Electrochemically stable frustrated Lewis pairs on dual-metal hydroxides for electrocatalytic CO2 reduction

Weining Zhang; Yuandong Yan; Jing Wang; Zhenhua Yang; Taozhu Li; Hu Li; Shicheng Yan; Tao Yu; Weiliu Fan; Zhigang Zou

doi:10.1039/d3dt00144j

Electrochemically stable frustrated Lewis pairs on dual-metal hydroxides for electrocatalytic CO₂ reduction

Dalton Trans. 2023 May 30;52(21):7129-7135. doi: 10.1039/d3dt00144j.

Authors

Weining Zhang^{1

2

3}, Yuandong Yan², Jing Wang⁴, Zhenhua Yang², Taozhu Li², Hu Li², Shicheng Yan², Tao Yu¹, Weiliu Fan⁴, Zhigang Zou^{1

2}

Affiliations

¹ Collaborative Innovation Center of Advanced Microstructures, Jiangsu Key Laboratory for Nano Technology, National Laboratory of Solid State Microstructures, School of Physics, Nanjing University, No. 22 Hankou Road, Nanjing, Jiangsu 210093, P. R. China.
² Eco-materials and Renewable Energy Research Center (ERERC), Collaborative Innovation Center of Advanced Microstructures, College of Engineering and Applied Sciences, Nanjing University, No. 22 Hankou Road, Nanjing, Jiangsu 210093, P. R. China. yscfei@nju.edu.cn.
³ School of Physics and Physical Engineering, Qufu Normal University, Qufu 273165, P. R. China.
⁴ School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, P. R. China.

PMID: 37159243
DOI: 10.1039/d3dt00144j

Abstract

The sluggish kinetics of CO₂ activation and reduction severely limit the energy conversion efficiency of electrocatalytic CO₂ reduction into fuels. Here, ZnSn(OH)₆ with an alternating arrangement of Zn(OH)₆ and Sn(OH)₆ octahedral units and SrSn(OH)₆ with an alternating arrangement of SrO₆ and Sn(OH)₆ octahedral units were adopted to check the effects of frustrated Lewis pairs (FLPs) on electrochemical CO₂ reduction. The FLPs were in situ electrochemically reconstructed on ZnSn(OH)₆ by reducing the electrochemically unstable Sn-OH to Sn-oxygen vacancies (Sn-O_Vs) as a Lewis acid site, which are able to create strong interactions with the adjacent electrochemically stable Zn-OH, a Lewis base site. Compared to SrSn(OH)₆ without FLPs, the higher formate selectivity of ZnSn(OH)₆ originates from the strong ability of FLPs to capture protons and activate CO₂via the electrostatic field of FLPs triggering better electron transfer and strong orbital interactions under negative potentials. Our findings may guide the design of electrocatalysts for CO₂ reduction with high catalytic performances.