Since the carbon neutrality target was proposed,many countries have been facing severe challenges to carbon emission reduction sustainably.This study is conducted using a tripartite evolutionary game model to explore ...Since the carbon neutrality target was proposed,many countries have been facing severe challenges to carbon emission reduction sustainably.This study is conducted using a tripartite evolutionary game model to explore the impact of the central environmental protection inspection(CEPI)on driving carbon emission reduction,and to study what factors influence the strategic choices of each party and how they interact with each other.The research results suggest that local governments and manufacturing enterprises would choose strategies that are beneficial to carbon reduction when CEPI increases.When the initial willingness of all parties increases 20%,50%—80%,the time spent for the whole system to achieve stability decreases from 100%,60%—30%.The evolutionary result of“thorough inspection,regulation implementation,low-carbon management”is the best strategy for the tripartite evolutionary game.Moreover,the smaller the cost and the larger the benefit,the greater the likelihood of the three-party game stability strategy appears.This study has important guiding significance for other developing countries to promote carbon emission reduction by environmental policy.展开更多
Bismuth-based materials(e.g., metallic, oxides and subcarbonate) are emerged as promising electrocatalysts for converting CO_(2) to formate. However, Bio-based electrocatalysts possess high overpotentials, while bismu...Bismuth-based materials(e.g., metallic, oxides and subcarbonate) are emerged as promising electrocatalysts for converting CO_(2) to formate. However, Bio-based electrocatalysts possess high overpotentials, while bismuth oxides and subcarbonate encounter stability issues. This work is designated to exemplify that the operando synthesis can be an effective means to enhance the stability of electrocatalysts under operando CO_(2)RR conditions. A synthetic approach is developed to electrochemically convert Bi^(O)Cl into Cl-containing subcarbonate(Bi_(2)O_(2)(CO_(3))_(x)Cl_(y)) under operando CO_(2)RR conditions. The systematic operando spectroscopic studies depict that BiOCl is converted to Bi_(2)O_(2)(CO_(3))_(x)Cl_(y) via a cathodic potential-promoted anion-exchange process. The operando synthesizedBi_(2)O_(2)(CO_(3))_(x)Cl_(y) can tolerate-1.0 V versus RHE, while for the wet-chemistry synthesized pure Bi_(2)O_(2)CO_(3),the formation of metallic Bio occurs at-0.6 V versus RHE. At-0.8 V versus RHE, Bi_(2)O_(2)(CO_(3))_(x)Cl_(y) can readily attain a FEHCOO-of 97.9%,much higher than that of the pure Bi_(2)O_(2)CO_(3)(81.3%). DFT calculations indicate that differing from the pure Bi_(2)O_(2)CO_(3)-catalyzed CO_(2)RR, where formate is formed via a *OCHO intermediate step that requires a high energy input energy of 2.69 eV to proceed, the formation of H COO-over Bi_(2)O_(2)(CO_(3))_(x)Cl_(y) has proceeded via a *COOH intermediate step that only requires low energy input of 2.56 eV.展开更多
Photocatalytic water splitting and carbon dioxide reduction provide us clean and sustainable energy resources. The carbon dioxide reduction is also the redemption of the greenhouse effect. MoS/TiOphotocatalysts based ...Photocatalytic water splitting and carbon dioxide reduction provide us clean and sustainable energy resources. The carbon dioxide reduction is also the redemption of the greenhouse effect. MoS/TiOphotocatalysts based on TiOnanoplates have been synthesized via a hydrothermal acidification route for water and carbon dioxide reduction reactions. This facile approach generates well dispersed Mo S3 with low crystallinity on the surface of TiOnanoplates. The as-synthesized MoS/TiOphotocatalyst showed considerable activity for both water reduction and carbon dioxide reduction. The thermal treatment effects of TiO, the loading percentage of MoSand the crystalline phase of TiOhave been investigated towards the photocatalytic performance. TiOnanoplate synthesized through hydrothermal reaction with the presence of HF acid is an ideal semiconductor material for the loading of MoSfor photocatalytic water and carbon dioxide reduction simultaneously in EDTA sacrificial solution.展开更多
We report the synthesis, characterisation and catalytic performance of two nature-inspired biomassderived electro-catalysts for the oxygen reduction reaction in fuel cells. The catalysts were prepared via pyrolysis of...We report the synthesis, characterisation and catalytic performance of two nature-inspired biomassderived electro-catalysts for the oxygen reduction reaction in fuel cells. The catalysts were prepared via pyrolysis of a real food waste（lobster shells） or by mimicking the composition of lobster shells using chitin and CaCO3 particles followed by acid washing. The simplified model of artificial lobster was prepared for better reproducibility. The calcium carbonate in both samples acts as a pore agent, creating increased surface area and pore volume, though considerably higher in artificial lobster samples due to the better homogeneity of the components. Various characterisation techniques revealed the presence of a considerable amount of hydroxyapatite left in the real lobster samples after acid washing and a low content of carbon（23%）, nitrogen and sulphur（〈1%）, limiting the surface area to 23 m^2/g, and consequently resulting in rather poor catalytic activity. However, artificial lobster samples, with a surface area of ≈200 m^2/g and a nitrogen doping of 2%, showed a promising onset potential, very similar to a commercially available platinum catalyst, with better methanol tolerance, though with lower stability in long time testing over 10,000 s.展开更多
An approach to the simultaneous reclamation of carbon and sulfur resources from CO2 and H2S has been proposed and effectively implemented with the aid of catalysts. A brief thermodynamic study reveals the potential of...An approach to the simultaneous reclamation of carbon and sulfur resources from CO2 and H2S has been proposed and effectively implemented with the aid of catalysts. A brief thermodynamic study reveals the potential of direct reduction of CO2 with H2S（15：15 mol% balanced with N2） for selective production of CO and elemental sulfur. The experiments carried out in a fixed-bed flow reactor over the temperature range of 400–800 °C give evidence of the importance of the employment of catalysts. Both the conversions of the reactants and the selectivities of the target products can be substantially promoted over most catalysts studied. Nevertheless, little difference appears among their catalytic performance. The results also prove that the presence of CO2 can remarkably enhance H2S conversion and the sulfur yield in comparison with H2S direct decomposition. A longtime reaction test on Mg O catalyst manifests its superior durability at high temperature（700 °C） and huge gas hourly space velocity（100,000 h-1）. Free radicals initiated by catalysts are supposed to dominate the reactions between CO2 and H2S.展开更多
Composites of carbon aerogel and graphite oxide（GO） were synthesized using a self-assembly method based on dispersive forces. Their surface was modified by treatment in hydrogen sulfide at 650 and800 ℃. The samples...Composites of carbon aerogel and graphite oxide（GO） were synthesized using a self-assembly method based on dispersive forces. Their surface was modified by treatment in hydrogen sulfide at 650 and800 ℃. The samples obtained were characterized by adsorption of nitrogen, TA-MS, XPS, potentiometric titration, and HRTEM and tested as catalysts for oxygen reduction reactions（ORR） in an alkaline medium.The synergistic effect of the composite（electrical conductivity, porosity and surface chemistry） leads to a good ORR catalytic activity. The onset potential for the composite of carbon aerogel heated at 800 ℃ is shifted to a more positive value and the number of electron transfer was 2e-at the potential 0.68 V versus RHE and it increased to 4e-with an increase in the negative values of the potential. An excellent tolerance to methanol crossover was also recorded.展开更多
The electronic structure of electrocatalysts plays a critical role in energy conversion,whereas for an efficient catalyst,it is challenging to modulate the orbitals.Herein,we present a new strategy to modulate the e_(...The electronic structure of electrocatalysts plays a critical role in energy conversion,whereas for an efficient catalyst,it is challenging to modulate the orbitals.Herein,we present a new strategy to modulate the e_(g) orbital occupancy of Pd by constructing composition-controllable Pd-Au metallic aerogels(MAs),optimizing the d-band center of Pd to achieve excellent performance for electrochemical carbon dioxide reduction reaction(CO_(2)RR).Specifically,Pd_(1)Au_(2) MAs achieve almost 100% Faraday efficiency(FE) of CO in the range of-0.40 to-0.80 V vs.reversible hydrogen electrode(RHE),as well as the long-term stability,being one of the best Pd-based materials for CO_(2)RR.The X-ray photoelectron spectroscopy(XPS) results and density functional theory(DFT) calculations demonstrate that the introduction of Au modulates the Pd e_(g) orbital occupancy,which significantly weakens *CO adsorption on Pd,reduces the CO_(2)RR energy barrier and consequently improves the electrocatalytic activity and stability for long-term applications.Our work highlights a new strategy for designing efficient electrocatalysts for CO_(2)RR and beyond.展开更多
Mixed metal oxide(MMO) represents a critical class of materials that can allow for obtaining a dynamic interface between its components:reduced metal and its metal oxide counterpart during an electrocatalytic reaction...Mixed metal oxide(MMO) represents a critical class of materials that can allow for obtaining a dynamic interface between its components:reduced metal and its metal oxide counterpart during an electrocatalytic reaction.Here,a synthetic method utilizing a MOF-derived micro/mesoporous carbon as a template to prepare sub-2 nm MMO catalysts for CO_(2) electro reduction is reported.Starting from the zeolite imidazolate framework(ZIF-8),the pyrolyzed derivatives were used to synthesize sub-2 nm Pd-Ni MMO with different compositions.The Ni-rich(Pd_(20)-Ni_(80)/ZC) catalyst exhibits unexpectedly superior performance for CO production with an improved Faradaic efficiency(FE) of 95.3% at the current density of 200 mA cm^(-2) at-0.56 V vs.reversible hydrogen electrode(RHE) compared to other Pd-Ni compositions.X-ray photoelectron spectroscopy(XPS) analysis confirms the presence of Ni^(2+) and Pd^(2+) in all compositions,demonstrating the presence of MMO.Density functional theory(DFT) calculation reveals that the lower CO binding energy on the surface of the Pd_(20)-Ni_(80) cluster eases CO desorption,thus increasing its production.This work provides a general synthetic strategy for MMO electrocatalysts and can pave a new way for screening multimetallic catalysts with a dynamic electrochemical interface.展开更多
This study addresses the comparative carbon emissions of different transportation modes within a unified evaluation framework,focusing on their carbon footprints from inception to disposal.Specifically,the entire life...This study addresses the comparative carbon emissions of different transportation modes within a unified evaluation framework,focusing on their carbon footprints from inception to disposal.Specifically,the entire life cycle carbon emissions of High-Speed Rail(HSR),battery electric vehicles,conventional internal combustion engine vehicles,battery electric buses,and conventional internal combustion engine buses are analyzed.The life cycle is segmented into vehicle manufacturing,fuel or electricity production,operational,and dismantlingrecycling stages.This analysis is applied to the Beijing-Tianjin intercity transportation system to explore emission reduction strategies.Results indicate that HSR demonstrates significant carbon emission reduction,with an intensity of only 24%-32% compared to private vehicles and 47%-89% compared to buses.Notably,HSR travel for Beijing-Tianjin intercity emits only 24% of private vehicle emissions,demonstrating the emission reduction benefits of transportation structure optimization.Additionally,predictive modeling reveals the potential for carbon emission reduction through energy structure optimization,providing a guideline for the development of effective transportation management systems.展开更多
Electrocatalytic reduction of CO_(2) to produce high value-added products is an important way to achieve sustainable production of green energy,but it is limited by high complexity of the catalyst structure and reacti...Electrocatalytic reduction of CO_(2) to produce high value-added products is an important way to achieve sustainable production of green energy,but it is limited by high complexity of the catalyst structure and reaction process,making the rational design of the catalyst and the targeted generation of specific products a huge challenge.Herein,based on the penta-octa-graphene(POG)with sp~2 and sp~3 hybrid as the prototype,we theoretically guide the design of CO_(2) electrocatalytic reduction(CO_(2)RR)catalyst over pure POG and TM doping POG(TM@POG).Our mechanistic study highlights two key factors in new pathway for CH_(4) production and catalytic performance,i.e.,TM provides electron transfer for the key intermediate*CHO,promoting the activation of CO_(2),and the type of protonation for CO_(2)RR is determined by the charge accumulation on the O atom of the intermediates.This reduces the complexity of the reaction and provides a predictive effect on the formation of intermediates.More importantly,the proper values of the Gibbs free energy indicate that TM@POG is an ideal catalyst candidate,especially the Fe@POG,which is superior to Cu(211)material.On this basis,three simple descriptors(Bader charge,d-band centerε_dand descriptorφ)based on the inherent properties of atoms were constructed to reveal the underlying causes of the improvement of catalytic activity.Our results provide a new understanding of the’structure-performance’relationship of carbon-based electrocatalysts,thus providing a useful strategy for the design of catalysts for CO_(2)RR.展开更多
The electrochemical CO_(2) reduction reaction(CO_(2)RR) to controllable chemicals is considered as a promising pathway to store intermittent renewable energy. Herein, a set of catalysts based on copper-nitrogendoped c...The electrochemical CO_(2) reduction reaction(CO_(2)RR) to controllable chemicals is considered as a promising pathway to store intermittent renewable energy. Herein, a set of catalysts based on copper-nitrogendoped carbon xerogel(Cu-N-C) are successfully developed varying the copper amount and the nature of the copper precursor, for the efficient CO_(2)RR. The electrocatalytic performance of Cu-N-C materials is assessed by a rotating ring-disc electrode(RRDE), technique still rarely explored for CO_(2)RR. For comparison, products are also characterized by online gas chromatography in a H-cell. The as-synthesized Cu-NC catalysts are found to be active and highly CO selective at low overpotentials(from -0.6 to -0.8 V vs.RHE) in 0.1 M KHCO_(3), while H_(2) from the competitive water reduction appears at larger overpotentials(-0.9 V vs. RHE). The optimum copper acetate-derived catalyst containing Cu-N_(4) moieties exhibits a CO_(2)-to-CO turnover frequency of 997 h^(-1) at -0.9 V vs. RHE with a H_(2)/CO ratio of 1.8. These results demonstrate that RRDE configuration can be used as a feasible approach for identifying electrolysis products from CO_(2)RR.展开更多
Cu catalysts can convert CO_(2) through an electrochemical reduction reaction into a variety of useful carbon-based products.However,this capability provides an obstacle to increasing the selectivity for a single prod...Cu catalysts can convert CO_(2) through an electrochemical reduction reaction into a variety of useful carbon-based products.However,this capability provides an obstacle to increasing the selectivity for a single product.Herein,we report a simple fabrication method for a Cu-Pd alloy catalyst for use in a membrane electrode assembly(MEA)-based CO_(2) electrolyzer for the electrochemical CO_(2) reduction reaction(ECRR)with high selectivity for CO production.When the composition of the Cu-Pd alloy catalyst was fabricated at 6:4,the selectivity for CO increased and the production of multi-carbon compounds and hydrogen is suppressed.Introducing a Cu-Pd alloy catalyst with 6:4 ratio as the cathode of the MEAbased CO_(2) electrolyzer showed a CO faradaic efficiency of 92.8%at 2.4 V_(cell).We assumed that these results contributed from the crystal planes on the surface of the Cu-Pd alloy.The phases of the Cu-Pd alloy catalyst were partially separated through annealing to fabricate a catalyst with high selectivity for CO at low voltage and C_(2)H_4 at high voltage.The results of CO-stripping testing confirmed that when Cu partially separates from the lattice of the Cu-Pd alloy,the desorption of~*CO is suppressed,suggesting that C-C coupling reaction is favored.展开更多
Employing crystal facets to regulate the catalytic properties in electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)has been well demonstrated on electrocatalysts containing single metals but rarely explored...Employing crystal facets to regulate the catalytic properties in electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)has been well demonstrated on electrocatalysts containing single metals but rarely explored for bimetallic systems.Here,we synthesize ZnSn(OH)_(6)(ZSO)microcrystals(MCs)with distinct facets and investigate the facet effects in eCO_(2)RR.Electrochemical studies and in situ Fourier Transform Infrared Spectroscopy(in situ-FTIR)reveal that ZSO MCs produce mainly C1 products of HCOOH and CO.The{111}facet of the ZSO MCS exhibits higher selectivity and faradaic efficiency(FE)than that of the{100}facet over a wide range of potentials(-0.9 V∼-1.3 V versus RHE).Density Functional Theory(DFT)calculations elucidate that the{111}facet is favorable to the adsorption/activation of CO_(2)molecules,the formation of intermediate in the rate-determining step,and the desorption of C1 products of CO and HCOOH molecules.展开更多
Carbon neutrality(or climate neutrality)has been a global consensus,and international experience exchange is essential.Given the differences in the degree of social development,resource endowment and technological lev...Carbon neutrality(or climate neutrality)has been a global consensus,and international experience exchange is essential.Given the differences in the degree of social development,resource endowment and technological level,each country should build a carbon-neutral plan based on its national conditions.Compared with other major developed countries(e.g.,Germany,the United States and Japan),China's carbon neutrality has much bigger challenges,including a heavy and time-pressured carbon reduction task and the current energy structure that is over-dependent on fossil fuels.Here we provide a comprehensive review of the status and prospects of the key technologies for low-carbon,near-zero carbon,and negative carbon emissions.Technological innovations associated with coal,oil-gas and hydrogen industries and their future potential in reducing carbon emissions are particularly explained and assessed.Based on integrated analysis of international experience from the world's major developed countries,in-depth knowledge of the current and future technologies,and China's energy and ecological resources potential,five lessons for the implementation of China's carbon neutrality are proposed:(1)transformation of energy production pattern from a coal-dominated pattern to a diversified renewable energy pattern;(2)renewable power-to-X and large-scale underground energy storage;(3)integration of green hydrogen production,storage,transport and utilization;(4)construction of clean energy systems based on smart sector coupling(ENSYSCO);(5)improvement of ecosystem carbon sinks both in nationwide forest land and potential desert in Northwest China.This paper provides an international perspective for a better understanding of the challenges and opportunities of carbon neutrality in China,and can serve as a theoretical foundation for medium-long term carbon neutral policy formulation.展开更多
Electrocatalytic carb on dioxide reducti on(CO_(2)R)presents a promising route to establish zero-e mission carb on cycle and store in termittent ren ewable energy into chemical fuels for steady energy supply.Methanol ...Electrocatalytic carb on dioxide reducti on(CO_(2)R)presents a promising route to establish zero-e mission carb on cycle and store in termittent ren ewable energy into chemical fuels for steady energy supply.Methanol is an ideal energy carrier as alternative fuels and one of the most important commodity chemicals.Nevertheless,methanol is currently mainly produced from fossil-based syngas,the production of which yields tremendous carb on emission globally.Direct CO_(2)R towards metha nol poses great potential to shift the paradigm of methanol production.In this perspective,we focus our discussions on producing methanol from electrochemical CO_(2)R,using metallomacrocyclic molecules as the model catalysts.We discuss the motivation of having methanol as the sole CO_(2)R product,the documented application of metallomacrocyclic catalysts for CO_(2)R,and recent advance in catalyzing CO_(2) to methanol with cobalt phthalocyanine-based catalysts.We attempt to understand the key factors in determining the activity,selectivity,and stability of electrocatalytic CO_(2)-to-methanol conversion,and to draw mechanistic insights from existing observations.Finally,we identify the challenges hindering methanol electrosynthesis directly from CO_(2) and some intriguing directions worthy of further investigation and exploration.展开更多
Carbon dioxide is an important medium of the global carbon cycle,and has the dual properties of realizing the conversion of organic matter in the ecosystem and causing the greenhouse effect.The fixed or available carb...Carbon dioxide is an important medium of the global carbon cycle,and has the dual properties of realizing the conversion of organic matter in the ecosystem and causing the greenhouse effect.The fixed or available carbon dioxide in the atmosphere is defined as"gray carbon",while the carbon dioxide that cannot be fixed or used and remains in the atmosphere is called"black carbon".Carbon neutral is the consensus of human development,but its implementation still faces many challenges in politics,resources,technology,market,and energy structure,etc.It is proposed that carbon replacement,carbon emission reduction,carbon sequestration,and carbon cycle are the four main approaches to achieve carbon neutral,among which carbon replacement is the backbone.New energy has become the leading role of the third energy conversion and will dominate carbon neutral in the future.Nowadays,solar energy,wind energy,hydropower,nuclear energy and hydrogen energy are the main forces of new energy,helping the power sector to achieve low carbon emissions."Green hydrogen"is the reserve force of new energy,helping further reduce carbon emissions in industrial and transportation fields.Artificial carbon conversion technology is a bridge connecting new energy and fossil energy,effectively reducing the carbon emissions of fossil energy.It is predicted that the peak value of China’s carbon dioxide emissions will reach 110×10^(8) t in 2030.The study predicts that China’s carbon emissions will drop to 22×10^(8) t,33×10^(8) t and 44×10^(8) t,respectively,in 2060 according to three scenarios of high,medium,and low levels.To realize carbon neutral in China,seven implementation suggestions have been put forward to build a new"three small and one large"energy structure in China and promote the realization of China’s energy independence strategy.展开更多
Palladium(Pd) nanostructures are highly promising electrocatalysts for the carbon dioxide electrochemical reduction(CO_(2) ER). At present, it is still challenge for the synthesis of Pd nanostructures with high activi...Palladium(Pd) nanostructures are highly promising electrocatalysts for the carbon dioxide electrochemical reduction(CO_(2) ER). At present, it is still challenge for the synthesis of Pd nanostructures with high activity, selectivity and stability. In this work, a facile PdII-complex pyrolysis method is applied to synthesize the high-quality one-dimensional heterostructured Pd/Pd O nanowires(Pd/Pd O H-NWs).The as-prepared Pd/Pd O H-NWs have a large electrochemically active surface area, abundant defects and Pd/Pd O heterostructure. Electrochemical measurement results reveal that Pd/Pd O H-NWs exhibit up to 94% CO Faraday efficiency with a current density of 11.6 m A cm^(-2) at an applied potential of -0.8 V. Meanwhile, Pd/Pd O H-NWs can achieve a stable catalytic process of 12 h for CO_(2) ER. Such outstanding CO_(2) ER performance of Pd/Pd O H-NWs has also been verified in the flow cell test. The density functional theory calculations indicate that Pd/Pd O heterostructure can significantly weaken the CO adsorption on Pd sites, which improves the CO tolerance and consequently enhances the catalytic performance of Pd/Pd O H-NWs for CO_(2) ER. This work highlights a facile complex pyrolysis strategy for the synthesis of Pd-based CO_(2) ER catalysts and provides a new application instance of metal/metal oxide heterostructure in electrocatalysis.展开更多
The CuO/CeO_(2) composites with strong metal-support interaction were synthesised,which can efficiently electroreduct CO_(2)to C(2)H_(4).The Faradaic efficiency(FE)of C_(2)H_(4) could reach 50.5%with a current density...The CuO/CeO_(2) composites with strong metal-support interaction were synthesised,which can efficiently electroreduct CO_(2)to C(2)H_(4).The Faradaic efficiency(FE)of C_(2)H_(4) could reach 50.5%with a current density of 18 mA cm^(-2).The strong metal-support interaction could not only enhance the adsorption and activation of CO_(2),but also can stablize the CuO.展开更多
Smartcombination of manifold carbonaceous materials with admirable functionalities(like full of pores/functional groups,high specific surface area) is still a mainstream/preferential way to address knotty issues of po...Smartcombination of manifold carbonaceous materials with admirable functionalities(like full of pores/functional groups,high specific surface area) is still a mainstream/preferential way to address knotty issues of polysulfides dissolution/shuttling and poor electrical conductivity for S-based cathodes.However,extensive use of conductive carbon fillers in cell designs/technology would induce electrolytic overconsumption and thereby shelve high-energy-density promise of Li-S cells.To cut down carbon usage,we propose the incorporation of multi-functionalized NiFe2O4 quantum dots(QDs) as affordable additive substitutes.The total carbon content can be greatly curtailed from 26%(in traditional S/C cathodes) to a low/commercial mass ratio(~5%).Particularly,note that NiFe2O4 QDs additives own superb chemisorption interactions with soluble Li2Sn molecules and proper catalytic features facilitating polysulfide phase conversions and can also strengthen charge-transfer capability/redox kinetics of overall cathode systems.Benefiting from these intrinsic properties,such hybrid cathodes demonstrate prominent rate behaviors(decent capacity retention with ~526 mAh g^-1 even at 5 A g^-1) and stable cyclic performance in LiNO3-free electrolytes(only ~0.08% capacity decay per cycle in 500 cycles at 0.2 A g^-1).This work may arouse tremendous research interest in seeking other alternative QDs and offer an economical/more applicable methodology to construct low-carbon-content electrodes for practical usage.展开更多
Electrochemical reduction of CO_(2)(CO_(2)ER) to formate has been a promising route to produce value-added chemicals.Developing low-cost and efficient electrocatalysts with high product selectivity is still a grand ch...Electrochemical reduction of CO_(2)(CO_(2)ER) to formate has been a promising route to produce value-added chemicals.Developing low-cost and efficient electrocatalysts with high product selectivity is still a grand challenge.Herein,a novel Ni nanoparticles-anchored CNT coated by mesoporous carbon with yolk-shell structure (CNT/Ni@mC) catalysis was designed for CO_(2)ER.Ni nanoparticles were confined in the cavity between CNT and mesoporous carbon shell and the confined space can be controlled by tuning the amount of silica precursor.The mesoporous carbon shell and confined space are beneficial to charge transmission during CO_(2)ER.In contrast to previous studies,the CNT/Ni@mC catalyst presents selectivity toward formate rather than CO.Electrochemical in situ attenuated total reflection Fourier transform infrared spectroscopy measurements indicate the presence of a COO* intermediate that converts to formate under CO_(2)ER conditions.The well-defined structural feature of the confined space of the Ni-based catalyst for selective CO_(2)ER to formate may facilitate in-depth mechanistic understandings on structural factors that affect CO_(2)ER performance.展开更多
基金the financial support from the Postdoctoral Science Foundation of China(2022M720131)Spring Sunshine Collaborative Research Project of the Ministry of Education(202201660)+3 种基金Youth Project of Gansu Natural Science Foundation(22JR5RA542)General Project of Gansu Philosophy and Social Science Foundation(2022YB014)National Natural Science Foundation of China(72034003,72243006,and 71874074)Fundamental Research Funds for the Central Universities(2023lzdxjbkyzx008,lzujbky-2021-sp72)。
文摘Since the carbon neutrality target was proposed,many countries have been facing severe challenges to carbon emission reduction sustainably.This study is conducted using a tripartite evolutionary game model to explore the impact of the central environmental protection inspection(CEPI)on driving carbon emission reduction,and to study what factors influence the strategic choices of each party and how they interact with each other.The research results suggest that local governments and manufacturing enterprises would choose strategies that are beneficial to carbon reduction when CEPI increases.When the initial willingness of all parties increases 20%,50%—80%,the time spent for the whole system to achieve stability decreases from 100%,60%—30%.The evolutionary result of“thorough inspection,regulation implementation,low-carbon management”is the best strategy for the tripartite evolutionary game.Moreover,the smaller the cost and the larger the benefit,the greater the likelihood of the three-party game stability strategy appears.This study has important guiding significance for other developing countries to promote carbon emission reduction by environmental policy.
基金financially supported by Australian Research Council Discovery Project(DP200100965)。
文摘Bismuth-based materials(e.g., metallic, oxides and subcarbonate) are emerged as promising electrocatalysts for converting CO_(2) to formate. However, Bio-based electrocatalysts possess high overpotentials, while bismuth oxides and subcarbonate encounter stability issues. This work is designated to exemplify that the operando synthesis can be an effective means to enhance the stability of electrocatalysts under operando CO_(2)RR conditions. A synthetic approach is developed to electrochemically convert Bi^(O)Cl into Cl-containing subcarbonate(Bi_(2)O_(2)(CO_(3))_(x)Cl_(y)) under operando CO_(2)RR conditions. The systematic operando spectroscopic studies depict that BiOCl is converted to Bi_(2)O_(2)(CO_(3))_(x)Cl_(y) via a cathodic potential-promoted anion-exchange process. The operando synthesizedBi_(2)O_(2)(CO_(3))_(x)Cl_(y) can tolerate-1.0 V versus RHE, while for the wet-chemistry synthesized pure Bi_(2)O_(2)CO_(3),the formation of metallic Bio occurs at-0.6 V versus RHE. At-0.8 V versus RHE, Bi_(2)O_(2)(CO_(3))_(x)Cl_(y) can readily attain a FEHCOO-of 97.9%,much higher than that of the pure Bi_(2)O_(2)CO_(3)(81.3%). DFT calculations indicate that differing from the pure Bi_(2)O_(2)CO_(3)-catalyzed CO_(2)RR, where formate is formed via a *OCHO intermediate step that requires a high energy input energy of 2.69 eV to proceed, the formation of H COO-over Bi_(2)O_(2)(CO_(3))_(x)Cl_(y) has proceeded via a *COOH intermediate step that only requires low energy input of 2.56 eV.
基金supported by the Fundamental Research Funds for the Central Universities of Chinathe Starting Research Funds of Shaanxi Normal University for Mainstay Young Scholars+2 种基金the National Environment Agency of Singapore under the Environment Technology Research Programme(ETRP)through Project No.ETRP 1002 103Singapore National Research Foundation(NRF)through the Singapore-Berkeley Research Initiative for Sustainable Energy(SinBeRISE)Cambridge Centre for Carbon Reduction in Chemical Technology(C4T)CREATE Programmes
文摘Photocatalytic water splitting and carbon dioxide reduction provide us clean and sustainable energy resources. The carbon dioxide reduction is also the redemption of the greenhouse effect. MoS/TiOphotocatalysts based on TiOnanoplates have been synthesized via a hydrothermal acidification route for water and carbon dioxide reduction reactions. This facile approach generates well dispersed Mo S3 with low crystallinity on the surface of TiOnanoplates. The as-synthesized MoS/TiOphotocatalyst showed considerable activity for both water reduction and carbon dioxide reduction. The thermal treatment effects of TiO, the loading percentage of MoSand the crystalline phase of TiOhave been investigated towards the photocatalytic performance. TiOnanoplate synthesized through hydrothermal reaction with the presence of HF acid is an ideal semiconductor material for the loading of MoSfor photocatalytic water and carbon dioxide reduction simultaneously in EDTA sacrificial solution.
基金the EU for the Intra European Marie Curie Research Fellowship (PIEFGA-2013-623227)
文摘We report the synthesis, characterisation and catalytic performance of two nature-inspired biomassderived electro-catalysts for the oxygen reduction reaction in fuel cells. The catalysts were prepared via pyrolysis of a real food waste（lobster shells） or by mimicking the composition of lobster shells using chitin and CaCO3 particles followed by acid washing. The simplified model of artificial lobster was prepared for better reproducibility. The calcium carbonate in both samples acts as a pore agent, creating increased surface area and pore volume, though considerably higher in artificial lobster samples due to the better homogeneity of the components. Various characterisation techniques revealed the presence of a considerable amount of hydroxyapatite left in the real lobster samples after acid washing and a low content of carbon（23%）, nitrogen and sulphur（〈1%）, limiting the surface area to 23 m^2/g, and consequently resulting in rather poor catalytic activity. However, artificial lobster samples, with a surface area of ≈200 m^2/g and a nitrogen doping of 2%, showed a promising onset potential, very similar to a commercially available platinum catalyst, with better methanol tolerance, though with lower stability in long time testing over 10,000 s.
基金financial supports from the Fushun Research Institute of Petroleum&Petrochemicals(no.KG12009)the Natural Science Foundation of China(no.21276077)the Fundamental Research Funds for Central Universities(no.WG1213011)
文摘An approach to the simultaneous reclamation of carbon and sulfur resources from CO2 and H2S has been proposed and effectively implemented with the aid of catalysts. A brief thermodynamic study reveals the potential of direct reduction of CO2 with H2S（15：15 mol% balanced with N2） for selective production of CO and elemental sulfur. The experiments carried out in a fixed-bed flow reactor over the temperature range of 400–800 °C give evidence of the importance of the employment of catalysts. Both the conversions of the reactants and the selectivities of the target products can be substantially promoted over most catalysts studied. Nevertheless, little difference appears among their catalytic performance. The results also prove that the presence of CO2 can remarkably enhance H2S conversion and the sulfur yield in comparison with H2S direct decomposition. A longtime reaction test on Mg O catalyst manifests its superior durability at high temperature（700 °C） and huge gas hourly space velocity（100,000 h-1）. Free radicals initiated by catalysts are supposed to dominate the reactions between CO2 and H2S.
基金supported by the Spanish Ministry of Economy and Competitiveness (Project CTQ2012-37925-C03-03)FEDER fundsby the Hungarian National Fund OTKA K109558
文摘Composites of carbon aerogel and graphite oxide（GO） were synthesized using a self-assembly method based on dispersive forces. Their surface was modified by treatment in hydrogen sulfide at 650 and800 ℃. The samples obtained were characterized by adsorption of nitrogen, TA-MS, XPS, potentiometric titration, and HRTEM and tested as catalysts for oxygen reduction reactions（ORR） in an alkaline medium.The synergistic effect of the composite（electrical conductivity, porosity and surface chemistry） leads to a good ORR catalytic activity. The onset potential for the composite of carbon aerogel heated at 800 ℃ is shifted to a more positive value and the number of electron transfer was 2e-at the potential 0.68 V versus RHE and it increased to 4e-with an increase in the negative values of the potential. An excellent tolerance to methanol crossover was also recorded.
基金financially supported by the National Natural Science Foundation of China (NSFC) (Grant No. 22105087)Natural Science Foundation of Jiangsu Province (Grant No. BK20210446)。
文摘The electronic structure of electrocatalysts plays a critical role in energy conversion,whereas for an efficient catalyst,it is challenging to modulate the orbitals.Herein,we present a new strategy to modulate the e_(g) orbital occupancy of Pd by constructing composition-controllable Pd-Au metallic aerogels(MAs),optimizing the d-band center of Pd to achieve excellent performance for electrochemical carbon dioxide reduction reaction(CO_(2)RR).Specifically,Pd_(1)Au_(2) MAs achieve almost 100% Faraday efficiency(FE) of CO in the range of-0.40 to-0.80 V vs.reversible hydrogen electrode(RHE),as well as the long-term stability,being one of the best Pd-based materials for CO_(2)RR.The X-ray photoelectron spectroscopy(XPS) results and density functional theory(DFT) calculations demonstrate that the introduction of Au modulates the Pd e_(g) orbital occupancy,which significantly weakens *CO adsorption on Pd,reduces the CO_(2)RR energy barrier and consequently improves the electrocatalytic activity and stability for long-term applications.Our work highlights a new strategy for designing efficient electrocatalysts for CO_(2)RR and beyond.
基金supported by the National Research Foundation of Korea (NRF) Grant funded by the Korean Government (MSIT) (RS-2023-00210114)supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (NRF-2021R1C1C1004264 and NRF2021R1A4A1032114)+1 种基金supported by the National Research Foundation of Korea (NRF) Grant funded by the Korean Government (MSIT) (NRF-2022R1A4A1019296)supported by the National R&D Program through the National Research Foundation of Korea (NRF), funded by the Ministry of Science and ICT (2021M3D1A2051636)。
文摘Mixed metal oxide(MMO) represents a critical class of materials that can allow for obtaining a dynamic interface between its components:reduced metal and its metal oxide counterpart during an electrocatalytic reaction.Here,a synthetic method utilizing a MOF-derived micro/mesoporous carbon as a template to prepare sub-2 nm MMO catalysts for CO_(2) electro reduction is reported.Starting from the zeolite imidazolate framework(ZIF-8),the pyrolyzed derivatives were used to synthesize sub-2 nm Pd-Ni MMO with different compositions.The Ni-rich(Pd_(20)-Ni_(80)/ZC) catalyst exhibits unexpectedly superior performance for CO production with an improved Faradaic efficiency(FE) of 95.3% at the current density of 200 mA cm^(-2) at-0.56 V vs.reversible hydrogen electrode(RHE) compared to other Pd-Ni compositions.X-ray photoelectron spectroscopy(XPS) analysis confirms the presence of Ni^(2+) and Pd^(2+) in all compositions,demonstrating the presence of MMO.Density functional theory(DFT) calculation reveals that the lower CO binding energy on the surface of the Pd_(20)-Ni_(80) cluster eases CO desorption,thus increasing its production.This work provides a general synthetic strategy for MMO electrocatalysts and can pave a new way for screening multimetallic catalysts with a dynamic electrochemical interface.
基金the financial support of the National Natural Science Foundation of China(U2268208)Science and Technology Program of China National Railway Group Co.,Ltd.(N2022×037).
文摘This study addresses the comparative carbon emissions of different transportation modes within a unified evaluation framework,focusing on their carbon footprints from inception to disposal.Specifically,the entire life cycle carbon emissions of High-Speed Rail(HSR),battery electric vehicles,conventional internal combustion engine vehicles,battery electric buses,and conventional internal combustion engine buses are analyzed.The life cycle is segmented into vehicle manufacturing,fuel or electricity production,operational,and dismantlingrecycling stages.This analysis is applied to the Beijing-Tianjin intercity transportation system to explore emission reduction strategies.Results indicate that HSR demonstrates significant carbon emission reduction,with an intensity of only 24%-32% compared to private vehicles and 47%-89% compared to buses.Notably,HSR travel for Beijing-Tianjin intercity emits only 24% of private vehicle emissions,demonstrating the emission reduction benefits of transportation structure optimization.Additionally,predictive modeling reveals the potential for carbon emission reduction through energy structure optimization,providing a guideline for the development of effective transportation management systems.
基金supported by the Natural Science Basic Research Program of Shaanxi(2023-JC-YB-065,2024JC-YBMS-788)the Foundation of Laboratory of Computational Physics(6142A05QN22017)。
文摘Electrocatalytic reduction of CO_(2) to produce high value-added products is an important way to achieve sustainable production of green energy,but it is limited by high complexity of the catalyst structure and reaction process,making the rational design of the catalyst and the targeted generation of specific products a huge challenge.Herein,based on the penta-octa-graphene(POG)with sp~2 and sp~3 hybrid as the prototype,we theoretically guide the design of CO_(2) electrocatalytic reduction(CO_(2)RR)catalyst over pure POG and TM doping POG(TM@POG).Our mechanistic study highlights two key factors in new pathway for CH_(4) production and catalytic performance,i.e.,TM provides electron transfer for the key intermediate*CHO,promoting the activation of CO_(2),and the type of protonation for CO_(2)RR is determined by the charge accumulation on the O atom of the intermediates.This reduces the complexity of the reaction and provides a predictive effect on the formation of intermediates.More importantly,the proper values of the Gibbs free energy indicate that TM@POG is an ideal catalyst candidate,especially the Fe@POG,which is superior to Cu(211)material.On this basis,three simple descriptors(Bader charge,d-band centerε_dand descriptorφ)based on the inherent properties of atoms were constructed to reveal the underlying causes of the improvement of catalytic activity.Our results provide a new understanding of the’structure-performance’relationship of carbon-based electrocatalysts,thus providing a useful strategy for the design of catalysts for CO_(2)RR.
基金Grant PID2020-115848RB-C21 "STORELEC" projectTED2021-129694B-C22 "DEFY-CO2" project funded by MCIN/AEI/10.13039/501100011033+3 种基金LMP253_ (2)1 project funded by Gobierno de AragónGrant IJC2019-041874-I funded by the MCIN/AEI/10.13039/501100011033CSIC for her JAE Intro ICU 2021-ICB-04 grantthe Y2020/EMT-6419 "CEOTRES" project funded by the Comunidad Autonoma de Madrid。
文摘The electrochemical CO_(2) reduction reaction(CO_(2)RR) to controllable chemicals is considered as a promising pathway to store intermittent renewable energy. Herein, a set of catalysts based on copper-nitrogendoped carbon xerogel(Cu-N-C) are successfully developed varying the copper amount and the nature of the copper precursor, for the efficient CO_(2)RR. The electrocatalytic performance of Cu-N-C materials is assessed by a rotating ring-disc electrode(RRDE), technique still rarely explored for CO_(2)RR. For comparison, products are also characterized by online gas chromatography in a H-cell. The as-synthesized Cu-NC catalysts are found to be active and highly CO selective at low overpotentials(from -0.6 to -0.8 V vs.RHE) in 0.1 M KHCO_(3), while H_(2) from the competitive water reduction appears at larger overpotentials(-0.9 V vs. RHE). The optimum copper acetate-derived catalyst containing Cu-N_(4) moieties exhibits a CO_(2)-to-CO turnover frequency of 997 h^(-1) at -0.9 V vs. RHE with a H_(2)/CO ratio of 1.8. These results demonstrate that RRDE configuration can be used as a feasible approach for identifying electrolysis products from CO_(2)RR.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government MSIT(2021R1A2C2093358,2021R1A4A3027878,2022M3I3A1081901)financial support from the Lotte Chemical Company。
文摘Cu catalysts can convert CO_(2) through an electrochemical reduction reaction into a variety of useful carbon-based products.However,this capability provides an obstacle to increasing the selectivity for a single product.Herein,we report a simple fabrication method for a Cu-Pd alloy catalyst for use in a membrane electrode assembly(MEA)-based CO_(2) electrolyzer for the electrochemical CO_(2) reduction reaction(ECRR)with high selectivity for CO production.When the composition of the Cu-Pd alloy catalyst was fabricated at 6:4,the selectivity for CO increased and the production of multi-carbon compounds and hydrogen is suppressed.Introducing a Cu-Pd alloy catalyst with 6:4 ratio as the cathode of the MEAbased CO_(2) electrolyzer showed a CO faradaic efficiency of 92.8%at 2.4 V_(cell).We assumed that these results contributed from the crystal planes on the surface of the Cu-Pd alloy.The phases of the Cu-Pd alloy catalyst were partially separated through annealing to fabricate a catalyst with high selectivity for CO at low voltage and C_(2)H_4 at high voltage.The results of CO-stripping testing confirmed that when Cu partially separates from the lattice of the Cu-Pd alloy,the desorption of~*CO is suppressed,suggesting that C-C coupling reaction is favored.
基金the Fundamental Research Funds for the Central Universities and the Fundamental Science Research of Harbin Institute of Technology(No.AUGA2160100119,AUGA9803100120,AUGA5710001120).
文摘Employing crystal facets to regulate the catalytic properties in electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)has been well demonstrated on electrocatalysts containing single metals but rarely explored for bimetallic systems.Here,we synthesize ZnSn(OH)_(6)(ZSO)microcrystals(MCs)with distinct facets and investigate the facet effects in eCO_(2)RR.Electrochemical studies and in situ Fourier Transform Infrared Spectroscopy(in situ-FTIR)reveal that ZSO MCs produce mainly C1 products of HCOOH and CO.The{111}facet of the ZSO MCS exhibits higher selectivity and faradaic efficiency(FE)than that of the{100}facet over a wide range of potentials(-0.9 V∼-1.3 V versus RHE).Density Functional Theory(DFT)calculations elucidate that the{111}facet is favorable to the adsorption/activation of CO_(2)molecules,the formation of intermediate in the rate-determining step,and the desorption of C1 products of CO and HCOOH molecules.
基金supported by the Henan Institute for Chinese Development Strategy of Engineering&Technology(Grant No.2022HENZDA02)by the Science&Technology Department of Sichuan Province Project(Grant No.2021YFH0010).
文摘Carbon neutrality(or climate neutrality)has been a global consensus,and international experience exchange is essential.Given the differences in the degree of social development,resource endowment and technological level,each country should build a carbon-neutral plan based on its national conditions.Compared with other major developed countries(e.g.,Germany,the United States and Japan),China's carbon neutrality has much bigger challenges,including a heavy and time-pressured carbon reduction task and the current energy structure that is over-dependent on fossil fuels.Here we provide a comprehensive review of the status and prospects of the key technologies for low-carbon,near-zero carbon,and negative carbon emissions.Technological innovations associated with coal,oil-gas and hydrogen industries and their future potential in reducing carbon emissions are particularly explained and assessed.Based on integrated analysis of international experience from the world's major developed countries,in-depth knowledge of the current and future technologies,and China's energy and ecological resources potential,five lessons for the implementation of China's carbon neutrality are proposed:(1)transformation of energy production pattern from a coal-dominated pattern to a diversified renewable energy pattern;(2)renewable power-to-X and large-scale underground energy storage;(3)integration of green hydrogen production,storage,transport and utilization;(4)construction of clean energy systems based on smart sector coupling(ENSYSCO);(5)improvement of ecosystem carbon sinks both in nationwide forest land and potential desert in Northwest China.This paper provides an international perspective for a better understanding of the challenges and opportunities of carbon neutrality in China,and can serve as a theoretical foundation for medium-long term carbon neutral policy formulation.
基金financial support through the StartUp Fund for Outstanding Talent with grant number A1098531023601307the National University of Singapore and Ministry of Education in Singapore for its financial support through Tier-1 projects with grant numbers R-279000-622-133 and R-279-000-622-731.
文摘Electrocatalytic carb on dioxide reducti on(CO_(2)R)presents a promising route to establish zero-e mission carb on cycle and store in termittent ren ewable energy into chemical fuels for steady energy supply.Methanol is an ideal energy carrier as alternative fuels and one of the most important commodity chemicals.Nevertheless,methanol is currently mainly produced from fossil-based syngas,the production of which yields tremendous carb on emission globally.Direct CO_(2)R towards metha nol poses great potential to shift the paradigm of methanol production.In this perspective,we focus our discussions on producing methanol from electrochemical CO_(2)R,using metallomacrocyclic molecules as the model catalysts.We discuss the motivation of having methanol as the sole CO_(2)R product,the documented application of metallomacrocyclic catalysts for CO_(2)R,and recent advance in catalyzing CO_(2) to methanol with cobalt phthalocyanine-based catalysts.We attempt to understand the key factors in determining the activity,selectivity,and stability of electrocatalytic CO_(2)-to-methanol conversion,and to draw mechanistic insights from existing observations.Finally,we identify the challenges hindering methanol electrosynthesis directly from CO_(2) and some intriguing directions worthy of further investigation and exploration.
文摘Carbon dioxide is an important medium of the global carbon cycle,and has the dual properties of realizing the conversion of organic matter in the ecosystem and causing the greenhouse effect.The fixed or available carbon dioxide in the atmosphere is defined as"gray carbon",while the carbon dioxide that cannot be fixed or used and remains in the atmosphere is called"black carbon".Carbon neutral is the consensus of human development,but its implementation still faces many challenges in politics,resources,technology,market,and energy structure,etc.It is proposed that carbon replacement,carbon emission reduction,carbon sequestration,and carbon cycle are the four main approaches to achieve carbon neutral,among which carbon replacement is the backbone.New energy has become the leading role of the third energy conversion and will dominate carbon neutral in the future.Nowadays,solar energy,wind energy,hydropower,nuclear energy and hydrogen energy are the main forces of new energy,helping the power sector to achieve low carbon emissions."Green hydrogen"is the reserve force of new energy,helping further reduce carbon emissions in industrial and transportation fields.Artificial carbon conversion technology is a bridge connecting new energy and fossil energy,effectively reducing the carbon emissions of fossil energy.It is predicted that the peak value of China’s carbon dioxide emissions will reach 110×10^(8) t in 2030.The study predicts that China’s carbon emissions will drop to 22×10^(8) t,33×10^(8) t and 44×10^(8) t,respectively,in 2060 according to three scenarios of high,medium,and low levels.To realize carbon neutral in China,seven implementation suggestions have been put forward to build a new"three small and one large"energy structure in China and promote the realization of China’s energy independence strategy.
基金supported by the National Natural Science Foundation of China(51873100)Natural Science Foundation of Shaanxi Province(2020JZ-23)+2 种基金the Fundamental Research Funds for the Central Universities(GK202101005 and 2021CBLZ004)the Innovation Team Project for Graduate Student at Shaanxi Normal University(TD2020048Y)the 111 Project(B14041)。
文摘Palladium(Pd) nanostructures are highly promising electrocatalysts for the carbon dioxide electrochemical reduction(CO_(2) ER). At present, it is still challenge for the synthesis of Pd nanostructures with high activity, selectivity and stability. In this work, a facile PdII-complex pyrolysis method is applied to synthesize the high-quality one-dimensional heterostructured Pd/Pd O nanowires(Pd/Pd O H-NWs).The as-prepared Pd/Pd O H-NWs have a large electrochemically active surface area, abundant defects and Pd/Pd O heterostructure. Electrochemical measurement results reveal that Pd/Pd O H-NWs exhibit up to 94% CO Faraday efficiency with a current density of 11.6 m A cm^(-2) at an applied potential of -0.8 V. Meanwhile, Pd/Pd O H-NWs can achieve a stable catalytic process of 12 h for CO_(2) ER. Such outstanding CO_(2) ER performance of Pd/Pd O H-NWs has also been verified in the flow cell test. The density functional theory calculations indicate that Pd/Pd O heterostructure can significantly weaken the CO adsorption on Pd sites, which improves the CO tolerance and consequently enhances the catalytic performance of Pd/Pd O H-NWs for CO_(2) ER. This work highlights a facile complex pyrolysis strategy for the synthesis of Pd-based CO_(2) ER catalysts and provides a new application instance of metal/metal oxide heterostructure in electrocatalysis.
基金supported by the National Key Research and Development Program of China(2017YFA0403102)National Natural Science Foundation of China(21573073,21733011)+1 种基金Beijing Municipal Science&Technology Commission(Z191100007219009)the Chinese Academy of Sciences(QYZDY-SSW-SLH013)。
文摘The CuO/CeO_(2) composites with strong metal-support interaction were synthesised,which can efficiently electroreduct CO_(2)to C(2)H_(4).The Faradaic efficiency(FE)of C_(2)H_(4) could reach 50.5%with a current density of 18 mA cm^(-2).The strong metal-support interaction could not only enhance the adsorption and activation of CO_(2),but also can stablize the CuO.
基金financial supports from National Natural Science Foundation of China (51802269 and 21773138)Chongqing Natural Science Foundation (cstc2018jcyjAX0624)+1 种基金Fundamental Research Funds for the Central Universities (XDJK2019AA002)Venture & Innovation Support Program for Chongqing overseas returnees (cx2018027)。
文摘Smartcombination of manifold carbonaceous materials with admirable functionalities(like full of pores/functional groups,high specific surface area) is still a mainstream/preferential way to address knotty issues of polysulfides dissolution/shuttling and poor electrical conductivity for S-based cathodes.However,extensive use of conductive carbon fillers in cell designs/technology would induce electrolytic overconsumption and thereby shelve high-energy-density promise of Li-S cells.To cut down carbon usage,we propose the incorporation of multi-functionalized NiFe2O4 quantum dots(QDs) as affordable additive substitutes.The total carbon content can be greatly curtailed from 26%(in traditional S/C cathodes) to a low/commercial mass ratio(~5%).Particularly,note that NiFe2O4 QDs additives own superb chemisorption interactions with soluble Li2Sn molecules and proper catalytic features facilitating polysulfide phase conversions and can also strengthen charge-transfer capability/redox kinetics of overall cathode systems.Benefiting from these intrinsic properties,such hybrid cathodes demonstrate prominent rate behaviors(decent capacity retention with ~526 mAh g^-1 even at 5 A g^-1) and stable cyclic performance in LiNO3-free electrolytes(only ~0.08% capacity decay per cycle in 500 cycles at 0.2 A g^-1).This work may arouse tremendous research interest in seeking other alternative QDs and offer an economical/more applicable methodology to construct low-carbon-content electrodes for practical usage.
基金the Natural Science Foundation of Hebei(B02020208088,H_(2)020206514)the S&T Program of Hebei(20544401D,20314401D,206Z4406G,21314402D,B2021208074,21344601D)the Tianjin Science and Technology Project(19YFSLQY00070)。
文摘Electrochemical reduction of CO_(2)(CO_(2)ER) to formate has been a promising route to produce value-added chemicals.Developing low-cost and efficient electrocatalysts with high product selectivity is still a grand challenge.Herein,a novel Ni nanoparticles-anchored CNT coated by mesoporous carbon with yolk-shell structure (CNT/Ni@mC) catalysis was designed for CO_(2)ER.Ni nanoparticles were confined in the cavity between CNT and mesoporous carbon shell and the confined space can be controlled by tuning the amount of silica precursor.The mesoporous carbon shell and confined space are beneficial to charge transmission during CO_(2)ER.In contrast to previous studies,the CNT/Ni@mC catalyst presents selectivity toward formate rather than CO.Electrochemical in situ attenuated total reflection Fourier transform infrared spectroscopy measurements indicate the presence of a COO* intermediate that converts to formate under CO_(2)ER conditions.The well-defined structural feature of the confined space of the Ni-based catalyst for selective CO_(2)ER to formate may facilitate in-depth mechanistic understandings on structural factors that affect CO_(2)ER performance.
