Modulating the d-Band Center of Palladium via Ethylene Glycol Modification: Accelerating Had Desorption for Enhanced Formate Electrooxidation

Zheng Tang; Lanlan Shi; Kaixin Zhang; Feike Zhang; Yanfei Sun; Xiaoxuan Wang; Yebo Yao; Xia Liu; Dewei Wang; Jiangzhou Xie; Zhiyu Yang; Yi-Ming Yan

doi:10.1021/acs.jpclett.4c00127

Modulating the d-Band Center of Palladium via Ethylene Glycol Modification: Accelerating H_ad Desorption for Enhanced Formate Electrooxidation

J Phys Chem Lett. 2024 Mar 28;15(12):3354-3362. doi: 10.1021/acs.jpclett.4c00127. Epub 2024 Mar 18.

Authors

Affiliations

¹ State Key Laboratory of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, People's Republic of China.
² School of Mechanical and Manufacturing Engineering, University of New South Wales, Sydney, New South Wales 2052, Australia.

PMID: 38498427
DOI: 10.1021/acs.jpclett.4c00127

Abstract

This study addresses the critical challenge in alkaline direct formate fuel cells (DFFCs) of slow formate oxidation reaction (FOR) kinetics as a result of strong hydrogen intermediate (H_ad) adsorption on Pd catalysts. We developed WO₃-supported Pd nanoparticles (EG-Pd/WO₃) via an organic reduction method using ethylene glycol (EG), aiming to modulate the d-band center of Pd and alter H_ad adsorption dynamics. Cyclic voltammetry demonstrated significantly improved H_ad desorption kinetics in EG-Pd/WO₃ catalysts. Density functional theory (DFT) calculations revealed that the presence of EG reduces the d-band center of Pd, leading to weaker Pd-H bonds and enhanced H_ad desorption during the FOR. This research provides a new approach to optimize catalyst efficiency in DFFCs, highlighting the potential for more effective and sustainable energy solutions through advanced material engineering.