Plasmon-Enhanced C-C Bond Cleavage toward Efficient Ethanol Electrooxidation

Yan Wei; Zijie Mao; Xian-Yin Ma; Chao Zhan; Wen-Bin Cai

doi:10.1021/acs.jpclett.2c03292

Plasmon-Enhanced C-C Bond Cleavage toward Efficient Ethanol Electrooxidation

J Phys Chem Lett. 2022 Dec 8;13(48):11288-11294. doi: 10.1021/acs.jpclett.2c03292. Epub 2022 Nov 30.

Authors

Yan Wei¹, Zijie Mao¹, Xian-Yin Ma¹, Chao Zhan², Wen-Bin Cai¹

Affiliations

¹ Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Collaborative Innovation Center of Chemistry for Energy Materials, Department of Chemistry, Fudan University, Shanghai 200438, China.
² State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.

PMID: 36449387
DOI: 10.1021/acs.jpclett.2c03292

Abstract

Ethanol, as a sustainable biomass fuel, is endowed with the merits of theoretically high energy density and environmental friendliness yet suffers from sluggish kinetics and low selectivity toward the desired complete electrooxidation (C1 pathway). Here, the localized surface plasmon resonance (LSPR) effect is explored as a manipulating knob to boost electrocatalytic ethanol oxidation reaction in alkaline media under ambient conditions by appropriate visible light. Under illumination, Au@Pt nanoparticles with plasmonic core and active shell exhibit concurrently higher activity (from 2.30 to 4.05 A mg_Pt^-1 at 0.8 V vs RHE) and C1 selectivity (from 9 to 38% at 0.8 V). In situ attenuated total reflection-surface enhanced infrared absorption spectroscopy (ATR-SEIRAS) provides a molecular level insight into the LSPR promoted C-C bond cleavage and the subsequent CO oxidation. This work not only extends the methodology hyphenating plasmonic electrocatalysis and in situ surface IR spectroscopy but also presents a promising approach for tuning complex reaction pathways.