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Engineering heterogenous catalysts for chemical CO_(2) utilization:Lessons from thermal catalysis and advantages of yolk@shell structured nanoreactors 被引量:4
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作者 Cameron Alexander Hurd Price Tomas Ramirez Reina Jian Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第6期304-324,I0008,共22页
The development of catalytic materials for the recycling CO_(2) through a myriad of available processes is an attractive field,especially given the current climate change.While there is increasing publication in this ... The development of catalytic materials for the recycling CO_(2) through a myriad of available processes is an attractive field,especially given the current climate change.While there is increasing publication in this field,the reported catalysts rarely deviate from the traditionally supported metal nanoparticle morphology,with the most simplistic method of enhancement being the addition of more metals to an already complex composition.Encapsulated catalysts,especially yolk@shell catalysts with hollow voids,offer answers to the most prominent issues faced by this field,coking and sintering,and further potential for more advanced phenomena,for example,the confinement effect,to promote selectivity or offer greater protection against coking and sintering.This work serves to demonstrate the current position of catalyst development in the fields of thermal CO_(2) reforming and hydrogenation,summarizing the most recent work available and most common metals used for these reactions,and how yolk@shell catalysts can offer superior performance and survivability in thermal CO_(2) reforming and hydrogenation to the more traditional structure.Furthermore,this work will briefly demonstrate the bespoke nature and highly variable yolk@shell structure.Moreover,this review aims to illuminate the spatial confinement effect and how it enhances yolk@shell structured nanoreactors is presented. 展开更多
关键词 Yolk@shell CO_(2)utilization REFORMING HYDROGENATION Confinement effect
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Towards Practical Application of Li-S Battery with High Sulfur Loading and Lean Electrolyte:Will Carbon-Based Hosts Win This Race? 被引量:2
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作者 Yi Gong Jing Li +7 位作者 Kai Yang Shaoyin Li Ming Xu Guangpeng Zhang Yan Shi Qiong Cai Huanxin Li Yunlong Zhao 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第9期384-422,共39页
As the need for high-energy–density batteries continues to grow, lithium-sulfur(Li–S) batteries have become a highly promising next-generation energy solution due to their low cost and exceptional energy density com... As the need for high-energy–density batteries continues to grow, lithium-sulfur(Li–S) batteries have become a highly promising next-generation energy solution due to their low cost and exceptional energy density compared to commercially available Li-ion batteries. Research into carbon-based sulfur hosts for Li–S batteries has been ongoing for over two decades, leading to a significant number of publications and patents.However, the commercialization of Li–S batteries has yet to be realized. This can be attributed, in part, to the instability of the Li metal anode. However, even when considering just the cathode side, there is still no consensus on whether carbon-based hosts will prove to be the best sulfur hosts for the industrialization of Li–S batteries. Recently, there has been controversy surrounding the use of carbon-based materials as the ideal sulfur hosts for practical applications of Li–S batteries under high sulfur loading and lean electrolyte conditions. To address this question, it is important to review the results of research into carbon-based hosts, assess their strengths and weaknesses, and provide a clear perspective. This review systematically evaluates the merits and mechanisms of various strategies for developing carbon-based host materials for high sulfur loading and lean electrolyte conditions. The review covers structural design and functional optimization strategies in detail, providing a comprehensive understanding of the development of sulfur hosts. The review also describes the use of efficient machine learning methods for investigating Li–S batteries. Finally, the outlook section lists and discusses current trends, challenges, and uncertainties surrounding carbon-based hosts, and concludes by presenting our standpoint and perspective on the subject. 展开更多
关键词 Li-S batteries Carbon materials Structural design Functional modification Machine learning
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Optimization and statistical analysis of Au-ZnO/Al_2O_3 catalyst for CO oxidation
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作者 Wenjin Yan Xinli Jia +1 位作者 Tao Chen Yanhui Yang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2013年第3期498-505,共8页
In our former work [Catal. Today 174 (2011) 127], 12 heterogeneous catalysts were screened for CO oxidation, and Au-ZnO/Al2O3 was chosen and optimized in terms of weight loadings of Au and ZnO. The present study fol... In our former work [Catal. Today 174 (2011) 127], 12 heterogeneous catalysts were screened for CO oxidation, and Au-ZnO/Al2O3 was chosen and optimized in terms of weight loadings of Au and ZnO. The present study follows on to consider the impact of process parameters (catalyst preparation and reaction conditions), in conjunction with catalyst composition (weight loadings of Au and ZnO, and the total weight of the catalyst), as the optimization of the process parameters simultaneously optimized the catalyst composition. The optimization target is the reactivity of this important reaction. These factors were first optimized using response surface methodology (RSM) with 25 experiments, to obtain the optimum: 100 mg of 1.0%Au-4.1%ZnO/Al2O3 catalyst with 220℃ calcination and 100℃ reduction. After optimization, the main effects and interactions of these five factors were studied using statistical sensitivity analysis (SA). Certain observations from SA were verified by reaction mechanism, reactivity test and/or characterization techniques, while others need further investigation. 展开更多
关键词 carbon monoxide oxidation data-based modeling design of experiments gold catalysts heterogeneous catalysis rapid optimization
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Thermodynamic modelling of unloaded and loaded N,N-diethylethanolamine solutions
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作者 Monica Garcia Hanna K.Knuutila Sai Gu 《Green Energy & Environment》 SCIE 2016年第3期246-257,共12页
Chemical absorption is a crucial step for several chemical processes such as ammonia production, coal gasification, methane reforming,ethylene oxide manufacturing and treatment of associated gas streams [1]. It is con... Chemical absorption is a crucial step for several chemical processes such as ammonia production, coal gasification, methane reforming,ethylene oxide manufacturing and treatment of associated gas streams [1]. It is considered one of the main processes to eliminate CO_2 emissions from power plants by post-combustion.Use of new solvents are of high interest in chemical absorption for carbon capture. For the design of the absorption and desorption columns it is essential to know the vapour-liquid equilibrium(VLE), heat of absorption and densities. N,N-diethylethanolamine(DEEA) appeared as one of the amines with the lowest amount of energy needed for its regeneration [2], which would directly decrease the operation costs. DEEA has a high CO_2 loading of 1 mol/mol of amine compared to the traditional MEA solvent(0.5 mol/mol amine) and is obtained from renewable sources[1]. The main weakness is its low absorption rate and consequently the use of promoters is desirable.In this work, a thermodynamic model based on the electrolyte non-random two-liquid theory(eNRTL) was created and fitted to correlate and predict the partial and total pressures of the unloaded and loaded aqueous DEEA solutions. New interaction parameters were obtained for the binary and tertiary system. This model represents the vapour pressures of the pure components, DEEA and H_2 O, with AARD of 1.9% and 1.73%respectively. Furthermore, the fitted model predicts the total pressure above the binary system, H_2O-DEEA, with AARD of 0.05%. The excess of enthalpy and densities are predicted with AARD of 5.63% and 1.38% respectively. The tertiary system, H_2O-DEEA-CO_2, is fitted for 2 M and5 M DEEA solutions with loading between 0.042 and 0.9 mol CO_2/mol amine up to 80 ℃. Results of CO_2 partial pressures and total pressures are reproduced, with AARD of 19.45% and 16.18% respectively. Densities are predicted with an AARD of 1.52%. 展开更多
关键词 DEEA CO2 capture Chemical absorption MODELLING
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Metal-organic-framework-derived formation of Co–N-doped carbon materials for efficient oxygen reduction reaction 被引量:3
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作者 Hao Tian Chi Zhang +5 位作者 Panpan Su Zhangfeng Shen Hao Liu Guoxiu Wang Shaomin Liu Jian Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2020年第1期137-143,I0005,共8页
Non-precious metal nitrogen-doped carbonaceous materials have attracted tremendous attention in the field of electrochemical energy storage and conversion.Herein,we report the designed synthesis of a novel series of C... Non-precious metal nitrogen-doped carbonaceous materials have attracted tremendous attention in the field of electrochemical energy storage and conversion.Herein,we report the designed synthesis of a novel series of Co-N-C nanocomposites and their evaluation of electrochemical properties.Novel yolkshell structured Co nanoparticles@polymer materials are fabricated from the facile coating polymer strategy on the surface of ZIF-67.After calcination in nitrogen atmosphere,the Co–N–C nanocomposites in which cobalt metal nanoparticles are embedded in the highly porous and graphitic carbon matrix are successfully achieved.The cobalt nanoparticles containing cobalt metal crystallites with an oxidized shell and/or smaller(or amorphous)cobalt-oxide deposits appear on the surface of graphitic carbons.The prepared Co–N–C nanoparticles showed favorable electrocatalytic activity for oxygen reduction reactions,which is attributed to its high graphitic degree,large surface area and the large amount existence of Co–N active sites. 展开更多
关键词 Metal-organic-framework Resin polymer Oxygen reduction reaction ELECTROCATALYSTS
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Conversion of CO_(2)to added value products via rWGS using Fe-promoted catalysts:Carbide,metallic Fe or a mixture?
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作者 Q iZhang Laura Pastor-Pérez +1 位作者 Qiang Wang Tomas Ramirez Reina 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第3期635-646,I0017,共13页
Fe-based catalysts are efficient systems for CO_(2)conversion via reverse water-gas shift(rWGS)reaction.Nevertheless,the nature of the active phase,namely metallic iron,iron oxide or iron carbide remains a subject of ... Fe-based catalysts are efficient systems for CO_(2)conversion via reverse water-gas shift(rWGS)reaction.Nevertheless,the nature of the active phase,namely metallic iron,iron oxide or iron carbide remains a subject of debate which our paper is meant to close.Fe0 is a much better catalyst for the rWGS than Fe_(3)C.The activity of Fe0 can be promoted by the addition of Cs and Cu whose presence hinders iron carburisation while favouring both higher conversion and enhanced selectivity.When the samples are aged in the rWGS reaction mixture during stability test a new phase appear:Fe_(5)C_(2),resulting in a more active but less selective catalysts than Fe0 for the rWGS reaction.Hence our results indicate that we could potentially achieve an optimal activity/selective balance upon finely tuning the proportion Fe/Fe_(5)C_(2).Beyond the fundamental information concerning active phase we have observed the presence of advanced Fischer-Tropsch-like products at ambient pressure opening new opportunities for the design of hybrid rWGS/Fischer-Tropsch systems. 展开更多
关键词 CO_(2)conversion rWGS Fe carbide Fe catalysts Hybrid catalysts
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“H_(2)-free” demethoxylation of guaiacol in subcritical water using Pt supported on N-doped carbon catalysts:A cost-effective strategy for biomass upgrading
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作者 Laura Pastor-Pérez Wei Jin +4 位作者 Juan J.Villora-Picó Qiang Wang M.Mercedes Pastor-Blas Antonio Sepúlveda-Escribano Tomas R.Reina 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第7期377-385,共9页
"H_(2)-free" HDO is a revolutionary route to circumvent the limitations of H_(2)-fed HDO reactors for biomass upgrading.This work demonstrates the viability of this economically appealing route when an adequ... "H_(2)-free" HDO is a revolutionary route to circumvent the limitations of H_(2)-fed HDO reactors for biomass upgrading.This work demonstrates the viability of this economically appealing route when an adequate catalyst is implemented.Herein,we have developed a new family of Pt catalysts supported on N-doped activated carbons for the H_(2)-free HDO process of guaiacol.Several N-donors have been used to tune the catalyst’s structural and electronic properties.As a general trend,the N-promoted samples are more selective towards oxygen-depleted products.The best performing material,namely Pt/PANI-AC reached outstanding guaiacol conversion values-ca.75% at 300℃ while displaying reasonable stability for multiple recycling operations.The advanced performance is ascribed to the modified electronic and acid-base properties which favor guaiacol activation and C-O cleavage,as well as the excellent dispersion of the Pt nano particles. 展开更多
关键词 Biomass upgrading N-doped carbon PT HDO GUAIACOL H_(2)-free
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Amorphous phosphorus chalcogenide as an anode material for lithiumion batteries with high capacity and long cycle life
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作者 Jiale Yu Haiyan Zhang +5 位作者 Yingxi Lin Junyao Shen Yiwen Xie Xifeng Huang Qiong Cai Haitao Huang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第5期658-668,共11页
The ever-increasing demands for modern energy storage applications drive the search for novel anode materials of lithium(Li)-ion batteries(LIBs) with high storage capacity and long cycle life, to outperform the conven... The ever-increasing demands for modern energy storage applications drive the search for novel anode materials of lithium(Li)-ion batteries(LIBs) with high storage capacity and long cycle life, to outperform the conventional LIBs anode materials. Hence, we report amorphous ternary phosphorus chalcogenide(aP_(4)SSe_(2)) as an anode material with high performance for LIBs. Synthesized via the mechanochemistry method, the a-P_(4)SSe_(2) compound is endowed with amorphous feature and offers excellent cycling stability(over 1500 mA h g^(-1) capacity after 425 cycles at 0.3 A g^(-1)), owing to the advantages of isotropic nature and synergistic effect of multielement forming Li-ion conductors during battery operation. Furthermore,as confirmed by ex situ X-ray diffraction(XRD) and transmission electron microscope(TEM), the a-P_(4)SSe_(2)anode material has a reversible and multistage Li-storage mechanism, which is extremely beneficial to long cycle life for batteries. Moreover, the autogenous intermediate electrochemical products with fast ionic conductivity can facilitate Li-ion diffusion effectively. Thus, the a-P_(4)SSe_(2)electrode delivers excellent rate capability(730 mA h g^(-1)capacity at 3 A g^(-1)). Through in situ electrochemical impedance spectra(EIS) measurements, it can be revealed that the resistances of charge transfer(R_(SEI)) and solid electrolyte interphase(R_(Ct)) decrease along with the formation of Li-ion conductors whilst the ohmic resistance(R_(Ω)) remains unchanged during the whole electrochemical process, thus resulting in rapid reaction kinetics and stable electrode to obtain excellent rate performance and cycling ability for LIBs. Moreover, the formation mechanism and electrochemical superiority of the a-P_(4)SSe_(2)phase, and its expansion to P_(4)S_(3-x)Se_(x)(x = 0, 1, 2, 3) family can prove its significance for LIBs. 展开更多
关键词 Lithium-ion batteries Amorphous anode materials Lithium ionic conductor High capacity Long cycle life
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Effect of structural parameters on the setting performance of plug slips during hydraulic fracturing
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作者 Chao Zheng Zeng-Kai Liu +4 位作者 Xin-Lei Wu Aibaibu Abulimiti Jie Qin Xue-Fei Zheng Yong-Hong Liu 《Petroleum Science》 SCIE CAS CSCD 2022年第2期731-742,共12页
Slip is one of the most critical components for the frac plug,which would lodge into the casing and lock the frac plug in place during the setting and anchoring process.However,fracture failure of slip significantly a... Slip is one of the most critical components for the frac plug,which would lodge into the casing and lock the frac plug in place during the setting and anchoring process.However,fracture failure of slip significantly affects the hydraulic fracturing effects and has attracted tremendous attention.In this paper,a three-dimensional contact model is applied to explore the setting process of slip.The effects of key structural parameters such as apex angle,inclination angle,and wedge angle on the contact characteristics of slip are systematically investigated.Numerical results indicate that the maximum contact stress appears at the contact area between slip tooth and the casing’s inner wall.Besides,the maximum contact stress generally increases with the increase of apex angle and inclination angle,while decrease linearly with the rise in the wedge angle.Experimental results show that the slip teeth get blunt and appear severe plastic deformation,which arises from stress concentration.Comparison of biting area indicates that the experimental results are about 21.3%larger,which still have a reasonable agreement with the numerical results.These obtained results can guide the parametric selection of plug slip and other similar components. 展开更多
关键词 Hydraulic fracturing Plug slips Setting performance Fracture failure
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