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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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Electrochemical reduction of carbon dioxide to produce formic acid coupled with oxidative conversion of biomass
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作者 Xi Liu Yifan Wang +2 位作者 Zhiwei Dai Daihong Gao Xuebing Zhao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第5期705-729,共25页
Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(... Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(2) due to its high energy value as estimated by market price per energy unit and wide application in chemical industry.Biomass is the most abundant renewable resource in the natural world.Coupling biomass oxidative conversion with CO_(2)RR driven by renewable electricity would well achieve carbon negativity.In this work,we comprehensively reviewed the current research progress on CO_(2)RR to produce HCOOH and coupled system for conversion of biomass and its derivatives to produce value-added products.Sn-and Bi-based electrocatalysts are discussed for CO_(2)RR with regards to the structure of the catalyst and reaction mechanisms.Electro-oxidation reactions of biomass derived sugars,alcohols,furan aldehydes and even polymeric components of lignocellulose were reviewed as alternatives to replace oxygen evolution reaction(OER)in the conventional electrolysis process.It was recommended that to further improve the efficiency of the coupled system,future work should be focused on the development of more efficient and stable catalysts,careful design of the electrolytic cells for improving the mass transfer and development of environment-friendly processes for recovering the formed formate and biomass oxidation products. 展开更多
关键词 Electrochemical reduction of CO_(2) Formic acid oxidative conversion of biomass LIGNOCELLULOSE Coupled system
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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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Unraveling the roles of atomically-dispersed Au in boosting photocatalytic CO_(2)reduction and aryl alcohol oxidation
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作者 Jian Lei Nan Zhou +3 位作者 Shuaikang Sang Sugang Meng Jingxiang Low Yue Li 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第10期163-173,共11页
Atomically-dispersed metal-based materials represent an emerging class of photocatalysts attributed to their high catalytic activity,abundant surface active sites,and efficient charge separation.Nevertheless,the roles... Atomically-dispersed metal-based materials represent an emerging class of photocatalysts attributed to their high catalytic activity,abundant surface active sites,and efficient charge separation.Nevertheless,the roles of different forms of atomically-dispersed metals(i.e.,single-atoms and atomic clusters)in photocatalytic reactions remain ambiguous.Herein,we developed an ethylenediamine(EDA)-assisted reduction method to controllably synthesize atomically dispersed Au in the forms of Au single atoms(Au_(SA)),Au clusters(Au_(C)),and a mixed-phase of Au_(SA)and Au_(C)(Au_(SA+C))on CdS.In addition,we elucidate the synergistic effect of Au_(SA)and Au_(C)in enhancing the photocatalytic performance of CdS substrates for simultaneous CO_(2)reduction and aryl alcohol oxidation.Specifically,Au_(SA)can effectively lower the energy barrier for the CO_(2)→*COOH conversion,while Au_(C)can enhance the adsorption of alcohols and reduce the energy barrier for dehydrogenation.As a result,the Au_(SA)and Au_(C)co-loaded CdS show impressive overall photocatalytic CO_(2)conversion performance,achieving remarkable CO and BAD production rates of 4.43 and 4.71 mmol g^(−1)h^(−1),with the selectivities of 93%and 99%,respectively.More importantly,the solar-to-chemical conversion efficiency of Au_(SA+C)/CdS reaches 0.57%,which is over fivefold higher than the typical solar-to-biomass conversion efficiency found in nature(ca.0.1%).This study comprehensively describes the roles of different forms of atomically-dispersed metals and their synergistic effects in photocatalytic reactions,which is anticipated to pave a new avenue in energy and environmental applications. 展开更多
关键词 Photocatalysis Atomically-dispersed metal SINGLE-ATOM CO_(2)reduction Aryl alcohol oxidation
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Cu-Zn-based alloy/oxide interfaces for enhanced electroreduction of CO_(2) to C_(2+) products 被引量:5
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作者 Zi-Yang Zhang Hao Tian +3 位作者 Lei Bian Shi-Ze Liu Yuan Liu Zhong-Li Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第8期90-97,I0004,共9页
The electrochemical CO_(2)reduction reaction to produce multi-carbon(C_(2+)) hydrocarbons or oxygenate compounds is a promising route to obtain a renewable fuel of high energy density.However,producing C_(2+)at high c... The electrochemical CO_(2)reduction reaction to produce multi-carbon(C_(2+)) hydrocarbons or oxygenate compounds is a promising route to obtain a renewable fuel of high energy density.However,producing C_(2+)at high current densities is still a challenge.Herein,we develop a Cu-Zn alloy/Cu-Zn aluminate oxide composite electrocatalytic system for enhanced conversion of CO_(2)to C_(2+)products.The Cu-Zn-Al-Layered Double Hydroxide(LDH) is used as a precursor to decompose into uniform Cu-Zn oxide/Cu-Zn aluminate pre-catalyst.Under electrochemical reduction,Cu-Zn oxide generates Cu-Zn alloy while Cu-Zn aluminate oxide remains unchanged.The alloy and oxide are closely stacked and arranged alternately,and the aluminate oxide induces the strong electron interaction of Cu,Zn and Al,creating a large number of highly active reaction interfaces composed of 0 to+3 valence metal sites.With the help of the interface effect,the optimized Cu_(9)Zn_(1)/Cu_(0.8)Zn_(0.2)Al_(2)O_(4)catalyst achieves a Faradaic efficiency of 88.5% for C_(2+)products at a current density of 400 mA cm^(-2)at-1.15 V versus reversible hydrogen electrode.The in-situ Raman and attenuate total reflectance-infrared absorption spectroscopy(ATR-IRAS) spectra show that the aluminate oxide at the interface significantly enhances the adsorption and activation of CO_(2)and the dissociation of H2O and strengthens the adsorption of CO intermediates,and the alloy promotes the C-C coupling to produce C_(2+)products.This work provides an efficient strategy to construct highly active reaction interfaces for industrial-scale electrochemical CO_(2)RR. 展开更多
关键词 Electrochemical CO_(2)reduction reaction C_(2+)products Cu-Zn alloy Cu-Zn aluminate oxide Interface
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A core-shell copper oxides-cobalt oxides heterostructure nanowire arrays for nitrate reduction to ammonia with high yield rate 被引量:2
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作者 Hui Liu Jingsha Li +5 位作者 Feng Du Luyun Yang Shunyuan Huang Jingfeng Gao Changming Li Chunxian Guo 《Green Energy & Environment》 SCIE EI CAS CSCD 2023年第6期1619-1629,共11页
Electrochemical nitrate reduction to ammonia(NRA) can realize the green synthesis of ammonia(NH3) at ambient conditions, and also remove nitrate contamination in water. However, the current catalysts for NRA still fac... Electrochemical nitrate reduction to ammonia(NRA) can realize the green synthesis of ammonia(NH3) at ambient conditions, and also remove nitrate contamination in water. However, the current catalysts for NRA still face relatively low NH3yield rate and poor stability. We present here a core-shell heterostructure comprising cobalt oxide anchored on copper oxide nanowire arrays(CuO NWAs@Co_(3)O_(4)) for efficient NRA. The CuO NWAs@Co_(3)O_(4)demonstrates significantly enhanced NRA performance in alkaline media in comparison with plain CuO NWAs and Co_(3)O_(4)flocs. Especially, at-0.23 V vs. RHE, NH_(3) yield rate of the CuO NWAs@Co_(3)O_(4)reaches 1.915 mmol h^(-1)cm^(-2),much higher than those of CuO NWAs(1.472 mmol h^(-1)cm^(-2)), Co_(3)O_(4)flocs(1.222 mmol h^(-1)cm^(-2)) and recent reported Cu-based catalysts.It is proposed that the synergetic effects of the heterostructure combing atom hydrogen adsorption and nitrate reduction lead to the enhanced NRA performance. 展开更多
关键词 Electrocatalytic nitrate reduction Ammonia production Core–shell heterostructure Copper oxides nanowire arrays Cobalt oxidesflocs
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Activation of Transition Metal(Fe,Co and Ni)-Oxide Nanoclusters by Nitrogen Defects in Carbon Nanotube for Selective CO_(2) Reduction Reaction 被引量:1
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作者 Yi Cheng Jinfan Chen +7 位作者 Chujie Yang Huiping Wang Bernt Johannessen Lars Thomsen Martin Saunders Jianping Xiao Shize Yang San Ping Jiang 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第1期253-263,共11页
The electrochemical carbon dioxide reduction reaction(CO_(2)RR),which can produce value-added chemical feedstocks,is a proton-coupled-electron process with sluggish kinetics.Thus,highly efficient,cheap catalysts are u... The electrochemical carbon dioxide reduction reaction(CO_(2)RR),which can produce value-added chemical feedstocks,is a proton-coupled-electron process with sluggish kinetics.Thus,highly efficient,cheap catalysts are urgently required.Transition metal oxides such as CoO_(x),FeO_(x),and NiO_(x)are low-cost,low toxicity,and abundant materials for a wide range of electrochemical reactions,but are almost inert for CO_(2)RR.Here,we report for the first time that nitrogen doped carbon nanotubes(N-CNT)have a surprising activation effect on the activity and selectivity of transition metal-oxide(MO_(x)where M=Fe,Ni,and Co)nanoclusters for CO_(2)RR.MO_(x)supported on N-CNT,MO_(x)/N-CNT,achieves a CO yield of 2.6–2.8 mmol cm−2 min−1 at an overpotential of−0.55 V,which is two orders of magnitude higher than MO_(x)supported on acid treated CNTs(MO_(x)/O-CNT)and four times higher than pristine N-CNT.The faraday efficiency for electrochemical CO_(2)-to-CO conversion is as high as 90.3%at overpotential of 0.44 V.Both in-situ XAS measurements and DFT calculations disclose that MO_(x)nanoclusters can be hydrated in CO_(2)saturated KHCO_(3),and the N defects of N-CNT effectively stabilize these metal hydroxyl species under carbon dioxide reduction reaction conditions,which can split the water molecules and provide local protons to inhibit the poisoning of active sites under carbon dioxide reduction reaction conditions. 展开更多
关键词 activation effect electrochemical CO_(2)reduction reaction N defect proton-coupled electron transfer process transition metal oxide nanocluster
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Rapid and durable oxygen reduction reaction enabled by a perovskite oxide with self-cleaning surface
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作者 Shengli Pang Yifan Song +7 位作者 Meng Cui Xin Tang Chao Long Lingfeng Ke Gongmei Yang Ting Fang Yong Guan Chonglin Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第8期333-340,I0010,共9页
The growth of electrochemically inert segregation layers on the surface of solid oxide fuel cell cathodes has become a bottleneck restricting the development of perovskite-structured oxygen reduction catalysts.Here,we... The growth of electrochemically inert segregation layers on the surface of solid oxide fuel cell cathodes has become a bottleneck restricting the development of perovskite-structured oxygen reduction catalysts.Here,we report a new discovery in which enriched Ba and Fe ions on the near-surface of Nd_(1/2)Ba_(1/2)Co_(1/3)Fe_(1/3)Mn_(1/3)O_(3-δ)spontaneously agglomerate into dispersed Ba_(5)Fe_(2)O_(8) nanoparticles and maintain a highly active and durable perovskite structure on the surface.This unique surface selfcleaning phenomenon is related to the low average potential energy of Ba_(5)Fe_(2)O_(8),which is grown on the near-surface layer.The electrochemically inert Ba_(5)Fe_(2)O_(8) segregation layer on the near-surface of the perovskite catalyst achieves self-cleaning by regulating the formation energy of enriched metal oxides.This self-cleaned perovskite surface exhibits an ultrafast oxygen exchange rate,high catalytic activity for the oxygen reduction reaction,and good adaptability to the actual working conditions of solid oxide fuel cell stacks.This study paves a new way for overcoming the stubborn problem of perovskite catalyst surface deactivation and enriches the scientific knowledge of surface catalysis. 展开更多
关键词 Surface chemistry Energy materials ELECTROCATALYSIS Perovskite oxide Oxygen reduction reaction Solid oxide fuel cells
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Sub-2 nm mixed metal oxide for electrochemical reduction of carbon dioxide to carbon monoxide
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作者 Devina Thasia Wijaya Andi Haryanto +2 位作者 Hyun Woo Lim Kyoungsuk Jin Chan Woo Lee 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第9期303-310,共8页
Mixed metal oxide(MMO) represents a critical class of materials that can allow for obtaining a dynamic interface between its components:reduced metal and its metal oxide counterpart during an electrocatalytic reaction... Mixed metal oxide(MMO) represents a critical class of materials that can allow for obtaining a dynamic interface between its components:reduced metal and its metal oxide counterpart during an electrocatalytic reaction.Here,a synthetic method utilizing a MOF-derived micro/mesoporous carbon as a template to prepare sub-2 nm MMO catalysts for CO_(2) electro reduction is reported.Starting from the zeolite imidazolate framework(ZIF-8),the pyrolyzed derivatives were used to synthesize sub-2 nm Pd-Ni MMO with different compositions.The Ni-rich(Pd_(20)-Ni_(80)/ZC) catalyst exhibits unexpectedly superior performance for CO production with an improved Faradaic efficiency(FE) of 95.3% at the current density of 200 mA cm^(-2) at-0.56 V vs.reversible hydrogen electrode(RHE) compared to other Pd-Ni compositions.X-ray photoelectron spectroscopy(XPS) analysis confirms the presence of Ni^(2+) and Pd^(2+) in all compositions,demonstrating the presence of MMO.Density functional theory(DFT) calculation reveals that the lower CO binding energy on the surface of the Pd_(20)-Ni_(80) cluster eases CO desorption,thus increasing its production.This work provides a general synthetic strategy for MMO electrocatalysts and can pave a new way for screening multimetallic catalysts with a dynamic electrochemical interface. 展开更多
关键词 Carbon dioxide reduction Mixed metal oxide NANOALLOY Carbon monoxide Metal-organic framework
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Tuning the charge distribution and crystal field of iron single atoms via iron oxide integration for enhanced oxygen reduction reaction in zinc-air batteries
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作者 Feifei Zhang Yinlong Zhu +9 位作者 Yijun Zhong Jing Zou Yu Chen Lianhai Zu Zhouyou Wang Jack Jon Hinsch Yun Wang Lian Zhang Zongping Shao Huanting Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第10期154-163,I0006,共11页
Metal-air batteries face a great challenge in developing efficient and durable low-cost oxygen reduction reaction(ORR)electrocatalysts.Single-atom iron catalysts embedded into nitrogen doped carbon(Fe-N-C)have emerged... Metal-air batteries face a great challenge in developing efficient and durable low-cost oxygen reduction reaction(ORR)electrocatalysts.Single-atom iron catalysts embedded into nitrogen doped carbon(Fe-N-C)have emerged as attractive materials for potential replacement of Pt in ORR,but their catalytic performance was limited by the symmetrical electronic structure distribution around the single-atom Fe site.Here,we report our findings in significantly enhancing the ORR performance of Fe-N-C by moderate Fe_(2)O_(3) integration via the strong electronic interaction.Remarkably,the optimized catalyst(M-Fe_(2)O_(3)/Fe_(SA)@NC)exhibits excellent activity,durability and good tolerance to methanol,outperforming the benchmark Pt/C catalyst.When M-Fe_(2)O_(3)/Fe_(SA)@NC catalyst was used in a practical zinc-air battery assembly,peak power density of 155 mW cm^(-2)and specific capacity of 762 mA h g_(Zn)^(-1)were achieved and the battery assembly has shown superior cycling stability over a period of 200 h.More importantly,theoretical studies suggest that the introduction of Fe_(2)O_(3) can evoke the crystal field alteration and electron redistribution on single Fe atoms,which can break the symmetric charge distribution of Fe-N_(4) and thereby optimize the corresponding adsorption energy of intermediates to promote the O_(2)reduction.This study provides a new pathway to promote the catalytic performance of single-atom catalysts. 展开更多
关键词 Single-atom catalysts oxide nanoclusters Electronic interactions Oxygen reduction reaction Zn-air battery
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In operando-formed interface between silver and perovskite oxide for efficient electroreduction of carbon dioxide to carbon monoxide
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作者 Xinhao Wu Yanan Guo +11 位作者 Yuxing Gu Fenghua Xie Mengran Li Zhiwei Hu Hong-Ji Lin Chih-Wen Pao Yu-Cheng Huang Chung-Li Dong Vanessa KPeterson Ran Ran Wei Zhou Zongping Shao 《Carbon Energy》 SCIE CSCD 2023年第4期81-93,共13页
Electrochemical carbon dioxide(CO_(2))reduction(ECR)is a promising technology to produce valuable fuels and feedstocks from CO_(2).Despite large efforts to develop ECR catalysts,the investigation of the catalytic perf... Electrochemical carbon dioxide(CO_(2))reduction(ECR)is a promising technology to produce valuable fuels and feedstocks from CO_(2).Despite large efforts to develop ECR catalysts,the investigation of the catalytic performance and electrochemical behavior of complex metal oxides,especially perovskite oxides,is rarely reported.Here,the inorganic perovskite oxide Ag-doped(La_(0.8)Sr_(0.2))_(0.95)Ag_(0.05)MnO_(3-δ)(LSA0.05M)is reported as an efficient electrocatalyst for ECR to CO for the first time,which exhibits a Faradaic efficiency(FE)of 84.3%,a remarkable mass activity of 75Ag^(-1)(normalized to the mass of Ag),and stability of 130 h at a moderate overpotential of 0.79 V.The LSA0.05M catalyst experiences structure reconstruction during ECR,creating the in operando-formed interface between the perovskite and the evolved Ag phase.The evolved Ag is uniformly distributed with a small particle size on the perovskite surface.Theoretical calculations indicate the reconstruction of LSA0.05M during ECR and reveal that the perovskite-Ag interface provides adsorption sites for CO_(2) and accelerates the desorption of the*CO intermediate to enhance ECR.This study presents a novel high-performance perovskite catalyst for ECR andmay inspire the future design of electrocatalysts via the in operando formation of metal-metal oxide interfaces. 展开更多
关键词 electrochemical CO_(2)reduction faradaic efficiencies interfaces perovskite oxides
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Conversion of ferric oxide to magnetite by hydrothermal reduction in Bayer digestion process 被引量:4
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作者 李小斌 刘楠 +4 位作者 齐天贵 王一霖 周秋生 彭志宏 刘桂华 《Transactions of Nonferrous Metals Society of China》 SCIE EI CAS CSCD 2015年第10期3467-3474,共8页
Digesting aluminum-bearing minerals and converting ferric oxide to magnetite simultaneously in Bayer digestion process is crucially important to deal with high-iron diasporic bauxite economically for alumina productio... Digesting aluminum-bearing minerals and converting ferric oxide to magnetite simultaneously in Bayer digestion process is crucially important to deal with high-iron diasporic bauxite economically for alumina production.The reaction behaviors of hydrothermal reduction of ferric oxide in alkali solution were studied by both thermodynamic calculation and experimental investigation.The thermodynamic calculation indicates that Fe3O4 can be formed by the conversion of Fe2O3 at proper redox potentials in alkaline solution.The experimental results show that the formation ratio of Fe3O4 either through the reaction of Fe and Fe2O3 or through the reaction of Fe and H2O in alkaline aqueous solution increases remarkably with raising the temperature and alkali concentration,suggesting that Fe(OH)3- and Fe(OH)4- form by dissolving Fe and Fe2O3,respectively,in alkaline aqueous solution and further react to form Fe3O4.Moreover,aluminate ions have little influence on the hydrothermal reduction of Fe2O3 in alkaline aqueous solution,and converting iron minerals to magnetite can be realized in the Bayer digestion process of diasporic bauxite. 展开更多
关键词 Bayer process DIGESTION hydrothermal reduction ferric oxide MAGNETITE
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Catalytic reduction of SO_2 by CO over CeO_2-TiO_2 mixed oxides 被引量:5
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作者 张丽 秦毅红 +3 位作者 陈白珍 彭亚光 何汉兵 袁依 《Transactions of Nonferrous Metals Society of China》 SCIE EI CAS CSCD 2016年第11期2960-2965,共6页
The structure and catalytic desulfurization characteristics of CeO2-TiO2 mixed oxides were investigated by means ofX-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and catalytic activity tests. Acco... The structure and catalytic desulfurization characteristics of CeO2-TiO2 mixed oxides were investigated by means ofX-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and catalytic activity tests. According to the results, a CeO2-TiO2solid solution is formed when the mole ratio of cerium to titanium n(Ce):n(Ti) is 5:5 or greater, and the most suitable n(Ce):n(Ti) isdetermined as 7:3, over which the conversion rate of SO2 and the yield of sulfur at 500℃ reach 93% and 99%, respectively.According to the activity testing curve, Ce0.7Ti0.3O2 (n(Ce):n(Ti)=7:3) without any pretreatment can be gradually activated by reagentgas after about 10 min, and reaches a steady activation status 60 min later. The XPS results of Ce0.7Ti0.3O2 after different time ofSO2+CO reaction show that CeO2 is the active component that offers the redox couple Ce4+/Ce3+ and the labile oxygen vacancies, andTiO2 only functions as a catalyst structure stabilizer during the catalytic reaction process. After 48 h of catalytic reaction at 500℃,Ce0.7Ti0.3O2 still maintains a stable structure without being vulcanized, demonstrating its good anti-sulfur poisoning performance. 展开更多
关键词 CeO2-TiO2 mixed oxides solid solution catalytic reduction carbon monoxide sulfur dioxide
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Manganese extraction by reduction-acid leaching from low-grade manganese oxide ores using CaS as reductant 被引量:2
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作者 李昌新 钟宏 +3 位作者 王帅 薛建荣 武芳芳 张振宇 《Transactions of Nonferrous Metals Society of China》 SCIE EI CAS CSCD 2015年第5期1677-1684,共8页
The extraction of manganese from low-grade manganese oxide ores using Ca S derived from Ca SO4 as reductant was investigated. The effects of mass ratio of Ca S to ore, reduction temperature, reduction time, liquid to ... The extraction of manganese from low-grade manganese oxide ores using Ca S derived from Ca SO4 as reductant was investigated. The effects of mass ratio of Ca S to ore, reduction temperature, reduction time, liquid to solid ratio(L/S ratio), stirring speed, leaching temperature, leaching time and H2SO4 concentration on the leaching rates of Mn and Fe during the reduction–acid leaching process were discussed. The leaching rates of 96.47% for Mn and 19.24% for Fe were obtained under the optimized conditions of mass ratio of Ca S to manganese oxide ore 1:6.7, L/S ratio 5:1, stirring speed 300 r/min, reduction temperature of 95 °C for 2.0 h in the reduction process and leaching stirring speed of 200 r/min, H2SO4 concentration of 1.5 mol/L, leaching temperature of 80 °C for 5 min in the leaching process. In addition, this process can be employed in the recovery of manganese from various manganese oxide ores, and Mn leaching rate above 95% is obtained. 展开更多
关键词 MANGANESE manganese oxide ore calcium sulfide reduction LEACHING
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Acetic acid-assisted mild dealloying of fine CuPd nanoalloys achieving compressive strain toward high-efficiency oxygen reduction and ethanol oxidation electrocatalysis 被引量:5
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作者 Danye Liu Yu Zhang +5 位作者 Hui Liu Peng Rao Lin Xu Dong Chen Xinlong Tian Jun Yang 《Carbon Energy》 SCIE CSCD 2023年第7期112-120,共9页
Dealloying by which the transition metal is partially or completely leached from an alloy precursor is an effective way to optimize the fundamental effects for further enhancing the electrocatalysis of a catalyst.Here... Dealloying by which the transition metal is partially or completely leached from an alloy precursor is an effective way to optimize the fundamental effects for further enhancing the electrocatalysis of a catalyst.Herein,to address the deficiencies associated with the commonly used dealloying methods,for example,electrochemical and sulfuric acid/nitric acid treatment,we report an acetic acid-assisted mild strategy to dealloy Cu atoms from the outer surface layers of CuPd alloy nanoparticles to achieve high-efficiency electrocatalysis for oxygen reduction and ethanol oxidation in an alkaline electrolyte.The leaching of Cu atoms by acetic acid exerts an additional compressive strain effect on the surface layers and exposes more active Pd atoms,which is beneficial for boosting the catalytic performance of a dealloyed catalyst for the oxygen reduction reaction(ORR)and the ethanol oxidation reaction(EOR).In particular,for ORR,the CuPd nanoparticles with a Pd/Cu molar ratio of 2:1 after acetic dealloying show a half-wave potential of 0.912 V(vs.RHE)and a mass activity of 0.213 AmgPd^(-1) at 0.9 V,respectively,while for EOR,the same dealloyed sample has a mass activity and a specific activity of 8.4 Amg^(-1) and 8.23 mA cm^(-2),respectively,much better than their dealloyed counterparts at other temperatures and commercial Pd/C as well as a Pt/C catalyst. 展开更多
关键词 compressive strain effect DEALLOYING ELECTROCATALYSIS ethanol oxidation reaction oxygen reduction reaction
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Novel Perovskite Oxide Hybrid Nanofibers Embedded with Nanocatalysts for Highly Efficient and Durable Electrodes in Direct CO_(2) Electrolysis
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作者 Akromjon Akhmadjonov Kyung Taek Bae Kang Taek Lee 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第5期214-230,共17页
The unique characteristics of nanofibers in rational electrode design enable effec-tive utilization and maximizing material properties for achieving highly efficient and sustainable CO_(2) reduction reactions( CO_(2)R... The unique characteristics of nanofibers in rational electrode design enable effec-tive utilization and maximizing material properties for achieving highly efficient and sustainable CO_(2) reduction reactions( CO_(2)RRs)in solid oxide elec-trolysis cells(SOECs).However,practical appli-cation of nanofiber-based electrodes faces chal-lenges in establishing sufficient interfacial contact and adhesion with the dense electrolyte.To tackle this challenge,a novel hybrid nanofiber electrode,La_(0.6)Sr_(0.4)Co_(0.15)Fe_(0.8)Pd_(0.05)O_(3-δ)(H-LSCFP),is developed by strategically incorporating low aspect ratio crushed LSCFP nanofibers into the excess porous interspace of a high aspect ratio LSCFP nanofiber framework synthesized via electrospinning technique.After consecutive treatment in 100% H_(2) and CO_(2) at 700°C,LSCFP nanofibers form a perovskite phase with in situ exsolved Co metal nanocatalysts and a high concentration of oxygen species on the surface,enhancing CO_(2) adsorption.The SOEC with the H-LSCFP electrode yielded an outstanding current density of 2.2 A cm^(-2) in CO_(2) at 800°C and 1.5 V,setting a new benchmark among reported nanofiber-based electrodes.Digital twinning of the H-LSCFP reveals improved contact adhesion and increased reaction sites for CO_(2)RR.The present work demonstrates a highly catalytically active and robust nanofiber-based fuel electrode with a hybrid structure,paving the way for further advancements and nanofiber applications in CO_(2)-SOECs. 展开更多
关键词 NANOFIBERS Fuel electrodes Digital twinning CO_(2)reduction reaction Solid oxide electrolysis cells
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Conducting Polymer-Based e-Refinery for Sustainable Hydrogen Peroxide Production
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作者 Zhixing Wu Penghui Ding +7 位作者 Viktor Gueskine Robert Boyd Eric Daniel G■owacki Magnus Odén Xaνier Crispin Magnus Berggren Emma M.Björk Mikhail Vagin 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第2期334-342,共9页
Electrocatalysis enables the industrial transition to sustainable production of chemicals using abundant precursors and electricity from renewable sources.De-centralized production of hydrogen peroxide(H_(2)O_(2))from... Electrocatalysis enables the industrial transition to sustainable production of chemicals using abundant precursors and electricity from renewable sources.De-centralized production of hydrogen peroxide(H_(2)O_(2))from water and oxygen of air is highly desirable for daily life and industry.We report an effective electrochemical refinery(e-refinery)for H_(2)O_(2)by means of electrocatalysis-controlled comproportionation reaction(2_(H)O+o→2HO),feeding pure water and oxygen only.Mesoporous nickel(Ⅱ)oxide(NiO)was used as electrocatalyst for oxygen evolution reaction(OER),producing oxygen at the anode.Conducting polymer poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS)drove the oxygen reduction reaction(ORR),forming H_(2)O_(2)on the cathode.The reactions were evaluated in both half-cell and device configurations.The performance of the H_(2)O_(2)e-refinery,assembled on anion-exchange solid electrolyte and fed with pure water,was limited by the unbalanced ionic transport.Optimization of the operation conditions allowed a conversion efficiency of 80%. 展开更多
关键词 conducting polymer hydrogen peroxide nickel(Ⅱ)oxide oxygen evolution reaction oxygen reduction reaction
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Understanding the roles of Brønsted/Lewis acid sites on manganese oxide-zeolite hybrid catalysts for low-temperature NH_(3)-SCR
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作者 Hyun Sub Kim Hwangho Lee +2 位作者 Hongbeom Park Inhak Song Do Heui Kim 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第10期79-88,共10页
Although metal oxide-zeolite hybrid materials have long been known to achieve enhanced catalytic activity and selectivity in NO_(x)removal reactions through the inter-particle diffusion of intermediate species,their s... Although metal oxide-zeolite hybrid materials have long been known to achieve enhanced catalytic activity and selectivity in NO_(x)removal reactions through the inter-particle diffusion of intermediate species,their subsequent reaction mechanism on acid sites is still unclear and requires investigation.In this study,the distribution of Brønsted/Lewis acid sites in the hybrid materials was precisely adjusted by introducing potassium ions,which not only selectively bind to Brønsted acid sites but also potentially affect the formation and diffusion of activated NO species.Systematic in situ diffuse reflectance infrared Fourier transform spectroscopy analyses coupled with selective catalytic reduction of NO_(x)with NH_(3)(NH_(3)-SCR)reaction demonstrate that the Lewis acid sites over MnO_(x)are more active for NO reduction but have lower selectivity to N_(2)than Brønsted acids sites.Brønsted acid sites primarily produce N_(2),whereas Lewis acid sites primarily produce N_(2)O,contributing to unfavorable N_(2)selectivity.The Brønsted acid sites present in Y zeolite,which are stronger than those on MnO_(x),accelerate the NH_(3)-SCR reaction in which the nitrite/nitrate species diffused from the MnO_(x)particles rapidly convert into the N_(2).Therefore,it is important to design the catalyst so that the activated NO species formed in MnO_(x)diffuse to and are selectively decomposed on the Brønsted acid sites of H-Y zeolite rather than that of MnO_(x)particle.For the physically mixed H-MnO_(x)+H-Y sample,the abundant Brønsted/Lewis acid sites in H-MnO_(x)give rise to significant consumption of activated NO species before their inter-particle diffusion,thereby hindering the enhancement of the synergistic effects.Furthermore,we found that the intercalated K+in K-MnO_(x)has an unexpected favorable role in the NO reduction rate,probably owing to faster diffusion of the activated NO species on K-MnO_(x)than H-MnO_(x).This study will help to design promising metal oxide-zeolite hybrid catalysts by identifying the role of the acid sites in two different constituents. 展开更多
关键词 Hybrid metal oxide-zeolite The role of acid sites Manganese oxides Physical mixing Selective catalytic reduction of NOx with NH3
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Synthesis of a chabazite-supported copper catalyst with full mesopores for selective catalytic reduction of nitrogen oxides at low temperature 被引量:9
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作者 刘计省 刘坚 +4 位作者 赵震 宋卫余 韦岳长 段爱军 姜桂元 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第5期750-759,共10页
A series of meso‐microporous copper‐supporting chabazite molecular sieve(CuSAPO‐34) catalysts with excellent performance in low‐temperature ammonia selective catalytic reduction(NH3‐SCR)have been synthesized ... A series of meso‐microporous copper‐supporting chabazite molecular sieve(CuSAPO‐34) catalysts with excellent performance in low‐temperature ammonia selective catalytic reduction(NH3‐SCR)have been synthesized via a one‐pot hydrothermal crystallization method. The physicochemical properties of the catalysts were characterized by scanning electron microscopy, transmission electron microscopy, N2 adsorption‐desorption measurements, X‐ray diffraction, 27 Al magic angle spinning nuclear magnetic resonance, diffuse reflectance ultraviolet‐visible spectroscopy, inductively coupled plasma‐atomic emission spectroscopy, X‐ray photoelectron spectroscopy, temperature‐programmed reduction measurements, and electron paramagnetic resonance analysis. The formation of micro‐mesopores in the Cu‐SAPO‐34 catalysts decreases diffusion resistance and greatly improves the accessibility of reactants to catalytic active sites. The main active sites for NH3‐SCR reaction are the isolated Cu^2+ species displaced into the ellipsoidal cavity of the Cu‐SAPO‐34 catalysts. 展开更多
关键词 One-pot synthesis Meso-microporous Cu-SAPO-34 Low temperature Selective catalytic reduction Nitrogen oxides
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Metal-organic framework-based materials as key components in electrocatalytic oxidation and reduction reactions
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作者 Soheila Sanati Ali Morsali Hermenegildo García 《Journal of Energy Chemistry》 SCIE EI CSCD 2023年第12期540-567,I0014,共29页
Studies have extensively addressed the development of electrocatalytic technologies for energy storage and conversion,fuel production,and environmental protection.Electrode processes such as different oxidation and re... Studies have extensively addressed the development of electrocatalytic technologies for energy storage and conversion,fuel production,and environmental protection.Electrode processes such as different oxidation and reduction reactions play a vital and significant role in these technologies.In this regard,efficient,inexpensive,and stable electrocatalysts capable can significantly promote electrochemical reactions.Unique features of metal–organic frameworks(MOFs)such as their high porosity,tunable structure,size,and pore shape,high surface area,and redox properties have introduced them as an ideal electrocatalyst candidate.This review is thus aimed at elucidating the role of MOF-based materials(pristine,derivatives and composites)as efficient electrocatalysts in energy and sensing-related oxidation and reduction reactions such as oxygen reduction reaction(ORR),hydrogen oxidation reaction(HOR),carbon dioxide reduction reaction(CO_(2)RR),urea oxidation reaction(UOR),alcohol oxidation reaction(AOR),nitrogen reduction reaction(NRR),and glucose oxidation reaction(GOR)in advanced energy and sensing devices.Also,the structure–property relationship of the electrocatalyst was elaborated for each electrocatalytic reaction.Finally,perspectives on the potential research topics for practical use of MOF-based electrocatalysts are addressed.The present review can improve the interest in MOF-based electrocatalysts to study different oxidation and reduction reactions in energy and sensing systems. 展开更多
关键词 Metal-organic frameworks ELECTROCATALYST oxidation reaction reduction reaction
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