Selective CO 2 Reduction to Ethylene Mediated by Adaptive Small-molecule Engineering of Copper-based Electrocatalysts.

Autor: Chen S; 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, P. R. China., Ye C; Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China., Wang Z; 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, P. R. China., Li P; 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, P. R. China., Jiang W; Qian Xuesen Laboratory of Space Technology, China Academy of Space Technology, Beijing, 100094, P. R. China., Zhuang Z; Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China., Zhu J; State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, International School of Materials Science and Engineering, Wuhan University of Technology, Wuhan, 430070, P. R China., Zheng X; Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China., Zaman S; Key Laboratory of Energy Conversion and Storage Technologies, Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen, 518055, P. R. China., Ou H; Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China., Lv L; State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, International School of Materials Science and Engineering, Wuhan University of Technology, Wuhan, 430070, P. R China., Tan L; Key Laboratory of Energy Conversion and Storage Technologies, Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen, 518055, P. R. China., Su Y; 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, P. R. China., Ouyang J; School of Biomedical Engineering, Guangzhou Medical University, Guangzhou, 511436, P. R. China., Wang D; Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2023 Dec 11; Vol. 62 (50), pp. e202315621. Date of Electronic Publication: 2023 Nov 13.
DOI: 10.1002/anie.202315621
Abstrakt: Electrochemical CO 2 reduction reaction (CO 2 RR) over Cu catalysts exhibits enormous potential for efficiently converting CO 2 to ethylene (C 2 H 4 ). However, achieving high C 2 H 4 selectivity remains a considerable challenge due to the propensity of Cu catalysts to undergo structural reconstruction during CO 2 RR. 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 2 reduction to C 2 H 4 products. An excellent Faraday efficiency (FE) of 63.6 % on C 2 H 4 with a current density of 497.2 mA cm -2 in flow cell was achieved, about 6.5 times higher than the pristine Cu catalyst which mainly produce CH 4 . The in situ X-ray absorption spectroscopy and Raman studies reveal that the hydroxyl group in TA stabilizes Cu δ+ during the CO 2 RR. Furthermore, theoretical calculations demonstrate that the Cu δ+ /Cu 0 interfaces lower the activation energy barrier for *CO dimerization, and hydroxyl species stabilize the *COH intermediate via hydrogen bonding, thereby promoting C 2 H 4 production. Such molecule engineering modulated electronic structure provides a promising strategy to achieve highly selective CO 2 reduction to value-added chemicals.
(© 2023 Wiley-VCH GmbH.)
Databáze: MEDLINE
Externí odkaz: