Synergized Cu/Pb Core/Shell Electrocatalyst for High-Efficiency CO2Reduction to C2+Liquids

Wang，Pengtang1,2; Yang，Hao3; Xu，Yong4; Huang，Xiaoqing1,2; Wang，Juan1; Zhong，Miao5; Cheng，Tao3; Shao，Qi1,6

2021-01-26

10.1021/acsnano.0c07869

ACS Nano   影响因子和分区

1936-0851

1936-086X

The design of efficient copper-based (Cu-based) carbon dioxide reduction (CO2RR) electrocatalysts is crucial for converting CO2 to value-added liquid products. In this work, we demonstrate that the strong synergy between Cu core and ultrathin lead (Pb) shell (0.7 nm) in the Cu/Pb core/shell nanocrystals (NCs, CuPb-0.7/C) significantly boosts the electrocatalytic reduction of CO2 toward C2+ products (products with at least two carbon atoms). Specifically, when applying in a flow cell system, the Faradaic efficiency (FE) of total C2+ products and the selectivity of C2+ liquid products are as high as 81.6% and 49.5%, respectively. Moreover, the current density of C2+ liquid products reaches 196.8 mA cm-2, outperforming most of the reported Cu-based catalysts for CO2RR toward the production of C2+ liquid products. Density functional theory calculations indicate that the synergized Cu/Pb core/shell NCs reduce the formation energies of*COOH and*OCCOH intermediates, as the two critical intermediates for the reduction of CO2 to CO and the formation of C2+ products, respectively, and leads to the significant increase in the selectivity of C2+ liquid products. This study provides a efficient Cu-based catalyst for the reduction of CO2, highlighting the importance of synergistic effect for the design of electrocatalysts in catalysis.

CO2reduction reaction copper core-shell lead synergy

SCI ; EI

英语

NI论文

其他

Ministry of Science and Technology["2017YFA0208200","2016YFA0204100"] ; National Natural Science Foundation of China[21571135,21905188,21975148] ; Natural Science Foundation of Jiangsu Higher Education Institutions[SBK20190810] ; Jiangsu Province Natural Science Fund for Distinguished Young Scholars[BK20170003] ; Jiangsu Province High-Level Talents[JNHB-106] ; China Postdoctoral Science Foundation["2019M651937","2019M660128"] ; Guangdong Provincial Key Laboratory of Energy Materials for Electric Power[2018B030322001]

Chemistry ; Science & Technology - Other Topics ; Materials Science

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:000613942700077

AMER CHEMICAL SOC

20210509872216

Carbon dioxide ; Density functional theory ; Efficiency ; Electrocatalysts ; Lead compounds ; Liquids ; Pollution control ; Product design

Chemical Agents and Basic Industrial Chemicals:803 ; Inorganic Compounds:804.2 ; Production Engineering:913.1 ; Probability Theory:922.1

2-s2.0-85100142299

Scopus

1.College of Chemistry,Chemical Engineering and Materials Science,Soochow University,Jiangsu,215123,China
2.College of Chemistry and Chemical Engineering,Xiamen University,Xiamen,361005,China
3.Institute of Functional Nano and Soft Materials (FUNSOM),Soochow University,Jiangsu,215123,China
4.Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage Devices,Collaborative Innovation Center of Advanced Energy Materials,School of Materials and Energy,Guangdong University of Technology,Guangzhou,510006,China
5.College of Engineering and Applied Sciences,Nanjing University,Jiangsu,215093,China
6.Guangdong Provincial Key Laboratory of Energy Materials for Electric Power,Southern University of Science and Technology,Shenzhen,518055,China

Wang，Pengtang,Yang，Hao,Xu，Yong,et al. Synergized Cu/Pb Core/Shell Electrocatalyst for High-Efficiency CO2Reduction to C2+Liquids[J]. ACS Nano,2021,15(1):1039-1047.

Wang，Pengtang.,Yang，Hao.,Xu，Yong.,Huang，Xiaoqing.,Wang，Juan.,...&Shao，Qi.(2021).Synergized Cu/Pb Core/Shell Electrocatalyst for High-Efficiency CO2Reduction to C2+Liquids.ACS Nano,15(1),1039-1047.

Wang，Pengtang,et al."Synergized Cu/Pb Core/Shell Electrocatalyst for High-Efficiency CO2Reduction to C2+Liquids".ACS Nano 15.1(2021):1039-1047.