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Modified electronic structure and enhanced hydroxyl adsorption make quaternary Pt-based nanosheets efficient anode electrocatalysts for formic acid-/alcohol-air fuel cells
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作者 Fengling Zhao Qiang Yuan +2 位作者 Siyang Nie Liang Wu Xun Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第5期142-150,共9页
Surface/interface engineering of a multimetallic nanostructure with diverse electrocatalytic properties for direct liquid fuel cells is desirable yet challenging.Herein,using visible light,a class of quaternary Pt_(1)... Surface/interface engineering of a multimetallic nanostructure with diverse electrocatalytic properties for direct liquid fuel cells is desirable yet challenging.Herein,using visible light,a class of quaternary Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)ultrathin nanosheets is fabricated and used as high-performance anode electrocatalysts for formic acid-/alcohol-air fuel cells.The modified electronic structure of Pt,enhanced hydroxyl adsorption,and abundant exterior defects afford Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C high intrinsic anodic electrocatalytic activity to boost the power densities of direct formic acid-/methanol-/ethanol-/ethylene glycol-/glycerol-air fuel cells,and the corresponding peak power density of Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C is respectively 129.7,142.3,105.4,124.3,and 128.0 mW cm^(-2),considerably outperforming Pt/C.Operando in situ Fourier transform infrared reflection spectroscopy reveals that formic acid oxidation on Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C occurs via a CO_(2)-free direct pathway.Density functional theory calculations show that the presence of Ag,Bi,and Te in Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)suppresses CO^(*)formation while optimizing dehydrogenation steps and synergistic effect and modified Pt effectively enhance H_(2)O dissociation to improve electrocatalytic performance.This synthesis strategy can be extended to 43 other types of ultrathin multimetallic nanosheets(from ternary to octonary nanosheets),and efficiently capture precious metals(i.e.,Pd,Pt,Rh,Ru,Au,and Ag)from different water sources. 展开更多
关键词 pt-based nanosheets Modifiedelectronic structure Enhanced hydroxyl adsorption Formicacidand alcohol oxidation Direct liquid fuel cells
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Direct atomic-level insight into oxygen reduction reaction on size-dependent Pt-based electrocatalysts from density functional theory calculations
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作者 Fangren Qian Lishan Peng +2 位作者 Yujuan Zhuang Lei Liu Qingjun Chen 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2023年第9期140-146,共7页
Developing novel oxygen reduction reaction(ORR)catalysts with high activity is urgent for proton exchange membrane fuel cells.Herein,we investigated a group of size-dependent Pt-based catalysts as promising ORR cataly... Developing novel oxygen reduction reaction(ORR)catalysts with high activity is urgent for proton exchange membrane fuel cells.Herein,we investigated a group of size-dependent Pt-based catalysts as promising ORR catalysts by density functional theory calculations,ranging from single-atom,nanocluster to bulk Pt catalysts.The results showed that the ORR overpotential of these Pt-based catalysts increased when its size enlarged to the nanoparticle scale or reduced to the single-atom scale,and the Pt_(38)cluster had the lowest ORR overpotential(0.46 V)compared with that of Pt_(111)(0.57 V)and single atom Pt(0.7 V).Moreover,we established a volcano curve relationship between the ORR overpotential and binding energy of O*(ΔE_(O*),confirming the intermediate species anchored on Pt38cluster with suitable binding energy located at top of volcano curve.The interaction between intermediate species and Pt-based catalysts were also investigated by the charge distribution and projected density of state and which further confirmed the results of volcano curve. 展开更多
关键词 Density functional theory(DFT) calculations pt-based electrocatalysts Oxygen reduction reaction
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Carbon dots regulate the interface electron transfer and catalytic kinetics of Pt-based alloys catalyst for highly efficient hydrogen oxidation 被引量:4
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作者 Jie Wu Yunjie Zhou +6 位作者 Haodong Nie Kaiqiang Wei Hui Huang Fan Liao Yang Liu Mingwang Shao Zhenhui Kang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第3期61-67,I0003,共8页
The regulation of interface electron-transfer and catalytic kinetics is very important to design the efficient electrocatalyst for alkaline hydrogen oxidation reaction(HOR).Here,we show the Pt-Ni alloy nanoparticles(P... The regulation of interface electron-transfer and catalytic kinetics is very important to design the efficient electrocatalyst for alkaline hydrogen oxidation reaction(HOR).Here,we show the Pt-Ni alloy nanoparticles(PtNi_(2))have an enhanced HOR activity compared with single component Pt catalyst.While,the interface electron-transfer kinetics of PtNi_(2)catalyst exhibits a very wide electron-transfer speed distribution.When combined with carbon dots(CDs),the interface charge transfer of PtNi_(2)-CDs composite is optimized,and then the PtNi_(2)-5 mg CDs exhibits about 2.67 times and 4.04 times higher mass and specific activity in 0.1 M KOH than that of 20%commercial Pt/C.In this system,CDs also contribute to trapping H^(+)and H_(2)O generated during HOR,tuning hydrogen binding energy(HBE),and regulating interface electron transfer.This work provides a deep understanding of the interface catalytic kinetics of Pt-based alloys towards highly efficient HOR catalysts design. 展开更多
关键词 pt-based alloys Carbon dots Interface electron transfer Interface catalytic kinetics Hydrogen oxidation reaction
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Recent progress of Pt-based oxygen reduction reaction catalysts for proton exchange membrane fuel cells
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作者 Feng Zhan Kun-Song Hu +4 位作者 Jin-Hua Mai Li-Sheng Zhang Zhen-Guo Zhang Huan He Xin-Hua Liu 《Rare Metals》 SCIE EI CAS CSCD 2024年第6期2444-2468,共25页
With the increasing consumption of fossil fuels,proton exchange membrane fuel cells(PEMFCs)have attracted considerable attention as green and sustainable energy conversion devices.The slow kinetics of the cathodic oxy... With the increasing consumption of fossil fuels,proton exchange membrane fuel cells(PEMFCs)have attracted considerable attention as green and sustainable energy conversion devices.The slow kinetics of the cathodic oxygen reduction reaction(ORR)has a major impact on the performance of PEMFCs,and although platinum(Pt)can accelerate the reaction rate of the ORR,the scarcity and high cost of Pt resources still limit the development of PEMFCs.Therefore,the development of low-cost high-performance ORR catalysts is essential for the commercial application and development of PEMFCs.This paper reviews the research progress of researchers on Pt-based ORR catalysts in recent years,including Pt/C catalysts,Pt-based alloy catalysts,Pt-based intermetallic compounds,and Pt-based single-atom catalysts(SACs),with a focus on Pt-based alloy catalysts with different nanostructures.We described in detail the difficulties and solutions in the research process of various ORR catalysts and explained the principle of their activity enhancement with density functional theory(DFT).In addition,an outlook on the development of Pt-based catalysts is given,and reducing the amount of Pt used and improving the performance of catalysts are the directions to work on in the coming period. 展开更多
关键词 pt-based catalysts PEMFCS pt-based intermetallic compounds Single-atom catalysts
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Progress and prospect of Pt-based catalysts for electrocatalytic hydrogen oxidation reactions 被引量:2
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作者 Xu Zhang Ying Xie Lei Wang 《Nano Research》 SCIE EI CSCD 2024年第3期960-981,共22页
To achieve the goals of the peak carbon dioxide emissions and carbon neutral,the development and utilization of sustainable clean energy are extremely important.Hydrogen fuel cells are an important system for converti... To achieve the goals of the peak carbon dioxide emissions and carbon neutral,the development and utilization of sustainable clean energy are extremely important.Hydrogen fuel cells are an important system for converting hydrogen energy into electrical energy.However,the slow hydrogen oxidation reaction(HOR)kinetics under alkaline conditions has limited its development.Therefore,elucidating the catalytic mechanism of HOR in acidic and alkaline media is of great significance for the construction of highly active and stable catalysts.In terms of practicality,Pt is still the primary choice for commercialization of fuel cells.On the above basis,we first introduced the hydrogen binding energy theory and bifunctional theory used to describe the HOR activity,as well as the pH dependence.After that,the rational design strategies of Pt-based HOR catalysts were systematically classified and summarized from the perspective of activity descriptors.In addition,we further emphasized the importance of theoretical simulations and in situ characterization in revealing the HOR mechanism,which is crucial for the rational design of catalysts.Moreover,the practical application of Pt-based HOR catalysts in fuel cells was also presented.In closing,the current challenges and future development directions of HOR catalysts were discussed.This review will provide a deep understanding for exploring the mechanism of highly efficient HOR catalysts and the development of fuel cells. 展开更多
关键词 pt-based catalysts hydrogen oxidation reaction(HOR) electrocatalytic mechanism hydrogen binding energy theory bifunctional theory
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Strain engineering of Pt-based electrocatalysts for oxygen reaction reduction
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作者 Zeyu WANG Yanru LIU +4 位作者 Shun CHEN Yun ZHENG Xiaogang FU Yan ZHANG Wanglei WANG 《Frontiers in Energy》 SCIE EI CSCD 2024年第2期241-262,共22页
Proton exchange membrane fuel cells(PEMFCs)are playing irreplaceable roles in the construction of the future sustainable energy system.However,the insufficient performance of platinum(Pt)-based electrocatalysts for ox... Proton exchange membrane fuel cells(PEMFCs)are playing irreplaceable roles in the construction of the future sustainable energy system.However,the insufficient performance of platinum(Pt)-based electrocatalysts for oxygen reduction reaction(ORR)hinders the overall efficiency of PEMFCs.Engineering the surface strain of catalysts is considered an effective way to tune their electronic structures and therefore optimize catalytic behavior.In this paper,insights into strain engineering for improving Pt-based catalysts toward ORR are elaborated in detail.First,recent advances in understanding the strain effects on ORR catalysts are comprehensively discussed.Then,strain engineering methodologies for adjusting Ptbased catalysts are comprehensively discussed.Finally,further information on the various challenges and potential prospects for strain modulation of Pt-based catalysts is provided. 展开更多
关键词 strain engineering pt-based catalysts oxygen reduction reaction(ORR) catalytic performance proton exchange membrane fuel cells(PEMFCs)
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Melting mechanisms of Pt-based multimetallic spherical nanoparticles by molecular dynamics simulation
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作者 Chun-Yu Cheng Yuan-Yuan Guo +3 位作者 Yi-Ming Zou Amanda Jiamin Ong Alfred ling Yoong Tok Shuzhou Li 《Rare Metals》 SCIE EI CAS CSCD 2023年第2期406-417,共12页
The melting mechanisms of Pt-based multimetallic nanoparticles(NPs)are important to help determine their optimal melting processes.To understand the melting and coalescence behaviors of heterogeneous NPs(Pd-Pt NPs)wit... The melting mechanisms of Pt-based multimetallic nanoparticles(NPs)are important to help determine their optimal melting processes.To understand the melting and coalescence behaviors of heterogeneous NPs(Pd-Pt NPs)with various sizes and compositions,molecular dynamics(MD)simulation was employed.The MD results for larger Pd-Pt NPs with an effective diameter of4.6-7.8 nm show that PtPd alloy can form at Pd/Pt interface before Pd NP melted completely,while for Pt-core/Pdshell NP and Pd-core/Pt-shell NP,PtPd alloy formed only after Pd portion melted completely.For smaller Pd-Pt NPs with an effective diameter of 2.5-4.0 nm,PdPt alloy is not formed until both Pd and Pt NPs melted completely.Besides,the coalescence process of Pd-Pt NPs depends on the melting temperature of Pt NP when Pt composition is higher than 20 at%.Furthermore,the melting mechanisms of Pd/Pt/Ir trimetallic NPs are investigated.A two-step melting process occurs in Pd-Pt-Ir NPs and Ir-core/Ptshell/Pd-shell NP,and the melting sequence of Pd-core/Ptshell/Ir-shell NP and Pt-core/Pd-shell/Ir-shell NP is different from Pd/Pt bimetallic NPs. 展开更多
关键词 Molecular dynamics(MD) Melting mechanism pt-based Multimetallic Heterogeneous structure
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Tuning metal-support interaction of Pt-based electrocatalysts for hydrogen energy conversion
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作者 Shenzhou Li Tanyuan Wang Qing Li 《Science China Chemistry》 SCIE EI CAS CSCD 2023年第12期3398-3414,共17页
Pt-based electrocatalysts hold great promise for key electrocatalytic reactions in hydrogen-related energy conversion devices.Generally,the catalytic performance is significantly influenced by metal-support interactio... Pt-based electrocatalysts hold great promise for key electrocatalytic reactions in hydrogen-related energy conversion devices.Generally,the catalytic performance is significantly influenced by metal-support interactions(MSI)in the catalysts,making the tuning of MSI in Pt-based catalysts a highly intriguing research focus.In this review,the catalytic mechanism of Pt-based electrocatalysts is firstly introduced.Subsequently,the effects of MSI on supported Pt electrocatalysts are summarized into four types:geometric effects,electronic effects,synergistic effects,and structural reconfiguration.Finally,the prospect of optimizing the performance of Pt-based electrocatalysts by engineering MSI is exhibited,with the aim of inspiring innovation and advancement of supported Pt catalysts,thereby facilitating the development and utilization of hydrogen energy. 展开更多
关键词 metal-support interaction pt-based catalysts ELECTROCATALYSIS hydrogen evolution reaction oxygen reduction reaction
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Pt–C interactions in carbon-supported Pt-based electrocatalysts
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作者 Yu-Xuan Xiao Jie Ying +1 位作者 Hong-Wei Liu Xiao-Yu Yang 《Frontiers of Chemical Science and Engineering》 SCIE EI CSCD 2023年第11期1677-1697,共21页
Carbon-supported Pt-based materials are highly promising electrocatalysts.The carbon support plays an important role in the Pt-based catalysts by remarkably influencing the growth,particle size,morphology,dispersion,e... Carbon-supported Pt-based materials are highly promising electrocatalysts.The carbon support plays an important role in the Pt-based catalysts by remarkably influencing the growth,particle size,morphology,dispersion,electronic structure,physiochemical property and function of Pt.This review summarizes recent progress made in the development of carbon-supported Pt-based catalysts,with special emphasis being given to how activity and stability enhancements are related to Pt–C interactions in various carbon supports,including porous carbon,heteroatom doped carbon,carbon-based binary support,and their corresponding electrocatalytic applications.Finally,the current challenges and future prospects in the development of carbon-supported Pt-based catalysts are discussed. 展开更多
关键词 Pt-C interactions pt-based materials carbon support electrocatalysis
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High-throughput synthesis of size-controlled Pt-based catalysts
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作者 Zhuoran Deng Liqiang Zhao Daojian Cheng 《Particuology》 SCIE EI CSCD 2023年第12期232-240,共9页
Pt catalysts are commonly used for chemical reaction processes due to its high catalytic activity and selectivity.Notably,the size of metal particles often has a significant impact on the performance of the metal-load... Pt catalysts are commonly used for chemical reaction processes due to its high catalytic activity and selectivity.Notably,the size of metal particles often has a significant impact on the performance of the metal-loaded catalysts.Therefore,developing highly efficiently synthesis method for the size control of Pt catalysts has great development prospects and research value.In this study,high-throughput size tuning of Pt-based catalysts was achieved by carbonizing the carriers.The experimental and characterization results showed that the size of the loaded Pt nanoparticles varied with different concentrations of glucose solution during carriers carbonization process.The reduction of 4-nitrophenol as a template reaction indicated that the reaction rate constant of the catalyst is approximately linear with the size of Pt particles.Importantly,a laboratory-built high-throughput synthesis system was applied for the catalyst synthesis,which enhances the automation of the laboratory exploratory experiments and makes it possible to synthesize catalysts with controllable size in batches. 展开更多
关键词 High-throughput synthesis Size modulation pt-based catalysts 4-Nitrophenol reduction
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A general strategy for bimetallic Pt-based nano-branched structures as highly active and stable oxygen reduction and methanol oxidation bifunctional catalysts 被引量:8
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作者 Wenjuan Lei Menggang Li +5 位作者 Lin He Xun Meng Zijie Mu Yongsheng Yu Frances MRoss Weiwei Yang 《Nano Research》 SCIE EI CAS CSCD 2020年第3期638-645,共8页
The morphology and size of Pt-based bimetallic alloys are known to determine their electrocatalytic performance in reactions relevant to fuel cells.Here,we report a general approach for preparing Pt-M(M=Fe,Co and Ni)b... The morphology and size of Pt-based bimetallic alloys are known to determine their electrocatalytic performance in reactions relevant to fuel cells.Here,we report a general approach for preparing Pt-M(M=Fe,Co and Ni)bimetallic nano-branched structure(NBs)by a simple high temperature solution-phase synthesis.As-prepared Pt-M NBs show a polycrystalline structure and are rich in steps and kinks on the surface,which promote them favorable bifunctional catalytic properties in acidic electrolytes,specifically in terms of the oxygen reduction reaction(ORR)and methanol oxidation reaction(MOR).Specially,Pt-Co NBs/C catalyst shows 6.1 and 5.3 times higher in specific activity(SA)and mass activity(MA)for ORR than state-of-the-art commercial Pt/C catalysts,respectively.Moreover,it exhibits a loss of 4.0%in SA and 14.4%in MA after 10,000 cycles of accelerated durability tests(ADTs)compared with the initial activities.In addition,we also confirmed the superior MOR activity of Pt-Co NBs/C catalyst in acidic electrolytes.For Pt-M NBs with other alloying metals,the ORR and MOR activities are both higher than commercial catalysts and are in the sequence of Pt-Co/C>Pt-Fe/C>Pt-Ni/C>commercial Pt/C(or PtRu/C).The improved activities and durability can benefit from the morphological and compositional effects.This synthesis approach may be applied to develop bifunctional catalysts with enhanced ORR and MOR properties for future fuel cells designs. 展开更多
关键词 pt-based bimetallic alloy nano-branched structure electrocatalysts oxygen reduction reaction methanol oxidation reaction
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Controlled Synthesis of Carbon-Supported Pt-Based Electrocatalysts for Proton Exchange Membrane Fuel Cells 被引量:2
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作者 Huiyuan Liu Jian Zhao Xianguo Li 《Electrochemical Energy Reviews》 SCIE EI 2022年第4期138-189,共52页
Proton exchange membrane fuel cells are playing an increasing role in postpandemic economic recovery and climate action plans.However,their performance,cost,and durability are significantly related to Pt-based electro... Proton exchange membrane fuel cells are playing an increasing role in postpandemic economic recovery and climate action plans.However,their performance,cost,and durability are significantly related to Pt-based electrocatalysts,hampering their large-scale commercial application.Hence,considerable efforts have been devoted to improving the activity and durability of Pt-based electrocatalysts by controlled synthesis in recent years as an effective method for decreasing Pt use,and consequently,the cost.Therefore,this review article focuses on the synthesis processes of carbon-supported Pt-based electrocatalysts,which significantly affect the nanoparticle size,shape,and dispersion on supports and thus the activity and durability of the prepared electrocatalysts.The reviewed processes include(i)the functionalization of a commercial carbon support for enhanced catalyst-support interaction and additional catalytic effects,(ii)the methods for loading Pt-based electrocatalysts onto a carbon support that impact the manufacturing costs of electrocatalysts,(iii)the preparation of spheri-cal and nonspherical Pt-based electrocatalysts(polyhedrons,nanocages,nanoframes,one-and two-dimensional nanostruc-tures),and(iv)the postsynthesis treatments of supported electrocatalysts.The influences of the supports,key experimental parameters,and postsynthesis treatments on Pt-based electrocatalysts are scrutinized in detail.Future research directions are outlined,including(i)the full exploitation of the potential functionalization of commercial carbon supports,(ii)scaled-up one-pot synthesis of carbon-supported Pt-based electrocatalysts,and(iii)simplification of postsynthesis treatments.One-pot synthesis in aqueous instead of organic reaction systems and the minimal use of organic ligands are preferred to simplify the synthesis and postsynthesis treatment processes and to promote the mass production of commercial carbon-supported Pt-based electrocatalysts. 展开更多
关键词 Carbon-supported pt-based electrocatalysts Synthesis Shape Functionalization of commercial carbon support Postsynthesis treatment
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Engineering oxygen vacancies on Tb-doped ceria supported Pt catalyst for hydrogen production through steam reforming of long-chain hydrocarbon fuels
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作者 Zhourong Xiao Changxuan Zhang +5 位作者 Peng Li Desong Wang Xiangwen Zhang Li Wang Jijun Zou Guozhu Li 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第4期181-192,共12页
Steam reforming of long-chain hydrocarbon fuels for hydrogen production has received great attention for thermal management of the hypersonic vehicle and fuel-cell application.In this work,Pt catalysts supported on Ce... Steam reforming of long-chain hydrocarbon fuels for hydrogen production has received great attention for thermal management of the hypersonic vehicle and fuel-cell application.In this work,Pt catalysts supported on CeO_(2)and Tb-doped CeO_(2)were prepared by a precipitation method.The physical structure and chemical properties of the as-prepared catalysts were characterized by powder X-ray diffraction,scanning electron microscopy,transmission electron microscopy,Raman spectroscopy,H_(2)temperature programmed reduction,and X-ray photoelectron spectroscopy.The results show that Tb-doped CeO_(2)supported Pt possesses abundant surface oxygen vacancies,good inhibition of ceria sintering,and strong metal-support interaction compared with CeO_(2)supported Pt.The catalytic performance of hydrogen production via steam reforming of long-chain hydrocarbon fuels(n-dodecane)was tested.Compared with 2Pt/CeO_(2),2Pt/Ce_(0.9)Tb_(0.1)O_(2),and 2Pt/Ce_(0.5)Tb_(0.5)O_(2),the 2Pt/Ce_(0.7)Tb_(0.3)O_(2)has higher activity and stability for hydrogen production,on which the conversion of n-dodecane was maintained at about 53.2%after 600 min reaction under 700℃at liquid space velocity of 9 ml·g^(-1)·h^(-1).2Pt/CeO_(2)rapidly deactivated,the conversion of n-dodecane was reduced to only 41.6%after 600 min. 展开更多
关键词 Steam reforming N-DODECANE Hydrogen production pt-based catalyst Oxygen vacancy CeO_(2)
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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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Low carbon alcohol fuel electrolysis of hydrogen generation catalyzed by a novel and effective Pt–CoTe/C bifunctional catalyst system
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作者 Yang Zhou Lice Yu +2 位作者 Jinfa Chang Ligang Feng Jiujun Zhang 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第4期758-770,共13页
Low carbon alcohol fuels electrolysis under ambient conditions is promising for green hydrogen generation instead of the traditional alcohol fuels steam reforming technique,and highly efficient bifunctional catalysts ... Low carbon alcohol fuels electrolysis under ambient conditions is promising for green hydrogen generation instead of the traditional alcohol fuels steam reforming technique,and highly efficient bifunctional catalysts for membrane electrode fabrication are required to drive the electrolysis reactions.Herein,the efficient catalytic promotion effect of a novel catalyst promoter,CoTe,on Pt is demonstrated for low carbon alcohol fuels of methanol and ethanol electrolysis for hydrogen generation.Experimental and density functional theory calculation results indicate that the optimized electronic structure of Pt–CoTe/C resulting from the synergetic effect between Pt and CoTe further regulates the adsorption energies of CO and H*that enhances the catalytic ability for methanol and ethanol electrolysis.Moreover,the good water activation ability of CoTe and the strong electronic effect of Pt and CoTe increased the tolerance ability to the poisoning species as demonstrated by the CO-stripping technique.The high catalytic kinetics and stability,as well as the promotion effect,were also carefully discussed.Specifically,71.9%and 75.5%of the initial peak current density was maintained after 1000 CV cycles in acid electrolyte for methanol and ethanol oxidation;and a low overpotential of 30 and 35 mV was required to drive the hydrogen evolution reaction in methanol and ethanol solution at the current density of 10 mA cm^(-2).In the two-electrode system for alcohol fuels electrolysis,using the optimal Pt–CoTe/C catalyst as bi-functional catalysts,the cell potential of 0.66 V(0.67 V)was required to achieve 10 mA cm^(-2) for methanol(ethanol)electrolysis,much smaller than that of water electrolysis(1.76 V).The current study offers a novel platform for hydrogen generation via low carbon alcohol fuel electrolysis,and the result is helpful to the catalysis mechanism understanding of Pt assisted by the novel promoter. 展开更多
关键词 Methanol electrolysis Ethanol electrolysis Cobalt telluride pt-based electrocatalyst Hydrogen evolution reaction
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Rational modulation of electronic structure in PtAuCuNi alloys boosts efficient electrocatalytic ethanol oxidation assisted with energy-saving hydrogen evolution
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作者 Hu Yao Yinan Zheng +3 位作者 Xin Yu Songjie Hu Baolian Su Xiaohui Guo 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第6期557-567,I0014,共12页
Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient strategy.Herein,we prepared a type of nove... Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient strategy.Herein,we prepared a type of novel quaternary alloy catalyst(PtAuCuNi@NF)that exhibits excellent activity for EOR(0.215 V at 10 mA cm^(-2))and hydrogen evolution reaction(HER)(7 mV at 10 mA cm^(-2)).Experimental results demonstrated that both Cu and Ni modulated the electronic environment around Pt and Au.The electron-rich active center facilitates the rapid adsorption and dissociation of reactants and intermediates for both EOR and HER.Impressively,in the ethanol-assisted overall water splitting(E-OWS),a current density of 10 mA cm^(-2)was achieved at 0.28 V.Moreover,an advanced acid-base self-powered system(A-Bsps)that can achieve a self-powered voltage of 0.59 V was assembled.Accordingly,the self-driven hydrogen production with zero external power supply was realized by integrating A-Bsps with the E-OWS equipment.The interesting results can provide a feasible strategy for designing and developing advanced nanoalloy-based materials for clean energy integration and use in various fields. 展开更多
关键词 pt-based alloy Electronic structure Ethanol oxidation Self-powered system Overall water splitting
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Series Reports from Professor Wei's Group of Chongqing University:Advancements in Electrochemical Energy Conversions(1/4):Report 1:High-performance Oxygen Reduction Catalysts for Fuel Cells
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作者 Fa-Dong Chen Zhuo-Yang Xie +5 位作者 Meng-Ting Li Si-Guo Chen Wei Ding Li Li Jing Li Zi-Dong Wei 《电化学(中英文)》 CAS 北大核心 2024年第7期1-27,共27页
Two major challenges,high cost and short lifespan,have been hindering the commercialization process of lowtemperature fuel cells.Professor Wei's group has been focusing on decreasing cathode Pt loadings without lo... Two major challenges,high cost and short lifespan,have been hindering the commercialization process of lowtemperature fuel cells.Professor Wei's group has been focusing on decreasing cathode Pt loadings without losses of activity and durability,and their research advances in this area over the past three decades are briefly reviewed herein.Regarding the Pt-based catalysts and the low Pt usage,they have firstly tried to clarify the degradation mechanism of Pt/C catalysts,and then demonstrated that the activity and stability could be improved by three strategies:regulating the nanostructures of the active sites,enhancing the effects of support materials,and optimizing structures of the three-phase boundary.For Pt-free catalysts,especialiy carbon-based ones,several strategies that they proposed to enhance the activity of nitrogen-/heteroatom-doped carbon catalysts are firstly presented.Then,an indepth understanding of the degradation mechanism for carbon-based catalysts is discussed,and followed by the corresponding stability enhancement strategies.Also,the carbon-based electrode at the micrometer-scale,faces the challenges such as low active-site density,thick catalytic layer,and the effect of hydrogen peroxide,which require rational structure design for the integral cathodic electrode.This review finally gives a brief conclusion and outlook about the low cost and long lifespan of cathodic oxygen reduction catalysts. 展开更多
关键词 Fuel cell Oxygen reduction reaction pt-based catalyst Carbon-based catalyst
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Shape-Controlled Synthesis of Platinum-Based Nanocrystals and Their Electrocatalytic Applications in Fuel Cells 被引量:3
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作者 Can Li N.Clament Sagaya Selvam Jiye Fang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第6期190-219,共30页
To achieve environmentally benign energy conversion with the carbon neutrality target via electrochemical reactions, the innovation of electrocatalysts plays a vital role in the enablement of renewable resources. Nowa... To achieve environmentally benign energy conversion with the carbon neutrality target via electrochemical reactions, the innovation of electrocatalysts plays a vital role in the enablement of renewable resources. Nowadays, Pt-based nanocrystals(NCs) have been identified as one class of the most promising candidates to efficiently catalyze both the half-reactions in hydrogen-and hydrocarbonbased fuel cells. Here, we thoroughly discuss the key achievement in developing shape-controlled Pt and Pt-based NCs, and their electrochemical applications in fuel cells. We begin with a mechanistic discussion on how the morphology can be precisely controlled in a colloidal system, followed by highlighting the advanced development of shape-controlled Pt, Pt-alloy, Pt-based core@shell NCs, Pt-based nanocages, and Pt-based intermetallic compounds. We then select some case studies on models of typical reactions(oxygen reduction reaction at the cathode and small molecular oxidation reaction at the anode) that are enhanced by the shape-controlled Pt-based nanocatalysts. Finally, we provide an outlook on the potential challenges of shape-controlled nanocatalysts and envision their perspective with suggestions. 展开更多
关键词 SHAPE-CONTROL Colloidal synthesis pt-based nanocrystals Electrochemical catalysis
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High-entropy L1_(2)-Pt(FeCoNiCuZn)_(3) intermetallics for ultrastable oxygen reduction reaction 被引量:1
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作者 Qian Zhang Tao Shen +5 位作者 Min Song Shuang Wang Jialin Zhang Xiao Huang Shanfu Lu Deli Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第11期158-166,I0004,共10页
Enhancing the stability of Pt-based electrocatalysts for the sluggish cathodic oxygen reduction reaction(ORR)is critical for proton exchange membrane fuel cells(PEMFCs).Herein,high-entropy intermetallic(HEI)L1_(2)-Pt(... Enhancing the stability of Pt-based electrocatalysts for the sluggish cathodic oxygen reduction reaction(ORR)is critical for proton exchange membrane fuel cells(PEMFCs).Herein,high-entropy intermetallic(HEI)L1_(2)-Pt(FeCoNiCuZn)3is designed for durable ORR catalysis.Benefiting from the unique HEI structure and the enhanced intermetallic phase stability,Pt(FeCoNiCuZn)3/C nanoparticles demonstrate significantly improved stability over Pt/C and PtCu_(3)/C catalysts.The Pt(FeCoNiCuZn)3/C exhibits a negligible decay of the half-wave potential during 30,000 potential cycles from 0.6 to 1.0 V,whereas Pt/C and PtCu_(3)/C are negatively shifted by 46 and 36 m V,respectively.Even after 10,000 cycles at potential up to 1.5 V,the mass activity of Pt(FeCoNiCuZn)3/C still shows~70%retention.As evidenced by the structural characterizations,the HEI structure of Pt(FeCoNiCuZn)3/C is well maintained,while PtCu_(3)/C nanoparticles undergo severe Cu leaching and particle growth.In addition,when assembled Pt(FeCoNiCuZn)3/C as the cathode in high-temperature PEMFC of 160℃,the H_(2)-O_(2)fuel cell delivers almost no degradation even after operating for 150 h,demonstrating the potential for fuel cell applications.This work provides a facile design strategy for the development of high-performance ultrastable electrocatalysts. 展开更多
关键词 High-entropy intermetallics pt-based electrocatalysts Oxygen reduction reaction High stability
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Greatly Enhanced Methanol Oxidation Reaction of CoPt Truncated Octahedral Nanoparticles by External Magnetic Fields
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作者 Mengyuan Zhu Yi Wang +8 位作者 Yanfei Wu Jialong Liu Jingyan Zhang He Huang Xinqi Zheng Jianxin Shen Ruijie Zhao Wenda Zhou Shouguo Wang 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第5期201-210,共10页
Tunable behavior in electrocatalysis by external multifields,such as magnetic field,thermal field,and electric field,is the most promising strategy to expand the theory,design,and synthesis of state-of-the-art catalys... Tunable behavior in electrocatalysis by external multifields,such as magnetic field,thermal field,and electric field,is the most promising strategy to expand the theory,design,and synthesis of state-of-the-art catalysts and the cell in the near future.Here,a systematic investigation for the effect of external magnetic field and thermal field on methanol oxidation reactions(MOR)in magnetic nanoparticles is reported.For Co_(42)Pt_(58)truncated octahedral nanoparticles(TONPs),the catalytic performance in MOR is greatly increased to the maximum of 14.1%by applying a magnetic field up to 3000 Oe,and it shows a monotonical increase with increasing working temperature.The magnetic enhanced effect is closely related to the Co content of Co_(x)Pt_(100-x)TONPs.Furthermore,the enhancement effect under a magnetic field is more obvious for Co_(42)Pt_(58)TONPs annealed at 650℃.First-principle calculation points out that the magnetic fields can facilitate the dehydrogenation of both methanol and water by suppression of entropy of the electron spin and lowering of the activation barrier,where OH_(ad)intermediates on Co sites play a more important role.The application of magnetic fields together with thermal fields in MOR provides a new prospect to manipulate the performance of direct methanol fuel cells,which will accelerate their potential applications. 展开更多
关键词 external magnetic fields first-principle calculation methanol oxidation reaction pt-based magnetic nanomaterials
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