Manipulating Cu Nanoparticle Surface Oxidation States Tunes Catalytic Selectivity toward CH4 or C2+ Products in CO2 Electroreduction

Fan, Qikui1,2; Zhang, Xue3; Ge, Xiaohu4; Bai, Licheng3; He, Dongsheng5; Qu, Yunteng6; Kong, Chuncai7; Bi, Jinglei7; Ding, Dawei8; Cao, Yueqiang4; Duan, Xuezhi4; Wang, Jin1; Yang, Jian1; Wu, Yuen6

2021-08-01

10.1002/aenm.202101424

Advanced Energy Materials   影响因子和分区

1614-6832

1614-6840

Herein, a facile seed-assisted strategy for preparing Cu nanoparticles (NPs) with polyvinyl pyrrolidone (PVP) capping is presented. Compared to the Cu NPs with deficient PVP protection, the Cu NPs capped with a sufficient amount of PVP remain almost completely as Cu-0 species. In contrast, the Cu NPs that are considered PVP deficient form an oxide structure in which the inner layer is face-centered cubic Cu and the outer layer is, at least in part, made up of Cu2O species. Furthermore, to eliminate CO2 molecule diffusion and simultaneously obtain significant current density (200 mA cm(-2)) for industrial applications, a flow cell configuration is used for carbon dioxide electro reduction reaction (CO2RR) testing in 0.5 m potassium hydroxide solution. The Cu NPs with zero valence deliver Faradaic efficiencies (FEs) for the CO2 reduction to CH4 of over 70%, with a current density exceeding 200 mA cm(-2), outstripping the performances of the majority of the reported CO2 electrocatalysts. Interestingly, the distribution of products catalyzed by the Cu NPs with +1 valence includes multicarbon products (C2+) such as C2H4, C2H5OH, CH3COOH, and C3H7OH with combined FEs of >80%, with current densities of up to 300 mA cm(-2). The above results unambiguously establish that surface oxidation of Cu species plays a crucial role in the CO2RR.

CO (2) electroreduction Cu nanoparticles Cu oxidation

SCI ; EI

英语

其他

Guangdong Basic and Applied Basic Research Foundation[2020A1515110499] ; Shenzhen University Young Teacher Research Project[000002110713] ; National Natural Science Foundation of China[22022508,22008251] ; Guangdong Natural Science Fund for Distinguished Young Scholars[2016A030306020] ; Shaanxi Natural Science Basic Research Program[2020JZ-03] ; China Postdoctoral Science Foundation["2019M663690","2020M682869"] ; Shenzhen Science and Technology Research Funding[JCYJ20180302145547204]

Chemistry ; Energy & Fuels ; Materials Science ; Physics

Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:000681243500001

WILEY-V C H VERLAG GMBH

20213210727394

Acetic acid ; Carbon dioxide ; Catalytic oxidation ; Copper oxides ; Current density ; Electrocatalysts ; Electrolytic reduction ; Nanoparticles ; Oxide minerals ; Potassium hydroxide

Minerals:482.2 ; Ore Treatment:533.1 ; Copper:544.1 ; Electricity: Basic Concepts and Phenomena:701.1 ; Nanotechnology:761 ; Chemical Agents and Basic Industrial Chemicals:803 ; Organic Compounds:804.1 ; Inorganic Compounds:804.2 ; Solid State Physics:933

Web of Science

1.Shenzhen Univ, Shenzhen Key Lab Special Funct Mat, Guangdong Res Ctr Interfacial Engn Funct Mat, Coll Mat Sci & Engn, 1066 Xueyuan Ave, Shenzhen 518071, Guangdong, Peoples R China
2.Shenzhen Univ, Key Lab Optoelect Devices & Syst, Coll Phys & Optoelect Engn Inst, 3688 Nanhai Ave, Shenzhen 518060, Guangdong, Peoples R China
3.Chinese Acad Sci, Ctr Mat & Interfaces, Shenzhen Inst Adv Technol, 1068 Xueyuan Ave, Shenzhen 518055, Guangdong, Peoples R China
4.East China Univ Sci & Technol, State Key Lab Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China
5.Southern Univ Sci & Technol China, Core Res Facil, Southern Univ Sci & Technol, 1088 Xueyuan Ave, Shenzhen 518055, Guangdong, Peoples R China
6.Univ Sci & Technol China, Sch Chem & Mat Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Hefei Natl Lab Phys Sci Microscale, 96 JinZhaiRoad Baohe Dist, Hefei 230026, Peoples R China
7.Xi An Jiao Tong Univ, Sch Phys, MOE Key Lab Nonequilibrium Synth & Modulat Conden, Key Lab Adv Mat & Mesoscop Phys Shaanxi Prov,Sch, 28 Xianning West Rd, Xian 710049, Shaanxi, Peoples R China
8.Xi An Jiao Tong Univ, Sch Chem, State Key Lab Elect Insulat & Power Equipment, 28 Xianning West Rd, Xian 710049, Shaanxi, Peoples R China

Fan, Qikui,Zhang, Xue,Ge, Xiaohu,et al. Manipulating Cu Nanoparticle Surface Oxidation States Tunes Catalytic Selectivity toward CH4 or C2+ Products in CO2 Electroreduction[J]. Advanced Energy Materials,2021,11.

Fan, Qikui.,Zhang, Xue.,Ge, Xiaohu.,Bai, Licheng.,He, Dongsheng.,...&Wu, Yuen.(2021).Manipulating Cu Nanoparticle Surface Oxidation States Tunes Catalytic Selectivity toward CH4 or C2+ Products in CO2 Electroreduction.Advanced Energy Materials,11.

Fan, Qikui,et al."Manipulating Cu Nanoparticle Surface Oxidation States Tunes Catalytic Selectivity toward CH4 or C2+ Products in CO2 Electroreduction".Advanced Energy Materials 11(2021).