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A post-modification strategy to precisely construct dual-atom sites for oxygen reduction electrocatalysis
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作者 Juan Wang Xinyan Liu +9 位作者 Chang-Xin Zhao Yun-Wei Song Jia-Ning Liu Xi-Yao Li Chen-Xi Bi Xin Wan Jianglan Shui Hong-Jie Peng Bo-Quan Li Jia-Qi Huang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第3期511-517,I0012,共8页
Dual-atom catalysts(DACs) afford promising potential for oxygen reduction electrocatalysis due to their high atomic efficiency and high intrinsic activity.However,precise construction of dual-atom sites remains a chal... Dual-atom catalysts(DACs) afford promising potential for oxygen reduction electrocatalysis due to their high atomic efficiency and high intrinsic activity.However,precise construction of dual-atom sites remains a challenge.In this work,a post-modification strategy is proposed to precisely fabricate DACs for oxygen reduction electrocatalysis.Concretely,a secondary metal precursor is introduced to the primary single-atom sites to introduce direct metal-metal interaction,which ensures the formation of desired atom pair structure during the subsequent pyrolysis process and allows for successful construction of DACs.The as-prepared FeCo-NC DAC exhibits superior oxygen reduction electrocatalytic activity with a half-wave potential of 0,91 V vs.reversible hydrogen electrode.Zn-air batteries equipped with the FeCo-NC DAC demonstrate higher peak power density than those with the Pt/C benchmark.More importantly,this post-modification strategy is demonstrated universal to achieve a variety of dual-atom sites.This work presents an effective synthesis methodology for precise construction of catalytic materials and propels their applications in energy-related devices. 展开更多
关键词 Dual-atom catalysts electrocatalysis oxygen reduction reaction Post-modification Zinc–air batteries
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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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Inner-pore reduction nucleation of palladium nanoparticles in highly conductive wurster-type covalent organic frameworks for efficient oxygen reduction electrocatalysis 被引量:1
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作者 Weiwen Wang Lu Zhang +4 位作者 Tianping Wang Zhen Zhang Xiangnan Wang Chong Cheng Xikui Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第2期543-552,I0014,共11页
Covalent organic frameworks(COFs)have emerged as a class of promising supports for electrocatalysis because of their advantages including good crystallinity,highly ordered pores,and structural diversity.However,their ... Covalent organic frameworks(COFs)have emerged as a class of promising supports for electrocatalysis because of their advantages including good crystallinity,highly ordered pores,and structural diversity.However,their poor conductivity represents the main obstruction to their practical application.Here,we reported a novel synthesis strategy for synergistically endowing a triphenylamine-based COFs with improved electrical conductivity and excellent catalytic activity for oxygen reduction,via the in-situ redox deposition and confined growth of palladium nanoparticles inside the porous structure of COFs using reductive triphenylamine frameworks as reducing agent;meanwhile,the triphenylamine unit was oxidized to radical cation structure and affords radical cation COFs with conductivity as high as3.2*10^(-1) S m^(-1).Such a uniform confine palladium nanoparticle on highly conductive COFs makes it an efficient electrocatalyst for four-electron oxygen reduction reaction(4e-ORR),showing excellent activities and fast kinetics with a remarkable half-wave potential(E_(1/2))of 0.865 V and an ultralow Tafel slope of 39.7 mV dec^(-1) in alkaline media even in the absence of extra commercial conductive fillers.The generality of this strategy was proved by preparing the different metal and metal alloy nanoparticles supported on COFs(Au@COF,Pt@COF,AuPd@COF,AgPd@COF,and PtPd@COF)using reductive triphenylamine frameworks as reducing agent.This work not only provides a facile strategy for the fabrication of highly conductive COF supported ORR electrocatalysts,but also sheds new light on the practical application of Zn-air battery. 展开更多
关键词 Covalent organic frameworks Wurster-type structure In-situ reduction nucleation Palladium nanoparticles oxygen reduction electrocatalysis
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A cobalt(Ⅱ)porphyrin with a tethered imidazole for efficient oxygen reduction and evolution electrocatalysis 被引量:1
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作者 Xialiang Li Ping Li +10 位作者 Jindou Yang Lisi Xie Ni Wang Haitao Lei Chaochao Zhang Wei Zhang Yong-Min Lee Weiqiang Zhang Shunichi Fukuzumi Wonwoo Nam Rui Cao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第1期617-621,I0015,共6页
Electrocatalytic oxygen reduction and evolution reactions are involved in new energy conversion and storage technologies,such as various fuel cells and metal-air batteries and also water splitting devices[1,2].However... Electrocatalytic oxygen reduction and evolution reactions are involved in new energy conversion and storage technologies,such as various fuel cells and metal-air batteries and also water splitting devices[1,2].However,both reactions are very slow in kinetics,and thus catalysts are required[3,4]. 展开更多
关键词 Molecular electrocatalysis Cobalt porphyrin Axial ligand effect oxygen reduction reaction oxygen evolution reaction
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Scalable solid-phase synthesis of defect-rich graphene for oxygen reduction electrocatalysis 被引量:1
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作者 Chunxiao Dong Li Yang +4 位作者 Cheng Lian Xiaoling Yang Yihua Zhu Hongliang Jiang Chunzhong Li 《Green Energy & Environment》 SCIE EI CSCD 2023年第1期224-232,共9页
Defect-engineered carbon materials have been emerged as promising electrocatalysts for oxygen reduction reaction(ORR)in metal-air batteries.Developing a facile strategy for the preparation of highly active nanocarbon ... Defect-engineered carbon materials have been emerged as promising electrocatalysts for oxygen reduction reaction(ORR)in metal-air batteries.Developing a facile strategy for the preparation of highly active nanocarbon electrocatalysts remains challenging.Herein,a low-cost and simple route is developed to synthesize defective graphene by pyrolyzing the mixture of glucose and carbon nitride.Molecular dynamics simulations reveal that the graphene formation is ascribed to two-dimensional layered feature of carbon nitride,and high compatibility of carbon nitride/glucose systems.Structural measurements suggest that the graphene possesses rich edge and topological defects.The graphene catalyst exhibits higher power density than commercial Pt/C catalyst in a primary Zn-air battery.Combining experimental results and theoretical thermodynamic analysis,it is identified that graphitic nitrogen-modified topological defects at carbon framework edges are responsible for the decent ORR performance.The strategy presented in this work can be can be scaled up readily to fabricate defective carbon materials. 展开更多
关键词 Carbon materials electrocatalysis oxygen reduction reaction Solid-phase synthesis Zn-air battery
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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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Tin-mediated carbon-confined Pt_(3)Co ordered intermetallic nanoparticles as highly efficient and durable oxygen reduction electrocatalysts for rechargeable zinc-air batteries
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作者 Ruotao Yang Chuhan Dai +4 位作者 Laiwei Zhang Ruirui Wang Kui Yin Bo Liu Ziliang Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第11期169-179,共11页
The development of electrocatalysts for the oxygen reduction reaction(ORR) that bears high selectivity,exceptional activity,and long-term stability is crucial for advancing various green energy technologies.Intermetal... The development of electrocatalysts for the oxygen reduction reaction(ORR) that bears high selectivity,exceptional activity,and long-term stability is crucial for advancing various green energy technologies.Intermetallics composed of platinum and transition metals are considered to be promising candidates for this purpose.However,they typically face challenges such as unfavorable intrinsic activity and a propensity for particle aggregation,diminishing their ORR performance.Against this backdrop,we present our findings on a N-doped carbon confined Pt_(3)Co intermetallic doped with p-block metal tin(Pt_(3)Co_(x)Sn_(1-x)/NC).The introduction of Sn induces lattice strain due to its larger atomic size,which leads to the distortion of the Pt_(3)Co lattice structure,while the coupling of carbon polyhedra inhibits the particle aggregation.The optimized Pt_(3)Co_(0.8)Sn_(0.2)/NC catalyst demonstrates an impressive half-wave potential of 0.86 V versus RHE,surpassing both Pt_(3)Co/NC and Pt_(3)Sn/NC catalysts.Moreover,the Pt_(3)Co_(0.8)Sn_(0.2)/NC exhibits a mass-specific activity as high as 1.4 A mg_(Pt)^(-1),ranking it in the top level among the intermetallicsbased ORR electrocatalysts.When further employed as a cathode material in a self-assembled zinc-air battery,it shows stable operation for over 80 h.These results underscore the significant impact of lattice strain engineering through the strategic doping of p-block metal in the carbon-confined Pt_(3)Co intermetallic,thereby enhancing the catalytic efficiency for the ORR. 展开更多
关键词 Lattice strain Pt-based intermetallic N-doped carbon electrocatalysis oxygen reduction reaction
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Modulation of Electronic States in Bimetallic-doped Nitrogen-Carbon Based Nanoparticles for Enhanced Oxygen Reduction Kinetics
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作者 Chen Gong Chenyu Yang +2 位作者 Wanlin Zhou Hui Su Qinghua Liu 《Chinese Journal of Chemical Physics》 SCIE EI CAS CSCD 2024年第4期513-521,I0042-I0060,I0094,共29页
Controlling the local electronic structure of active ingredients to improve the adsorption desorption characteristics of oxygen-containing intermediates over the electrochemical liquid-solid interfaces is a critical c... Controlling the local electronic structure of active ingredients to improve the adsorption desorption characteristics of oxygen-containing intermediates over the electrochemical liquid-solid interfaces is a critical challenge in the field of oxygen reduction reaction(ORR)catalysis.Here,we offer a simple approach for modulating the electronic states of metal nanocrystals by bimetal co-doping into carbon-nitrogen substrate,allowing us to modulate the electronic structure of catalytic active centers.To test our strategy,we designed a typical bimetallic nanoparticle catalyst(Fe-Co NP/NC)to flexibly alter the reaction kinetics of ORR.Our results from synchrotron Xray absorption spectroscopy and X-ray photoelectron spectroscopy showed that the co-doping of iron and cobalt could optimize the intrinsic charge distribution of Fe-Co NP/NC catalyst,promoting the oxygen reduction kinetics and ultimately achieving remarkable ORR activity.Consequently,the carefully designed Fe-Co NP/NC exhibits an ultra-high kinetic current density at the operating voltage(71.94 mA/cm^(2)at 0.80 V),and the half-wave potential achieves 0.915 V,which is obviously better than that of the corresponding controls including Fe NP/NC,Co NP/NC.Our findings provide a unique perspective for optimizing the electronic structure of active centers to achieve higher ORR catalytic activity and faster kinetics. 展开更多
关键词 oxygen reduction reaction Reaction kinetics Electronic state modulation CODOPING electrocatalysis
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Multiatom activation of single-atom electrocatalysts via remote coordination for ultrahigh-rate two-electron oxygen reduction 被引量:3
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作者 Xiaoqing Liu Rui Chen +5 位作者 Wei Peng Lichang Yin De'an Yang Feng Hou Liqun Wang Ji Liang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第1期622-630,I0015,共10页
Electrocatalytic oxygen reduction via a two-electron pathway(2e^(-)-ORR)is a promising and eco-friendly route for producing hydrogen peroxide(H_(2)O_(2)).Single-atom catalysts(SACs)typically show excellent selectivity... Electrocatalytic oxygen reduction via a two-electron pathway(2e^(-)-ORR)is a promising and eco-friendly route for producing hydrogen peroxide(H_(2)O_(2)).Single-atom catalysts(SACs)typically show excellent selectivity towards 2e^(-)-ORR due to their unique electronic structures and geometrical configurations.The very low density of single-atom active centers,however,often leads to unsatisfactory H_(2)O_(2)yield rate,significantly inhibiting their practical feasibility.Addressing this,we herein introduce fluorine as a secondary doping element into conventional SACs,which does not directly coordinate with the singleatom metal centers but synergize with them in a remote manner.This strategy effectively activates the surrounding carbon atoms and converts them into highly active sites for 2e^(-)-ORR.Consequently,a record-high H_(2)O_(2)yield rate up to 27 mol g^(-1)h^(-1)has been achieved on the Mo–F–C catalyst,with high Faradaic efficiency of 90%.Density functional theory calculations further confirm the very kinetically facile 2e^(-)-ORR over these additional active sites and the superiority of Mo as the single-atom center to others.This strategy thus not only provides a high-performance electrocatalyst for 2e^(-)-ORR but also should shed light on new strategies to significantly increase the active centers number of SACs. 展开更多
关键词 Hydrogen peroxide oxygen reduction reaction Two-electron pathway Remote coordination electrocatalysis
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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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Pd nanoparticles embedded in N-Enriched MOF-Derived architectures for efficient oxygen reduction reaction in alkaline media
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作者 Daqiang Yan Lin Zhang +3 位作者 Lei Shen Runyu Hu Weiping Xiao Xiaofei Yang 《Green Energy & Environment》 SCIE EI CAS CSCD 2023年第4期1205-1215,共11页
Developing high efficient Pd-based electrocatalysts for oxygen reduction reaction(ORR) is still challenging for alkaline membrane fuel cell,since the strong oxygen adsorption energy and easy agglomerative intrinsic pr... Developing high efficient Pd-based electrocatalysts for oxygen reduction reaction(ORR) is still challenging for alkaline membrane fuel cell,since the strong oxygen adsorption energy and easy agglomerative intrinsic properties. In order to simultaneously solve these problems, Pd/Co_(3)O_(4)–N–C multidimensional materials with porous structures is designed as the ORR catalysts. In details, the ZIF-67 with polyhedral structure was firstly synthesized and then annealed at high-temperature to prepare the N-doped Co_(3)O_(4)carbon-based material, which was used to homogeneously confine Pd nanoparticles and obtained the Pd/Co_(3)O_(4)–N–C series catalysts. The formation of Co–N and C–N bond could provide efficient active sites for ORR. Simultaneously, the strong electronic interaction in the interface between the Pd and N-doped Co_(3)O_(4)could disperse and avoid the agglomeration of Pd nanoparticles and ensure the exposure of active sites, which is crucial to lower the energy barrier toward ORR and substantially enhance the ORR kinetics. Hence, the Pd/Co_(3)O_(4)–N–C nanocompounds exhibited excellent ORR catalytic performance, ideal Pd mass activity, and durability in 0.1 mol L-1KOH solution compared with Co_(3)O_(4)–N–C and Pd/C. The scalable synthesis method, relatively low cost, and excellent electrochemical ORR performance indicated that the obtained Pd/Co_(3)O_(4)–N–C electrocatalyst had the potential for application on fuel cells. 展开更多
关键词 oxygen reduction reaction electrocatalysis Pd/Co_(3)O_(4)–N–C Carbon-based materials Co–N and C–N bond
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Controlling of coordination state of Ru_(x)N_(y) clusters for efficient oxygen reduction electrocatalysis
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作者 Weiyang Fu Yihuan Yu +3 位作者 Tongtong Liu Yinliang Cao Zhengping Zhang Feng Wang 《Nano Research》 SCIE EI CSCD 2024年第3期1035-1041,共7页
Ruthenium(Ru)is an attractive potential alternative to platinum as an electrocatalyst for the oxygen reduction reaction(ORR),in virtue of its high catalytic selectivity and relatively low price.In this work,a series o... Ruthenium(Ru)is an attractive potential alternative to platinum as an electrocatalyst for the oxygen reduction reaction(ORR),in virtue of its high catalytic selectivity and relatively low price.In this work,a series of well-dispersed nitrogen-coordinated Ru-clusters on carbon black(Ru_(x)N_(y)/C)were prepared by pyrolyzing different Ru-containing sandwich compounds as the Ru sources.The higher thermal stability of these complexed sandwich precursors(bis(1,2,3,4,5-pentamethylcyclopentadienyl)Ru(II)monomer,dichloro(p-cymene)Ru(II)dimer,and chloro(1,2,3,4,5-pentamethylcyclopentadienyl)Ru(II)tetramer)affords the control of coordinated state for the resulting Ru-clusters,in comparison of that derived from ruthenium chlorides.After the pyrolysis treatment,the Ru coordinated state in Ru_(x)N_(y)/C,with the Ru–N and Ru–Ru bonds,still showed the structural inheritance from the Ru(II)monomer,dimer,and tetramer,but using ruthenium chlorides as the Ru source resulted in the nanoscale Ru agglomerations.The ORR testing exhibited that the Ru_(x)N_(y)/C sample derived from the Ru(II)tetramer(Ru_(x)N_(y)/C-T)presents the higher catalytic activity than the other obtained samples in either alkaline or acidic electrolytes.Even in the acidic electrolyte,Ru_(x)N_(y)/C-T shows the comparable ORR activity to that of Pt/C catalysts,and it shows the superior tolerance against methanol and CO.The X-ray absorption spectroscopy and density functional theory calculations demonstrate that these tetra-nuclear Ru-clusters could be the most active site due to their broadened d-orbital bands and lower energy d-band center than those of other subnano species and nanocrystals,and their favorable Yeager-type adsorption of O_(2)-molecules is also contributed to promoting O–O bond cleavage and accelerating the ORR process. 展开更多
关键词 ruthenium clusters coordination environment sandwich compounds electrocatalysis oxygen reduction reaction
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Oxygen reduction electrocatalysis:From conventional to single-atomic platinum-based catalysts for proton exchange membrane fuel cells
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作者 Cheng YUAN Shiming ZHANG Jiujun ZHANG 《Frontiers in Energy》 SCIE EI CSCD 2024年第2期206-222,共17页
Platinum(Pt)-based materials are still the most efficient and practical catalysts to drive the sluggish kinetics of cathodic oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs).However,their c... Platinum(Pt)-based materials are still the most efficient and practical catalysts to drive the sluggish kinetics of cathodic oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs).However,their catalysis and stability performance still need to be further improved in terms of corrosion of both carbon support and Pt catalyst particles as well as Pt loading reduction.Based on the developed synthetic strategies of alloying/nanostructuring Pt particles and modifying/innovating supports in developing conventional Pt-based catalysts,Pt single-atom catalysts(Pt SACs)as the recently burgeoning hot materials with a potential to achieve the maximum utilization of Pt are comprehensively reviewed in this paper.The design thoughts and synthesis of various isolated,alloyed,and nanoparticlecontained Pt SACs are summarized.The single-atomic Pt coordinating with non-metals and alloying with metals as well as the metal-support interactions of Pt single-atoms with carbon/non-carbon supports are emphasized in terms of the ORR activity and stability of the catalysts.To advance further research and development of Pt SACs for viable implementation in PEMFCs,various technical challenges and several potential research directions are outlined. 展开更多
关键词 oxygen reduction electrocatalysis Pt singleatom catalysts conventional Pt-based catalysts design thoughts and synthesis metal-support interactions
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Fabrication of a highly dispersed Pd_(core)@Pt_(shell) electrocatalyst for the oxygen reduction reaction
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作者 曹龙生 蒋尚峰 +4 位作者 张耕 唐雪君 秦晓平 邵志刚 衣宝廉 《Chinese Journal of Catalysis》 CSCD 北大核心 2017年第7期1196-1206,共11页
Core-shell nanostructures have been widely investigated to improve the electrocatalytic perfor-mance of platinum. However, organic precursors, surfactants or high temperature are usually nec-essary during the prepa... Core-shell nanostructures have been widely investigated to improve the electrocatalytic perfor-mance of platinum. However, organic precursors, surfactants or high temperature are usually nec-essary during the preparation procedure. Unfortunately, these requirements limit the application of these methods on a large scale. Herein, a Pdcore@ Pt shell nanostructure was fabricated through the reduction of fcPtCU by dissociated hydrogen at room temperature without the assistance o f either a surfactant or a high-boiling point solvent. The shell thickness of this nanostructure was successfully controlled by varying the amount of fcPtCU; core-shell nanoparticles with a shell thickness of 0.45, 0.75 and 0.90 nm w ere obtained, as determined by TEM. The remarkable crystallinity and epitaxial growth of the Pdcore@ Pt shell nanostructure were revealed by HRTEM and EDS. According to ICP and XPS, surface segregation of Pt was established. The impressive ORR performance was attributed to the weak adsorption strength of the OHads species, which resulted from the electron transfer impact between the Pdcore and Ptshell. The facile and clean preparation method can be used to prepare other core-shell nanostructures under a mild atmosphere. 展开更多
关键词 Pdcore@Pt shell Dissociated hydrogen oxygen reduction electrocatalysis Core shell
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Hydrothermal synthesis of titanium-supported nanoporous palladium-copper electrocatalysts for formic acid oxidation and oxygen reduction reaction
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作者 易清风 肖兴中 刘云清 《Transactions of Nonferrous Metals Society of China》 SCIE EI CAS CSCD 2013年第4期1184-1190,共7页
Nanoporous Pd and binary Pd-Cu particles were prepared by a hydrothermal method using ethylene glycol as a reduction agent and they were directly immobilized on Ti substrates named as Ti-supported Pd-based catalysts. ... Nanoporous Pd and binary Pd-Cu particles were prepared by a hydrothermal method using ethylene glycol as a reduction agent and they were directly immobilized on Ti substrates named as Ti-supported Pd-based catalysts. Their electrocatalytic activity for formic acid oxidation and oxygen reduction reaction (ORR) in alkaline media was examined by voltammetric techniques. Among the as-prepared catalysts, nanoPdslCu19/Ti catalyst presents the highest current density of 39.8 mA/cm2 at -0.5 V or 66.4 mA/cm2 at -0.3 V for formic acid oxidation. The onset potential of ORR on the nanoPdslCU19/Ti catalyst presents an about 70 mV positive shift compared to that on the nanoPd/Ti, and the current density of ORR at -0.3 V is 2.12 mA/cm2, which is 3.7 times larger than that on the nanoPd/Ti. 展开更多
关键词 Pd electrode Pd-Cu electrode formic acid oxidation oxygen reduction reaction NANOPARTICLE electrocatalysis
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Rare earth alloy nanomaterials in electrocatalysis 被引量:1
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作者 Yifei Li Xilin Yuan +5 位作者 Ping Wang Lulin Tang Miao He Pangen Li Jiang Li Zhenxing Li 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第8期574-594,I0014,共22页
With the rapid development of society and economy, the excessive consumption of fossil energy has led to the global energy and environment crisis. In order to explore the sustainable development of new energy, researc... With the rapid development of society and economy, the excessive consumption of fossil energy has led to the global energy and environment crisis. In order to explore the sustainable development of new energy, research based on electrocatalysis has attracted extensive attention in the academic circle. The main challenge in this field is to develop nano-catalysts with excellent electrocatalytic activity and selectivity for target products. The state of the active site in catalyst plays a decisive role in the activity and selectivity of the reaction. In order to design efficient and excellent catalysts, it is an effective means to adjust the electronic structure of catalysts. Electronic effects are also called ligand effects. By alloying with rare earth(RE) elements, electrons can be redistributed between RE elements and transition metal elements, achieving accurate design of the electronic structure of the active site in the alloy. Because of the unique electronic structure of RE, it has been paid attention in the field of catalysis. The outermost shell structure of RE elements is basically the same as that of the lower shell, except that the number of electrons in the 4f orbital is different, but the energy level is similar, so their properties are very similar. When RE elements form compounds, both the f electrons in the outermost shell and the d electrons in the lower outer shell can participate in bonding. In addition, part of the 4f electrons in the third outer shell can also participate in bonding.In order to improve the performance of metal catalysts, alloying provides an effective method to design advanced functional materials. RE alloys can integrate the unique electronic structure and catalytic behavior of RE elements into metal materials, which not only provides an opportunity to adjust the electronic structure and catalytic activity of the active component, but also enhances the structural stability of the alloy and is expected to significantly improve the catalytic performance of the catalyst. From the perspective of electronic and catalytic activity, RE elements have unique electronic configuration and lanthanide shrinkage effect. Alloying with RE elements will make the alloy have more abundant electronic structure, activity, and spatial arrangement, effectively adjusting the reaction kinetics of the electrochemical process of the catalyst. In this paper, the composition,structure, synthesis of RE alloys and their applications in the field of electrocatalysis are summarized, including the hydrogen evolution reaction, the oxygen evolution reaction, the oxygen reduction reaction, the methanol oxidation reaction, the ethanol oxidation reaction, and other catalytic reactions. At the same time, the present challenges of RE alloy electrocatalytic materials are summarized and their future development direction is pointed out. In the field of electrocatalysis, the cost of catalyst is too high and the stability is not strong. Therefore, the testing process should be related to the actual application, and the test method should be standardized, so as to carry forward the field of electrocatalysis. 展开更多
关键词 Rare earth Alloy nanomaterials electrocatalysis Preparation methods Hydrogen evolution reaction oxygen reduction reaction Methanol oxidation reaction Ethanol oxidation reaction
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Oxygen vacancy enhancing mechanism of nitrogen reduction reaction property in Ru/TiO2 被引量:11
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作者 Shan Cheng Yi-Jing Gao +7 位作者 Yi-Long Yan Xu Gao Shao-Hua Zhang Gui-Lin Zhuang Sheng-Wei Deng Zhong-Zhe Wei Xing Zhong Jian-Guo Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2019年第12期144-151,共8页
To search the new effective nitrogen reduction reaction(NRR)electrocatalyst is very important for the ammonia-based industry.Herein,we reported the design of a novel NRR electrocatalyst with Ru NPs loaded on oxygen-va... To search the new effective nitrogen reduction reaction(NRR)electrocatalyst is very important for the ammonia-based industry.Herein,we reported the design of a novel NRR electrocatalyst with Ru NPs loaded on oxygen-vacancy TiO2(Ru/TiO2-Vo).Structural characterizations revealed that oxygen vacancy was loaded in the matrix of Ru/TiO2-Vo.Electrocatalytic results indicated that Ru/TiO2-Vo showed good NRR performance(2.11μg h^-1 cm^-2).Contrast tests showed that NRR property of Ru/TiO2-Vo was much better than those of Ru/TiO-12(B)(0.53μg hcm^-2)and Ru/P25(0.42μg h^-1 cm^-2).Furthermore,density functional theory calculation results indicated catalytic mechanism of NRR and rate-determining step(*N2+1/2 H2→*N+*NH)was the potential-determining step with the overpotential requirement of 0.21 V.A combination of electronic structure analysis and catalytic measurement shed light on the synergistic effect of Ru and oxygen vacancy on the NRR performance. 展开更多
关键词 Nitrogen reduction reaction electrocatalysis oxygen vacancy DFT
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Creation of Triple Hierarchical Micro-Meso-Macroporous N-doped Carbon Shells with Hollow Cores Toward the Electrocatalytic Oxygen Reduction Reaction 被引量:11
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作者 Ruohao Xing Tingsheng Zhou +4 位作者 Yao Zhou Ruguang Ma Qian Liu Jun Luo Jiacheng Wang 《Nano-Micro Letters》 SCIE EI CAS 2018年第1期20-33,共14页
A series of triple hierarchical micro-mesomacroporous N-doped carbon shells with hollow cores have been successfully prepared via etching N-doped hollow carbon spheres with CO_2 at high temperatures.The surface areas,... A series of triple hierarchical micro-mesomacroporous N-doped carbon shells with hollow cores have been successfully prepared via etching N-doped hollow carbon spheres with CO_2 at high temperatures.The surface areas, total pore volumes and microporepercentages of the CO_2-activated samples evidently increase with increasing activation temperature from 800 to950 °C, while the N contents show a contrary trend from7.6 to 3.8 at%. The pyridinic and graphitic nitrogen groups are dominant among various N-containing groups in the samples. The 950 °C-activated sample(CANHCS-950) has the largest surface area(2072 m^2 g^(-1)), pore volume(1.96 cm^3 g^(-1)), hierarchical micro-mesopore distributions(1.2, 2.6 and 6.2 nm), hollow macropore cores(*91 nm)and highest relative content of pyridinic and graphitic N groups. This triple micro-meso-macropore system could synergistically enhance the activity because macropores could store up the reactant, mesopores could reduce the transport resistance of the reactants to the active sites, and micropores could be in favor of the accumulation of ions.Therefore, the CANHCS-950 with optimized structure shows the optimal and comparable oxygen reduction reaction(ORR) activity but superior methanol tolerance and long-term durability to commercial Pt/C with a 4 e--dominant transfer pathway in alkaline media. These excellent properties in combination with good stability and recyclability make CANHCSs among the most promising metal-free ORR electrocatalysts reported so far in practical applications. 展开更多
关键词 Hierarchical pores Hollow cores N doping electrocatalysis oxygen reduction reaction
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Recent developments in electrocatalysts and future prospects for oxygen reduction reaction in polymer electrolyte membrane fuel cells 被引量:8
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作者 Maryam Kiani Jie Zhang +5 位作者 Yan Luo Chunping Jiang Jinlong Fan Gang Wang Jinwei Chen Ruilin Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2018年第4期1124-1139,共16页
The main difficulty in the extensive commercial use of polymer electrolyte membrane fuel cells (PEMFCs) is the use of noble metals such as Pt-based electrocatalyst at the cathode, which is essential to ease the oxyg... The main difficulty in the extensive commercial use of polymer electrolyte membrane fuel cells (PEMFCs) is the use of noble metals such as Pt-based electrocatalyst at the cathode, which is essential to ease the oxygen reduction reaction (ORR) in fuel cells (FCs). To eliminate the high loading of Pt-based electrocatalysts to minimize the cost, extensive study has been carried out over the previous decades on the non-noble metal catalysts. Development in enhancing the ORR performance of FCs is mainly due to the doped carbon materials, Fe and Co-based electrocatalysts, these materials could be considered as probable substitutes for Pt-based catalysts. But the stability of these non-noble metal electrocatalysts is low and the durability of these metals remains unclear. The three basic reasons of instability are: (i) oxidative occurrence by H2O2, (ii) leakage of the metal site and (iii) protonation by probable anion adsorption of the active site. Whereas leakage of the metal site has been almost solved, more work is required to understand and avoid losses from oxidative attack and protonation. The ORR performance such as stability tests are usually run at low current densities and the lifetime is much shorter than desired need. Therefore, improvement in the ORR activity and stability afe the key issues of the non-noble metal electrocatalyst. Based on the consequences obtained in this area, numerous future research directions are projected and discussed in this paper. Hence, this review is focused on improvement of stability and durability of the non-noble metal electrocatalyst. 展开更多
关键词 Non-noble metal electrocatalysts Polymer electrolyte membrane fuel cells(PEMFCs) oxygen reduction reaction(ORR) electrocatalysis Stability
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Facile synthesis of Mo2C nanoparticles on N-doped carbon nanotubes with enhanced electrocatalytic activity for hydrogen evolution and oxygen reduction reactions 被引量:3
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作者 Yue-Jun Song Jin-Tao Ren +3 位作者 Gege Yuan Yali Yao Xinying Liu Zhong-Yong Yuan 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2019年第11期68-77,共10页
Developing low-cost and highly-efficient electrocatalysts for renewable energy conversion technologies has attracted even-increasing attention. Molybdenum carbide materials have recently emerged as a type of promising... Developing low-cost and highly-efficient electrocatalysts for renewable energy conversion technologies has attracted even-increasing attention. Molybdenum carbide materials have recently emerged as a type of promising catalysts for electrocatalytic reactions due to the earth-abundance and Pt-resembled electrical properties. In this work, taking the advantage of the interaction between the basic groups of the Mo(VI)-melamine polymer and the acidic groups on the surface of the oxidized carbon nanotubes(CNTs), N-doped CNTs supported Mo2C nanoparticles(Mo2C/NCNT) are prepared, which exhibit outstanding electrocatalytic activity and durability for both the hydrogen evolution and oxygen reduction reactions. The impressive performance of Mo2C/NCNT can be attributed to the small size of Mo2C particles, the large exposure ratio of surface sites and the presence of N-doped CNTs. This work enlarges the multi-field applications of molybdenum carbide-base materials as promising non-precious metal electrocatalysts, which is of great significance for sustainable energy-related technologies. 展开更多
关键词 N-DOPING Carbon NANOTUBES Molybdenum carbides Hydrogen evolution REACTION oxygen reduction REACTION electrocatalysis
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