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Nano Research 2022年第5期15卷 3920-3926页

作者： Mingyu Chu Jialu Huang Jin Gong Yi Qu Guoling Chen Hu Yang Xuchun Wang Qixuan Zhong Chengwei Deng Muhan Cao Jinxing Chen Xiaolei Yuan Qiao Zhang School of Chemistry and Chemical Engineering Nantong University9 Seyuan RoadNantong 226019China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesSoochow UniversityNo.199 Ren’ai RoadSuzhou 215123China Department of Chemistry University of Western OntarioLondonOntario N6A5B7Canada State Key Laboratory of Space Power-sources Technology Shanghai Institute of Space Power-Sources2965 Dongchuan RoadShanghai 200245China

Highly active and durable Pd-based electrocatalysts for ethanol oxidation reaction(EOR)play a crucial role in the commercialization of direct ethanol fuel cells(DEFCs).However,the poisonous intermediates(especially adsorbed CO species(COad))formed during the EOR process can easily adsorb and block the active sites on Pd electrodes,which in turn limits the catalytic efficiency.Hence,we present a series of Pd-based composites with a strong coupling interface consisting of Pd nanosheets and amorphous Bi(OH)_(3)species.The incorporation of Bi(OH)3 can induce an electron-rich state adjacent to the Pd sites and effectively separate the Pd ensemble,leading to excellent CO tolerance.The optimal Pd-Bi(OH)_(3)NSs catalyst manifests a mass activity of 2.2 A·mgPd^(-1),which is 5.7 and 2.0 times higher than that of Pd NSs and commercial Pd/C catalyst,respectively.Further CO-stripping experiments and CO-DRIFTS tests confirm the excellent CO tolerance on Pd-Bi(OH)3 NSs electrode,leading to the enhanced EOR durability.

关键词： Pd nanosheets Bi(OH)_(3)species ethanol oxidation reaction Co tolerance

General strategy for evaluating the d-band center shift and ethanol oxidation reaction pathway towards Pt-based electrocatalysts

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Science China Chemistry 2023年第1期66卷 279-288页

作者： Jin-Hong Zheng Guang Li Jun-Ming Zhang Ningyan Cheng Li-Fei Ji Jian Yang Jialin Zhang Bin-Wei Zhang Yan-Xia Jiang Shi-Gang Sun State Key Laboratory of Physical Chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China School of Chemistry and Chemical Engineering Chongqing UniversityChongqing 401331China Center of Advanced Energy Technology and Electrochemistry Institute of Advanced Interdisciplinary StudiesChongqing UniversityChongqing 400044China Key Laboratory of Magnetic Molecules&Magnetic Information Materials Ministry of Education School of Chemical and Material ScienceShanxi Normal UniversityTaiyuan 030031China Information Materials and Intelligent Sensing Laboratory of Anhui Province Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationInstitutes of Physical Science and Information TechnologyAnhui UniversityHefei 230039China

The catalytic performance of Pt-based catalysts depends sensitively on their d-band centers.Nevertheless,there are still huge challenges to evaluate their d-band centers from experimental technologies,and modulate them to analyze their selectivity in ethanol oxidation reaction(EOR).Here,Pt1Au1alloy supported on the commercial carbon material(Pt_(1)Au_(1)/C)is employed as a typical example to investigate its d-band center shift of surface Pt,and as electrocatalysts to study its selectivity towards EOR.Significantly,a highly reliable in situ Fourier-transform infrared spectroscopy CO-probe strategy is developed to characterize the d-band center shift of surface Pt.The modified electronic effect and site effect of Pt_(1)Au_(1)/C dictated the adsorption configuration of intermediate species and the OH species coverage,thereby influencing its selectivity.More importantly,we developed a universal cyclic voltammetry peak differentiation fitting method as an electrochemical analysis technique to investigate CO_(2)selectivity,which is potentially extendable to other Pt-based electrocatalysts.

关键词： PtAu in situ FTIRS d-band center ethanol oxidation reaction CV peak differentiation fitting method

Porous Pt nanoframes decorated with Bi(OH)3 as highly efficient and stable electrocatalyst for ethanol oxidation reaction

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Nano Research 2020年第1期13卷 265-272页

作者： Xiaolei Yuan Bei Jiang Muhan Cao Congyang Zhang Xiaozhi Liu Qinghua Zhang Fenglei Lyu Lin Gu Qiao Zhang School of Chemistry and Chemical Engineering Nantong University9 Seyuan RoadNantong226019China Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesSWC for Synchrotron Radiation ResearchSoochow University199 Ren’ai RoadSuzhou215123China Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing100190China School of Physical Sciences University of Chinese Academy of SciencesBeijing100049China Key Laboratory of Green Chemistry and Technology Ministry of EducationCollege of ChemistrySichuan UniversityChengdu610064China

High-quality Pt-based catalysts are highly desirable for ethanol oxidation reaction(EOR),which is of critical importance for the commercial applications of direct ethanol fuel cells(DEFCs).However,most of the Pt-based catalysts have suffered from high cost and low operation durability.Herein a two-step method has been developed to synthesize porous Pt nanoframes decorated with Bi(OH)3,which show excellent catalytic activity and operation durability in both alkaline and acidic media.For example,the nanoframes show a mass activity of 6.87 A·mgPt−1 in alkaline media,which is 13.5-fold higher than that of commercial Pt/C.More importantly,the catalyst can be reactivated simply,which shows negligible activity loss after running for 180,000 s.Further in situ attenuated total reflection-infrared(ATR-IR)absorption spectroscopy and CO-stripping experiments indicate that surface Bi(OH)3 species can greatly facilitate the formation of adsorbed OH species and subsequently remove carbonaceous poison,resulting in a significantly enhanced stability towards EOR.This work may favor the tailoring of desired electrocatalysts with high activity and durability for future commercial application of DEFCs.

关键词： Pt nanoframe ethanol oxidation reaction bismuth hydroxide CO tolerance in situ infrared spectroscopy durability

Flexible Au micro-array electrode with atomic-scale Au thin film for enhanced ethanol oxidation reaction

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Nano Research 2021年第1期14卷 311-319页

作者： Xun Cao Dongdong Peng Cao Wu Yongmin He Chaojiang Li Bowei Zhang Changcun Han Junsheng Wu Zheng Liu Yizhong Huang College of Sciencey Hubei University of Technology 28 Nanli RoadHongshan DistrictWuhan 430068China School of Materials Science and Engineering Nanyang Technological University50 Nanyang AvenueSingapore 639798Singapore International Laboratory for Insulation and Energy Efficiency Materials College of Materials Science and TechnologyNanjing University of Aeronautics and Astronautics29 Jiangjun AvenueJiangning DistrictNanjing 211100China School of Mechanical Engineering Beijing Institute of Technology5 South Zhongguancun StreetHaidian DistrictBeijing 100081China Institute for Advanced Materials and Technology University of Science and Technology Beijing30 Xueyuan RoadHaidian DistrictBeijing 100083China

The catalysis of Au thin film could be improved by fabrication of array structures in large area.In this work,nanoimprint lithography has been developed tofabricate flexible Au micro-array(MA)electrodes with~100%coverage.Advanced electron microscopy characterisations have directly visualised the atomic-scale three-dimensional(3D)nanostructures with a maximum depth of 6 atomic layers.In-situ observation unveils the crystal growth in the form of twinning.High double layer capacitance brings about large number of active sites on the Au thin film and has a logarithmic relationship with mesh grade.Electrochemistry testing shows that the Au MAs perform much better ethanol oxidation reaction than the planar sample;MAs with higher mesh grade have a greater active site utilisation ratio(ASUR),which is important to build electrochemical double layer for efficient charge transfer.Further improvement on ASUR is expected for greater electrocatalytic performance and potential application in direct ethanol fuel cell.

关键词： atomic-scale three-dimensional(3D)nanostructures atomic-scale active sites in-situ observations flexible electrode ethanol oxidation reaction active site utilisation ratio

Crystal phase-controlled growth of PtCu and PtCo alloys on 4H Au nanoribbons for electrocatalytic ethanol oxidation reaction

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Nano Research 2020年第7期13卷 1970-1975页

作者： Jie Wang Jian Zhang Guigao Liu Chongyi Ling Bo Chen Jingtao Huang Xiaozhi Liu Bing Li An-Liang Wang Zhaoning Hu Ming Zhou Ye Chen Hongfei Cheng Jiawei Liu Zhanxi Fan Nailiang Yang Chaoliang Tan Lin Gu Jinlan Wang Hua Zhang Department of Chemistry City University of Hong KongHong KongChina Center for Programmable Materials School of Materials Science and EngineeringNanyang Technological University50 Nanyang AvenueSingapore 639798Singapore School of Physics Southeast UniversityNanjing 211189China Institute of Physics Beijing National Laboratory for Condensed Matter PhysicsChinese Academy of SciencesBeijing 100190China Institute of Materials Research and Engineering(IMRE) Agency for Science Technology and Research(A*STAR)Singapore 138634Singapore Hong Kong Branch of National Precious Metals Material Engineering Research Center(NPMM) City University of Hong KongHong KongChina

Crystal phase can greatly affect the physicochemical properties and applications of nanomaterials.However,it stil remains a great challenge to synthesize nanostructures with the same composition and morphology but different phases in order to explore the phase-dependent properties and applications.Herein,we report the crystal phase-controlled synthesis of PtCu alloy shells on 4H Au nanoribbons(NRBs),referred to as 4H-Au NRBs,to form the 4H-Au@PtCu core-shell NRBs.By tuning the thickness of PtCu,4H-PtCu and face-centered cubic(cc)phase PICu(cc-PtCu)alloy shells are successtully grown on the 4H-Au NRB cores.This thickness-dependent phase-controlled growth strategy can also be used to grow PtCo alloys with 4H or fcc phase on 4H-Au NRBs.Significantly,when used as electrocatalysts for the ethanol oxidation reaction(EOR)in alkaline media,the 4H-Au@4H-PtCu NRBs show much better EOR performance than the 4H-Au@fcc-PtCu NRBs,and both of them possess superior performance compared to the commercial Pt black.Our study provides a strategy on phase-contolled synthesis of nanomaterials used for crystal phase-dependent applications.

关键词： crystal phase 4H hexagonal face-ce ntered cubic ethanol oxidation reaction phase engineering of nanomaterials

Self-supporting trimetallic PtAuBi aerogels as electrocatalyst for ethanol oxidation reaction

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Chinese Journal of Structural Chemistry 2023年第8期42卷 21-30页

作者： Chu Li Xiaoguo Tie Yulin Min Qunjie Xu Qiaoxia Li Shanghai Key Laboratory of Materials Protection and Advanced Materials in Electric Power College of Environmental and Chemical EngineeringShanghai University of Electric PowerYangpu District2588 Changyang RoadShanghai200090China Shanghai Institute of Pollution Control and Ecological Security Shanghai200090China

The creation of anodic ethanol oxidation reaction catalysts with superior all-around performance for direct ethanol fuel cells(DEFCs)has continued to attract the attention of researchers.An ultrathin trimetallic PtAuBi aerogel with branching,rough-surfaced 1D nanowires that self-assemble into a 3D porous network structure has been created in this study.It has a mass activity(MA)of 8045 mA mgPt^(-1)in an alkaline medium,which is 7.56 times greater than that of commercial Pt/C(1064 mA mgPt^(-1)).Notably,the catalytic activity and resistance to CO poisoning of PtAuBi aerogels are improved by the addition of an efficient"active additive"Au.The results analysis reveals that the increased performance of PtAuBi aerogel is mostly attributable to the integrated function of the 3D porous network structure,the downward shift of the Pt d-band center,and the synergistic effect of the"Pt-Bi"and/or"Pt-Au"dual active sites.

关键词： PtAuBi aerogels ethanol oxidation reaction Carbon monoxide tolerance Direct ethanol fuel cells

Rare earth alloy nanomaterials in electrocatalysis

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能源化学:英文版 2023年第8期83卷 574-594,I0014页

作者： Yifei Li Xilin Yuan Ping Wang Lulin Tang Miao He Pangen Li Jiang Li Zhenxing Li State Key Laboratory of Heavy Oil Processing College of New Energy and MaterialsChina University of Petroleum(Beijing)Beijing 102249China

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 th

关键词： Rare earth Alloy nanomaterials Electrocatalysis Preparation methods Hydrogen evolution reaction Oxygen reduction reaction Methanol oxidation reaction ethanol oxidation reaction

Rh-Cu alloy nano-dendrites with enhanced electrocatalytic ethanol oxidation activity

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Journal of Energy Chemistry 2023年第7期82卷 343-349,I0008页

作者： Di Liu Zhejiaji Zhu Jiani Li Li-Wei Chen Hui-Zi Huang Xiao-Ting Jing An-Xiang Yin Ministry of Education Key Laboratory of Cluster Science Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsAdvanced Technology Research Institute(Jinan)School of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China

The application of direct ethanol fuel cell(DEFC)has been bottlenecked by the sluggish ethanol oxidation reaction(EOR).Efficient electrocatalysts for the C-C bond cleavage are essential to promote EOR with high efficiency and C1 selectivity.Here,we prepared Rh-Cu alloy nano-dendrites(RhCu NDs)with abundant surface steps through controlled co-reduction,which exhibited significantly enhanced activity and C1 selectivity(0.47 m A cm_((ECSA))^(-2),472.4 mA mg_(Rh)^(-1),and 38.9%)than Rh NDs(0.32 mA cm((ECSA))-2,322.1 mA mgRh-1,and 21.4%)and commercially available Rh/C(0.18 mA cm_((ECSA))^(-2),265.4 mA mg_(Rh)^(-1),and 14.9%).Theoretical calculations and CO-stripping experiments revealed that alloying with Cu could modulate the surface electronic structures of Rh to resist CO-poisoning while strengthening ethanol adsorption.In situ Fourier transform infrared spectroscopy(FTIR)indicated that the surface steps on RhCu NDs further promoted the C-C bond cleavage to increase the C1 selectivity.Therefore,optimizing the surface geometric and electronic structures of nanocrystals by rational composition and morphology control can provide a promising strategy for developing practical DEFC devices.

关键词： Rh-Cu alloy Nano-dendrites Electrocatalysis ethanol oxidation reaction In situ FTIR

Enabling high-efficiency ethanol oxidation on NiFe-LDH via deprotonation promotion and absorption inhibition

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Journal of Energy Chemistry 2023年第10期85卷 76-82,I0004页

作者： Jiawei Shi Huawei He Yinghua Guo Feng Ji Jing Li Yi Zhang Chengwei Deng Liyuan Fan Weiwei Cai Hydrogen Energy Technology Innovation Center of Hubei Province Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430074HubeiChina State Key Laboratory of Space Power-Sources Technology Shanghai Institute of Space Power SourcesShanghai 200245China College of Science and Engineering James Cook University1 James Cook DriveTownsvilleQLD 4811Australia

Nucleophile oxidation reaction(NOR), represented by ethanol oxidation reaction(EOR), is a promising pathway to replace oxygen evolution reaction(OER). EOR can effectively reduce the driving voltage of hydrogen production in direct water splitting. In this work, large current and high efficiency of EOR on a Ni, Fe layered double hydroxide(NiFe-LDH) catalyst were simultaneously achieved by a facile fluorination strategy. F in NiFe-LDH can reduce the activation energy of the dehydrogenation reaction, thus promoting the deprotonation process of NiFe-LDH to achieve a lower EOR onset potential. It also weakens the absorption of OH-and nucleophile electrooxidation products on the surface of NiFe-LDH at a higher potential, achieving a high current density and EOR selectivity, according to density functional theory calculations. Based on our experiment results, the optimized fluorinated NiFe-LDH catalyst achieves a low potential of 1.386 V to deliver a 10 mA cm^(-2)EOR. Moreover, the Faraday efficiency is greater than 95%, with a current density ranging from 10 to 250 mA cm^(-2). This work provides a promising pathway for an efficient and cost-effective NOR catalyst design for economic hydrogen production.

关键词： ethanol oxidation reaction High efficiency Ni Fe layered double hydroxide Fluorination strategy Deprotonation

Enhancement of CH_(3)CO^(*) adsorption by editing d-orbital states of Pd to boost C–C bond cleavage of ethanol eletrooxidation

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Science China Chemistry 2024年第2期67卷 696-704页

作者： Yuchen Qin Fengqi Wang Pei Liu Jinyu Ye Qian Wang Yao Wang Guangce Jiang Lijie Liu Pengfang Zhang Xiaobiao Liu Xin Zheng Yunlai Ren Junjun Li Zhicheng Zhang College of Sciences Henan Agricultural UniversityZhengzhou450000China Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of ChemistrySchool of ScienceTianjin University&Collaborative Innovation Center of Chemical Science and EngineeringTianjin300072China College of Chemistry and Chemical Engineering Xiamen UniversityXiamen361005China Department of Analysis Sinopec Engineering Group Luoyang R&D Center of TechnologyLuoyang471000China School of Chemical and Material Engineering Jiangnan UniversityWuxi214211China Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology Liaocheng UniversityLiaocheng252000China

Improving the complete ethanol electrooxidation on Pd-based catalysts in alkaline media has drawn widely attention due to the high mass energy density.However,the weak adsorption energy of CH_(3)CO^(*) on Pd restricts the C–C bond cleavage.Inspired by the molecular orbital theory,we proposed the d-state-editing strategy to construct more unoccupied d-states of Pd for the enhanced interaction with CH_(3)CO^(*) to break C–C bonds.As expected,the reduced number of e_g electrons and more unoccupied d-states of Pd successfully formed on as-prepared porous Rh Au–Pd Cu nanosheets(PNSs).Theoretical calculations show that the optimized d-states of Rh Au–Pd Cu PNS can effectively improve the adsorption of CH_(3)CO^(*) and drastically reduce the energy barrier of C–C bond cleavage,thus boosting the complete oxidation of ethanol.The charge ratio of C_1 pathway on Rh Au–Pd Cu PNSs is 51.5%,more than 2 times higher than that of Pd NSs.Our finding provides an innovative perspective for the design of highly-efficient noble-based electrocatalysts.

关键词： C–C bond cleavage CH_(3)CO^(*)adsorption unoccupied d-states ethanol oxidation reaction RhAu–PdCu porous nanosheets