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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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The photo-decomposition and self-restructuring dynamic equilibrium mechanism of Cu_(2)(OH)_(2)CO_(3)for stable photocatalytic CO_(2)reduction 被引量:1
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作者 Yaqing Zhi Haoning Mao +5 位作者 Guangxing Yang Qiao Zhang Zhiting Liu Yonghai Cao Siyuan Yang Feng Peng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第5期104-112,共9页
Developing suitable photocatalysts and understanding their intrinsic catalytic mechanism remain key challenges in the pursuit of highly active,good selective,and long-term stable photocatalytic CO_(2)reduction(PCO_(2)... Developing suitable photocatalysts and understanding their intrinsic catalytic mechanism remain key challenges in the pursuit of highly active,good selective,and long-term stable photocatalytic CO_(2)reduction(PCO_(2)R)systems.Herein,monoclinic Cu_(2)(OH)_(2)CO_(3)is firstly proven to be a new class of photocatalyst,which has excellent catalytic stability and selectivity for PCO_(2)R in the absence of any sacrificial agent and cocatalysts.Based on a Cu_(2)(OH)_(2)^(13)CO_(3)photocatalyst and 13CO_(2)two-sided^(13)C isotopic tracer strategy,and combined with in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)analysis and density functional theory(DFT)calculations,two main CO_(2)transformation routes,and the photo-decomposition and self-restructuring dynamic equilibrium mechanism of Cu_(2)(OH)_(2)CO_(3)are definitely revealed.The PCO_(2)R activity of Cu_(2)(OH)_(2)CO_(3)is comparable to some of state-of-the-art novel photocatalysts.Significantly,the PCO_(2)R properties can be further greatly enhanced by simply combining Cu_(2)(OH)_(2)CO_(3)with typical TiO_(2)to construct composites photocatalyst.The highest CO_(2)and CH_(4)production rates by 7.5 wt%Cu_(2)(OH)_(2)CO_(3)-TiO_(2)reach 16.4μmol g^(-1)h^(-1)and 116.0μmol g^(-1)h^(-1),respectively,which are even higher than that of some of PCO_(2)R systems containing sacrificial agents or precious metals modified photocatalysts.This work provides a better understanding for the PCO_(2)R mechanism at the atomic levels,and also indicates that basic carbonate photocatalysts have broad application potential in the future. 展开更多
关键词 CO_(2)photocatalytic reduction PHOTOCATALYSIS Basic copper carbonate SELF-RECONSTRUCTION PHOTOCATALYST
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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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Understanding Bridging Sites and Accelerating Quantum Efficiency for Photocatalytic CO_(2) Reduction 被引量:1
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作者 Kangwang Wang Zhuofeng Hu +8 位作者 Peifeng Yu Alina M.Balu Kuan Li Longfu Li Lingyong Zeng Chao Zhang Rafael Luque Kai Yan Huixia Luo 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第1期68-84,共17页
We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in... We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in S_(v)–In_(2)S_(3)@2H–MoTe_(2).The X-ray absorption near-edge structure shows that the formation of S_(v)–In_(2)S_(3)@2H–MoTe_(2) adjusts the coordination environment via interface engineering and forms Mo–S polarized sites at the interface.The interfacial dynamics and catalytic behavior are clearly revealed by ultrafast femtosecond transient absorption,time-resolved,and in situ diffuse reflectance–Infrared Fourier transform spectroscopy.A tunable electronic structure through steric interaction of Mo–S bridging bonds induces a 1.7-fold enhancement in S_(v)–In_(2)S_(3)@2H–MoTe_(2)(5)photogenerated carrier concentration relative to pristine S_(v)–In_(2)S_(3).Benefiting from lower carrier transport activation energy,an internal quantum efficiency of 94.01%at 380 nm was used for photocatalytic CO_(2)RR.This study proposes a new strategy to design photocatalyst through bridging sites to adjust the selectivity of photocatalytic CO_(2)RR. 展开更多
关键词 Quantum efficiency Electronic structure Steric interaction Bridging sites CO_(2)reduction
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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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An Integrated Analysis on the Synergistic Reduction of Carbon and Pollution Emissions from China’s Iron and Steel Industry 被引量:1
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作者 Quanyin Tan Fei Liu Jinhui Li 《Engineering》 SCIE EI CAS CSCD 2024年第9期111-121,共11页
Decarbonization and decontamination of the iron and steel industry(ISI),which contributes up to 15%to anthropogenic CO_(2) emissions(or carbon emissions)and significant proportions of air and water pollutant emissions... Decarbonization and decontamination of the iron and steel industry(ISI),which contributes up to 15%to anthropogenic CO_(2) emissions(or carbon emissions)and significant proportions of air and water pollutant emissions in China,are challenged by the huge demand for steel.Carbon and pollutants often share common emission sources,indicating that emission reduction could be achieved synergistically.Here,we explored the inherent potential of measures to adjust feedstock composition and technological structure and to control the size of the ISI to achieve carbon emission reduction(CER)and pollution emission reduction(PER).We investigated five typical pollutants in this study,namely,petroleum hydrocarbon pollutants and chemical oxygen demand in wastewater,particulate matter,SO_(2),and NO_(x) in off gases,and examined synergies between CER and PER by employing cross elasticity for the period between 2022 and 2035.The results suggest that a reduction of 8.7%-11.7%in carbon emissions and 20%-31%in pollution emissions(except for particulate matter emissions)could be achieved by 2025 under a high steel scrap ratio(SSR)scenario.Here,the SSR and electric arc furnace(EAF)ratio serve critical roles in enhancing synergies between CER and PER(which vary with the type of pollutant).However,subject to a limited volume of steel scrap,a focused increase in the EAF ratio with neglection of the available supply of steel scrap to EAF facilities would lead to an increase carbon and pollution emissions.Although CER can be achieved through SSR and EAF ratio optimization,only when the crude steel production growth rate remains below 2.2%can these optimization measures maintain the emissions in 2030 at a similar level to that in 2021.Therefore,the synergistic effects between PER and CER should be considered when formulating a development route for the ISI in the future. 展开更多
关键词 Iron and steel industry Carbon and pollution emissions Synergistic reduction Technological structure Steel scrap Cross-elasticity
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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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Pre-reduction of WO_(3)-Co_(3)O_(4)by H_(2)-C_(2)H_4 in a fluidized bed 被引量:1
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作者 Huijun Shang Hengli Li +2 位作者 Weijun Li Feng Pan Zhan Du 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第2期273-284,共12页
In order to avoid the formation ofηphase(W_(6)Co_(6)C or W_(3)Co_(3)C)that adversely affects the sintering process and its products in the preparation process of ultra-fine WC-Co powder,a technical route of prereduct... In order to avoid the formation ofηphase(W_(6)Co_(6)C or W_(3)Co_(3)C)that adversely affects the sintering process and its products in the preparation process of ultra-fine WC-Co powder,a technical route of prereduction of WO_(3)-Co_(3)O_(4)to WO_(2)-Co and then deep reduction carbonization to WC-Co powder has been proposed.This study mainly investigates the influence of gas partial pressure on the pre-reduction process of WO_(3)-Co_(3)O_(4)under a mixed atmosphere of H_(2)-C_(2)H_(4)-Ar at 600℃and establishes the kinetic equations of pre-reduction and carbon evolution.The results indicate that increasing the partial pressure of hydrogen is conducive to the rapid and complete conversion of WO_(3) to WO_(2).High carbon content can be generated by the deposition of C_(2)H_(4),and it hinders the diffusion of the reducing gas;WO_(3)still cannot be completely reduced to WO_(2)as the partial pressure of C_(2)H_(4) increases to 60%.For the carbon evolution of C_(2)H_(4),the carbon amount is positively related to the H_(2)partial pressure,but it shows the highest amount and evolution rate when the ethylene partial pressure is 20%.Based on the reduction rate curves of WO_(3) and carbon evolution rate curves of C_(2)H_(4),the rate equations of pre-reduction and carbon evolution of WO_(3)-Co_(3)O_(4)system at 600℃are established.The pre-reduction reaction belongs to the first-order reaction,and its equation is expressed as follows:r=-(dw_(WO_(3)))/dt=(9±0.15)×10^(-2)×P_(H_(2))^(0.44)P_(C_(2)H_(4))&(0.57)The carbon deposition rate equation of C_(2)H_(4) can be expressed as follows:r=-(dc_C)/dt=r_f-r_b≌7.35×10^(-2)×P_(C_(2)H_(4))^(0.31) 展开更多
关键词 FLUIDIZATION WO_(3)-Co_(3)O_(4) reduction Carbon deposition Rate equation
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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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Attribute Reduction of Hybrid Decision Information Systems Based on Fuzzy Conditional Information Entropy 被引量:1
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作者 Xiaoqin Ma Jun Wang +1 位作者 Wenchang Yu Qinli Zhang 《Computers, Materials & Continua》 SCIE EI 2024年第5期2063-2083,共21页
The presence of numerous uncertainties in hybrid decision information systems(HDISs)renders attribute reduction a formidable task.Currently available attribute reduction algorithms,including those based on Pawlak attr... The presence of numerous uncertainties in hybrid decision information systems(HDISs)renders attribute reduction a formidable task.Currently available attribute reduction algorithms,including those based on Pawlak attribute importance,Skowron discernibility matrix,and information entropy,struggle to effectively manages multiple uncertainties simultaneously in HDISs like the precise measurement of disparities between nominal attribute values,and attributes with fuzzy boundaries and abnormal values.In order to address the aforementioned issues,this paper delves into the study of attribute reduction withinHDISs.First of all,a novel metric based on the decision attribute is introduced to solve the problem of accurately measuring the differences between nominal attribute values.The newly introduced distance metric has been christened the supervised distance that can effectively quantify the differences between the nominal attribute values.Then,based on the newly developed metric,a novel fuzzy relationship is defined from the perspective of“feedback on parity of attribute values to attribute sets”.This new fuzzy relationship serves as a valuable tool in addressing the challenges posed by abnormal attribute values.Furthermore,leveraging the newly introduced fuzzy relationship,the fuzzy conditional information entropy is defined as a solution to the challenges posed by fuzzy attributes.It effectively quantifies the uncertainty associated with fuzzy attribute values,thereby providing a robust framework for handling fuzzy information in hybrid information systems.Finally,an algorithm for attribute reduction utilizing the fuzzy conditional information entropy is presented.The experimental results on 12 datasets show that the average reduction rate of our algorithm reaches 84.04%,and the classification accuracy is improved by 3.91%compared to the original dataset,and by an average of 11.25%compared to the other 9 state-of-the-art reduction algorithms.The comprehensive analysis of these research results clearly indicates that our algorithm is highly effective in managing the intricate uncertainties inherent in hybrid data. 展开更多
关键词 Hybrid decision information systems fuzzy conditional information entropy attribute reduction fuzzy relationship rough set theory(RST)
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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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