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Precision tuning of highly efficient Pt-based ternary alloys on nitrogen-doped multi-wall carbon nanotubes for methanol oxidation reaction
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作者 Xingqun Zheng Zhengcheng Wang +3 位作者 Qian Zhou Qingmei Wang Wei He Shun Lu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第1期242-251,I0006,共11页
The electrochemical methanol oxidation is a crucial reaction in the conversion of renewable energy.To enable the widespread adoption of direct methanol fuel cells(DMFCs),it is essential to create and engineer catalyst... The electrochemical methanol oxidation is a crucial reaction in the conversion of renewable energy.To enable the widespread adoption of direct methanol fuel cells(DMFCs),it is essential to create and engineer catalysts that are both highly effective and robust for conducting the methanol oxidation reaction(MOR).In this work,trimetallic PtCoRu electrocatalysts on nitrogen-doped carbon and multi-wall carbon nanotubes(PtCoRu@NC/MWCNTs)were prepared through a two-pot synthetic strategy.The acceleration of CO oxidation to CO_(2) and the blocking of CO reduction on adjacent Pt active sites were attributed to the crucial role played by cobalt atoms in the as-prepared electrocatalysts.The precise control of Co atoms loading was achieved through precursor stoichiometry.Various physicochemical techniques were employed to analyze the morphology,element composition,and electronic state of the catalyst.Electrochemical investigations and theoretical calculations confirmed that the Pt_(1)Co_(3)Ru_(1)@NC/MWCNTs exhibit excellent electrocatalytic performance and durability for the process of MOR.The enhanced MOR activity can be attributed to the synergistic effect between the multiple elements resulting from precisely controlled Co loading content on surface of the electrocatalyst,which facilitates efficient charge transfer.This interaction between the multiple components also modifies the electronic structures of active sites,thereby promoting the conversion of intermediates and accelerating the MOR process.Thus,achieving precise control over Co loading in PtCoRu@NC/MWCNTs would enable the development of high-performance catalysts for DMFCs. 展开更多
关键词 Ternary alloys ELECTROCATALYSTS Methanol oxidation reaction Electron transfer Theoretical calculations
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Boosted Electrocatalytic Glucose Oxidation Reaction on Noble-Metal-Free MoO_(3)-Decorated Carbon Nanotubes
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作者 Yu-Long Men Ning Dou +3 位作者 Yiyi Zhao Yan Huang Lei Zhang Peng Liu 《Transactions of Tianjin University》 EI CAS 2024年第1期63-73,共11页
Electrocatalytic glucose oxidation reaction(GOR)has attracted much attention owing to its crucial role in biofuel cell fabrication.Herein,we load MoO_(3)nanoparticles on carbon nanotubes(CNTs)and use a discharge proce... Electrocatalytic glucose oxidation reaction(GOR)has attracted much attention owing to its crucial role in biofuel cell fabrication.Herein,we load MoO_(3)nanoparticles on carbon nanotubes(CNTs)and use a discharge process to prepare a noblemetal-free MC-60 catalyst containing MoO_(3),Mo_(2)C,and a Mo_(2)C–MoO_(3)interface.In the GOR,MC-60 shows activity as high as 745μA/(mmol/L cm^(2)),considerably higher than those of the Pt/CNT(270μA/(mmol/L cm^(2)))and Au/CNT catalysts(110μA/(mmol/L cm^(2))).In the GOR,the response minimum on MC-60 is as low as 8μmol/L,with a steady-state response time of only 3 s.Moreover,MC-60 has superior stability and anti-interference ability to impurities in the GOR.The better performance of MC-60 in the GOR is attributed to the abundant Mo sites bonding to C and O atoms at the MoO_(3)–Mo_(2)C interface.These Mo sites create active sites for promoting glucose adsorption and oxidation,enhancing MC-60 performance in the GOR.Thus,these results help to fabricate more effi cient noble-metal-free catalysts for the fabrication of glucose-based biofuel cells. 展开更多
关键词 Interface eff ect ELECTROCATALYSIS Molybdenum oxide GLUCOSE Oxidation reaction
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General approach for atomically dispersed precious metal catalysts toward hydrogen reaction 被引量:2
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作者 Ruisong Li Daoxiong Wu +8 位作者 Peng Rao Peilin Deng Jing Li Junming Luo Wei Huang Qi Chen Zhenye Kang Yijun Shen Xinlong Tian 《Carbon Energy》 SCIE CSCD 2023年第7期100-111,共12页
As a carbon-free energy carrier,hydrogen has become the pivot for future clean energy,while efficient hydrogen production and combustion still require precious metal-based catalysts.Single-atom catalysts(SACs)with hig... As a carbon-free energy carrier,hydrogen has become the pivot for future clean energy,while efficient hydrogen production and combustion still require precious metal-based catalysts.Single-atom catalysts(SACs)with high atomic utilization open up a desirable perspective for the scale applications of precious metals,but the general and facile preparation of various precious metal-based SACs remains challenging.Herein,a general movable printing method has been developed to synthesize various precious metal-based SACs,such as Pd,Pt,Rh,Ir,and Ru,and the features of highly dispersed single atoms with nitrogen coordination have been identified by comprehensive characterizations.More importantly,the synthesized Pt-and Ru-based SACs exhibit much higher activities than their corresponding nanoparticle counterparts for hydrogen oxidation reaction and hydrogen evolution reaction(HER).In addition,the Pd-based SAC delivers an excellent activity for photocatalytic hydrogen evolution.Especially for the superior mass activity of Ru-based SACs toward HER,density functional theory calculations confirmed that the adsorption of the hydrogen atom has a significant effect on the spin state and electronic structure of the catalysts. 展开更多
关键词 hydrogen evolution reaction hydrogen oxidation reaction photocatalytic hydrogen evolution reaction precious metals single-atom catalysts
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Studies on the Preparation of Bioactive Oligomerstilbene by Oxidative Coupling Reaction(Ⅰ)-Preparation of Shegansu B using Silver Oxide as Oxidant
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作者 Li Xin ZHOU Mao LIN(Institute of Materia Medica,Chinese Academy of Medical Sciences,Peking Union Medical College, Beijing 100050) 《Chinese Chemical Letters》 SCIE CAS CSCD 2000年第6期515-516,共2页
篢he oxidative coupling reaction of isorhapontigenin using sliver oxide as oxidant afforded a major product, named shegansu B(2), which was isolated from the roots of Belamcanda chinensis (L.)DC. Both the natural ... 篢he oxidative coupling reaction of isorhapontigenin using sliver oxide as oxidant afforded a major product, named shegansu B(2), which was isolated from the roots of Belamcanda chinensis (L.)DC. Both the natural and synthetic Shegansu B have the same potent antagonism activities of leukotriene B4,D4 receptor. 展开更多
关键词 ISORHAPONTIGENIN oligomerstilbene shegansu B oxidative coupling reaction silver oxide
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RuO_(2)-PdO nanowire networks with rich interfaces and defects supported on carbon toward the efficient alkaline hydrogen oxidation reaction
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作者 Yuanyuan Cong Fanchao Meng +5 位作者 Haibin Wang Di Dou Qiuping Zhao Chunlei Li Ningshuang Zhang Junying Tian 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第8期255-263,I0008,共10页
Interfacial engineering is a promising approach for enhancing electrochemical performance,but rich and efficient interfacial active sites remain a challenge in fabrication.Herein,RuO_(2)-PdO heterostructure nanowire n... Interfacial engineering is a promising approach for enhancing electrochemical performance,but rich and efficient interfacial active sites remain a challenge in fabrication.Herein,RuO_(2)-PdO heterostructure nanowire networks(NWs) with rich interfaces and defects supported on carbon(RuO_(2)-PdO NWs/C) for alkaline hydrogen oxidation reaction(HOR) was formed by a seed induction-oriented attachment-thermal treatment method for the first time.As expected,the RuO_(2)-PdO NWs/C(72.8% Ru atomic content in metal) exhibits an excellent activity in alkaline HOR with a mass specific exchange current density(jo,m) of 1061 A gRuPd-1,which is 3.1 times of commercial Pt/C and better than most of the reported nonPt noble metal HOR electrocatalysts.Even at the high potential(~0.5 V vs.RHE) or the presence of CO(5 vol%),the RuO_(2)-PdO NWs/C still effectively catalyzes the alkaline HOR.Structure/electrochemical analysis and theoretical calculations reveal that the interfaces between RuO_(2) and PdO act as the active sites.The electronic interactions between the two species and the rich defects for the interfacial active sites weaken the adsorption of Had,also strengthen the adsorption of OHad,and accelerate the alkaline HOR process.Moreover,OHadon RuO_(2) can spillover to the interfaces,keeping the RuO_(2)-PdO NWs/C with the stable current density at higher potential and high resistance to CO poisoning. 展开更多
关键词 Hydrogen oxidation reaction HETEROSTRUCTURE Nanowire networks DEFECTS Interfacial active sites
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Optimized Electronic Modification of S-Doped CuO Induced by Oxidative Reconstruction for Coupling Glycerol Electrooxidation with Hydrogen Evolution
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作者 Ruo‑Yao Fan Xue‑Jun Zhai +6 位作者 Wei‑Zhen Qiao Yu‑Sheng Zhang Ning Yu Na Xu Qian‑Xi Lv Yong‑Ming Chai Bin Dong 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第10期622-637,共16页
Glycerol(electrochemical) oxidation reaction(GOR) producing organic small molecule acid and coupling with hydrogen evolution reaction is a critical aspect of ensuring balanced glycerol capacity and promoting hydrogen ... Glycerol(electrochemical) oxidation reaction(GOR) producing organic small molecule acid and coupling with hydrogen evolution reaction is a critical aspect of ensuring balanced glycerol capacity and promoting hydrogen generation on a large scale. However, the development of highly efficient and selective non-noble metal-based GOR electrocatalysts is still a key problem. Here, an S-doped CuO nanorod array catalyst(S-CuO/CF) constructed by sulfur leaching and oxidative remodeling is used to drive GOR at low potentials: It requires potentials of only 1.23 and 1.33 V versus RHE to provide currents of 100 and 500 mA cm^(-2), respectively. Moreover, it shows satisfactory comprehensive performance(at 100 mA cm^(-2), V_(cell) = 1.37 V) when assembled as the anode in asymmetric coupled electrolytic cell. Furthermore, we propose a detailed cycle reaction pathway(in alkaline environment) of S-doped CuO surface promoting GOR to produce formic acid and glycolic acid. Among them, the C–C bond breaking and lattice oxygen deintercalation steps frequently involved in the reaction pathway are the key factors to determine the catalytic performance and product selectivity. This research provides valuable guidance for the development of transition metal-based electrocatalysts for GOR and valuable insights into the glycerol oxidation cycle reaction pathway. 展开更多
关键词 Glycerol oxidation reaction(GOR) Hydrogen evolution reaction(HER) CUO oxidative reconstruction Electronic modification
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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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Efficient solar fuel production enabled by an iodide oxidation reaction on atomic layer deposited MoS_(2)
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作者 Young Sun Park Gyumin Jang +12 位作者 Inkyu Sohn Hyungsoo Lee Jeiwan Tan Juwon Yun Sunihl Ma Jeongyoub Lee Chan Uk Lee Subin Moon Hayoung Im Seung-Min Chung Seungho Yu Hyungjun Kim Jooho Moon 《Carbon Energy》 SCIE EI CAS CSCD 2023年第12期200-214,共15页
Oxygen evolution reaction(OER)as a half-anodic reaction of water splitting hinders the overall reaction efficiency owing to its thermodynamic and kinetic limitations.Iodide oxidation reaction(IOR)with low thermodynami... Oxygen evolution reaction(OER)as a half-anodic reaction of water splitting hinders the overall reaction efficiency owing to its thermodynamic and kinetic limitations.Iodide oxidation reaction(IOR)with low thermodynamic barrier and rapid reaction kinetics is a promising alternative to the OER.Herein,we present a molybdenum disulfide(MoS_(2))electrocatalyst for a high-efficiency and remarkably durable anode enabling IOR.MoS_(2)nanosheets deposited on a porous carbon paper via atomic layer deposition show an IOR current density of 10 mA cm^(–2)at an anodic potential of 0.63 V with respect to the reversible hydrogen electrode owing to the porous substrate as well as the intrinsic iodide oxidation capability of MoS_(2)as confirmed by theoretical calculations.The lower positive potential applied to the MoS_(2)-based heterostructure during IOR electrocatalysis prevents deterioration of the active sites on MoS_(2),resulting in exceptional durability of 200 h.Subsequently,we fabricate a two-electrode system comprising a MoS_(2)anode for IOR combined with a commercial Pt@C catalyst cathode for hydrogen evolution reaction.Moreover,the photovoltaic–electrochemical hydrogen production device comprising this electrolyzer and a single perovskite photovoltaic cell shows a record-high current density of 21 mA cm^(–2)at 1 sun under unbiased conditions. 展开更多
关键词 iodide oxidation reaction molybdenum sulfide photovoltaic-electrochemical hydrogen production solar hydrogen
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Microwave-assisted exploration of the electron configuration-dependent electrocatalytic urea oxidation activity of 2D porous NiCo_(2)O_(4) spinel
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作者 Jun Wan Zhiao Wu +11 位作者 Guangyu Fang Jinglin Xian Jiao Dai Jiayue Guo Qingxiang Li Yongfei You Kaisi Liu Huimin Yu Weilin Xu Huiyu Jiang Minggui Xia Huanyu Jin 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第4期226-235,共10页
Urea holds promise as an alternative water-oxidation substrate in electrolytic cells.High-valence nickelbased spinel,especially after heteroatom doping,excels in urea oxidation reactions(UOR).However,traditional spine... Urea holds promise as an alternative water-oxidation substrate in electrolytic cells.High-valence nickelbased spinel,especially after heteroatom doping,excels in urea oxidation reactions(UOR).However,traditional spinel synthesis methods with prolonged high-temperature reactions lack kinetic precision,hindering the balance between controlled doping and highly active two-dimensional(2D)porous structures design.This significantly impedes the identification of electron configuration-dependent active sites in doped 2D nickel-based spinels.Herein,we present a microwave shock method for the preparation of 2D porous NiCo_(2)O_(4)spinel.Utilizing the transient on-off property of microwave pulses for precise heteroatom doping and 2D porous structural design,non-metal doping(boron,phosphorus,and sulfur)with distinct extranuclear electron disparities serves as straightforward examples for investigation.Precise tuning of lattice parameter reveals the impact of covalent bond strength on NiCo_(2)O_(4)structural stability.The introduced defect levels induce unpaired d-electrons in transition metals,enhancing the adsorption of electron-donating amino groups in urea molecules.Simultaneously,Bode plots confirm the impact mechanism of rapid electron migration caused by reduced band gaps on UOR activity.The prepared phosphorus-doped 2D porous NiCo_(2)O_(4),with optimal electron configuration control,outperforms most reported spinels.This controlled modification strategy advances understanding theoretical structure-activity mechanisms of high-performance 2D spinels in UOR. 展开更多
关键词 2D materials SPINEL Microwave ELECTROCATALYSIS Urea oxidation reaction
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Interfacial Electronic Modulation of Dual-Monodispersed Pt–Ni_(3)S_(2) as Efficacious Bi-Functional Electrocatalysts for Concurrent H_(2) Evolution and Methanol Selective Oxidation
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作者 Qianqian Zhao Bin Zhao +7 位作者 Xin Long Renfei Feng Mohsen Shakouri Alisa Paterson Qunfeng Xiao Yu Zhang Xian‑Zhu Fu Jing‑Li Luo 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第4期415-431,共17页
Constructing the efficacious and applicable bifunctional electrocatalysts and establishing out the mechanisms of organic electro-oxidation by replacing anodic oxygen evolution reaction(OER) are critical to the develop... Constructing the efficacious and applicable bifunctional electrocatalysts and establishing out the mechanisms of organic electro-oxidation by replacing anodic oxygen evolution reaction(OER) are critical to the development of electrochemicallydriven technologies for efficient hydrogen production and avoid CO_(2) emission. Herein, the hetero-nanocrystals between monodispersed Pt(~ 2 nm) and Ni_(3)S_(2)(~ 9.6 nm) are constructed as active electrocatalysts through interfacial electronic modulation, which exhibit superior bi-functional activities for methanol selective oxidation and H_(2) generation. The experimental and theoretical studies reveal that the asymmetrical charge distribution at Pt–Ni_(3)S_(2) could be modulated by the electronic interaction at the interface of dual-monodispersed heterojunctions, which thus promote the adsorption/desorption of the chemical intermediates at the interface. As a result, the selective conversion from CH_(3)OH to formate is accomplished at very low potentials(1.45 V) to attain 100 m A cm^(-2) with high electronic utilization rate(~ 98%) and without CO_(2) emission. Meanwhile, the Pt–Ni_(3)S_(2) can simultaneously exhibit a broad potential window with outstanding stability and large current densities for hydrogen evolution reaction(HER) at the cathode. Further, the excellent bi-functional performance is also indicated in the coupled methanol oxidation reaction(MOR)//HER reactor by only requiring a cell voltage of 1.60 V to achieve a current density of 50 m A cm^(-2) with good reusability. 展开更多
关键词 Dual-monodispersed heterostructure Electronic interactive modulation reaction mechanism Methanol oxidation reaction Hydrogen generation
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Metastable face-centered cubic ruthenium-based binary alloy for efficient alkaline hydrogen oxidation electrocatalysis
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作者 Yunbo Li Jianchao Yue +3 位作者 Chaoyi Yang Hongnan Jia Hengjiang Cong Wei Luo 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第5期207-215,共9页
Metastable nanostructured electrocatalyst with a completely different surface environment compared to conventional phase-based electrocatalyst often shows distinctive catalytic property.Although Ru-based electrocataly... Metastable nanostructured electrocatalyst with a completely different surface environment compared to conventional phase-based electrocatalyst often shows distinctive catalytic property.Although Ru-based electrocatalysts have been widely investigated toward hydrogen oxidation reaction(HOR)under alkaline electrolytes,these studies are mostly limited to conventional hexagonal-close-packed(hcp)phase,mainly arising from the lack of sufficient synthesis strategies.In this study,we report the precise synthesis of metastable binary RuW alloy with face-centered-cubic(fcc)phase.We find that the introduction of W can serve as fcc phase seeds and reduce the formation energy of metastable fcc-RuW alloy.Impressively,fcc-RuW exhibits remarkable alkaline HOR performance and stability with the activity of 0.67 mA cm_(Ru)^(-2)which is almost five and three times higher than that of hcp-Ru and commercial Pt/C,respectively,which is attributed to the optimized binding strength of adsorbed hydroxide intermediate derived from tailored electronic structure through W doping and phase engineering.Moreover,this strategy can also be applied to synthesize other metastable fcc-RuCr and fcc-RuMo alloys with enhanced HOR performances. 展开更多
关键词 Hydrogen oxidation reaction Metastable phase Face-centered cubic(fcc) Ru Phase engineering
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Pyridinic-N doping carbon layers coupled with tensile strain of FeNi alloy for activating water and urea oxidation
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作者 Guangfu Qian Wei Chen +5 位作者 Jinli Chen Li Yong Gan Tianqi Yu Miaojing Pan Xiaoyan Zhuo Shibin Yin 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第4期684-694,共11页
Exploitation of oxygen evolution reaction(OER)and urea oxidation reaction(UOR)catalysts with high activity and stability at large current density is a major challenge for energy-saving H_(2) production in water electr... Exploitation of oxygen evolution reaction(OER)and urea oxidation reaction(UOR)catalysts with high activity and stability at large current density is a major challenge for energy-saving H_(2) production in water electrolysis.Herein,we use the pyridinic-N doping carbon layers coupled with tensile strain of FeNi alloy activated by NiFe_(2)O_(4)(FeNi/NiFe_(2)O_(4)@NC)for efficiently increasing the performance of water and urea oxidation.Due to the tensile strain effect on FeNi/NiFe_(2)O_(4)@NC,it provides a favorable modulation on the electronic properties of the active center,thus enabling amazing OER(η_(100)=196 mV)and UOR(E_(10)=1.32 V)intrinsic activity.Besides,the carbon-coated layers can be used as armor to prevent FeNi alloy from being corroded by the electrolyte for enhancing the OER/UOR stability at large current density,showing high industrial practicability.This work thus provides a simple way to prepare high-efficiency catalyst for activating water and urea oxidation. 展开更多
关键词 Carbon-encapsulated Tensile strain Catalyst Oxygen evolution reaction Urea oxidation reaction
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Electron-distribution control via Pt/NC and MoC/NC dual junction:Boosted hydrogen electro-oxidation and theoretical study
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作者 Feng Zhou Xiaofeng Ke +8 位作者 Yihuang Chen Mei Zhao Yun Yang Youqing Dong Chao Zou Xi’an Chen Huile Jin Lijie Zhang Shun Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第1期513-520,I0011,共9页
The scarcity,high cost and susceptibility to CO of Platinum severely restrict its application in alkaline hydrogen oxidation reaction(HOR).Hybridizing Pt with other transition metals provides an effective strategy to ... The scarcity,high cost and susceptibility to CO of Platinum severely restrict its application in alkaline hydrogen oxidation reaction(HOR).Hybridizing Pt with other transition metals provides an effective strategy to modulate its catalytic HOR performance,but at the cost of mass activity due to the coverage of modifiers on Pt surface.Herein,we constructed dual junctions'Pt/nitrogen-doped carbon(Pt/NC)andδ-MoC/NC to modify electronic structure of Pt via interfacial electron transfer to acquire Pt-MoC@NC catalyst with electron-deficient Pt nanoparticles,simultaneously endowing it with high mass activity and durability of alkaline HOR.Moreover,the unique structure of Pt-MoC@NC endows Pt with a high COtolerance at 1,000 ppm CO/H_(2),a quality that commercial Pt-C catalyst lacks.The theoretical calculations not only confirm the diffusion of electrons from Pt/NC to Mo C/NC could occur,but also demonstrate the negative shift of Pt d-band center for the optimized binding energies of*H,*OH and CO. 展开更多
关键词 Hydrogen oxidation reaction Dual junctions CO-tolerance PLATINUM
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Asymmetric configuration activating lattice oxygen via weakening d-p orbital hybridization for efficient C/N separation in urea overall electrolysis
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作者 Chongchong Liu Peifang Wang +3 位作者 Bin Hu Xiaoli Liu Rong Huang Gang Zhou 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第5期233-239,共7页
Urea oxidation reaction(UOR)is proposed as an exemplary half-reaction in renewable energy applications because of its low thermodynamical potential.However,challenges persist due to sluggish reaction kinetics and comp... Urea oxidation reaction(UOR)is proposed as an exemplary half-reaction in renewable energy applications because of its low thermodynamical potential.However,challenges persist due to sluggish reaction kinetics and complex by-products separation.To this end,we introduce the lattice oxygen oxidation mechanism(LOM),propelling a novel UOR route using a modified CoFe layered double hydroxide(LDH)catalyst termed CFRO-7.Theoretical calculations and in-situ characterizations highlight the activated lattice oxygen(O_(L))within CFRO-7 as pivotal sites for UOR,optimizing the reaction pathway and accelerating the kinetics.For the urea overall electrolysis application,the LOM route only requires a low voltage of 1.54 V to offer a high current of 100 mA cm^(-2) for long-term utilization(>48 h).Importantly,the by-product NCO^(-)−is significantly suppressed,while the CO_(2)2/N_(2) separation is efficiently achieved.This work proposed a pioneering paradigm,invoking the LOM pathway in urea electrolysis to expedite reaction dynamics and enhance product selectivity. 展开更多
关键词 Lattice oxygen Urea oxidation reaction Overall electrolysis Products selectivity
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Engineering hierarchical quaternary superstructure of an integrated MOF-derived electrode for boosting urea electrooxidation assisted water electrolysis
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作者 Jianjun Tian Changsheng Cao +3 位作者 Yingchun He Muhammad Imran Khan Xin-Tao Wu Qi-Long Zhu 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第4期695-701,共7页
Controllable design of the catalytic electrodes with hierarchical superstructures is expected to improve their electrochemical performance.Herein,a self-supported integrated electrode(NiCo-ZLDH/NF)with a unique hierar... Controllable design of the catalytic electrodes with hierarchical superstructures is expected to improve their electrochemical performance.Herein,a self-supported integrated electrode(NiCo-ZLDH/NF)with a unique hierarchical quaternary superstructure was fabricated through a self-sacrificing template strategy from the metal–organic framework(Co-ZIF-67)nanoplate arrays,which features an intriguing well-defined hierarchy when taking the unit cells of the NiCo-based layered double hydroxide(NiCo-LDH)as the primary structure,the ultrathin LDH nanoneedles as the secondary structure,the mesoscale hollow plates of the LDH nanoneedle arrays as the tertiary structure,and the macroscale three-dimensional frames of the plate arrays as the quaternary structure.Notably,the distinctive structure of NiCo-ZLDH/NF can not only accelerate both mass and charge transfer,but also expose plentiful accessible active sites with high intrinsic activity,endowing it with an excellent electrochemical performance for urea oxidation reaction(UOR).Specially,it only required the low potentials of 1.335,1.368 and 1.388 V to deliver the current densities of 10,100 and 200 mA cm^(-2),respectively,much superior to those for typical NiCo-LDH.Employing NiCo-ZLDH/NF as the bifunctional electrode for both anodic UOR and cathodic HER,an energy-saving electrolysis system was further explored which can greatly reduce the needed voltage of 213 mV to deliver the current density of 100 mA cm^(-2),as compared to the conventional water electrolysis system composed of OER.This work manifests that it is prospective to explore the hierarchically nanostructured electrodes and the innovative electrolytic technologies for high-efficiency electrocatalysis. 展开更多
关键词 Hierarchical superstructures Metal–organic frameworks Layered double hydroxides Urea oxidation reaction Hydrogen evolution reaction
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Atomically dispersed Ni electrocatalyst for superior urea-assisted water splitting
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作者 Fang Luo Shuyuan Pan +3 位作者 Yuhua Xie Chen Li Yingjie Yu Zehui Yang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第3期1-6,I0002,共7页
Urea oxidation reaction(UOR) has been selected as substitution for oxygen evolution reaction ascribing to its low thermodynamic voltage as well as utilization of nickel as electrocatalyst.Herein,we report the formatio... Urea oxidation reaction(UOR) has been selected as substitution for oxygen evolution reaction ascribing to its low thermodynamic voltage as well as utilization of nickel as electrocatalyst.Herein,we report the formation of nickel single atoms(Ni-SAs) as exceptional bifunctional electrocatalyst toward UOR and hydrogen evolution reaction(HER) in urea-assisted water splitting.In UOR catalysis,Ni-SAs perform a superior catalytic performance than Ni-NP/NC and Pt/C ascribing to the formation of HOO-Ni-N_(4) structure evidenced by in-situ Raman spectroscopy,corresponding to a boosted mass activity by 175-fold at 1.4 V vs.RHE than Ni-NP/NC.Furthermore,Ni-SAs requires only 450 mV overpotential to obtain HER current density of 500 mA cm^(-2).136 mA cm^(-2) is achieved in urea-assisted water splitting at1.7 V for Ni-SAs,boosted by 5.7 times than Pt/C-IrO_(2) driven water splitting. 展开更多
关键词 Urea oxidation reaction Hydrogen evolution reaction Nickel single atoms Water splitting
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Rational design ternary platinum based electrocatalysts for effective methanol oxidation reaction 被引量:3
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作者 Hao Tian Daoxiong Wu +9 位作者 Jing Li Junming Luo Chunman Jia Zhongxin Liu Wei Huang Qi Chen Chong Michael Shim Peilin Deng Yijun Shen Xinlong Tian 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第7期230-235,I0007,共7页
Exploring effective, durable, and affordable electrocatalysts of methanol oxidation reaction(MOR) is of vital significance for the industrial application of direct methanol fuel cells. Herein, an efficient, general,an... Exploring effective, durable, and affordable electrocatalysts of methanol oxidation reaction(MOR) is of vital significance for the industrial application of direct methanol fuel cells. Herein, an efficient, general,and expandable method is developed to synthesis two-dimensional(2D) ternary Pt Bi M nanoplates(NPLs), in which various M(Co, Ni, Cu, Zn, Sn) is severed as the third component to the binary Pt Bi system. The MOR performance of Pt Bi M NPLs is entirely investigated, demonstrating that both the MOR activity and durability is enhanced with the introduction of the additional composition. Pt3Bi3Zn NPLs shows much higher MOR activity and stability than that of the Pt Bi counterparts, not to mention the current advanced Pt Ru/C and Pt/C catalysts. The prominent performances are attributed to the modulated electronic structure of the surface Pt in Pt Bi NPLs by the addition of Zn, resulting in a weakened affination between Pt and the adsorbed poisoning species(mainly CO) compared with Pt Bi NPLs, verified by density functional theory(DFT) calculations. In addition, the absorbed OH can be generated on the surface of Zn atom due to its favorable water activation properties, thus the CO removal on the adjacent Pt atoms is accelerated, further leading to a high activity and anti-poisoning performance of the resulting Pt_(3)Bi_(3)Zn catalyst. This work provides new insights and robust strategy for highly efficient MOR electrocatalyst with extraordinary anti-poisoning performance and stability. 展开更多
关键词 Fuel cells Ternary nanoplates DURABILITY Methanol oxidation reaction Anti-poisoning
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Recent advances in alkaline hydrogen oxidation reaction 被引量:3
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作者 Lixin Su Dan Gong +2 位作者 Yiming Jin Dean Wu Wei Luo 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第3期107-122,I0004,共17页
The development of highly efficient electrocatalysts toward hydrogen oxidation reaction(HOR)under alkaline media is essential for the commercialization of alkaline exchange membrane fuel cells(AEMFCs).However,the HOR ... The development of highly efficient electrocatalysts toward hydrogen oxidation reaction(HOR)under alkaline media is essential for the commercialization of alkaline exchange membrane fuel cells(AEMFCs).However,the HOR kinetics in alkaline is two to three orders of magnitude slower than that in acid.More critically,fundamental understanding of the sluggish kinetics derived from the p H effect is still debatable.In this review,the recent development of understanding HOR mechanism and rational design of advanced HOR electrocatalysts are summarized.First,recent advances in the theories focusing on fundamental understandings of HOR under alkaline electrolyte are comprehensively discussed.Then,from the aspect of intermediates binding energy,optimizing hydrogen binding energy(HBE)and increasing hydroxyl binding energy(OHBE),the strategies for designing efficient alkaline HOR catalysts are summarized.At last,perspectives for the future research on alkaline HOR are pointed out. 展开更多
关键词 Hydrogen oxidation reaction Hydrogen evolution reaction Alkaline electrolyte AEMFC Binding energy
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Nitrogen vacancies enriched Ce-doped Ni_(3)N hierarchical nanosheets triggering highly-efficient urea oxidation reaction in urea-assisted energy-saving electrolysis 被引量:2
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作者 Meng Li Xiaodong Wu +6 位作者 Kun Liu Yifan Zhang Xuechun Jiang Dongmei Sun Yawen Tang Kai Huang Gengtao Fu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第6期506-515,I0014,共11页
Urea oxidation reaction (UOR),which has favorable thermodynamic energy barriers compared with oxygen evolution reaction (OER),can provide more cost-effective electrons for the renewable energy systems,but is trapped b... Urea oxidation reaction (UOR),which has favorable thermodynamic energy barriers compared with oxygen evolution reaction (OER),can provide more cost-effective electrons for the renewable energy systems,but is trapped by its sluggish UOR kinetics and intricate reaction intermediates formation/desorption process.Herein,we report a novel and effective electrocatalyst consisting of carbon cloth supported nitrogen vacancies-enriched Ce-doped Ni_(3)N hierarchical nanosheets (Ce-Ni_(3)N @CC) to optimize the flat-footed UOR kinetics,especially the stiff rate-determine CO_(2)desorption step of UOR.Upon the introduction of valance state variable Ce,the resultant nitrogen vacancies enriched Ce-Ni_(3)N @CC exhibits an enhanced UOR performance where the operation voltage requires only 1.31 V to deliver the current density of 10 mA cm^(-2),which is superior to that of Ni_(3)N @CC catalyst (1.36 V) and other counterparts.Density functional theory (DFT) results demonstrate that the incorporation of Ce in Ni_(3)N lowers the formation energy of nitrogen vacancies,resulting in rich nitrogen vacancies in Ce-Ni_(3)N @CC.Moreover,the nitrogen vacancies together with Ce doping optimize the local charge distribution around Ni sites,and balance the adsorption energy of CO_(2)in the rate-determining step (RDS),as well as affect the initial adsorption structure of urea,leading to the superior UOR catalytic performance of Ce-Ni_(3)N @CC.When integrating the Ce-Ni_(3)N catalyst in UOR//HER and UOR//CO_(2)R flow electrolyzer,both of them perform well with low operation voltage and robust long-term stability,proofing that the thermodynamically favorable UOR can act as a suitable substitute anodic reaction compared with that of OER.Our findings here not only provide a novel UOR catalyst but also offer a promising design strategy for the future development of energy-related devices. 展开更多
关键词 Rare earth cerium Nickel nitride Nitrogen vacancies Charge redistribution Urea oxidation reaction
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Improved hydrogen oxidation reaction under alkaline conditions by Au–Pt alloy nanoparticles 被引量:2
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作者 Lijuan Lu Lishan Peng +3 位作者 Li Li Jing Li Xun Huang Zidong Wei 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2020年第1期52-56,I0003,共6页
This work demonstrates the outstanding performance of alloyed Au1 Pt1 nanoparticles on hydrogen oxidation reaction(HOR)in alkaline solution.Due to the weakened hydrogen binding energy caused by uniform incorporation o... This work demonstrates the outstanding performance of alloyed Au1 Pt1 nanoparticles on hydrogen oxidation reaction(HOR)in alkaline solution.Due to the weakened hydrogen binding energy caused by uniform incorporation of Au,the alloyed Au1Pt1/C nanoparticles exhibit superior HOR activity than commercial PtRu/C.On the contrary,the catalytic performance of the phase-segregated Au2Pt1/C and Au1Pt1/C bimetallic nanoparticles in HOR is significantly worse.Moreover,Au1Pt1/C shows a remarkable durability with activity dropping only 4% after 3000 CV cycles,while performance attenuation of commercial PtRu/C is high up to 15% under the same condition.Our results indicate that the alloyed Au1Pt1/C is a promising candidate to substitute commercial PtRu/C for hydrogen oxidation reaction in alkaline electrolyte. 展开更多
关键词 Hydrogen oxidation reaction Pt-Au alloy NANOPARTICLES Alkaline electrolyte
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