Journal of Energy Chemistry ›› 2023, Vol. 79 ›› Issue (4): 550-558.DOI: 10.1016/j.jechem.2023.01.026

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Self-catalytic induced interstitial C-doping of Pd nanoalloys for highly selective electrocatalytic dehydrogenation of formic acid

Jun Lia,b,c, Liying Caia, Xiaosi Lianga, Shuke Huanga, Xiaosha Wanga, Yongshuai Kanga, Yongjian Zhaoa, Lei Zhanga, Chenyang Zhaoa,*   

  1. aCollege of chemistry and environmental engineering, Shenzhen University, Shenzhen 518071, Guangdong, China;
    bKey laboratory of optoelectronic devices and systems of ministry of education and Guangdong province, College of physics and optoelectronic engineering, Shenzhen University, Shenzhen 518067, Guangdong, China;
    cCollege of chemistry and environmental engineering, Hanshan Normal University, Chaozhou 521041, Guangdong, China
  • Received:2022-11-02 Revised:2023-01-05 Accepted:2023-01-16 Online:2023-04-15 Published:2023-05-30
  • Contact: * E-mail address: cyzhao@szu.edu.cn (C. Zhao).

Abstract: Light-metalloid-atom-doped Pd interstitial nanoalloy is promising candidate for electrocatalysis because of the favorable electronic effect. Herein, an innovative method was developed to synthesize C-doped Pd interstitial nanoalloy using palladium acetate both as metal precursor and C dopant. Elaborate character-izations demonstrated that C atoms were successfully doped into the Pd lattice via self-catalytic decom-position of acetate ions. The as-synthesized C-doped Pd catalysts showed excellent activity and durable stability for formic acid electrooxidation. The mass activity and specific activity at 0.6 V of C-doped Pd were approximately 2.59 A/mg and 3.50 mA cm-2, i.e., 2.4 and 2.6 times of Pd, respectively. DFT calcu-lations revealed that interstitial doping with C atoms induced differentiation of Pd sites. The strong non-covalent interaction between the Pd sites and the key intermediates endowed Pd with high-selectivity to direct routes and enhanced CO tolerance. This work presents a sites-differentiation strategy for metallic catalysts to improve the electrocatalysis.

Key words: C-doped Palladium, Interstitial nanoalloy, Electrocatalysis, Formic acid oxidation reaction