Ternary Sn-Ti-O Electrocatalyst Boosts the Stability and Energy Efficiency of CO2 Reduction

Guobin Wen; Bohua Ren; Moon G Park; Jie Yang; Haozhen Dou; Zhen Zhang; Ya-Ping Deng; Zhengyu Bai; Lin Yang; Jeff Gostick; Gianluigi A Botton; Yongfeng Hu; Zhongwei Chen

doi:10.1002/anie.202004149

Ternary Sn-Ti-O Electrocatalyst Boosts the Stability and Energy Efficiency of CO₂ Reduction

Angew Chem Int Ed Engl. 2020 Jul 27;59(31):12860-12867. doi: 10.1002/anie.202004149. Epub 2020 Jun 3.

Authors

Guobin Wen^{1

2}, Bohua Ren², Moon G Park², Jie Yang³, Haozhen Dou², Zhen Zhang², Ya-Ping Deng², Zhengyu Bai¹, Lin Yang¹, Jeff Gostick², Gianluigi A Botton^{3

4}, Yongfeng Hu⁴, Zhongwei Chen²

Affiliations

¹ School of Chemistry and Chemical Engineering, Key Laboratory of Green Chemical Media and Reactions, Ministry of Education, Henan Normal University, Xinxiang, 453007, China.
² Department of Chemical Engineering, Waterloo Institute for Nanotechnology, Waterloo Institute for Sustainable Energy, University of Waterloo, Waterloo, Ontario, N2L 3G1, Canada.
³ Department of Materials Science and Engineering and Canadian Centre for Electron Microscopy, McMaster University, 1280 Main Street West, Hamilton, Ontario, L8S 4M1, Canada.
⁴ Canadian Light Source, University of Saskatchewan, Saskatoon, Saskatchewan, S7N 0X4, Canada.

PMID: 32379944
DOI: 10.1002/anie.202004149

Abstract

Simultaneously improving energy efficiency (EE) and material stability in electrochemical CO₂ conversion remains an unsolved challenge. Among a series of ternary Sn-Ti-O electrocatalysts, 3D ordered mesoporous (3DOM) Sn_0.3 Ti_0.7 O₂ achieves a trade-off between active-site exposure and structural stability, demonstrating up to 71.5 % half-cell EE over 200 hours, and a 94.5 % Faradaic efficiency for CO at an overpotential as low as 430 mV. DFT and X-ray absorption fine structure analyses reveal an electron density reconfiguration in the Sn-Ti-O system. A downshift of the orbital band center of Sn and a charge depletion of Ti collectively facilitate the dissociative adsorption of the desired intermediate COOH* for CO formation. It is also beneficial in maintaining a local alkaline environment to suppress H₂ and formate formation, and in stabilizing oxygen atoms to prolong durability. These findings provide a new strategy in materials design for efficient CO₂ conversion and beyond.

Keywords: carbon dioxide fixation; electrochemistry; interfaces; materials science; mesoporous materials.

Abstract

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