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Revealing structure-selectivity correlations in pulsed CO_(2)electrolysis via time-resolved operando synchrotron X-ray studies

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Nano Research 2022年第8期15卷 6860-6861页

作者： dunfeng gao State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

In the context of carbon neutrality,CO_(2)electrolysis powered by renewable energy sources holds great promise in converting CO_(2)to valuable chemicals and *** of the major challenges for practical application of CO_(2)electrolysis is control of selectivity with respect to specific products,especially multicarbon compounds like ethylene and ethanol[1–3].Through applying a series of oxidizing(anodic)and working(cathodic)potential pulses,facilitated C–C coupling,suppressed hydrogen evolution reaction and improved stability have been demonstrated over a group of Cu catalysts[4–7].Yet,mechanistic understandings behind the performance enhancement under dynamic pulsed reaction conditions are still in debate[8].

关键词： selectivity holds resolved

Heterogeneous Catalysis for CO_(2) Conversion into Chemicals and Fuels

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Transactions of Tianjin University 2022年第4期28卷 245-264页

作者： dunfeng gao Wanjun Li Hanyu Wang Guoxiong Wang Rui Cai State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China

Catalytic conversion of CO_(2)into chemicals and fuels is a viable method to reduce carbon emissions and achieve carbon *** thermal catalysis,electrocatalysis,and photo(electro)catalysis,CO_(2)can be converted into a wide range of valuable products,including CO,formic acid,methanol,methane,ethanol,acetic acid,propanol,light olefi ns,aromatics,and gasoline,as well as fi ne *** this mini-review,we summarize the recent progress in heterogeneous catalysis for CO_(2)conversion into chemicals and fuels and highlight some representative studies of diff erent conversion *** structure-performance correlations of typical catalytic materials used for the CO_(2)conversion reactions have been revealed by combining advanced in situ/operando spectroscopy and microscopy characterizations and density functional theory *** selectivity toward a single CO_(2)reduction product/fraction should be further improved at an industrially relevant CO_(2)conversion rate with considerable stability in the future.

关键词： CO_(2)conversion CO_(2)hydrogenation CO_(2)electroreduction Chemicals Fuels

Boosting CO_(2) electroreduction to formate via bismuth oxide clusters

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Nano Research 2023年第10期16卷 12050-12057页

作者： Xiaole Jiang Le Lin Youwen Rong Rongtan Li Qike Jiang Yaoyue Yang dunfeng gao Key Laboratory of Fundamental Chemistry of the State Ethnic Commission School of Chemistry and EnvironmentSouthwest Minzu UniversityChengdu 610041China State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China School of Science Dalian Maritime UniversityDalian 116026China University of Chinese Academy of Sciences Beijing 100049China

Supported metal(oxide)clusters,with both rich surface sites and high atom utilization efficiency,have shown improved activity and selectivity for many catalytic reactions over nanoparticle and single atom ***,the role of cluster catalysts has been rarely reported in CO_(2)electroreduction reaction(CO_(2)RR),which is a promising route for converting CO_(2)to liquid fuels like formic acid with renewable *** we develop a bismuth oxide(BiOn)cluster catalyst for highly efficient CO_(2)RR to *** BiOn cluster catalyst exhibits excellent activity,selectivity,and stability towards formate production,with a formate Faradaic efficiency of over 90%at a current density up to 500 mA·cm^(−2)in an alkaline membrane electrode assembly electrolyzer,corresponding to a mass activity as high as 3,750 A·gBi−*** electrolyzer with the BiOn cluster catalyst delivers a remarkable formate production rate of 0.56 mmol·min−1 at a high single-pass CO_(2)conversion of 44%.Density functional theory calculations indicate that Bi4O_(3)cluster is more favorable for stabilizing the HCOO^(*)intermediate than Bi(001)surface and single site BiC_(4)motif,rationalizing the improved formate production over the BiOn cluster *** work highlights the great importance of cluster catalysts in activity and selectivity control in electrocatalytic CO_(2)conversion.

关键词： CO_(2)electroreduction reaction formate bismuth oxide cluster catalyst membrane electrode assembly

Amorphous Sn(HPO_(4))_(2)-derived phosphorus-modified Sn/SnO_(x) core/shell catalyst for efficient CO_(2) electroreduction to formate

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Journal of Energy Chemistry 2023年第6期81卷 125-131,I0005页

作者： Chunfeng Cheng Tianfu Liu Yi Wang Pengfei Wei Jiaqi Sang Jiaqi Shao Yanpeng Song Yipeng Zang dunfeng gao Guoxiong Wang State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

Simultaneously achieving high activity,selectivity and stability for electrochemical CO_(2)reduction reaction(CO_(2)RR)remains great ***,a phosphorus-modified Sn/Sn Oxcore/shell(P-Sn/SnO_x)catalyst,derived from in situ electrochemical reduction of an amorphous Sn(HPO_(4))_(2) pre-catalyst,exhibits high CO_(2)RR *** total Faradaic efficiency(FE)of C_(1) products is close to 100%in a broad potential range from-0.49 to-1.02 V *** hydrogen electrode,and a total current density of 315.0 m A cm^(-2)is ***,the P-Sn/SnO_(x) catalyst maintains a formate FE of~90%for 120 *** functional theory calculations suggest that the phosphorus-modified Sn/SnO_(x) core/shell structure effectively facilitates formate production by enhancing CO_(2)adsorption and improving free energy profile of formate formation.

关键词： CO_(2)electroreduction Structural evolution Reaction intermediate Phosphorus modification Stability

Electrochemical synthesis of catalytic materials for energy catalysis

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Chinese Journal of Catalysis 2022年第4期43卷 1001-1016页

作者： dunfeng gao Hefei Li Pengfei Wei Yi Wang Guoxiong Wang Xinhe Bao State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

Electrocatalysis is a process dealing with electrochemical reactions in the interconversion of chemical energy and electrical *** synthesis of catalytically active nanostructures is one of the key challenges that hinder the practical application of many important energy‐related electrocatalytic *** with conventional wet‐chemical,solid‐state and vapor deposition synthesis,electrochemical synthesis is a simple,fast,cost‐effective and precisely controllable method for the preparation of highly efficient catalytic *** this review,we summarize recent progress in the electrochemical synthesis of catalytic materials such as single atoms,spherical and shaped nanoparticles,nanosheets,nanowires,core‐shell nanostructures,layered nanomaterials,dendritic nanostructures,hierarchically porous nanostructures as well as composite *** aspects of electrochemical synthesis and several main electrochemical synthesis methods are ***‐performance correlations between electrochemically synthesized catalysts and their unique electrocatalytic properties are exemplified using selected *** offer the reader with a basic guide to the synthesis of highly efficient catalysts using electrochemical methods,and we propose some research challenges and future opportunities in this field.

关键词： Catalytic material Electrochemical synthesis Electrocatalytic reaction Electrodeposition Cathodic corrosion Nanostructure

Ball-milling MoS_2/carbon black hybrid material for catalyzing hydrogen evolution reaction in acidic medium

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Journal of Energy Chemistry 2015年第5期24卷 608-613页

作者： Jiayuan Li dunfeng gao Jing Wang Shu Miao Guoxiong Wang Xinhe Bao State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences

Replacing platinum for catalyzing hydrogen evolution reaction （HER） in acidic medium remains great chal- lenges. Herein, we prepared few-layered MoS2 by ball milling as an efficient catalyst for HER in acidic medium, The activity of as-prepared MoS2 had a strong dependence on the ball milling time, Furthermore, Ketjen Black EC 300J was added into the ball-milled MoS2 followed by a second ball milling, and the resultant MoS2/carbon black hybrid material showed a much higher HER activity than MoS2 and carbon black alone. The enhanced activity of the MoS2/carbon black hybrid material was attributed to the increased abundance of catalytic edge sites of MoS） and excellent electrical coupling to the underlving carbon network.

关键词： Molybdenum disulfide Carbon black Hybrid material Ball milling Hydrogen evolution reaction Acidic medium

Gas-phase electrocatalytic reduction of carbon dioxide using electrolytic cell based on phosphoric acid-doped polybenzimidazole membrane

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Journal of Energy Chemistry 2014年第6期23卷 694-700页

作者： dunfeng gao Fan Cai Qinqin Xu Guoxiong Wang Xiulian Pan Xinhe Bao State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences

Carbon dioxide transformation to fuels or chemicals provides an attractive approach for its utilization as feedstock and its emission reduction. Herein, we report a gas-phase electrocatalytic reduction of CO2 in an electrolytic cell, constructed using phosphoric acid-doped polybenz- imidazole （PBI） membrane, which allowed operation at 170 ℃ Pt/C and PtMo/C with variable ratio of Pt/Mo were studied as the cathode catalysts. The results showed that PtMo/C catalysts significantly enhanced CO formation and inhibited CH4 formation compared with Pt/C catalyst. Characterization by X-ray diffraction, X-ray photoelectron spectroscopy and transmission electron microscopy revealed that most Mo species existed as MoO3 in PtMo/C catalysts and the interaction between Pt and MoOx was likely responsible for the enhanced CO formation rate although these bicomponent catalysts in general had a larger particle size than Pt/C catalyst.

关键词： carbon dioxide gas-phase electrocatalytic reduction platinum-molybdenum catalyst Faradaic efficiency formation rate

Copper-indium bimetallic catalysts for the selective electrochemical reduction of carbon dioxide

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Chinese Journal of Catalysis 2020年第9期41卷 1393-1400页

作者： Jiaqi Shao Yi Wang dunfeng gao Ke Ye Qi Wang Guoxiong Wang Key Laboratory of Superlight Materials and Surface Technology of Ministry of Education College of Materials Science and Chemical EngineeringHarbin Engineering UniversityHarbin 150001HeilongjiangChina State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Liaoning Key Materials Laboratory for Railway School of Materials and EngineeringDalian Jiaotong UniversityDalian 116028LiaoningChina

Copper-indium bimetallic catalysts with a dendritic structure are fabricated by a two-step electrodeposition method using a hydrogen evolution template for the CO2 electroreduction reaction(CO2RR).The dendritic Cu-In-30 catalyst electrodeposited for 30 min shows the highest specific surface area and exposes the most active sites,resulting in improved CO2RR *** dendritic Cu-In-30 catalyst exhibits distinctly higher formate partial current density(42.0 m A cm^-2)and Faradaic efficiency(87.4%)than those of the In-30 catalyst without the dendritic structure(the formate partial current density and Faradaic efficiency are 4.6 m A cm^-2 and 57.0%,respectively)at-0.85 V *** hydrogen electrode,ascribed to the increased specific surface *** Cu-In-30 catalyst can maintain stable performance for 12 h during the *** addition,the intrinsic current density of Cu-In-30 with the dendritic structure(4.8 m A cm^-2)is much higher than that of In-30 without the dendritic structure(2.1 m A cm^-2),indicating that the dendritic structure promotes the CO2RR,possibly due to additional coordination unsaturated atoms.

关键词： CO2 electroreduction reaction Copper Indium Electrodeposition Formate

CO2 electrolysis at industrial current densities using anion exchange membrane based electrolyzers

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Science China Chemistry 2020年第12期63卷 1711-1715页

作者： Pengfei Wei Hefei Li Long Lin dunfeng gao Xiaomin Zhang Huimin Gong Guangyan Qing Rui Cai Guoxiong Wang Xinhe Bao State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China

Significant progress on electrocatalytic CO2 reduction reaction (CO2RR) has been achieved in recent ***,the research and development of electrolyzer device for CO2RR is *** we use anion exchange membrane to develop zerogap electrolyzers for *** electrochemical properties of the electrolyzers with Pd/C and Cu cathodes are *** Pd/C cathode shows a current density of 200 mA cm^-2with CO Faradaic efficiency of 98%and energy efficiency of 48.8%,while the Cu cathode shows a current density of 350 mA cm^-2with total CO2RR Faradaic efficiency of 81.9%and energy efficiency of 30.5%.This work provides a promising demonstration of CO2 electrolyzer using anion exchange membrane for CO2 electrolysis at industrial current densities.

关键词： CO2 electrolysis electrolyzer industrial current density anion exchange membrane energy efficiency Pd/C catalyst Cu catalyst