Fast site-to-site electron transfer of high-entropy alloy nanocatalyst driving redox electrocatalysis

Hongdong Li; Yi Han; Huan Zhao; Wenjing Qi; Dan Zhang; Yaodong Yu; Wenwen Cai; Shaoxiang Li; Jianping Lai; Bolong Huang; Lei Wang

doi:10.1038/s41467-020-19277-9

Fast site-to-site electron transfer of high-entropy alloy nanocatalyst driving redox electrocatalysis

Nat Commun. 2020 Oct 28;11(1):5437. doi: 10.1038/s41467-020-19277-9.

Authors

Hongdong Li¹, Yi Han¹, Huan Zhao¹, Wenjing Qi², Dan Zhang^{1

3}, Yaodong Yu¹, Wenwen Cai¹, Shaoxiang Li³, Jianping Lai⁴, Bolong Huang⁵, Lei Wang^{6

7}

Affiliations

¹ Key Laboratory of Eco-chemical Engineering, Key Laboratory of Optic-electric Sensing and Analytical Chemistry of Life Science, Taishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and Technology, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, 266042, Qingdao, P. R. China.
² College of Chemistry, Chongqing Normal University, 401331, Chongqing, P. R. China.
³ Shandong Engineering Research Center for Marine Environment Corrosion and Safety Protection, College of Environment and Safety Engineering, Qingdao University of Science and Technology, 266042, Qingdao, P. R. China.
⁴ Key Laboratory of Eco-chemical Engineering, Key Laboratory of Optic-electric Sensing and Analytical Chemistry of Life Science, Taishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and Technology, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, 266042, Qingdao, P. R. China. jplai@qust.edu.cn.
⁵ Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong SAR, China. bhuang@polyu.edu.hk.
⁶ Key Laboratory of Eco-chemical Engineering, Key Laboratory of Optic-electric Sensing and Analytical Chemistry of Life Science, Taishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and Technology, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, 266042, Qingdao, P. R. China. inorchemwl@126.com.
⁷ Shandong Engineering Research Center for Marine Environment Corrosion and Safety Protection, College of Environment and Safety Engineering, Qingdao University of Science and Technology, 266042, Qingdao, P. R. China. inorchemwl@126.com.

Abstract

Designing electrocatalysts with high-performance for both reduction and oxidation reactions faces severe challenges. Here, the uniform and ultrasmall (~3.4 nm) high-entropy alloys (HEAs) Pt₁₈Ni₂₆Fe₁₅Co₁₄Cu₂₇ nanoparticles are synthesized by a simple low-temperature oil phase strategy at atmospheric pressure. The Pt₁₈Ni₂₆Fe₁₅Co₁₄Cu₂₇/C catalyst exhibits excellent electrocatalytic performance for hydrogen evolution reaction (HER) and methanol oxidation reaction (MOR). The catalyst shows ultrasmall overpotential of 11 mV at the current density of 10 mA cm^-2, excellent activity (10.96 A mg^-1_Pt at -0.07 V vs. reversible hydrogen electrode) and stability in the alkaline medium. Furthermore, it is also the efficient catalyst (15.04 A mg^-1_Pt) ever reported for MOR in alkaline solution. Periodic DFT calculations confirm the multi-active sites for both HER and MOR on the HEA surface as the key factor for both proton and intermediate transformation. Meanwhile, the construction of HEA surfaces supplies the fast site-to-site electron transfer for both reduction and oxidation processes.

Abstract

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