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

Dalton Trans

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.

Published: May 2023

AI Article Synopsis

  • The activation and reduction of CO are hindered by slow kinetics, affecting energy conversion efficiency in electrocatalytic processes.
  • Researchers examined ZnSn(OH) and SrSn(OH) to study the impact of frustrated Lewis pairs (FLPs) on CO reduction, leading to enhanced catalytic properties.
  • The electrochemical reconstruction of ZnSn(OH) generated Lewis acid-base interactions, resulting in improved formate selectivity and better electron transfer during CO activation compared to SrSn(OH) without FLPs.

Article Abstract

The sluggish kinetics of CO activation and reduction severely limit the energy conversion efficiency of electrocatalytic CO reduction into fuels. Here, ZnSn(OH) with an alternating arrangement of Zn(OH) and Sn(OH) octahedral units and SrSn(OH) with an alternating arrangement of SrO and Sn(OH) octahedral units were adopted to check the effects of frustrated Lewis pairs (FLPs) on electrochemical CO reduction. The FLPs were electrochemically reconstructed on ZnSn(OH) by reducing the electrochemically unstable Sn-OH to Sn-oxygen vacancies (Sn-O) 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) without FLPs, the higher formate selectivity of ZnSn(OH) originates from the strong ability of FLPs to capture protons and activate CO 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 CO reduction with high catalytic performances.

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http://dx.doi.org/10.1039/d3dt00144jDOI Listing

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