Selective CO2 Reduction to Ethylene Mediated by Adaptive Small-molecule Engineering of Copper-based Electrocatalysts

Chen，Shenghua1; Ye，Chengliang2; Wang，Ziwei4; Li，Peng4; Jiang，Wenjun5; Zhuang，Zechao2; Zhu，Jiexin6; Zheng，Xiaobo2; Zaman，Shahid7; Ou，Honghui2; Lv，Lei6; Tan，Lin7; Su，Yaqiong4; Ouyang，Jiang3; Wang，Dingsheng2

2023-12-11

10.1002/anie.202315621

Angewandte Chemie - International Edition   影响因子和分区

1433-7851

1521-3773

Electrochemical CO reduction reaction (CORR) over Cu catalysts exhibits enormous potential for efficiently converting CO to ethylene (CH). However, achieving high CH selectivity remains a considerable challenge due to the propensity of Cu catalysts to undergo structural reconstruction during CORR. Herein, we report an in situ molecule modification strategy that involves tannic acid (TA) molecules adaptive regulating the reconstruction of a Cu-based material to a pathway that facilitates CO reduction to CH products. An excellent Faraday efficiency (FE) of 63.6 % on CH with a current density of 497.2 mA cm in flow cell was achieved, about 6.5 times higher than the pristine Cu catalyst which mainly produce CH. The in situ X-ray absorption spectroscopy and Raman studies reveal that the hydroxyl group in TA stabilizes Cu during the CORR. Furthermore, theoretical calculations demonstrate that the Cu/Cu interfaces lower the activation energy barrier for *CO dimerization, and hydroxyl species stabilize the *COH intermediate via hydrogen bonding, thereby promoting CH production. Such molecule engineering modulated electronic structure provides a promising strategy to achieve highly selective CO reduction to value-added chemicals.

C2H4 CO2RR Cuδ+/Cu0 Hydrogen Bonding TA Molecule

SCI ; EI

英语

NI论文

其他

WOS:001103748100001

20234615062332

Activation energy ; Carbon dioxide ; Catalyst selectivity ; Copper ; Electrocatalysts ; Electronic structure ; Hydrogen bonds ; Molecules ; Reduction ; X ray absorption spectroscopy

Copper:544.1 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Inorganic Compounds:804.2 ; Atomic and Molecular Physics:931.3

CHEMISTRY

2-s2.0-85176297387

Scopus

1.National Innovation Platform (Center) for Industry-Education Integration of Energy Storage Technology,School of Chemical Engineering and Technology,Xi'an Jiaotong University,Xi'an,710049,China
2.Engineering Research Center of Advanced Rare Earth Materials,Department of Chemistry,Tsinghua University,Beijing,100084,China
3.School of Biomedical Engineering,Guangzhou Medical University,Guangzhou,511436,China
4.School of Chemistry,Xi'an Key Laboratory of Sustainable Energy Materials Chemistry,State Key Laboratory of Electrical Insulation and Power Equipment,Engineering Research Center of Energy Storage Materials and Devices,Ministry of Education,Xi'an Jiaotong University,Xi'an,710049,China
5.Qian Xuesen Laboratory of Space Technology,China Academy of Space Technology,Beijing,100094,China
6.State Key Laboratory of Advanced Technology for Materials Synthesis and Processing,International School of Materials Science and Engineering,Wuhan University of Technology,Wuhan,430070,China
7.Key Laboratory of Energy Conversion and Storage Technologies,Department of Mechanical and Energy Engineering,Southern University of Science and Technology,Shenzhen,518055,China

Chen，Shenghua,Ye，Chengliang,Wang，Ziwei,et al. Selective CO2 Reduction to Ethylene Mediated by Adaptive Small-molecule Engineering of Copper-based Electrocatalysts[J]. Angewandte Chemie - International Edition,2023,62(50).

Chen，Shenghua.,Ye，Chengliang.,Wang，Ziwei.,Li，Peng.,Jiang，Wenjun.,...&Wang，Dingsheng.(2023).Selective CO2 Reduction to Ethylene Mediated by Adaptive Small-molecule Engineering of Copper-based Electrocatalysts.Angewandte Chemie - International Edition,62(50).

Chen，Shenghua,et al."Selective CO2 Reduction to Ethylene Mediated by Adaptive Small-molecule Engineering of Copper-based Electrocatalysts".Angewandte Chemie - International Edition 62.50(2023).