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MOF-derived Cu embedded into N-doped mesoporous carbon as a robust support of PdAu nanocatalysts for ethanol electrooxidation

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Rare Metals 2024年第3期43卷 1083-1094页

作者： Yu-Fu Huang Peng Wu Jun-Ping Tang Jian Yang Jing Li Shuai Chen Xue-Ling Zhao ChengChen Bin-Wei Zhang Yan-Yun Ma Wei-Heng shi Dong-Hai Lin shi-gang sun School of Energy and Materials Shanghai Engineering Research Center of Advanced Thermal Functional MaterialsShanghai Key Laboratory of Engineering Materials Application and EvaluationShanghai Polytechnic UniversityShanghai201209China State Key Laboratory of Physical Chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China School of Chemistry and Chemical Engineering Chongqing UniversityChongqing401331China Center of Advanced Energy Technology and Electrochemistry Institute of Advanced Interdisciplinary StudiesChongqing UniversityChongqing400044China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou215123China Department of Materials Science and Engineering Drexel UniversityPhiladelphiaPA19104USA

Metal-organic frameworks(MOFs)h ave attracted widespread attention due to their large surface area and porous structure.Rationally designing the nanostructures of MOFs to promote their application in ethanol electrooxidation is still a challenge.Here,a novel Cu-NCNs(Cu-nitrogen-doped carbon nanotubes)support was synthesized by pyrolysis of melamine(MEL)and Cu-ZIF-8 together,and then,Pd-Au nanoalloys were loaded by sodium borohydride reduction method to prepare PdAu@Cu-NCNs catalysts.The generating mesoporous carbon with high specific surface area and favorable electron and mass transport can be used as a potential excellent carrier for PdAu nanoparticles.In addition,the balance of catalyst composition and surface structure was tuned by controlling the content of Pd and Au.Thus,the best-performed Pd_(2)Au_(2)@Cu-NCN-1000-2(where 1000 means the carrier calcination temperature,and 2 means the calcination constant temperature time)catalyst exhibits better long-term stability and electrochemical activity for ethanol oxidation in alkaline media(4.80 A·mg^(-1)),which is 5.05 times higher than that of commercial Pd/C(0.95 A·mg^(-1)).Therefore,this work is beneficial to further promoting the application of MOFs in direct ethanol fuel cells(DEFCs)and can be used as inspiration for the design of more efficient catalyst support structures.

关键词： Metal-organic frameworks(MOFs) N-doped Mesoporous carbon PdAu Ethanol electrooxidation

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Phosphorus-doping-tuned PtNi concave nanocubes with high-index facets for enhanced methanol oxidation reaction

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Nano Research 2022年第8期15卷 6961-6968页

作者： Aixin Fan Congli Qin Ruxia Zhao Haixiao sun Hui sun Xiaoping Dai Jin-Yu Ye shi-gang sun Yanhong Lu Xin Zhang School of Chemistry&Material Science Langfang Normal UniversityLangfang 065000China ShanDong Drug and Food Vacational Colleage Weihai 255000China State Key Laboratory of Heavy Oil Processing College of Chemical EngineeringChina University of PetroleumBeijing 102249China State Key Laboratory of Physical Chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Surface engineering has been found to be an efficient strategy to boost the catalytic performance of noble-metal-based nanocatalysts.In this work,a small amount of P was doped to the surface of PtNi concave cube(P-PtNi CNC).Interestingly,the P-PtNi CNC nanocatalyst shows an enhanced methanol oxidation reaction(MOR)performance with achieving 8.19 times of specific activity than that of comercial Pt/C.The electrochemical in situ Fourier transform infrared spectroscopy(FTIR)results reveal that the surface P doping promotes the adsorption energy of OH,enhancing the resistance against CO poisoning.Therefore,the intermediate adsorbed CO(COads)reacted with adsorbed OH(OHads)through the Langmuir–Hinshelwood(LH)mechanism to generate CO_(2)and release surface active sites for further adsorption.This work provides a promising strategy via the incorporation of non-metallic elements into the PtNi alloys bounded with high-index facets(HIFs)as efficient fuel cell catalysts.

关键词： P doping high-index facets methanol oxidation reaction in situ Fourier transform infrared spectroscopy

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Recent advances of bismuth-based electrocatalysts for CO_(2)reduction:Strategies,mechanism and applications

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Materials Reports(Energy) 2023年第2期3卷 4-26,I0002页

作者： Xiao-Du Liang Na Tian Sheng-Nan Hu Zhi-You Zhou shi-gang sun State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005PR China

Electrocatalytic CO_(2)reduction reaction(CO_(2)RR),driven by clean electric energy such as solar and wind,can not only alleviate environmental greenhouse effect stemming from excessive CO_(2)emissions,but also realize the storage of renewable energy,for it guarantees the production of value-added chemicals and fuels.Among CO_(2)RR products,formic acid shows great advantages in low energy consumption and high added-value,and thus producing formic acid is generally considered as a profitable line for CO_(2)RR.Bismuth-based electrocatalysts exhibit high formic acid selectivity in CO_(2)RR.Herein,we review the recent progress in bismuth-based electrocatalysts for CO_(2)RR,including material synthesis,performance optimization/validation,and electrolyzers.The effects of morphologies,structure,and composition of bismuth-based electrocatalysts on CO_(2)RR performance are highlighted.Simultaneously,in situ spectroscopic characterization and DFT calculations for reaction mechanism of CO_(2)RR on Bi-based catalysts are emphasized.The applications and optimization of electrolyzers with high current density for CO_(2)RR are summarized.Finally,conclusions and future directions in this field are prospected.

关键词： Bismuth-based electrocatalysts Electrochemical CO_(2)reduction reaction Formate Structure-activity relationship Electrolyzer

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Engineering iron-group bimetallic nanotubes as efficient bifunctional oxygen electrocatalysts for flexible Zn–air batteries

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eScience 2022年第5期2卷 546-556页

作者： Yanli Niu Shuaiqi Gong Xuan Liu Chen Xu Mingze Xu shi-gang sun Zuofeng Chen Shanghai Key Laboratory of Chemical Assessment and Sustainability School of Chemical Science and EngineeringTongji UniversityShanghai200092China State Key Lab of Physical Chemistry of Solid Surface College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China

Air cathode performance is essential for rechargeable zinc–air batteries(ZABs).In this study,we develop a self-templated synthesis technique for fabricating bimetallic alloys(FeNi_(3)),bimetallic nitrides(FeNi_(3)N)and heterostructured FeNi_(3)/FeNi_(3)N hollow nanotubes.Owing to its structural and compositional advantages,FeNi_(3)/FeNi_(3)N exhibits remarkable bifunctional oxygen electrocatalytic performance with an extremely small potential gap of 0.68V between the oxygen evolution reaction(OER)and oxygen reduction reaction(ORR).Theoretical calculations reveal reduced Gibbs free energy for the rate-limiting O–O bond formation during OER due to the self-adaptive surface reconfiguration,which induces a synergistic effect between Fe(Ni)OOH developed in situ on the surface and the inner FeNi_(3)/FeNi_(3)N.ZAB fabricated using the FeNi_(3)/FeNi_(3)N catalyst shows high power density,small charge/discharge voltage gap and excellent cycling stability.In addition to its excellent battery performance,the corresponding quasi-solid-state ZAB shows robust flexibility and integrability.The synthesis method is extended to prepare a CoFe/CoFeN oxygen electrocatalyst,demonstrating its applicability to other iron-group elements.

关键词： Bifunctional electrocatalysts Oxygen electrocatalysis Bimetallic nitrides Hollow nanotube structure Zn-air batteries

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Tracking the atomic pathways of Pt3Ni-Ni(OH)2 core-shell structures at the gas-liquid interface by in-situ liquid cell TEM

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Science China Chemistry 2020年第4期63卷 513-518页

作者： Junyu Zhang Gen Li Hong-gang Liao shi-gang sun State Key Lab of Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy MaterialsCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Using the in-situ liquid cell transmission electron microscopy, the three-stage growth of Pt3Ni-Ni(OH)2 core-shell structures at the gas-liquid interfaces was clearly observed, which consists of(1) a thermodynamically driven Pt3Ni alloy core by the monomer attachment,(2) a nickel(Ni) shell formation due to the depletion of the Pt salt precursor, and(3) the oxidation and of the Ni shell into Ni(OH)2 flakes. We also further observed the nucleation and growth of the Ni(OH)2 flakes on an existing layer either at the middle part or at the step edge. More interestingly, the dynamic transformation among a Pt3Ni alloy, Ni clusters and Ni(OH)2 flakes was also imaged even at a high electron dose rate.

关键词： Pt3Ni-Ni(OH)2 core-shell structure liquid cell electron microscopy gas-liquid interface dynamic transformation

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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

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Engineering Two-Phase Bifunctional Oxygen Electrocatalysts with Tunable and Synergetic Components for Flexible Zn-Air Batteries

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Nano-Micro Letters 2021年第8期13卷 175-190页

作者： Yanli Niu Xue Teng Shuaiqi Gong Mingze Xu shi-gang sun Zuofeng Chen Shanghai Key Laboratory of Chemical Assessment and Sustainability School of Chemical Science and EngineeringTongji UniversityShanghai 200092People’s Republic of China State Key Lab of Physical Chemistry of Solid Surface College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005People’s Republic of China

Metal-air batteries,like Zn-air batteries(ZABs)are usually suffered from low energy conversion efficiency and poor cyclability caused by the sluggish OER and ORR at the air cathode.Herein,a novel bimetallic Co/CoFe nanomaterial supported on nanoflower-like N-doped graphitic carbon(NC)was prepared through a strategy of coordination construction-cation exchange-pyrolysis and used as a highly efficient bifunctional oxygen electrocatalyst.Experimental characterizations and density functional theory calculations reveal the formation of Co/CoFe heterostructure and synergistic effect between metal layer and NC support,leading to improved electric conductivity,accelerated reaction kinetics,and optimized adsorption energy for intermediates of ORR and OER.The Co/CoFe@NC exhibits high bifunctional activities with a remarkably small potential gap of 0.70 V between the half-wave potential(E_(1/2))of ORR and the potential at 10 mA cm^(-2)(E_(j=10))of OER.The aqueous ZAB constructed using this air electrode exhibits a slight voltage loss of only 60 mV after 550-cycle test(360 h,15 days).A sodium polyacrylate(PANa)-based hydrogel electrolyte was synthesized with strong water-retention capability and high ionic conductivity.The quasi-solid-state ZAB by integrating the Co/CoFe@NC air electrode and PANa hydrogel electrolyte demonstrates excellent mechanical stability and cyclability under different bending states.

关键词： Bifunctional electrocatalysts Oxygen electrocatalysis Zn-air battery Co/CoFe heterointerface engineering Density functional theory calculations

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Multifunctional sulfur-immobilizing GO/MXene aerogels for highly-stable and long-cycle-life lithium-sulfur batteries

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稀有金属:英文版 2023年第8期42卷 2577-2591页

作者： Wen-Hao Yang Zhi-Cong Ni Dan You Ji-Yue Hou Bing-Nan Deng Rong-Wei Huang shi-gang sun Jin-Bao Zhao Xue Li Yi-Yong Zhang Ying-Jie Zhang Key Laboratory of Advanced Battery Materials of Yunnan Province College of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunming oouuyocnina State Key Laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy MaterialsCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Lithium-sulfur batteries are a promising candidate for next-generation energy storage due to their high theoretical energy density.However,S insulation and the lithium polysulfide intermediate’s shuttle effect greatly hinder its practical application.In this paper,a three-dimensional porous graphene oxide(GO)/MXene(Ti_(3)C_(2)T_(x))(GM)aerogel is designed and applied to a lithium-sulfur battery to settle the problem mentioned.In this strategy,two-dimensional(2D)GO sheets and highly conductive MXene nanosheets are integrated to form a 3D porous aerogel structure,creating a 3D conductive network and large polar surfaces,which can simultaneously achieve fast Li-ion/electron transport,strong chemical anchoring sulfur,and promot redox reactions between poly sulfides.Therefore,the cathode shows excellent sulfur utilization and cycle stability.The prepared GM electrode battery has been tested for nearly nine months at 0.1C,providing the high initial capacity of 1255.62 mAh·g^(-1)and maintaining615.7 mAh·g^(-1)after 450 cycles.

关键词： Lithium-sulfur battery Aerogel Graphene oxide(GO) Ti_(3)C_(2)T_(x) Multifunction

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Activating coordinative conjugated polymer via interfacial electron transfer for efficient CO_(2) electroreduction

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能源化学:英文版 2023年第8期83卷 313-323,I0009页

作者： Jing Zhang Jia-Jun Dai De-Quan Cao Heng Xu Xing-Yu Ding Chun-Hua Zhen Beate Paulus Jin-Yu Ye Qian Liang Jun-Ke Liu shi-Jun Xie Sai-Sai Deng Zhen Wang Jun-Tao Li Yao Zhou shi-gang sun College of Energy XiamenUniversityXiamen 361005FujianChina College of Chemistry and Chemical Engineering Xiamen UniversityXiamen 361005FujianChina Institute of Chemistry and Biochemistry Freie Universitat BerlinArnimallee 2214195 BerlinGermany

With tunable local electronic environment,high mass density of MN4sites,and ease of preparation,metal-organic conjugated coordinative polymer(CCP) with inherent electronic conductivity provides a promising alternative to the well-known M-N-C electrocatalysts.Herein,the coordination reaction between Cu^(2+)and 1,2,4,5-tetraaminobenzene(TAB) was conducted on the surface of metallic Cu nanowires,forming a thin layer of CuN4-based CCP(Cu-TAB) on the Cu nanowire.More importantly,interfacial transfer of electrons from Cu core to the CuN4-based CCP nanoshell was observed within the resulting CuTAB@Cu,which was found to enrich the local electronic density of the CuN4sites.As such,the CuTAB@Cu demonstrates much improved affinity to the*COOH intermediate formed from the rate determining step;the energy barrier for C-C coupling,which is critical to convert CO_(2)into C2products,is also decreased.Accordingly,it delivers a current density of-9.1 mA cm^(-2)at a potential as high as 0.558 V(vs.RHE) in H-type cell and a Faraday efficiency of 46.4% for ethanol.This work emphasizes the profound role of interfacial interaction in tuning the local electronic structure and activating the CuN4-based CCPs for efficient electroreduction of CO_(2).

关键词： Metal-organic solid compounds Conjugated coordinative polymer Solid-solid interfacial electron transfer MN_(4)sites Electrocatalysis

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A breakthrough in electrocatalysis of CO2 conversion

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National Science Review 2017年第2期4卷 155-156页

作者： Zhi-You Zhou shi-gang sun State Key Laboratory of Physical Chemistry of Solid Surfaces Xiamen University

Increasing consumption of fossil fuels has resulted in dramatic increase of COconcentration in the atmosphere,which results in a series of environmental problems such as the greenhouse effect and ocean acidification.Electrocatalytic reduction of COinto organic fuels and useful chemicals is a supreme way to convert CO.The electrochemical CO

关键词： In CO

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