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Boosted Electrocatalytic Glucose Oxidation Reaction on Noble-Metal-Free MoO_(3)-Decorated Carbon Nanotubes 被引量:1
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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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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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Revealing interfacial charge redistribution of homologous Ru-RuS_(2) heterostructure toward robust hydrogen oxidation reaction
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作者 Yi Liu Lianrui Cheng +5 位作者 Shuqing Zhou Yuting Yang Chenggong Niu Tayirjan Taylor Isimjan Bao Wang Xiulin Yang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第7期332-339,共8页
Precisely tailoring the surface electronic structures of electrocatalysts for optimal hydrogen binding energy and hydroxide binding energy is vital to improve the sluggish kinetics of hydrogen oxidation reac-tion(HOR)... Precisely tailoring the surface electronic structures of electrocatalysts for optimal hydrogen binding energy and hydroxide binding energy is vital to improve the sluggish kinetics of hydrogen oxidation reac-tion(HOR).Herein,we employ a partial desulfurization strategy to construct a homologous Ru-RuS_(2) heterostructure anchored on hollow mesoporous carbon nanospheres(Ru-RuS_(2)@C).The disparate work functions of the heterostructure contribute to the spontaneous formation of a unique built-in electric field,accelerating charge transfer and boosting conductivity of electrocatalyst.Consequently,Ru-RuS_(2)@C exhibits robust HOR electrocatalytic activity,achieving an exchange current density and mass activity as high as 3.56 mA cm^(-2) and 2.13 mAμg_(Ru)^(-1),respectively.exceeding those of state-of-the-art Pt/C and most contemporary Ru-based HOR electrocatalysts.Surprisingly,Ru-RuS_(2)@C can tolerate 1000 ppm of cO that lacks in Pt/C.Comprehensive analysis reveals that the directional electron transfer across Ru-RuS_(2) heterointerface induces local charge redistribution in interfacial region,which optimizes and balances the adsorption energies of H and OH species,as well as lowers the energy barrier for water formation,thereby promoting theHoR performance. 展开更多
关键词 HETEROSTRUCTURE Hollow spherical structure Hydrogen oxidation reaction Charge redistribution Density functional calculation
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Theoretical investigations on CO oxidation reaction catalyzed by gold nanoparticles 被引量:2
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作者 孙科举 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第10期1608-1618,共11页
It is crucial to understand the mechanism of low temperature CO oxidation reaction catalyzed by gold nanoparticles so as to find out the origin of the high catalytic reactivity and extend the indus‐trialization appli... It is crucial to understand the mechanism of low temperature CO oxidation reaction catalyzed by gold nanoparticles so as to find out the origin of the high catalytic reactivity and extend the indus‐trialization applications of nano gold catalysts. In this work, some theoretical works on CO adsorp‐tion, O2 adsorption, atomic oxygen adsorption, formation of surface gold oxide films, reaction mechanisms of CO oxidation involving O2 reaction with CO and O2 dissociation before reacting with CO on gold surfaces and Au/metal oxide were summarized, and the influences of coordination number, charge transfer and relativity of gold on CO oxidation reaction were briefly reviewed. It was found that CO reaction mechanism depended on the systems with or without oxide and the strong relativistic effects might play an important role in CO oxidation reaction on gold catalysts. In particular, the relativistic effects are related to the unique behaviors of CO adsorption, O adsorption, O2 activation on gold surfaces, effects of coordination number and the wide gap between the chem‐ical inertness of bulk gold and high catalytic activity of nano gold. The present work helps us to understand the CO oxidation reaction mechanism on gold catalysts and the influence of relativistic effects on gold catalysis. 展开更多
关键词 Carbon monoxide oxidation reaction Gold nanoparticle reaction mechanism Theoretical calculation Relativistic effect
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Hierarchically skeletal multi-layered Pt-Ni nanocrystals for highly efficient oxygen reduction and methanol oxidation reactions 被引量:6
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作者 Shibo Li Zhi Qun Tian +5 位作者 Yang Liu Zheng Jang Syed Waqar Hasan Xingfa Chen Panagiotis Tsiakaras Pei Kang Shen 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第4期648-657,共10页
Pt based materials are the most efficient electrocatalysts for the oxygen reduction reaction(ORR)and methanol oxidation reaction(MOR)in fuel cells.Maximizing the utilization of Pt based materials by modulating their m... Pt based materials are the most efficient electrocatalysts for the oxygen reduction reaction(ORR)and methanol oxidation reaction(MOR)in fuel cells.Maximizing the utilization of Pt based materials by modulating their morphologies to expose more active sites is a fundamental objective for the practical application of fuel cells.Herein,we report a new class of hierarchically skeletal Pt-Ni nanocrystals(HSNs)with a multi-layered structure,prepared by an inorganic acid-induced solvothermal method.The addition of H_(2)SO_(4)to the synthetic protocol provides a critical trigger for the successful growth of Pt-Ni nanocrystals with the desired structure.The Pt-Ni HSNs synthesized by this method exhibit enhanced mass activity of 1.25 A mgpt−1 at 0.9 V(versus the reversible hydrogen electrode)towards ORR in 0.1-M HClO_(4),which is superior to that of Pt-Ni multi-branched nanocrystals obtained by the same method in the absence of inorganic acid;it is additionally 8.9-fold higher than that of the commercial Pt/C catalyst.Meanwhile,it displays enhanced stability,with only 21.6%mass activity loss after 10,000 cycles(0.6–1.0 V)for ORR.Furthermore,the Pt-Ni HSNs show enhanced activity and anti-toxic ability in CO for MOR.The superb activity of the Pt-Ni HSNs for ORR and MOR is fully attributed to an extensively exposed electrochemical surface area and high intrinsic activity,induced by strain effects,provided by the unique hierarchically skeletal alloy structure.The novel open and hierarchical structure of Pt-Ni alloy provides a promising approach for significant improvements of the activity of Pt based alloy electrocatalysts. 展开更多
关键词 Hierarchically skeletal Pt-Ni NANOCRYSTALS SELF-ASSEMBLY Solvent thermal method Oxygen reduction reaction Methanol oxidation reaction Fuel cells ACTIVITY
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Rational design ternary platinum based electrocatalysts for effective methanol oxidation reaction 被引量:6
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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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General approach for atomically dispersed precious metal catalysts toward hydrogen reaction 被引量:6
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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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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:4
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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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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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Surface elemental distribution effect of Pt-Pb hexagonal nanoplates for electrocatalytic methanol oxidation reaction 被引量:2
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作者 Hee Jin Kim Yong-Deok Ahn +4 位作者 Jeonghyeon Kim Kyoung-Su Kim Yeon Uk Jeong Jong Wook Hong Sang-Il Choi 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2020年第5期813-819,共7页
Bimetallic Pt-based catalysts have been extensively investigated to enhance the performance of direct methanol fuel cells(DMFCs) because CO, a by-product, reduces the activity of the pure Pt catalysts. Herein, we synt... Bimetallic Pt-based catalysts have been extensively investigated to enhance the performance of direct methanol fuel cells(DMFCs) because CO, a by-product, reduces the activity of the pure Pt catalysts. Herein, we synthesized Pt-Pb hexagonal nanoplates as a model catalyst for the methanol oxidation reaction(MOR) and further controlled the Pt and Pb distributions on the surface of the nanoplates through acetic acid(HAc) treatment. As a result, we obtained Pt-Pb nanoplates and HAc-treated Pt-Pb nanoplates with homogeneous and heterogeneous distributions of the Pt-Pb alloy surfaces, respectively. We showed that the MOR activity and stability of the Pt-Pb nanoplates improved compared to those of the HAc-treated Pt-Pb nanoplates, mainly due to the enhanced CO tolerance and the modified electronic structure of Pt under the influence of the oxophilic Pb. 展开更多
关键词 Platinum Lead NANOPLATE Surface atomic distribution Methanol 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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Electrocatalysts development for hydrogen oxidation reaction in alkaline media:From mechanism understanding to materials design 被引量:1
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作者 Yang Qiu Xiaohong Xie +1 位作者 Wenzhen Li Yuyan Shao 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第12期2094-2104,共11页
Anion exchange membrane(AEM)fuel cells have gained great attention partially due to the advantage of using non-precious metal as catalysts.However,the reaction kinetics of hydrogen oxidation reaction(HOR)is two orders... Anion exchange membrane(AEM)fuel cells have gained great attention partially due to the advantage of using non-precious metal as catalysts.However,the reaction kinetics of hydrogen oxidation reaction(HOR)is two orders of magnitude slower in alkaline systems than in acid.To understand the slower kinetics of HOR in base,two major theories have been proposed,such as(1)pH dependent hydrogen binding energy as a major descriptor for HOR;and(2)bifunctional theory based on the contributions of both hydrogen and hydroxide adsorption for HOR in alkaline electrolyte.Here,we discuss the possible HOR mechanisms in alkaline electrolytes with the corresponding change in their Tafel behavior.Apart from the traditional Tafel-Volmer and Heyrovsky-Volmer HOR mechanisms,the recently proposed hydroxide adsorption step is also discussed to illustrate the difference in HOR mechanisms in acid and base.We further summarize the representative works of alkaline HOR catalyst design(e.g.,precious metals,alloy,intermetallic materials,Ni-based alloys,carbides,nitrides,etc.),and briefly describe their fundamental HOR reaction mechanism to emphasize the difference in elementary reaction steps in alkaline medium.The strategy of strengthening local interaction that facilitates both H2 desorption and Hads+OHads recombination is finally proposed for future HOR catalyst design in alkaline environment. 展开更多
关键词 Hydrogen oxidation reaction Alkaline electrolyte Fuel cell ELECTROCATALYST ELECTROCATALYSIS Hydrogen and hydroxide binding energy
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Simple Preparation of Crystal Co_3(BTC)_2·12H_2O and Its Catalytic Activity in CO Oxidation Reaction 被引量:1
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作者 谭海燕 LIU Cheng +1 位作者 YAN Yunfan 吴金平 《Journal of Wuhan University of Technology(Materials Science)》 SCIE EI CAS 2015年第1期71-75,共5页
Crystalline metal-organic framework cobalt (II) benzenetricarboxylate C%(BTC)2·12H2O (MOF-Co) has been prepared using solvothermal method. The reaction of cobalt (II) nitrate and 1,3,5-benzenetriearboxyl... Crystalline metal-organic framework cobalt (II) benzenetricarboxylate C%(BTC)2·12H2O (MOF-Co) has been prepared using solvothermal method. The reaction of cobalt (II) nitrate and 1,3,5-benzenetriearboxylic (BTC) acid in a mixed solution of N,N-dimethylformarnide (DMF)/C2H5OH/H2O (1:1:1, v/v) at low temperature for short reaction times produced this crystalline compound. Compared with traditional hydrothermal method, a mixed solution method for the synthesis of crystalline metal complex was found to be highly efficient. After water molecules were removed from this metal complex, its exposed nodes served as active sites. When this MOF-Co was employed in the oxidation of CO, it showed good catalytic properties causing 100% conversion of CO to CO2 at low temperature of 160 ℃. 展开更多
关键词 metal-organic framework solvothermal synthesis crystalline compound cobalt catalyst CO oxidation reaction
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Hydrogen evolution-assisted one-pot aqueous synthesis of hierarchical trimetallic PdNiRu nanochains for hydrazine oxidation reaction 被引量:1
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作者 Tao Yuan Aijun Wang +2 位作者 Keming Fang Zhigang Wang Jiuju Feng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2017年第6期1231-1237,共7页
A hydrogen evolution-assisted one-pot aqueous approach was developed for facile synthesis of trimetallic Pd Ni Ru alloy nanochain-like networks(Pd Ni Ru NCNs) by only using KBHas the reductant, without any specific ... A hydrogen evolution-assisted one-pot aqueous approach was developed for facile synthesis of trimetallic Pd Ni Ru alloy nanochain-like networks(Pd Ni Ru NCNs) by only using KBHas the reductant, without any specific additive(e.g. surfactant, polymer, template or seed). The products were mainly investigated by transmission electron microscopy(TEM), X-ray diffraction(XRD) and X-ray photoelectron spectroscopy(XPS). The hierarchical architectures were formed by the oriented assembly growth and the diffusioncontrolled deposition in the presence of many in-situ generated hydrogen bubbles. The architectures had the largest electrochemically active surface area(ECSA) of 84.32 mgPdthan Pd Ni nanoparticles(NPs,65.23 mgPd), Pd Ru NPs(23.12 mgPd), Ni Ru NPs(nearly zero), and commercial Pd black(6.01 mgPd), outperforming the referenced catalysts regarding the catalytic characters for hydrazine oxygen reaction(HOR). The synthetic route provides new insight into the preparation of other trimetallic nanocatalysts in fuel cells. 展开更多
关键词 Trimetallic alloy Nanochain networks Hydrogen evolution-assisted synthesis Diffusion-controlled deposition Hydrazine oxidation reaction
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Robust copper nanocrystal/nitrogen-doped carbon monoliths as carbon monoxide-resistant electrodes for methanol oxidation reaction 被引量:1
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作者 Fei Chen Na Wu +4 位作者 Meixu Zhai Xue Zhang Ruihong Guo Tuoping Hu Mingming Ma 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第7期247-255,共9页
Noble metal-based electrocatalysts present high activities for methanol oxidation reaction(MOR),but are limited by their high cost,low stability and poor resistance to carbon monoxide(CO) poisoning.The development of ... Noble metal-based electrocatalysts present high activities for methanol oxidation reaction(MOR),but are limited by their high cost,low stability and poor resistance to carbon monoxide(CO) poisoning.The development of active and stable non-noble metal electrocatalysts for MOR is desired,but remains a challenge.Herein,we report a simple strategy to make copper nanocrystal/nitrogen-doped carbon(Cu/N-C)monoliths,which can serve as active and robust electrodes for MOR.Copper nanocrystals were electrochemically deposited onto a conductive polyaniline hydrogel and calcined to form Cu/N-C monolith,where the active copper nanocrystals are protected by nitrogen-doped carbon.Owing to their extremely high electrical conductivity(1.25 × 10^(5) S cm^(-1)) and mechanical robustness,these Cu/N-C monoliths can be directly used as electrodes for MOR,without using substrates or additives.The optimal Cu/N-C(FT)@500 monolith shows a high MOR activity of 189 mA cm^(-2) at 0.6 V vs.SCE in alkaline methanol solution,superior to most of reported Cu-based MOR catalysts.Cu/N-C(FT)@500 also presents a better stability than Pt/C catalyst in the long-term MOR test at high current densities.Upon carbon monoxide(CO) poisoning,Cu/N-C(FT)@500 retains 96% of its MOR activity,far exceeding the performance of Pt/C catalyst(61% retention).Owing to its facile synthesis,outstanding activity,high stability and mechanical robustness,Cu/N-C(FT)@500 monolith is promising as a low-cost,efficient and CO-resistant electrocatalyst for MOR. 展开更多
关键词 Copper nanocrystal Methanol oxidation reaction Non-noble metal-based electrocatalysts Poison-resistant electrocatalysts Nitrogen-doped carbon
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Manipulating the electronic structure of Ni electrocatalyst through d‐p orbital hybridization induced by B‐doping for efficient alkaline hydrogen oxidation reaction 被引量:1
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作者 Pengyu Han Na Yao +1 位作者 Wei Zuo Wei Luo 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第6期1527-1534,共8页
Developing highly efficient platinum‐group‐metal‐free electrocatalysts towards hydrogen oxidation reaction(HOR)under alkaline electrolyte is critical for the development of alkaline exchange member fuel cells.Herei... Developing highly efficient platinum‐group‐metal‐free electrocatalysts towards hydrogen oxidation reaction(HOR)under alkaline electrolyte is critical for the development of alkaline exchange member fuel cells.Herein,we reported the synthesis of boron doped Ni electrocatalyst(B‐Ni/C)and its remarkable alkaline HOR performance,with a 10‐fold mass activity enhancement compared with that of undoped Ni catalyst.Experimental results and density functional theory calculations indicate the d‐p hybridization between the p orbital of B and the d orbital of Ni via B‐doping could lead to promoted OH adsorption and optimized hydrogen binding energy on Ni surface,which together with the reduced formation energy of water species,contributes to the enhanced HOR performance under alkaline electrolyte. 展开更多
关键词 Hydrogen oxidation reaction Hydrogen evolution reaction d‐p hybridization Boron doping Density functional theory
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Two-dimensional bimetallic coordination polymers as bifunctional evolved electrocatalysts for enhanced oxygen evolution reaction and urea oxidation reaction 被引量:1
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作者 Qiang Li Lele Lu +2 位作者 Jingwei Liu Wei Shi Peng Cheng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第12期230-238,I0005,共10页
Two-dimensional coordination polymers(CPs) have aroused tremendous interest as electrocatalysts because the catalytic performance could be fine-tuned by their well-designed coordination layers with highly accessible a... Two-dimensional coordination polymers(CPs) have aroused tremendous interest as electrocatalysts because the catalytic performance could be fine-tuned by their well-designed coordination layers with highly accessible and active metal sites.However,it remains great challenge for CP-based catalysts to be utilized for electrocatalytic oxidation reactions due to their inefficient activities and low catalytic stabilities.Herein,we applied a mixed-metal strategy to fabricate two-dimensional Co_xNi_(1-x)-CPs with dual active sites for electrocatalytic water and urea oxidation.By metal ratio regulation in the twodimensional layer,an optimized Co_(2/3)Ni_(1/3)-CP exhibits a water oxidation performance with an overpotential of 325 mV at a current density of 10 mA cm^(-2) and a Tafel slope of 86 mV dec^(-1) in alkaline solution for oxygen evolution reaction.Importantly,a lower potential than that of commercial RuO_(2) is observed over20 mA cm^(-2).Co_(2/3)Ni_(1/3)-CP also displays a potential of 1.381 V at 10 mA cm^(-2) for urea oxidation reaction and a Tafel slope of 124 mV dec^(-1).This mixed-metal strategy to maximize synergistic effect of different metal centers may ultimately lead to promising electrocatalysts for small molecule oxidation reaction. 展开更多
关键词 Coordination Polymers ELECTROCATALYSIS Oxygen Evolution reaction Urea Oxidation reaction
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Preparation of new sunscreen materials Ce_(1-x)Zn_xO_(2-x) via solid-state reaction at room temperature and study on their properties 被引量:5
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作者 WU Wenwei, LI Shushu, LIAO Sen, XIANG Feng, and WU Xuehang School of Chemistry and Chemical Engineering, Guangxi University, Nanning 530004, China 《Rare Metals》 SCIE EI CAS CSCD 2010年第2期149-153,共5页
Superfine cerium-zinc oxides Ce1-xZnxO2-x with x = 0, 0.1, 0.3, 0.5, and 1.0 were obtained by grinding Ce(SO4)2·4H2O, ZnSO4·7H2O and NH4HCO3 under the condition of surfactant PEG-400 being present at room ... Superfine cerium-zinc oxides Ce1-xZnxO2-x with x = 0, 0.1, 0.3, 0.5, and 1.0 were obtained by grinding Ce(SO4)2·4H2O, ZnSO4·7H2O and NH4HCO3 under the condition of surfactant PEG-400 being present at room temperature, washing the mixture with water to remove soluble inorganic salts, drying at 80°C, and calcining.The precursor and its calcined samples were characterized using thermogravimetry and differential thermal analyses(TG/DTA), UV-vis absorption spectroscopy, X-ray powder diffraction(XRD), and scanning electron microscopy(SEM).The results showed that superfine Ce1-xZnxO2-x behaved as an excellent UV-shielding material.The ZnO-doped CeO2 can facilitate the formation of crystalline state CeO2.The catalytic ability of products used in air oxidation of castor oil was investigated.The results showed that the catalytic abilities of products decreased with increasing zinc amount. 展开更多
关键词 cerium oxide zinc oxide solid-state reaction UV absorbency catalytic properties
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Catalytic activity of V_(2)CO_(2) MXene supported transition metal single atoms for oxygen reduction and hydrogen oxidation reactions:A density functional theory calculation study
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作者 Zhongjing Deng Xingqun Zheng +3 位作者 Mingming Deng Li Li Li Jing Zidong Wei 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第10期1659-1666,共8页
Two-dimensional(2D)MXene and single-atom(SA)catalysts are two frontier research fields in catalysis.2D materials with unique geometric and electronic structures can modulate the catalytic performance of supported SAs,... Two-dimensional(2D)MXene and single-atom(SA)catalysts are two frontier research fields in catalysis.2D materials with unique geometric and electronic structures can modulate the catalytic performance of supported SAs,which,in turn,affect the intrinsic activity of 2D materials.Density functional theory calculations were used to systematically explore the potential of O-terminated V2C MXene(V_(2)CO_(2))-supported transition metal(TM)SAs,including a series of 3d,4d,and 5d metals,as oxygen reduction reaction(ORR)and hydrogen oxidation reaction(HOR)catalysts.The combination of TM SAs and V_(2)CO_(2)changes their electronic structure and enriches the active sites,and consequently regulates the intermediate adsorption energy and catalytic activity for ORR and HOR.Among the investigated TM-V_(2)CO_(2)models,Sc-,Mn-,Rh-,and PtMCCh showed high ORR activity,while Sc-,Ti-,V-,Cr-,and Mn-V_(2)CO_(2)exhibited high HOR activity.Specifically,Mn-and Sc-V_(2)CO_(2)are expected to serve as highly efficient and cost-effective bifunctional catalysts for fuel cells because of their high catalytic activity and stability.This work provides theoretical guidance for the rational design of efficient ORR and HOR bifunctional catalysts. 展开更多
关键词 Single atoms catalyst MXenes Oxygen reduction reaction Hydrogen oxidation reaction Density functional theory Fuel cells
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Visualization of atomic scale reaction dynamics of supported nanocatalysts during oxidation and ammonia synthesis using in-situ environmental(scanning) transmission electron microscopy
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作者 Michael R.Ward Robert W.Mitchell +1 位作者 Edward D.Boyes Pratibha L.Gai 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第6期281-290,I0007,共11页
Reaction dynamics in gases at operating temperatures at the atomic level are the basis of heterogeneous gas-solid catalyst reactions and are crucial to the catalyst function.Supported noble metal nanocatalysts such as... Reaction dynamics in gases at operating temperatures at the atomic level are the basis of heterogeneous gas-solid catalyst reactions and are crucial to the catalyst function.Supported noble metal nanocatalysts such as platinum are of interest in fuel cells and as diesel oxidation catalysts for pollution control,and practical ruthenium nanocatalysts are explored for ammonia synthesis.Graphite and graphitic carbons are of interest as supports for the nanocatalysts.Despite considerable literature on the catalytic processes on graphite and graphitic supports,reaction dynamics of the nanocatalysts on the supports in different reactive gas environments and operating temperatures at the single atom level are not well understood.Here we present real time in-situ observations and analyses of reaction dynamics of Pt in oxidation,and practical Ru nanocatalysts in ammonia synthesis,on graphite and related supports under controlled reaction environments using a novel in-situ environmental(scanning) transmission electron microscope with single atom resolution.By recording snapshots of the reaction dynamics,the behaviour of the catalysts is imaged.The images reveal single metal atoms,clusters of a few atoms on the graphitic supports and the support function.These all play key roles in the mobility,sintering and growth of the catalysts.The experimental findings provide new structural insights into atomic scale reaction dynamics,morphology and stability of the nanocatalysts. 展开更多
关键词 In-situ visualization Atomic scale reaction dynamics In-situ environmental scanning transmission electron microscopy with single atom resolution Supported nanoparticles Ammonia synthesis Oxidation reactions
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