Supercapacitors are gaining popularity due to their high cycling stability,power density,and fast charge and discharge rates.Researchers are ex-ploring electrode materials,electrolytes,and separat-ors for cost-effecti...Supercapacitors are gaining popularity due to their high cycling stability,power density,and fast charge and discharge rates.Researchers are ex-ploring electrode materials,electrolytes,and separat-ors for cost-effective energy storage systems.Ad-vances in materials science have led to the develop-ment of hybrid nanomaterials,such as combining fil-amentous carbon forms with inorganic nanoparticles,to create new charge and energy transfer processes.Notable materials for electrochemical energy-stor-age applications include MXenes,2D transition met-al carbides,and nitrides,carbon black,carbon aerogels,activated carbon,carbon nanotubes,conducting polymers,carbon fibers,and nanofibers,and graphene,because of their thermal,electrical,and mechanical properties.Carbon materials mixed with conducting polymers,ceramics,metal oxides,transition metal oxides,metal hydroxides,transition metal sulfides,trans-ition metal dichalcogenide,metal sulfides,carbides,nitrides,and biomass materials have received widespread attention due to their remarkable performance,eco-friendliness,cost-effectiveness,and renewability.This article explores the development of carbon-based hybrid materials for future supercapacitors,including electric double-layer capacitors,pseudocapacitors,and hy-brid supercapacitors.It investigates the difficulties that influence structural design,manufacturing(electrospinning,hydro-thermal/solvothermal,template-assisted synthesis,electrodeposition,electrospray,3D printing)techniques and the latest car-bon-based hybrid materials research offer practical solutions for producing high-performance,next-generation supercapacitors.展开更多
Electrocatalytic carbon dioxide(CO_(2))reduction is an important way to achieve carbon neutrality by converting CO_(2)in-to high-value-added chemicals using electric energy.Carbon-based materials are widely used in va...Electrocatalytic carbon dioxide(CO_(2))reduction is an important way to achieve carbon neutrality by converting CO_(2)in-to high-value-added chemicals using electric energy.Carbon-based materials are widely used in various electrochemical reactions,including electrocatalytic CO_(2)reduction,due to their low cost and high activity.In recent years,defect engineering has attracted wide attention by constructing asymmetric defect centers in the materials,which can optimize the physicochemical properties of the mater-ial and improve its electrocatalytic activity.This review summarizes the types,methods of formation and defect characterization tech-niques of defective carbon-based materials.The advantages of defect engineering and the advantages and disadvantages of various defect formation methods and characterization techniques are also evaluated.Finally,the challenges of using defective carbon-based materials in electrocatalytic CO_(2)reduction are investigated and opportunities for their use are discussed.It is believed that this re-view will provide suggestions and guidance for developing defective carbon-based materials for CO_(2)reduction.展开更多
The use of three-dimensional(3D)electrodes in water treatment is competitive because of their high catalytic efficiency,low energy consumption and promising development.The use of particle electrodes is a key research...The use of three-dimensional(3D)electrodes in water treatment is competitive because of their high catalytic efficiency,low energy consumption and promising development.The use of particle electrodes is a key research focus in this technology.They are usually in the form of particles that fill the space between the cathode and anode,and the selection of materials used is important.Carbon-based materials are widely used because of their large specific surface area,good adsorption performance,high chemical stability and low cost.The principles of 3D electrode technology are introduced and recent research on its use for degrading organic pollutants using carbon-based particle electrodes is summarized.The classification of particle electrodes is introduced and the challenges for the future development of carbon-based particle electrodes in wastewater treatment are discussed.展开更多
Carbon-based perovskite solar cells have attracted much attention,due to their low cost,simple preparation process and high chemical stability.However,the devices exhibit low photoelectric conversion efficiency,owing ...Carbon-based perovskite solar cells have attracted much attention,due to their low cost,simple preparation process and high chemical stability.However,the devices exhibit low photoelectric conversion efficiency,owing to the presence of defects and interface impedance between the perovskite active layer and the contact interface.In order to minimize the interfacial defects and improve the charge transfer performance between the perovskite layer and the contact interface,cetyltrimethylammonium chloride(CTAC)was introduced into the lower interface of HTL-free carbon-based perovskite solar cells,because CTAC can be used as interface modification material to passivate the buried interface of perovskite and promote grain growth.It was found that CTAC can not only passivate the interface defects of perovskite,but also improve the crystalline quality of perovskite.As a result,the photovoltaic conversion efficiency of reaches 17.18%,which is 12.5%higher than that of the control group.After 20 days in air with 60%RH humidity,the cell can still maintain more than 90%of the initial efficiency,which provides a new strategy for interfacial passivation of perovskite solar cells.展开更多
Transformation of urea and glycerol to glycerol carbonate is an environmental friendly and economical process.Catalysts play an indispensable role in the process.Although many catalysts have been developed,the perform...Transformation of urea and glycerol to glycerol carbonate is an environmental friendly and economical process.Catalysts play an indispensable role in the process.Although many catalysts have been developed,the performance of the catalysts still cannot meet the needs of industrialization.In this paper,research progress of the homogeneous and heterogeneous catalysts of the reaction over the past 20 years were reviewed systematically.According to the types and active centers of catalysts,the catalysts were classified systematically and analyzed in detail.The typical reaction mechanisms were also summarized.The research and development direction of catalysts is made more explicit through systematic classification and mechanism analysis.The article reveals more novel catalysts have been designed and used for the reaction,such as mixed metal oxides with special structures,solid wastes and non-metallic materials.This work summarized the current state of research and prospected possible routes for design of novel catalysts.It is hoped that this review can provide some references for developing efficient catalysts.展开更多
Carbon nanotubes(CNTs)supported CoB and CoBSn catalysts were synthesized for hydrogen production via NaBH4 hydrolysis.The roles of Sn-promoter and the effect of CNTs treatment on CoB catalysts were evaluated and discu...Carbon nanotubes(CNTs)supported CoB and CoBSn catalysts were synthesized for hydrogen production via NaBH4 hydrolysis.The roles of Sn-promoter and the effect of CNTs treatment on CoB catalysts were evaluated and discussed.It is found that after the addition of Sn promoter,the specific surface area and the generation of active CoB phase are increased,while the oxidation treatment of CNTs results in more loading amounts of active components and enrichment of electron at active sites as well as large surface area.Consequently,the Sn-doped CoB catalysts supported on CNTs with oxidation treatment exhibits a significantly improved activity with a high H_(2)generation rate of 2640 mL/(min·g).Meanwhile,this catalyst shows a low activation energy of 43.7 kJ/mol and relatively high reusability.展开更多
In recent years,numer-ous single-atom catalysts(SACs)have been synthesized to activate persulfate(PS)by a non-radical pathway because of its high se-lectivity,and activity for the cata-lyst.Metal-nitrogen-carbon(M-N_(...In recent years,numer-ous single-atom catalysts(SACs)have been synthesized to activate persulfate(PS)by a non-radical pathway because of its high se-lectivity,and activity for the cata-lyst.Metal-nitrogen-carbon(M-N_(x)-C)has been identified as the key active site in SACs.Although methods for preparing SACs have been extensively reported,a systematic summary of the direct construction of M-N_(x)-C,espe-cially unconventional metal-nitrogen-carbon(UM-N_(x)-C,x≠4),on SACs for PS non-radical activation has still not been reported.The role of the M-N_(x)-C active sites on PS non-radical activation is discussed and methods for the formation of M-N_(x)-C and UM-N_(x)-C active sites in SACs and the effect of catalyst carriers such as carbon nitride(g-C_(3)N_(4)),MOFs,COFs,and other car-bon materials are reviewed.Direct and indirect methods,especially for UM-N_(x)-C active site formation,are also elaborated.Factors affecting the formation of a M-N_(x)-C active site on SACs are also discussed.Prospects for the use of M-N_(x)-C active sites for the non-radical activation of PS by SACs to remove organic contaminants from wastewater are evaluated.展开更多
By simplifying catalyst-product separation and reducing phosphorus waste,heterogeneous hydroformylation offers a more sustainable alternative to homogeneous processes.However,heterogeneous hydroformylation catalysts d...By simplifying catalyst-product separation and reducing phosphorus waste,heterogeneous hydroformylation offers a more sustainable alternative to homogeneous processes.However,heterogeneous hydroformylation catalysts developed thus far still suffer from the issues of much lower activity and metal leaching,which severely hinder their practical application.Here,we demonstrate that incorporating phosphorus(P)atoms into graphitic carbon nitride(PCN)supports facilitates charge transfer from Rh to the PCN support,thus largely enhancing electronic metal-support interactions(EMSIs).In the styrene hydroformylation reaction,the activity of Rh_(1)/PCN single-atom catalysts(SACs)with varying P contents exhibited a volcano-shaped relationship with P doping,where the Rh_(1)/PCN SAC with optimal P doping showed exceptional activity,approximately 5.8-and 3.3-fold greater than that of the Rh_(1)/g-C_(3)N_(4)SAC without P doping and the industrial homogeneous catalyst HRh(CO)(PPh_(3))_(3),respectively.In addition,the optimal Rh_(1)/PCN SAC catalyst also demonstrated largely enhanced multicycle stability without any visible metal aggregation owing to the increased EMSIs,which sharply differed from the severe metal aggregation of large nanoparticles on the Rh_(1)/g-C_(3)N_(4)SAC.Mechan-istic studies revealed that the enhanced catalytic performance could be attributed to electron-deficient Rh species,which reduced CO adsorption while simultaneously promoting alkene adsorption through increased EMSIs.These findings suggest that tuning EMSIs is an effective way to achieve SACs with high activity and durability.展开更多
Direct ethanol fuel cells(DEFCs)are a promising alternative to conventional energy sources,offering high energy density,environmental sustainability,and operational safety.Compared to methanol fuel cells,DEFCs exhibit...Direct ethanol fuel cells(DEFCs)are a promising alternative to conventional energy sources,offering high energy density,environmental sustainability,and operational safety.Compared to methanol fuel cells,DEFCs exhibit lower toxicity and a more mature preparation process.Unlike hydrogen fuel cells,DEFCs provide superior storage and transport feasibility,as well as cost-effectiveness,significantly enhancing their commercial viability.However,the stable C-C bond in ethanol creates a high activation energy barrier,often resulting in incomplete electrooxidation.Current commercial platinum(Pt)-and palladium(Pd)-based catalysts demonstrate low C-C bond cleavage efficiency(<7.5%),severely limiting DEFC energy output and power density.Furthermore,high catalyst costs and insufficient activity impede large-scale commercialization.Recent advances in DEFC anode catalyst design have focused on optimizing material composition and elucidating catalytic mechanisms.This review systematically examines developments in ethanol electrooxidation catalysts over the past five years,highlighting strategies to improve C1 pathway selectivity and C-C bond activation.Key approaches,such as alloying,nanostructure engineering,and interfacial synergy effects,are discussed alongside their mechanistic implications.Finally,we outline current challenges and future prospects for DEFC commercialization.展开更多
The weak adsorption energy of oxygen-containing intermediates on Co center leads to a considerable performance dis-parity between Co-N-C and costly Pt benchmark in catalyzing oxygen reduction reaction(ORR).In this wor...The weak adsorption energy of oxygen-containing intermediates on Co center leads to a considerable performance dis-parity between Co-N-C and costly Pt benchmark in catalyzing oxygen reduction reaction(ORR).In this work,we strategi-cally engineer the active site structure of Co-N-C via B substitution,which is accomplished by the pyrolysis of ammonium borate.During this process,the in-situ generated NH_(3)gas plays a critical role in creating surface defects and boron atoms substituting nitrogen atoms in the carbon structure.The well-designed CoB_(1)N_(3)active site endows Co with higher charge density and stronger adsorption energy toward oxygen species,potentially accelerating ORR kinetics.As expected,the resulting Co-B/N-C catalyst exhibited superior ORR performance over Co-N-C counterpart,with 40 mV,and fivefold en-hancement in half-wave potential and turnover frequency(TOF).More importantly,the excellent ORR performance could be translated into membrane electrode assembly(MEA)in a fuel cell test,delivering an impressive peak power density of 824 mW·cm^(-2),which is currently the best among Co-based catalysts under the same conditions.This work not only demon-strates an effective method for designing advanced catalysts,but also affords a highly promising non-precious metal ORR electrocatalyst for fuel cell applications.展开更多
Electrocatalytic reduction of carbon dioxide(CO_(2))to carbon monoxide(CO)is an effective strategy to achieve carbon neutrality.High selective and low-cost catalysts for the electrocatalytic reduction of CO_(2)have re...Electrocatalytic reduction of carbon dioxide(CO_(2))to carbon monoxide(CO)is an effective strategy to achieve carbon neutrality.High selective and low-cost catalysts for the electrocatalytic reduction of CO_(2)have received increasing attention.In contrast to the conventional tube furnace method,the high-temperature shock(HTS)method enables ultra-fast thermal processing,superior atomic efficiency,and a streamlined synthesis protocol,offering a simplified method for the preparation of high-performance single-atom catalysts(SACs).The reports have shown that nickel-based SACs can be synthesized quickly and conveniently using the HTS method,making their application in CO_(2)reduction reactions(CO_(2)RR)a viable and promising avenue for further exploration.In this study,the effect of heating temperature,metal loading and different nitrogen(N)sources on the catalyst morphology,coordination environment and electrocatalytic performance were investigated.Under optimal conditions,0.05Ni-DCD-C-1050 showed excellent performance in reducing CO_(2)to CO,with CO selectivity close to 100%(−0.7 to−1.0 V vs RHE)and current density as high as 130 mA/cm^(2)(−1.1 V vs RHE)in a flow cell under alkaline environment.展开更多
The nitrogen-coordinated metal single-atom catalysts(M−N−C SACs)with an ultra-high metal loading synthetized by direct high-temperature pyrolysis have been widely reported.However,most of metal single atoms in these c...The nitrogen-coordinated metal single-atom catalysts(M−N−C SACs)with an ultra-high metal loading synthetized by direct high-temperature pyrolysis have been widely reported.However,most of metal single atoms in these catalysts were buried in the carbon matrix,resulting in a low metal utilization and inaccessibility for adsorption of reactants during the catalytic process.Herein,we reported a facile synthesis based on the hard-soft acid-base(HSAB)theory to fabricate Co single-atom catalysts with highly exposed metal atoms ligated to the external pyridinic-N sites of a nitrogen-doped carbon support.Benefiting from the highly accessible Co active sites,the prepared Co−N−C SAC exhibited a superior oxygen reduction reactivity comparable to that of the commercial Pt/C catalyst,showing a high turnover frequency(TOF)of 0.93 e^(−)·s^(-1)·site^(-1)at 0.85 V vs.RHE,far exceeding those of some representative SACs with a ultra-high metal content.This work provides a rational strategy to design and prepare M−N−C single-atom catalysts featured with high site-accessibility and site-density.展开更多
Hanyu Xu 1,Xuedan Song 1,*,Qing Zhang 1,Chang Yu 1,Jieshan Qiu 1,2,*1 Liaoning Key Lab for Energy Materials and Chemical Engineering,State Key Laboratory of Fine Chemicals,School of Chemical Engineering,Dalian Univers...Hanyu Xu 1,Xuedan Song 1,*,Qing Zhang 1,Chang Yu 1,Jieshan Qiu 1,2,*1 Liaoning Key Lab for Energy Materials and Chemical Engineering,State Key Laboratory of Fine Chemicals,School of Chemical Engineering,Dalian University of Technology,Dalian 116024,Liaoning Province,China.展开更多
Owing to outstanding hydrophilicity and ionic interaction,layered double hydroxides(LDHs)have emerged as a promising carrier for high performance catalysts.However,the synthesis of new specialized catalytic LDHs for d...Owing to outstanding hydrophilicity and ionic interaction,layered double hydroxides(LDHs)have emerged as a promising carrier for high performance catalysts.However,the synthesis of new specialized catalytic LDHs for degradation of antibiotics still faces some challenges.In this study,a CoFe_(2)O_(4)/MgAl-LDH composite catalyst was synthesized using a hydrothermal coprecipitation method.Comprehensive characterization reveals that the surface of MgAl-LDH is covered with nanometer CoFe_(2)O_(4) particles.The specific surface area of CoFe_(2)O_(4)/MgAl-LDH is 82.84 m^(2)·g^(-)1,which is 2.34 times that of CoFe_(2)O_(4).CoFe_(2)O_(4)/MgAl-LDH has a saturation magnetic strength of 22.24 A·m^(2)·kg^(-1) facilitating efficient solid-liquid separation.The composite catalyst was employed to activate peroxymonosulfate(PMS)for the efficient degradation of tetracycline hydrochloride(TCH).It is found that the catalytic performance of CoFe_(2)O_(4)/MgAl-LDH significantly exceeds that of CoFe_(2)O_(4).The maximum TCH removal reaches 98.2%under the optimal conditions([TCH]=25 mg/L,[PMS]=1.5 mmol/L,CoFe_(2)O_(4)/MgAl-LDH=0.20 g/L,pH 7,and T=25℃).Coexisting ions in the solution,such as SO_(4)^(2-),Cl-,H_(2)PO_(4)^(-),and CO_(3)^(2-),have a negligible effect on catalytic performance.Cyclic tests demonstrate that the catalytic performance of CoFe_(2)O_(4)/MgAl-LDH remains 67.2%after five cycles.Mechanism investigations suggest that O_(2)^(•-)and ^(1)O_(2) produced by CoFe_(2)O_(4)/MgAl-LDH play a critical role in the catalytic degradation.展开更多
With ongoing global warming and increasing energy demands,the CH_(4)-CO_(2)reforming reaction(dry reforming of methane,DRM)has garnered significant attention as a promising carbon capture and utilization technology.Ni...With ongoing global warming and increasing energy demands,the CH_(4)-CO_(2)reforming reaction(dry reforming of methane,DRM)has garnered significant attention as a promising carbon capture and utilization technology.Nickel-based catalysts are renowned for their outstanding activity and selectivity in this process.The impact of metal-support interaction(MSI),on Ni-based catalyst performance has been extensively researched and debated recently.This paper reviews the recent research progress of MSI on Ni-based catalysts and their characterization and modulation strategies in catalytic reactions.From the perspective of MSI,the effects of different carriers(metal oxides,carbon materials and molecular sieves,etc.)are introduced on the dispersion and surface structure of Ni active metal particles,and the effect of MSI on the activity and stability of DRM reactions on Ni-based catalysts is discussed in detail.Future research should focus on better understanding and controlling MSI to improve the performance and durability of nickel-based catalysts in CH_(4)-CO_(2)reforming,advancing cleaner energy technologies.展开更多
Combustion catalyst is a key modifier for the performance of composite solid propellant.To exploit highefficiency combustion catalyst,a fascinating bimetallic metal-organic framework[MnCo(EIM)_(2)(DCA)_(2)]n(1)was con...Combustion catalyst is a key modifier for the performance of composite solid propellant.To exploit highefficiency combustion catalyst,a fascinating bimetallic metal-organic framework[MnCo(EIM)_(2)(DCA)_(2)]n(1)was constructed by an active dicyandiamide(DCA)linker,Mn^(2+),Co^(2+)centers,and an 1-ethylimidazole(EIM)ligand.1 possesses good thermal stability(Tp=205℃),high energy density(Eg=24.34 kJ/g,Ev=35.93 kJ/cm^(3)),and insensitivity to impact and frictional stimulus.The catalytic effects of 1 contrasted to monometallic coordination compounds Mn(EIM)_(4)(DCA)_(2)(2)and Co(EIM)_(4)(DCA)_(2)(3)on the thermal decomposition of AP/RDX composite were investigated by a DSC method.The decomposition peak temperatures of AP and RDX of the composite decreased to 335.8℃ and 206.4℃,respectively,and the corresponding activation energy decreased by 27.3%and 43.6%,respectively,which are better than the performances of monometallic complexes 2 and 3.The gas products in the whole thermal decomposition stage of the sample were measured by TG-MS and TG-IR,and the catalytic mechanism of 1 to AP/RDX was further analyzed.This work reveal potential application of bimetallic MOFs in the composite solid propellants.展开更多
Single-atom catalysts(SACs)are promising for oxygen reduction reaction(ORR)on account of their excellent catalytic activity and maximum utilization of atoms.However,due to the complicated preparation processes and exp...Single-atom catalysts(SACs)are promising for oxygen reduction reaction(ORR)on account of their excellent catalytic activity and maximum utilization of atoms.However,due to the complicated preparation processes and expensive reagents used,the cost of SACs is usually too high to put into practical application.The development of cost-effective and sustainable SACs remains a great challenge.Herein,a low-cost method employing biomass is designed to prepare efficient single-atom Fe-N-C catalysts(SA-Fe-N-C).Benefiting from the confinement effect of porous carbon support and the coordination effect of glucose,SA-Fe-N-C is derived from cheap flour by the two-step pyrolysis.Atomically dispersed Fe atoms exist in the form of Fe-N_(x),which acts as active sites for ORR.The catalyst shows outstanding activity with a half-wave potential(E_(1/2))of 0.86 V,which is better than that of Pt/C(0.84 V).Additionally,the catalyst also exhibits superior stability.The ORR catalyzed by SA-Fe-N-C proceeds via an efficient 4e transfer pathway.The high performance of SA-Fe-N-C also benefits from its porous structure,extremely high specific surface area(1450.1 m^(2)/g),and abundant micropores,which are conducive to increasing the density of active sites and fully exposing them.This work provides a cost-effective strategy to synthesize SACs from cheap biomass,achieving a balance between performance and cost.展开更多
Two major challenges,high cost and short lifespan,have been hindering the commercialization process of lowtemperature fuel cells.Professor Wei's group has been focusing on decreasing cathode Pt loadings without lo...Two major challenges,high cost and short lifespan,have been hindering the commercialization process of lowtemperature fuel cells.Professor Wei's group has been focusing on decreasing cathode Pt loadings without losses of activity and durability,and their research advances in this area over the past three decades are briefly reviewed herein.Regarding the Pt-based catalysts and the low Pt usage,they have firstly tried to clarify the degradation mechanism of Pt/C catalysts,and then demonstrated that the activity and stability could be improved by three strategies:regulating the nanostructures of the active sites,enhancing the effects of support materials,and optimizing structures of the three-phase boundary.For Pt-free catalysts,especialiy carbon-based ones,several strategies that they proposed to enhance the activity of nitrogen-/heteroatom-doped carbon catalysts are firstly presented.Then,an indepth understanding of the degradation mechanism for carbon-based catalysts is discussed,and followed by the corresponding stability enhancement strategies.Also,the carbon-based electrode at the micrometer-scale,faces the challenges such as low active-site density,thick catalytic layer,and the effect of hydrogen peroxide,which require rational structure design for the integral cathodic electrode.This review finally gives a brief conclusion and outlook about the low cost and long lifespan of cathodic oxygen reduction catalysts.展开更多
文摘Supercapacitors are gaining popularity due to their high cycling stability,power density,and fast charge and discharge rates.Researchers are ex-ploring electrode materials,electrolytes,and separat-ors for cost-effective energy storage systems.Ad-vances in materials science have led to the develop-ment of hybrid nanomaterials,such as combining fil-amentous carbon forms with inorganic nanoparticles,to create new charge and energy transfer processes.Notable materials for electrochemical energy-stor-age applications include MXenes,2D transition met-al carbides,and nitrides,carbon black,carbon aerogels,activated carbon,carbon nanotubes,conducting polymers,carbon fibers,and nanofibers,and graphene,because of their thermal,electrical,and mechanical properties.Carbon materials mixed with conducting polymers,ceramics,metal oxides,transition metal oxides,metal hydroxides,transition metal sulfides,trans-ition metal dichalcogenide,metal sulfides,carbides,nitrides,and biomass materials have received widespread attention due to their remarkable performance,eco-friendliness,cost-effectiveness,and renewability.This article explores the development of carbon-based hybrid materials for future supercapacitors,including electric double-layer capacitors,pseudocapacitors,and hy-brid supercapacitors.It investigates the difficulties that influence structural design,manufacturing(electrospinning,hydro-thermal/solvothermal,template-assisted synthesis,electrodeposition,electrospray,3D printing)techniques and the latest car-bon-based hybrid materials research offer practical solutions for producing high-performance,next-generation supercapacitors.
文摘Electrocatalytic carbon dioxide(CO_(2))reduction is an important way to achieve carbon neutrality by converting CO_(2)in-to high-value-added chemicals using electric energy.Carbon-based materials are widely used in various electrochemical reactions,including electrocatalytic CO_(2)reduction,due to their low cost and high activity.In recent years,defect engineering has attracted wide attention by constructing asymmetric defect centers in the materials,which can optimize the physicochemical properties of the mater-ial and improve its electrocatalytic activity.This review summarizes the types,methods of formation and defect characterization tech-niques of defective carbon-based materials.The advantages of defect engineering and the advantages and disadvantages of various defect formation methods and characterization techniques are also evaluated.Finally,the challenges of using defective carbon-based materials in electrocatalytic CO_(2)reduction are investigated and opportunities for their use are discussed.It is believed that this re-view will provide suggestions and guidance for developing defective carbon-based materials for CO_(2)reduction.
文摘The use of three-dimensional(3D)electrodes in water treatment is competitive because of their high catalytic efficiency,low energy consumption and promising development.The use of particle electrodes is a key research focus in this technology.They are usually in the form of particles that fill the space between the cathode and anode,and the selection of materials used is important.Carbon-based materials are widely used because of their large specific surface area,good adsorption performance,high chemical stability and low cost.The principles of 3D electrode technology are introduced and recent research on its use for degrading organic pollutants using carbon-based particle electrodes is summarized.The classification of particle electrodes is introduced and the challenges for the future development of carbon-based particle electrodes in wastewater treatment are discussed.
基金National Natural Science Foundation of China (52162028)Natural Science Foundation of Jiangxi Province (20232ACB204011,20224BAB204001)+3 种基金Education Department of Jiangxi Province (GJJ2201001)Jingdezhen Municipal Science and Technology Bureau (2023GY001-16,2023ZDGG001 and 20224SF005-08)Opening Project of National Engineering Research Center for Domestic&Building Ceramics (GCZX2301)State Key Laboratory of New Ceramics and Fine Processing in Tsinghua University (KF202309,KF202414)。
文摘Carbon-based perovskite solar cells have attracted much attention,due to their low cost,simple preparation process and high chemical stability.However,the devices exhibit low photoelectric conversion efficiency,owing to the presence of defects and interface impedance between the perovskite active layer and the contact interface.In order to minimize the interfacial defects and improve the charge transfer performance between the perovskite layer and the contact interface,cetyltrimethylammonium chloride(CTAC)was introduced into the lower interface of HTL-free carbon-based perovskite solar cells,because CTAC can be used as interface modification material to passivate the buried interface of perovskite and promote grain growth.It was found that CTAC can not only passivate the interface defects of perovskite,but also improve the crystalline quality of perovskite.As a result,the photovoltaic conversion efficiency of reaches 17.18%,which is 12.5%higher than that of the control group.After 20 days in air with 60%RH humidity,the cell can still maintain more than 90%of the initial efficiency,which provides a new strategy for interfacial passivation of perovskite solar cells.
基金supported by Fundamental Research Program of Shanxi Province(202203021221303)。
文摘Transformation of urea and glycerol to glycerol carbonate is an environmental friendly and economical process.Catalysts play an indispensable role in the process.Although many catalysts have been developed,the performance of the catalysts still cannot meet the needs of industrialization.In this paper,research progress of the homogeneous and heterogeneous catalysts of the reaction over the past 20 years were reviewed systematically.According to the types and active centers of catalysts,the catalysts were classified systematically and analyzed in detail.The typical reaction mechanisms were also summarized.The research and development direction of catalysts is made more explicit through systematic classification and mechanism analysis.The article reveals more novel catalysts have been designed and used for the reaction,such as mixed metal oxides with special structures,solid wastes and non-metallic materials.This work summarized the current state of research and prospected possible routes for design of novel catalysts.It is hoped that this review can provide some references for developing efficient catalysts.
基金supported by National Natural Science Foundation of China(22276144).
文摘Carbon nanotubes(CNTs)supported CoB and CoBSn catalysts were synthesized for hydrogen production via NaBH4 hydrolysis.The roles of Sn-promoter and the effect of CNTs treatment on CoB catalysts were evaluated and discussed.It is found that after the addition of Sn promoter,the specific surface area and the generation of active CoB phase are increased,while the oxidation treatment of CNTs results in more loading amounts of active components and enrichment of electron at active sites as well as large surface area.Consequently,the Sn-doped CoB catalysts supported on CNTs with oxidation treatment exhibits a significantly improved activity with a high H_(2)generation rate of 2640 mL/(min·g).Meanwhile,this catalyst shows a low activation energy of 43.7 kJ/mol and relatively high reusability.
文摘In recent years,numer-ous single-atom catalysts(SACs)have been synthesized to activate persulfate(PS)by a non-radical pathway because of its high se-lectivity,and activity for the cata-lyst.Metal-nitrogen-carbon(M-N_(x)-C)has been identified as the key active site in SACs.Although methods for preparing SACs have been extensively reported,a systematic summary of the direct construction of M-N_(x)-C,espe-cially unconventional metal-nitrogen-carbon(UM-N_(x)-C,x≠4),on SACs for PS non-radical activation has still not been reported.The role of the M-N_(x)-C active sites on PS non-radical activation is discussed and methods for the formation of M-N_(x)-C and UM-N_(x)-C active sites in SACs and the effect of catalyst carriers such as carbon nitride(g-C_(3)N_(4)),MOFs,COFs,and other car-bon materials are reviewed.Direct and indirect methods,especially for UM-N_(x)-C active site formation,are also elaborated.Factors affecting the formation of a M-N_(x)-C active site on SACs are also discussed.Prospects for the use of M-N_(x)-C active sites for the non-radical activation of PS by SACs to remove organic contaminants from wastewater are evaluated.
基金supported by the Petrochemical Research Institute Foundation(21-CB-09-01)the National Natural Science Foundation of China(22302186,22025205)+1 种基金the China Postdoctoral Science Foundation(2022M713030,2023T160618)the Fundamental Research Funds for the Central Universities(WK2060000058,WK2060000038).
文摘By simplifying catalyst-product separation and reducing phosphorus waste,heterogeneous hydroformylation offers a more sustainable alternative to homogeneous processes.However,heterogeneous hydroformylation catalysts developed thus far still suffer from the issues of much lower activity and metal leaching,which severely hinder their practical application.Here,we demonstrate that incorporating phosphorus(P)atoms into graphitic carbon nitride(PCN)supports facilitates charge transfer from Rh to the PCN support,thus largely enhancing electronic metal-support interactions(EMSIs).In the styrene hydroformylation reaction,the activity of Rh_(1)/PCN single-atom catalysts(SACs)with varying P contents exhibited a volcano-shaped relationship with P doping,where the Rh_(1)/PCN SAC with optimal P doping showed exceptional activity,approximately 5.8-and 3.3-fold greater than that of the Rh_(1)/g-C_(3)N_(4)SAC without P doping and the industrial homogeneous catalyst HRh(CO)(PPh_(3))_(3),respectively.In addition,the optimal Rh_(1)/PCN SAC catalyst also demonstrated largely enhanced multicycle stability without any visible metal aggregation owing to the increased EMSIs,which sharply differed from the severe metal aggregation of large nanoparticles on the Rh_(1)/g-C_(3)N_(4)SAC.Mechan-istic studies revealed that the enhanced catalytic performance could be attributed to electron-deficient Rh species,which reduced CO adsorption while simultaneously promoting alkene adsorption through increased EMSIs.These findings suggest that tuning EMSIs is an effective way to achieve SACs with high activity and durability.
基金supported by the National Natural Science Foundation of China(22472023,22202037)the Jilin Province Science and Technology Development Program(20250102077JC)the Fundamental Research Funds for the Central Universities(2412024QD014,2412023QD019).
文摘Direct ethanol fuel cells(DEFCs)are a promising alternative to conventional energy sources,offering high energy density,environmental sustainability,and operational safety.Compared to methanol fuel cells,DEFCs exhibit lower toxicity and a more mature preparation process.Unlike hydrogen fuel cells,DEFCs provide superior storage and transport feasibility,as well as cost-effectiveness,significantly enhancing their commercial viability.However,the stable C-C bond in ethanol creates a high activation energy barrier,often resulting in incomplete electrooxidation.Current commercial platinum(Pt)-and palladium(Pd)-based catalysts demonstrate low C-C bond cleavage efficiency(<7.5%),severely limiting DEFC energy output and power density.Furthermore,high catalyst costs and insufficient activity impede large-scale commercialization.Recent advances in DEFC anode catalyst design have focused on optimizing material composition and elucidating catalytic mechanisms.This review systematically examines developments in ethanol electrooxidation catalysts over the past five years,highlighting strategies to improve C1 pathway selectivity and C-C bond activation.Key approaches,such as alloying,nanostructure engineering,and interfacial synergy effects,are discussed alongside their mechanistic implications.Finally,we outline current challenges and future prospects for DEFC commercialization.
基金the National Key Research and Development Program of China(2022YFB4004100)National Natural Science Foundation of China(22272161,22179126)+1 种基金the Jilin Province Science and Technology Development Program(YDZJ202202CXJD011,20240101019JC)Jilin Province major science and technology project(222648GX0105103875)for financial supports.
文摘The weak adsorption energy of oxygen-containing intermediates on Co center leads to a considerable performance dis-parity between Co-N-C and costly Pt benchmark in catalyzing oxygen reduction reaction(ORR).In this work,we strategi-cally engineer the active site structure of Co-N-C via B substitution,which is accomplished by the pyrolysis of ammonium borate.During this process,the in-situ generated NH_(3)gas plays a critical role in creating surface defects and boron atoms substituting nitrogen atoms in the carbon structure.The well-designed CoB_(1)N_(3)active site endows Co with higher charge density and stronger adsorption energy toward oxygen species,potentially accelerating ORR kinetics.As expected,the resulting Co-B/N-C catalyst exhibited superior ORR performance over Co-N-C counterpart,with 40 mV,and fivefold en-hancement in half-wave potential and turnover frequency(TOF).More importantly,the excellent ORR performance could be translated into membrane electrode assembly(MEA)in a fuel cell test,delivering an impressive peak power density of 824 mW·cm^(-2),which is currently the best among Co-based catalysts under the same conditions.This work not only demon-strates an effective method for designing advanced catalysts,but also affords a highly promising non-precious metal ORR electrocatalyst for fuel cell applications.
基金supported by the National Key R&D Program of China(2024YFB4106400)National Natural Science Foundation of China(22209200,52302331)。
文摘Electrocatalytic reduction of carbon dioxide(CO_(2))to carbon monoxide(CO)is an effective strategy to achieve carbon neutrality.High selective and low-cost catalysts for the electrocatalytic reduction of CO_(2)have received increasing attention.In contrast to the conventional tube furnace method,the high-temperature shock(HTS)method enables ultra-fast thermal processing,superior atomic efficiency,and a streamlined synthesis protocol,offering a simplified method for the preparation of high-performance single-atom catalysts(SACs).The reports have shown that nickel-based SACs can be synthesized quickly and conveniently using the HTS method,making their application in CO_(2)reduction reactions(CO_(2)RR)a viable and promising avenue for further exploration.In this study,the effect of heating temperature,metal loading and different nitrogen(N)sources on the catalyst morphology,coordination environment and electrocatalytic performance were investigated.Under optimal conditions,0.05Ni-DCD-C-1050 showed excellent performance in reducing CO_(2)to CO,with CO selectivity close to 100%(−0.7 to−1.0 V vs RHE)and current density as high as 130 mA/cm^(2)(−1.1 V vs RHE)in a flow cell under alkaline environment.
基金supported by Shanxi Province Science Foundation for Youths(202203021212300)Taiyuan University of Science and Technology Scientific Research Initial Funding(20212064)Outstanding Doctoral Award Fund in Shanxi Province(20222060).
文摘The nitrogen-coordinated metal single-atom catalysts(M−N−C SACs)with an ultra-high metal loading synthetized by direct high-temperature pyrolysis have been widely reported.However,most of metal single atoms in these catalysts were buried in the carbon matrix,resulting in a low metal utilization and inaccessibility for adsorption of reactants during the catalytic process.Herein,we reported a facile synthesis based on the hard-soft acid-base(HSAB)theory to fabricate Co single-atom catalysts with highly exposed metal atoms ligated to the external pyridinic-N sites of a nitrogen-doped carbon support.Benefiting from the highly accessible Co active sites,the prepared Co−N−C SAC exhibited a superior oxygen reduction reactivity comparable to that of the commercial Pt/C catalyst,showing a high turnover frequency(TOF)of 0.93 e^(−)·s^(-1)·site^(-1)at 0.85 V vs.RHE,far exceeding those of some representative SACs with a ultra-high metal content.This work provides a rational strategy to design and prepare M−N−C single-atom catalysts featured with high site-accessibility and site-density.
文摘Hanyu Xu 1,Xuedan Song 1,*,Qing Zhang 1,Chang Yu 1,Jieshan Qiu 1,2,*1 Liaoning Key Lab for Energy Materials and Chemical Engineering,State Key Laboratory of Fine Chemicals,School of Chemical Engineering,Dalian University of Technology,Dalian 116024,Liaoning Province,China.
基金University Synergy Innovation Program of Anhui Province(GXXT-2022-083)Science and Technology Plan Project of Wuhu City,China(2023kx12)Anhui Provincial Department of Education New Era Education Project(2023xscx070)。
文摘Owing to outstanding hydrophilicity and ionic interaction,layered double hydroxides(LDHs)have emerged as a promising carrier for high performance catalysts.However,the synthesis of new specialized catalytic LDHs for degradation of antibiotics still faces some challenges.In this study,a CoFe_(2)O_(4)/MgAl-LDH composite catalyst was synthesized using a hydrothermal coprecipitation method.Comprehensive characterization reveals that the surface of MgAl-LDH is covered with nanometer CoFe_(2)O_(4) particles.The specific surface area of CoFe_(2)O_(4)/MgAl-LDH is 82.84 m^(2)·g^(-)1,which is 2.34 times that of CoFe_(2)O_(4).CoFe_(2)O_(4)/MgAl-LDH has a saturation magnetic strength of 22.24 A·m^(2)·kg^(-1) facilitating efficient solid-liquid separation.The composite catalyst was employed to activate peroxymonosulfate(PMS)for the efficient degradation of tetracycline hydrochloride(TCH).It is found that the catalytic performance of CoFe_(2)O_(4)/MgAl-LDH significantly exceeds that of CoFe_(2)O_(4).The maximum TCH removal reaches 98.2%under the optimal conditions([TCH]=25 mg/L,[PMS]=1.5 mmol/L,CoFe_(2)O_(4)/MgAl-LDH=0.20 g/L,pH 7,and T=25℃).Coexisting ions in the solution,such as SO_(4)^(2-),Cl-,H_(2)PO_(4)^(-),and CO_(3)^(2-),have a negligible effect on catalytic performance.Cyclic tests demonstrate that the catalytic performance of CoFe_(2)O_(4)/MgAl-LDH remains 67.2%after five cycles.Mechanism investigations suggest that O_(2)^(•-)and ^(1)O_(2) produced by CoFe_(2)O_(4)/MgAl-LDH play a critical role in the catalytic degradation.
基金supported by the Natural Science Foundation of Shanxi Province(202203021221155)the Foundation of National Key Laboratory of High Efficiency and Low Carbon Utilization of Coal(J23-24-902)。
文摘With ongoing global warming and increasing energy demands,the CH_(4)-CO_(2)reforming reaction(dry reforming of methane,DRM)has garnered significant attention as a promising carbon capture and utilization technology.Nickel-based catalysts are renowned for their outstanding activity and selectivity in this process.The impact of metal-support interaction(MSI),on Ni-based catalyst performance has been extensively researched and debated recently.This paper reviews the recent research progress of MSI on Ni-based catalysts and their characterization and modulation strategies in catalytic reactions.From the perspective of MSI,the effects of different carriers(metal oxides,carbon materials and molecular sieves,etc.)are introduced on the dispersion and surface structure of Ni active metal particles,and the effect of MSI on the activity and stability of DRM reactions on Ni-based catalysts is discussed in detail.Future research should focus on better understanding and controlling MSI to improve the performance and durability of nickel-based catalysts in CH_(4)-CO_(2)reforming,advancing cleaner energy technologies.
基金supported by the National Natural Science Foundation of China(Grant No.22175025)State Key Laboratory of Explosion Science and Safety Protection(Grant No.YBKT22-03)+1 种基金the Natural Science Foundation of Chongqing(Grant No.CSTB2023 NSCQ-LZX0098)the Chongqing Municipal Education Commis-sion(Grant No.KJZD-M202301404).
文摘Combustion catalyst is a key modifier for the performance of composite solid propellant.To exploit highefficiency combustion catalyst,a fascinating bimetallic metal-organic framework[MnCo(EIM)_(2)(DCA)_(2)]n(1)was constructed by an active dicyandiamide(DCA)linker,Mn^(2+),Co^(2+)centers,and an 1-ethylimidazole(EIM)ligand.1 possesses good thermal stability(Tp=205℃),high energy density(Eg=24.34 kJ/g,Ev=35.93 kJ/cm^(3)),and insensitivity to impact and frictional stimulus.The catalytic effects of 1 contrasted to monometallic coordination compounds Mn(EIM)_(4)(DCA)_(2)(2)and Co(EIM)_(4)(DCA)_(2)(3)on the thermal decomposition of AP/RDX composite were investigated by a DSC method.The decomposition peak temperatures of AP and RDX of the composite decreased to 335.8℃ and 206.4℃,respectively,and the corresponding activation energy decreased by 27.3%and 43.6%,respectively,which are better than the performances of monometallic complexes 2 and 3.The gas products in the whole thermal decomposition stage of the sample were measured by TG-MS and TG-IR,and the catalytic mechanism of 1 to AP/RDX was further analyzed.This work reveal potential application of bimetallic MOFs in the composite solid propellants.
基金Project(52174338)supported by the National Natural Science Foundation of ChinaProjects(2022JJ20086,2021JJ30796)supported by the Natural Science Foundation of Hunan Province,China+1 种基金Project(2023CXQD005)supported by the Central South University Innovation-Driven Research Programme,ChinaProject(23B0841)supported by the Education Department of Hunan Provincial Government,China。
文摘Single-atom catalysts(SACs)are promising for oxygen reduction reaction(ORR)on account of their excellent catalytic activity and maximum utilization of atoms.However,due to the complicated preparation processes and expensive reagents used,the cost of SACs is usually too high to put into practical application.The development of cost-effective and sustainable SACs remains a great challenge.Herein,a low-cost method employing biomass is designed to prepare efficient single-atom Fe-N-C catalysts(SA-Fe-N-C).Benefiting from the confinement effect of porous carbon support and the coordination effect of glucose,SA-Fe-N-C is derived from cheap flour by the two-step pyrolysis.Atomically dispersed Fe atoms exist in the form of Fe-N_(x),which acts as active sites for ORR.The catalyst shows outstanding activity with a half-wave potential(E_(1/2))of 0.86 V,which is better than that of Pt/C(0.84 V).Additionally,the catalyst also exhibits superior stability.The ORR catalyzed by SA-Fe-N-C proceeds via an efficient 4e transfer pathway.The high performance of SA-Fe-N-C also benefits from its porous structure,extremely high specific surface area(1450.1 m^(2)/g),and abundant micropores,which are conducive to increasing the density of active sites and fully exposing them.This work provides a cost-effective strategy to synthesize SACs from cheap biomass,achieving a balance between performance and cost.
基金supported by the National Key Research and Development Program of China(No.2020YFB1506002,2019YFB1504503,2016YFB0101202)National 973 Program of China(No.2012CB215501)National Natural Science Foundation of China(No.52021004,22022502(2021),21822803(2019),21576031(2016),51272297(2013),20936008(2010),20676156(2007),20376088(2004),20176066(2002),29976047(2000)).
文摘Two major challenges,high cost and short lifespan,have been hindering the commercialization process of lowtemperature fuel cells.Professor Wei's group has been focusing on decreasing cathode Pt loadings without losses of activity and durability,and their research advances in this area over the past three decades are briefly reviewed herein.Regarding the Pt-based catalysts and the low Pt usage,they have firstly tried to clarify the degradation mechanism of Pt/C catalysts,and then demonstrated that the activity and stability could be improved by three strategies:regulating the nanostructures of the active sites,enhancing the effects of support materials,and optimizing structures of the three-phase boundary.For Pt-free catalysts,especialiy carbon-based ones,several strategies that they proposed to enhance the activity of nitrogen-/heteroatom-doped carbon catalysts are firstly presented.Then,an indepth understanding of the degradation mechanism for carbon-based catalysts is discussed,and followed by the corresponding stability enhancement strategies.Also,the carbon-based electrode at the micrometer-scale,faces the challenges such as low active-site density,thick catalytic layer,and the effect of hydrogen peroxide,which require rational structure design for the integral cathodic electrode.This review finally gives a brief conclusion and outlook about the low cost and long lifespan of cathodic oxygen reduction catalysts.
