Acta Phys. -Chim. Sin. ›› 2026, Vol. 42 ›› Issue (7): 100287.doi: 10.1016/j.actphy.2026.100287

• ARTICLE • Previous Articles     Next Articles

Charge redistribution on Pd mediated by electronically asymmetric carbon for boosting ethanol oxidation

Xincan Zhou1,2, Xueyao Wang1,3, Xiaokang Chen1,4, Di Lan2, Yuting Gao5, Xiaoxia Wang1, Daohao Li1, Shuchao Zhang1,6,*(), Lijie Zhang1,*(), Guanglei Wu1,*()   

  1. 1 State Key Laboratory of Bio-fibers and Eco-textiles, College of Materials Science and Engineering, Qingdao University, Qingdao 266237, Shandong Province, China
    2 School of Automotive Materials, Hubei University of Automotive Technology, Shiyan 442002, Hubei Province, China
    3 School of Environmental Science and Engineering, Shandong University, Qingdao 266237, Shandong Province, China
    4 Institute of Frontier Chemistry, School of Chemistry and Chemical Engineering, Shandong University, Qingdao 266237, Shandong Province, China
    5 Shandong Institute of Scientific and Technical Information, Jinan 250101, Shandong Province, China
    6 Department of Blood Transfusion, The Affiliated Hospital of Qingdao University, Qingdao University, Qingdao 266003, Shandong Province, China
  • Received:2025-12-19 Revised:2026-03-12 Accepted:2026-03-12 Published:2026-05-22
  • Contact: Email: zhangshuchao@qdu.edu.cn (Shuchao Zhang)lijiezh@qdu.edu.cn (Lijie Zhang)wuguanglei@qdu.edu.cn/wuguanglei@mail.xjtu.edu.cn (Guanglei Wu)

Abstract:

Pd-based materials as the promising catalysts for ethanol oxidation reaction (EOR) are still intrinsically limited by the surface electronic-structure trade-off between ethanol adsorption and CH3CO intermediate desorption. Herein, the Pd supported on N/S co-doped carbon (Pd@SNC) catalyst is synthesized, in which the doped S and N atoms could transfer moderate amounts electron to Pd, leading to opportune electron structure of Pd. Moreover, the moderate negative shift of d-band center demonstrate that the opportune Pd electron structure can strengthen adsorption of ethanol/OH− and promote the desorption of intermediate (CH3CO*), which may facilitate the kinetics. As a result, Pd@SNC exhibiting the highest catalytic activity for EOR (945.49 mA mgPd−1), surpassing to that of Pd@NC and Pd@C. Due to the fact that the electronic structure of Pd is properly regulated by co-doped N and S atoms, as shown by the theoretical calculation results, Pd@SNC exhibits the lowest reaction energy barrier of the dehydrogenation during the process of EOR.

Key words: Pd-based catalyst, Ethanol oxidation, Heteroatoms doping, Metal-support interaction, Electronic structure