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Strong synergy between physical and chemical properties:Insight into optimization of atomically dispersed oxygen reduction catalysts 被引量:4
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作者 Yifan Zhang Linsheng Liu +4 位作者 Yuxuan Li Xueqin Mu Shichun Mu Suli Liu Zhihui Dai 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第4期36-49,共14页
Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utiliz... Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utilization and exceptional catalytic functionality.Furthermore,accurately controlling atomic physical properties including spin,charge,orbital,and lattice degrees of atomically dispersed catalysts can realize the optimized chemical properties including maximum atom utilization efficiency,homogenous active centers,and satisfactory catalytic performance,but remains elusive.Here,through physical and chemical insight,we review and systematically summarize the strategies to optimize atomically dispersed ORR catalysts including adjusting the atomic coordination environment,adjacent electronic orbital and site density,and the choice of dual-atom sites.Then the emphasis is on the fundamental understanding of the correlation between the physical property and the catalytic behavior for atomically dispersed catalysts.Finally,an overview of the existing challenges and prospects to illustrate the current obstacles and potential opportunities for the advancement of atomically dispersed catalysts in the realm of electrocatalytic reactions is offered. 展开更多
关键词 Atomically dispersed catalysts Coordination environment Electronic orbitals Inter-site distance effect Oxygen reduction reaction
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Cu-Based Materials for Enhanced C_(2+) Product Selectivity in Photo-/Electro-Catalytic CO_(2) Reduction: Challenges and Prospects 被引量:1
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作者 Baker Rhimi Min Zhou +2 位作者 Zaoxue Yan Xiaoyan Cai Zhifeng Jiang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第4期25-66,共42页
Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues and the energy shortages. Among the materials utilized for ca... Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues and the energy shortages. Among the materials utilized for catalytic reduction of CO_(2), Cu-based materials are highly advantageous owing to their widespread availability, cost-effectiveness, and environmental sustainability. Furthermore, Cu-based materials demonstrate interesting abilities in the adsorption and activation of carbon dioxide, allowing the formation of C_(2+) compounds through C–C coupling process. Herein, the basic principles of photocatalytic CO_(2) reduction reactions(PCO_(2)RR) and electrocatalytic CO_(2) reduction reaction(ECO_(2)RR) and the pathways for the generation C_(2+) products are introduced. This review categorizes Cu-based materials into different groups including Cu metal, Cu oxides, Cu alloys, and Cu SACs, Cu heterojunctions based on their catalytic applications. The relationship between the Cu surfaces and their efficiency in both PCO_(2)RR and ECO_(2)RR is emphasized. Through a review of recent studies on PCO_(2)RR and ECO_(2)RR using Cu-based catalysts, the focus is on understanding the underlying reasons for the enhanced selectivity toward C_(2+) products. Finally, the opportunities and challenges associated with Cu-based materials in the CO_(2) catalytic reduction applications are presented, along with research directions that can guide for the design of highly active and selective Cu-based materials for CO_(2) reduction processes in the future. 展开更多
关键词 Photocatalytic CO_(2)reduction Cu-based materials Electrocatalytic CO_(2)reduction
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Numerical Study on Reduction in Aerodynamic Drag and Noise of High-Speed Pantograph 被引量:1
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作者 Deng Qin Xing Du +1 位作者 Tian Li Jiye Zhang 《Computer Modeling in Engineering & Sciences》 SCIE EI 2024年第5期2155-2173,共19页
Reducing the aerodynamic drag and noise levels of high-speed pantographs is important for promoting environmentally friendly,energy efficient and rapid advances in train technology.Using computational fluid dynamics t... Reducing the aerodynamic drag and noise levels of high-speed pantographs is important for promoting environmentally friendly,energy efficient and rapid advances in train technology.Using computational fluid dynamics theory and the K-FWH acoustic equation,a numerical simulation is conducted to investigate the aerodynamic characteristics of high-speed pantographs.A component optimization method is proposed as a possible solution to the problemof aerodynamic drag and noise in high-speed pantographs.The results of the study indicate that the panhead,base and insulator are the main contributors to aerodynamic drag and noise in high-speed pantographs.Therefore,a gradual optimization process is implemented to improve the most significant components that cause aerodynamic drag and noise.By optimizing the cross-sectional shape of the strips and insulators,the drag and noise caused by airflow separation and vortex shedding can be reduced.The aerodynamic drag of insulator with circular cross section and strips with rectangular cross section is the largest.Ellipsifying insulators and optimizing the chamfer angle and height of the windward surface of the strips can improve the aerodynamic performance of the pantograph.In addition,the streamlined fairing attached to the base can eliminate the complex flow and shield the radiated noise.In contrast to the original pantograph design,the improved pantograph shows a 21.1%reduction in aerodynamic drag and a 1.65 dBA reduction in aerodynamic noise. 展开更多
关键词 High-speed pantograph aerodynamic drag aerodynamic noise reduction optimizing
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Oxygen‑Coordinated Single Mn Sites for Efficient Electrocatalytic Nitrate Reduction to Ammonia 被引量:2
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作者 Shengbo Zhang Yuankang Zha +8 位作者 Yixing Ye Ke Li Yue Lin Lirong Zheng Guozhong Wang Yunxia Zhang Huajie Yin Tongfei Shi Haimin Zhang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第1期147-159,共13页
Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites... Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites with atomically dispersed oxygen(O)coordination on bacterial cellulose-converted graphitic carbon(Mn-O-C).Evidence of the atomically dispersed Mn-(O-C_(2))_(4)moieties embedding in the exposed basal plane of carbon surface is confirmed by X-ray absorption spectroscopy.As a result,the as-synthesized Mn-O-C catalyst exhibits superior NitRR activity with an NH_(3)yield rate(RNH_(3))of 1476.9±62.6μg h^(−1)cm^(−2)at−0.7 V(vs.reversible hydrogen electrode,RHE)and a faradaic efficiency(FE)of 89.0±3.8%at−0.5 V(vs.RHE)under ambient conditions.Further,when evaluated with a practical flow cell,Mn-O-C shows a high RNH_(3)of 3706.7±552.0μg h^(−1)cm^(−2)at a current density of 100 mA cm−2,2.5 times of that in the H cell.The in situ FT-IR and Raman spectroscopic studies combined with theoretical calculations indicate that the Mn-(O-C_(2))_(4)sites not only effectively inhibit the competitive hydrogen evolution reaction,but also greatly promote the adsorption and activation of nitrate(NO_(3)^(−)),thus boosting both the FE and selectivity of NH_(3)over Mn-(O-C_(2))_(4)sites. 展开更多
关键词 Atomically dispersed Oxygen coordination Nitrate reduction reaction In situ spectroscopic studies Hydrogen evolution reaction
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Research on a Monte Carlo global variance reduction method based on an automatic importance sampling method 被引量:1
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作者 Yi-Sheng Hao Zhen Wu +3 位作者 Shen-Shen Gao Rui Qiu Hui Zhang Jun-Li Li 《Nuclear Science and Techniques》 SCIE EI CAS CSCD 2024年第5期200-215,共16页
Global variance reduction is a bottleneck in Monte Carlo shielding calculations.The global variance reduction problem requires that the statistical error of the entire space is uniform.This study proposed a grid-AIS m... Global variance reduction is a bottleneck in Monte Carlo shielding calculations.The global variance reduction problem requires that the statistical error of the entire space is uniform.This study proposed a grid-AIS method for the global variance reduction problem based on the AIS method,which was implemented in the Monte Carlo program MCShield.The proposed method was validated using the VENUS-Ⅲ international benchmark problem and a self-shielding calculation example.The results from the VENUS-Ⅲ benchmark problem showed that the grid-AIS method achieved a significant reduction in the variance of the statistical errors of the MESH grids,decreasing from 1.08×10^(-2) to 3.84×10^(-3),representing a 64.00% reduction.This demonstrates that the grid-AIS method is effective in addressing global issues.The results of the selfshielding calculation demonstrate that the grid-AIS method produced accurate computational results.Moreover,the grid-AIS method exhibited a computational efficiency approximately one order of magnitude higher than that of the AIS method and approximately two orders of magnitude higher than that of the conventional Monte Carlo method. 展开更多
关键词 Monte Carlo Global variance reduction Reactor shielding Automatic importance sampling
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Single-atom catalysts for the electrochemical reduction of carbon dioxide into hydrocarbons and oxygenates 被引量:1
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作者 Karl Adrian Gandionco Juwon Kim +2 位作者 Lieven Bekaert Annick Hubin Jongwoo Lim 《Carbon Energy》 SCIE EI CAS CSCD 2024年第3期64-117,共54页
The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic ... The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic material and renewable energy-generated electricity drive the conversion of carbon dioxide into high-value chemicals and carbon-neutral fuels.Over the past few years,single-atom catalysts have been intensively studied as they could provide near-unity atom utilization and unique catalytic performance.Single-atom catalysts have become one of the state-of-the-art catalyst materials for the electrochemical reduction of carbon dioxide into carbon monoxide.However,it remains a challenge for single-atom catalysts to facilitate the efficient conversion of carbon dioxide into products beyond carbon monoxide.In this review,we summarize and present important findings and critical insights from studies on the electrochemical carbon dioxide reduction reaction into hydrocarbons and oxygenates using single-atom catalysts.It is hoped that this review gives a thorough recapitulation and analysis of the science behind the catalysis of carbon dioxide into more reduced products through singleatom catalysts so that it can be a guide for future research and development on catalysts with industry-ready performance for the electrochemical reduction of carbon dioxide into high-value chemicals and carbon-neutral fuels. 展开更多
关键词 ELECTROCATALYSIS electrochemical CO_(2)reduction hydrocarbons OXYGENATES single-atom catalysts
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Porous metal oxides in the role of electrochemical CO_(2) reduction reaction 被引量:1
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作者 Ziqi Zhang Jinyun Xu +9 位作者 Yu Zhang Liping Zhao Ming Li Guoqiang Zhong Di Zhao Minjing Li Xudong Hu Wenju Zhu Chunming Zheng Xiaohong Sun 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第1期373-398,I0009,共27页
The global energy-related CO_(2) emissions have rapidly increased as the world economy heavily relied on fossil fuels.This paper explores the pressing challenge of CO_(2) emissions and highlights the role of porous me... The global energy-related CO_(2) emissions have rapidly increased as the world economy heavily relied on fossil fuels.This paper explores the pressing challenge of CO_(2) emissions and highlights the role of porous metal oxide materials in the electrocatalytic reduction of CO_(2)(CO_(2)RR).The focus is on the development of robust and selective catalysts,particularly metal and metal-oxide-based materials.Porous metal oxides offer high surface area,enhancing the accessibility to active sites and improving reaction kinetics.The tunability of these materials allows for tailored catalytic behavior,targeting optimized reaction mechanisms for CO_(2)RR.The work also discusses the various synthesis strategies and identifies key structural and compositional features,addressing challenges like high overpotential,poor selectivity,and low stability.Based on these insights,we suggest avenues for future research on porous metal oxide materials for electrochemical CO_(2) reduction. 展开更多
关键词 CO_(2)reduction Carbon dioxide TRANSFORMATION Porous metal oxides ELECTROCATALYSIS
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Surface engineering of ZnO electrocatalyst by N doping towards electrochemical CO_(2) reduction 被引量:1
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作者 Rohini Subhash Kanase Getasew Mulualem Zewdie +7 位作者 Maheswari Arunachalam Jyoti Badiger Suzan Abdelfattah Sayed Kwang-Soon Ahn Jun-Seok Ha Uk Sim Hyeyoung Shin Soon Hyung Kang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第1期71-81,I0002,共12页
The discovery of efficient,selective,and stable electrocatalysts can be a key point to produce the largescale chemical fuels via electrochemical CO_(2) reduction(ECR).In this study,an earth-abundant and nontoxic ZnO-b... The discovery of efficient,selective,and stable electrocatalysts can be a key point to produce the largescale chemical fuels via electrochemical CO_(2) reduction(ECR).In this study,an earth-abundant and nontoxic ZnO-based electrocatalyst was developed for use in gas-diffusion electrodes(GDE),and the effect of nitrogen(N)doping on the ECR activity of ZnO electrocatalysts was investigated.Initially,a ZnO nanosheet was prepared via the hydrothermal method,and nitridation was performed at different times to control the N-doping content.With an increase in the N-doping content,the morphological properties of the nanosheet changed significantly,namely,the 2D nanosheets transformed into irregularly shaped nanoparticles.Furthermore,the ECR performance of Zn O electrocatalysts with different N-doping content was assessed in 1.0 M KHCO_(3) electrolyte using a gas-diffusion electrode-based ECR cell.While the ECR activity increased after a small amount of N doping,it decreased for higher N doping content.Among them,the N:ZnO-1 h electrocatalysts showed the best CO selectivity,with a faradaic efficiency(FE_(CO))of 92.7%at-0.73 V vs.reversible hydrogen electrode(RHE),which was greater than that of an undoped Zn O electrocatalyst(FE_(CO)of 63.4%at-0.78 V_(RHE)).Also,the N:ZnO-1 h electrocatalyst exhibited outstanding durability for 16 h,with a partial current density of-92.1 mA cm^(-2).This improvement of N:ZnO-1 h electrocatalyst can be explained by density functional theory calculations,demonstrating that this improvement of N:ZnO-1 h electrocatalyst comes from(ⅰ)the optimized active sites lowering the free energy barrier for the rate-determining step(RDS),and(ⅱ)the modification of electronic structure enhancing the electron transfer rate by N doping. 展开更多
关键词 ZNO N-doped ZnO Gas-diffusion electrode CO Selectivity Electrochemical CO_(2)reduction
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Model reduction of fractional impedance spectra for time–frequency analysis of batteries, fuel cells, and supercapacitors 被引量:1
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作者 Weiheng Li Qiu-An Huang +6 位作者 Yuxuan Bai Jia Wang Linlin Wang Yuyu Liu Yufeng Zhao Xifei Li Jiujun Zhang 《Carbon Energy》 SCIE EI CAS CSCD 2024年第1期108-141,共34页
Joint time–frequency analysis is an emerging method for interpreting the underlying physics in fuel cells,batteries,and supercapacitors.To increase the reliability of time–frequency analysis,a theoretical correlatio... Joint time–frequency analysis is an emerging method for interpreting the underlying physics in fuel cells,batteries,and supercapacitors.To increase the reliability of time–frequency analysis,a theoretical correlation between frequency-domain stationary analysis and time-domain transient analysis is urgently required.The present work formularizes a thorough model reduction of fractional impedance spectra for electrochemical energy devices involving not only the model reduction from fractional-order models to integer-order models and from high-to low-order RC circuits but also insight into the evolution of the characteristic time constants during the whole reduction process.The following work has been carried out:(i)the model-reduction theory is addressed for typical Warburg elements and RC circuits based on the continued fraction expansion theory and the response error minimization technique,respectively;(ii)the order effect on the model reduction of typical Warburg elements is quantitatively evaluated by time–frequency analysis;(iii)the results of time–frequency analysis are confirmed to be useful to determine the reduction order in terms of the kinetic information needed to be captured;and(iv)the results of time–frequency analysis are validated for the model reduction of fractional impedance spectra for lithium-ion batteries,supercapacitors,and solid oxide fuel cells.In turn,the numerical validation has demonstrated the powerful function of the joint time–frequency analysis.The thorough model reduction of fractional impedance spectra addressed in the present work not only clarifies the relationship between time-domain transient analysis and frequency-domain stationary analysis but also enhances the reliability of the joint time–frequency analysis for electrochemical energy devices. 展开更多
关键词 battery fuel cell supercapacitor fractional impedance spectroscopy model reduction time-frequency analysis
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Bimetallic In_(2)O_(3)/Bi_(2)O_(3) Catalysts Enable Highly Selective CO_(2) Electroreduction to Formate within Ultra-Broad Potential Windows 被引量:1
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作者 Zhongxue Yang Hongzhi Wang +7 位作者 Xinze Bi Xiaojie Tan Yuezhu Zhao Wenhang Wang Yecheng Zou Huai ping Wang Hui Ning Mingbo Wu 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第1期257-264,共8页
CO_(2)electrochemical reduction reaction(CO_(2)RR)to formate is a hopeful pathway for reducing CO_(2)and producing high-value chemicals,which needs highly selective catalysts with ultra-broad potential windows to meet... CO_(2)electrochemical reduction reaction(CO_(2)RR)to formate is a hopeful pathway for reducing CO_(2)and producing high-value chemicals,which needs highly selective catalysts with ultra-broad potential windows to meet the industrial demands.Herein,the nanorod-like bimetallic ln_(2)O_(3)/Bi_(2)O_(3)catalysts were successfully synthesized by pyrolysis of bimetallic InBi-MOF precursors.The abundant oxygen vacancies generated from the lattice mismatch of Bi_(2)O_(3)and ln_(2)O_(3)reduced the activation energy of CO_(2)to*CO_(2)·^(-)and improved the selectivity of*CO_(2)·^(-)to formate simultaneously.Meanwhile,the carbon skeleton derived from the pyrolysis of organic framework of InBi-MOF provided a conductive network to accelerate the electrons transmission.The catalyst exhibited an ultra-broad applied potential window of 1200 mV(from-0.4 to-1.6 V vs RHE),relativistic high Faradaic efficiency of formate(99.92%)and satisfactory stability after 30 h.The in situ FT-IR experiment and DFT calculation verified that the abundant oxygen vacancies on the surface of catalysts can easily absorb CO_(2)molecules,and oxygen vacancy path is dominant pathway.This work provides a convenient method to construct high-performance bimetallic catalysts for the industrial application of CO_(2)RR. 展开更多
关键词 bimetallic catalyst CO_(2)electrochemical reduction reaction FORMATE oxygen vacancy wide potential window
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Exploring the impact of Nafion modifier on electrocatalytic CO_(2) reduction over Cu catalyst 被引量:1
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作者 Yingshi Su Yonghui Cheng +6 位作者 Zhen Li Yanjia Cui Caili Yang Ziyi Zhong Yibing Song Gongwei Wang Lin Zhuang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第1期543-551,I0012,共10页
Nafion as a universal polymer ionomer was widely applied for nanocatalysts electrode preparation.However,the effect of Nafion on electrocatalytic performance was often overlooked,especially for CO_(2)electrolysis.Here... Nafion as a universal polymer ionomer was widely applied for nanocatalysts electrode preparation.However,the effect of Nafion on electrocatalytic performance was often overlooked,especially for CO_(2)electrolysis.Herein,the key roles of Nafion for CO_(2)RR were systematically studied on Cu nanoparticles(NPs)electrocatalyst.We found that Nafion modifier not only inhibit hydrogen evolution reaction(HER)by decreasing the accessibility of H_(2)O from electrolyte to Cu NPs,and increase the CO_(2)concentration at electrocatalyst interface for enhancing the CO_(2)mass transfer process,but also activate CO_(2)molecule by Lewis acid-base interaction between Nafion and CO_(2)to accelerate the formation of^(*)CO,which favor of C–C coupling for boosting C_(2)product generation.Owing to these features,the HER selectivity was suppressed from 40.6%to 16.8%on optimal Cu@Nafion electrode at-1.2 V versus reversible hydrogen electrode(RHE),and as high as 73.5%faradaic efficiencies(FEs)of C_(2)products were achieved at the same applied potential,which was 2.6 times higher than that on bare Cu electrode(~28.3%).In addition,Nafion also contributed to the long-term stability by hinder Cu NPs morphology reconstruction.Thus,this work provides insights into the impact of Nafion on electrocatalytic CO_(2)RR performance. 展开更多
关键词 Nafion modifier CO_(2)reduction Cu nanoparticles In situ ATR-SEIRAS C_(2)product
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Preferentially selective extraction of lithium from spent LiCoO_(2)cathodes by medium-temperature carbon reduction roasting 被引量:1
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作者 Daixiang Wei Wei Wang +6 位作者 Longjin Jiang Zhidong Chang Hualei Zhou Bin Dong Dekun Gao Minghui Zhang Chaofan Wu 《International Journal of Minerals,Metallurgy and Materials》 SCIE EI CAS CSCD 2024年第2期315-322,共8页
Lithium recovery from spent lithium-ion batteries(LIBs)have attracted extensive attention due to the skyrocketing price of lithium.The medium-temperature carbon reduction roasting was proposed to preferential selectiv... Lithium recovery from spent lithium-ion batteries(LIBs)have attracted extensive attention due to the skyrocketing price of lithium.The medium-temperature carbon reduction roasting was proposed to preferential selective extraction of lithium from spent Li-CoO_(2)(LCO)cathodes to overcome the incomplete recovery and loss of lithium during the recycling process.The LCO layered structure was destroyed and lithium was completely converted into water-soluble Li2CO_(3)under a suitable temperature to control the reduced state of the cobalt oxide.The Co metal agglomerates generated during medium-temperature carbon reduction roasting were broken by wet grinding and ultrasonic crushing to release the entrained lithium.The results showed that 99.10%of the whole lithium could be recovered as Li2CO_(3)with a purity of 99.55%.This work provided a new perspective on the preferentially selective extraction of lithium from spent lithium batteries. 展开更多
关键词 spent LiCoO_(2)cathodes medium-temperature carbon reduction lithium extraction priority crystal transformation macro-scopic transport resistance
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Optimum Profiles of Endwall Contouring for Enhanced Net Heat Flux Reduction and Aerodynamic Performance 被引量:1
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作者 Arjun K S Tide P S Biju N 《Journal of Harbin Institute of Technology(New Series)》 CAS 2024年第2期80-92,共13页
Successfully utilized non-axisymmetric endwalls to enhance turbine efficiencies(aerodynamic and turbine inlet temperatures)by controlling the characteristics of the secondary flow in a blade passage.This is accomplish... Successfully utilized non-axisymmetric endwalls to enhance turbine efficiencies(aerodynamic and turbine inlet temperatures)by controlling the characteristics of the secondary flow in a blade passage.This is accomplished by steady-state numerical hydrodynamics and deep knowledge of the field of flow.Because of the interaction between mainstream and purge flow contributing supplementary losses in the stage,non-axisymmetric endwalls are highly susceptible to the inception of purge flow exit compared to the flat and any advantage rapidly vanishes.The conclusions reveal that the supreme endwall pattern could yield a lowering of the gross pressure loss at the design stage and is related to the size of the top-loss location being productively lowered.This has led to diminished global thermal exchange lowered in the passage of the vane alone.The reverse flow adjacent to the suction side corner of the endwall is migrated farther from the vane surface,as the deviated pressure spread on the endwall accelerates the flow and progresses the reverse flow core still downstream.The depleted association between the tornado-like vortex and the corner vortex adjacent to the suction side corner of the endwall is the dominant mechanism of control in the contoured end wall.In this publication,we show that the non-axisymmetric endwall contouring by selective numerical shape change method at most prominent locations is advantageous in lowering the thermal load in turbines to augment the net heat flux reduction as well as the aerodynamic performance using multi-objective optimization. 展开更多
关键词 endwall contouring turbine VANE heat transfer phantom cooling coolant injection net heat flux reduction aerodynamic performance
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Comprehensive understanding of the thriving electrocatalytic nitrate/nitrite reduction to ammonia under ambient conditions
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作者 Xinying Zhao Yuzhuo Jiang +5 位作者 Mengfan Wang Yunfei Huan Qiyang Cheng Yanzheng He Tao Qian Chenglin Yan 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第5期459-483,共25页
Ammonia(NH_(3))is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH_(3)synthesis is highly dependent on the... Ammonia(NH_(3))is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH_(3)synthesis is highly dependent on the conventional Haber–Bosch process that operates under harsh conditions,which consumes large quantities of fossil fuels and releases a large amount of carbon dioxide.As an alternative,electrosynthesis is a prospective method for producing NH_(3)under normal temperature and pressure conditions.Although electrocatalytic nitrogen reduction to ammonia has attracted considerable attentions,the low solubility of N_(2)and high N≡N cracking energy render the achievements of high NH_(3) yield rate and Faradaic efficiency difficult.Nitrate and nitrite(NO_(x)^(-))are common N-containing pollutants.Due to their high solubilities and low dissociation energy of N=O,NO_(x)^(-)−are ideal raw materials for NH_(3) production.Therefore,electrocatalytic NO_(x)^(-)−reduction to NH_(3)(eNO_(x)RR)is a prospective strategy to simultaneously realise environmental protection and NH_(3) synthesis.This review offers a comprehensive understanding of the thriving eNO_(x)RR under ambient conditions.At first,the popular theory and mechanism of eNO_(x)RR and a summary of the measurement system and evaluation criteria are introduced.Thereafter,various strategies for developing NO_(x)−reduction catalysts are systematically presented and discussed.Finally,the challenges and possible prospects of electrocatalytic NO_(x)^(-1) reduction are outlined to facilitate energy-saving and environmentally friendly large-scale synthesis of NH_(3) in the future. 展开更多
关键词 Electrocatalytic nitrate reduction Electrocatalytic nitrite reduction Ammonia synthesis Pollutant removal ELECTROSYNTHESIS
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Engineering of oxygen vacancy and bismuth cluster assisted ultrathin Bi_(12)O_(17)Cl_(2)nanosheets with efficient and selective photoreduction of CO_(2)to CO 被引量:1
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作者 Meili Guan Ni Lu +7 位作者 Xuan Zhang Qiuwan Wang Jian Bao Guiye Chen Hao Yu Huaming Li Jiexiang Xia Xuezhong Gong 《Carbon Energy》 SCIE EI CAS CSCD 2024年第4期1-11,共11页
The photocatalytic conversion of CO_(2)into solar‐powered fuels is viewed as a forward‐looking strategy to address energy scarcity and global warming.This work demonstrated the selective photoreduction of CO_(2)to C... The photocatalytic conversion of CO_(2)into solar‐powered fuels is viewed as a forward‐looking strategy to address energy scarcity and global warming.This work demonstrated the selective photoreduction of CO_(2)to CO using ultrathin Bi_(12)O_(17)Cl_(2)nanosheets decorated with hydrothermally synthesized bismuth clusters and oxygen vacancies(OVs).The characterizations revealed that the coexistences of OVs and Bi clusters generated in situ contributed to the high efficiency of CO_(2)–CO conversion(64.3μmol g^(−1)h^(−1))and perfect selectivity.The OVs on the facet(001)of the ultrathin Bi_(12)O_(17)Cl_(2)nanosheets serve as sites for CO_(2)adsorption and activation sites,capturing photoexcited electrons and prolonging light absorption due to defect states.In addition,the Bi‐cluster generated in situ offers the ability to trap holes and the surface plasmonic resonance effect.This study offers great potential for the construction of semiconductor hybrids as multiphotocatalysts,capable of being used for the elimination and conversion of CO_(2)in terms of energy and environment. 展开更多
关键词 Bi cluster Bi_(12)O_(17)Cl_(2)nanosheet oxygen vacancy photocatalytic CO_(2)reduction
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Oxidation Evolution and Activity Origin of N-Doped Carbon in the Oxygen Reduction Reaction
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作者 Jiaqi Wu Chuanqi Cheng +2 位作者 Shanshan Lu Bin Zhang Yanmei Shi 《Transactions of Tianjin University》 EI CAS 2024年第4期369-379,共11页
N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively studied.However,a negletcted fact is that the operating potential of the ORR is higher ... N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively studied.However,a negletcted fact is that the operating potential of the ORR is higher than the theoretical oxida-tion potential of carbon,possibly leading to the oxidation of carbon materials.Consequently,the infl uence of the structural oxidation evolution on ORR performance and the real active sites are not clear.In this study,we discover a two-step oxida-tion process of N-doped carbon during the ORR.The fi rst oxidation process is caused by the applied potential and bubbling oxygen during the ORR,leading to the oxidative dissolution of N and the formation of abundant oxygen-containing functional groups.This oxidation process also converts the reaction path from the four-electron(4e)ORR to the two-electron(2e)ORR.Subsequently,the enhanced 2e ORR generates oxidative H_(2)O_(2),which initiates the second stage of oxidation to some newly formed oxygen-containing functional groups,such as quinones to dicarboxyls,further diversifying the oxygen-containing functional groups and making carboxyl groups as the dominant species.We also reveal the synergistic eff ect of multiple oxygen-containing functional groups by providing additional opportunities to access active sites with optimized adsorption of OOH*,thus leading to high effi ciency and durability in electrocatalytic H_(2)O_(2) production. 展开更多
关键词 Oxygen reduction reaction N-doped carbon Reaction path Structural evolution Oxidation in reduction
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Behavior and mechanism of pre-oxidation improvement on fluidization in the fluidized reduction of titanomagnetite
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作者 Haoyan Sun Ajala Adewole Adetoro +1 位作者 Zhiqiang Wang Qingshan Zhu 《International Journal of Minerals,Metallurgy and Materials》 SCIE EI CAS CSCD 2024年第11期2458-2465,共8页
The direct reduction process is an important development direction of low-carbon ironmaking and efficient comprehensive utilization of poly-metallic iron ore,such as titanomagnetite.However,the defluidization of reduc... The direct reduction process is an important development direction of low-carbon ironmaking and efficient comprehensive utilization of poly-metallic iron ore,such as titanomagnetite.However,the defluidization of reduced iron particles with a high metallization degree at a high temperature will seriously affect the operation of fluidized bed reduction.Coupling the pre-oxidation enhancing reduction and the particle surface modification of titanomagnetite,the behavior and mechanism of pre-oxidation improvement on fluidization in the fluidized bed reduction of titanomagnetite are systematically studied in this paper.Pre-oxidation treatment of titanomagnetite can significantly lower the critical stable reduction fluidization gas velocity to 0.17 m/s,which is reduced by 56%compared to that of titanomagnetite reduction without pre-oxidation,while achieving a metallization degree of>90%,Corresponding to the different reduction fluidization behaviors,three pre-oxidation operation regions have been divided,taking oxidation degrees of 26%and 86%as the boundaries.Focusing on the particle surface morphology evolution in the pre-oxidation-reduction process,the relationship between the surface morphology of pre-oxidized ore and the reduced iron with fluidization properties is built.The improving method of pre-oxidation on the reduction fluidization provides a novel approach to prevent defluidization by particle surface modification,especially for the fluidized bed reduction of poly-metallic iron ore. 展开更多
关键词 FLUIDIZATION direct reduction PRE-OXIDATION TITANOMAGNETITE iron whisker
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Attribute Reduction Method Based on Sequential Three-Branch Decision Model
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作者 Peiyu Su Fu Li 《Applied Mathematics》 2024年第4期257-266,共10页
Attribute reduction is a research hotspot in rough set theory. Traditional heuristic attribute reduction methods add the most important attribute to the decision attribute set each time, resulting in multiple redundan... Attribute reduction is a research hotspot in rough set theory. Traditional heuristic attribute reduction methods add the most important attribute to the decision attribute set each time, resulting in multiple redundant attribute calculations, high time consumption, and low reduction efficiency. In this paper, based on the idea of sequential three-branch decision classification domain, attributes are treated as objects of three-branch division, and attributes are divided into core attributes, relatively necessary attributes, and unnecessary attributes using attribute importance and thresholds. Core attributes are added to the decision attribute set, unnecessary attributes are rejected from being added, and relatively necessary attributes are repeatedly divided until the reduction result is obtained. Experiments were conducted on 8 groups of UCI datasets, and the results show that, compared to traditional reduction methods, the method proposed in this paper can effectively reduce time consumption while ensuring classification performance. 展开更多
关键词 Attribute reduction Three-Branch Decision Sequential Three-Branch Decision
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The manipulation of rectifying contact of Co and nitrogen-doped carbon hierarchical superstructures toward high-performance oxygen reduction reaction
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作者 Jing Li Tingyu Lu +6 位作者 Yu Fang Guangyao Zhou Mingyi Zhang Huan Pang Jun Yang Yawen Tang Lin Xu 《Carbon Energy》 SCIE EI CAS CSCD 2024年第9期338-349,共12页
Rational design and construction of oxygen reduction reaction(ORR)electrocatalysts with high activity,good stability,and low price are essential for the practical applications of renewable energy conversion devices,su... Rational design and construction of oxygen reduction reaction(ORR)electrocatalysts with high activity,good stability,and low price are essential for the practical applications of renewable energy conversion devices,such as metal-air batteries.Electronic modification through constructing metal/semiconductor Schottky heterointerface represents a powerful strategy to enhance the electrochemical performance.Herein,we demonstrate a concept of Schottky electrocatalyst composed of uniform Co nanoparticles in situ anchored on the carbon nanotubes aligned on the carbon nanosheets(denoted as Co@N-CNTs/NSs hereafter)toward ORR.Both experimental findings and theoretical simulation testify that the rectifying contact could impel the voluntary electron flow from Co to N-CNTs/NSs and create an internal electric field,thereby boosting the electron transfer rate and improving the intrinsic activity.As a consequence,the Co@N-CNTs/NSs deliver outstanding ORR activity,impressive long-term durability,excellent methanol tolerance,and good performance as the air-cathode in the Zn-air batteries.The design concept of Schottky contact may provide the innovational inspirations for the synthesis of advanced catalysts in sustainable energy conversion fields. 展开更多
关键词 Co-based ELECTROCATALYSTS oxygen reduction reaction rectifying CONTACT Zn-air BATTERIES
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Pyrolysis of Copper Phthalocyanine as Non-noble Metal Electrocatalysts for Oxygen Reduction Reaction
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作者 ZHANG Lijuan LU Jinhua +1 位作者 WANG Yan LI Xiang 《Journal of Wuhan University of Technology(Materials Science)》 SCIE EI CAS CSCD 2024年第5期1087-1092,共6页
We investigated the relationship between oxygen reduction reaction(ORR)activity and the pyrolysis temperature(650-850℃)of CuPc in alkaline solution.The highly active sites were formed through the decomposition of CuP... We investigated the relationship between oxygen reduction reaction(ORR)activity and the pyrolysis temperature(650-850℃)of CuPc in alkaline solution.The highly active sites were formed through the decomposition of CuPc or Cu-N_(4) structure after releasing 4-nitrophthalonitrile.Cu-Nx incorporated with carbon were the main active sites.The XPS measurement results show that,at lower temperature,the contents of pyridinic-N and pyrrolic-N account for the most of the total N.As the temperature is higher than 750℃,the content of graphitic N(26.11%)increases and pyridinic-N(58.81%)becomes the dominant specie.When the temperature is higher than 850℃,the content of graphitic N increases remarkably and becomes the dominant species.Moreover,the specific surface areas decrease with increased pyrolysis temperature.Benefiting from the synergistic effect,the pyrolysis temperature at 750℃of CuPc displays superior electrocatalytic properties.The obtained results reveal that the fabricated non-noble metal catalysts can be used as low-cost,efficient catalyst for water splitting ORR in metal-air batteries and fuel cells. 展开更多
关键词 copper phthalocyanine PYROLYSIS ELECTROCATALYTIC oxygen reduction reaction
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