Single-atom catalyst for high-performance methanol oxidation

Zhiqi Zhang; Jiapeng Liu; Jian Wang; Qi Wang; Yuhao Wang; Kai Wang; Zheng Wang; Meng Gu; Zhenghua Tang; Jongwoo Lim; Tianshou Zhao; Francesco Ciucci

doi:10.1038/s41467-021-25562-y

Single-atom catalyst for high-performance methanol oxidation

Nat Commun. 2021 Sep 2;12(1):5235. doi: 10.1038/s41467-021-25562-y.

Authors

Zhiqi Zhang^#¹, Jiapeng Liu^#¹, Jian Wang^#², Qi Wang³, Yuhao Wang¹, Kai Wang⁴, Zheng Wang¹, Meng Gu³, Zhenghua Tang⁴, Jongwoo Lim², Tianshou Zhao¹, Francesco Ciucci^{5

6}

Affiliations

¹ Department of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology, Hong Kong, China.
² Department of Chemistry, College of Science, Seoul National University, Seoul, South Korea.
³ Department of Materials Science and Engineering, Guangdong Provincial Key Laboratory of Energy Materials for Electric Power, Southern University of Science and Technology, Shenzhen, China.
⁴ Guangzhou Key Laboratory for Surface Chemistry of Energy Materials and New Energy Research Institute, School of Environment and Energy, South China University of Technology, Guangzhou Higher Education Mega Centre, Guangzhou, China.
⁵ Department of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology, Hong Kong, China. francesco.ciucci@ust.hk.
⁶ Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Hong Kong, China. francesco.ciucci@ust.hk.

^# Contributed equally.

Abstract

Single-atom catalysts have been widely investigated for several electrocatalytic reactions except electrochemical alcohol oxidation. Herein, we synthesize atomically dispersed platinum on ruthenium oxide (Pt₁/RuO₂) using a simple impregnation-adsorption method. We find that Pt₁/RuO₂ has good electrocatalytic activity towards methanol oxidation in an alkaline media with a mass activity that is 15.3-times higher than that of commercial Pt/C (6766 vs. 441 mA mg^‒1_Pt). In contrast, single atom Pt on carbon black is inert. Further, the mass activity of Pt₁/RuO₂ is superior to that of most Pt-based catalysts previously developed. Moreover, Pt₁/RuO₂ has a high tolerance towards CO poisoning, resulting in excellent catalytic stability. Ab initio simulations and experiments reveal that the presence of Pt‒O_3f (3-fold coordinatively bonded O)‒Ru_cus (coordinatively unsaturated Ru) bonds with the undercoordinated bridging O in Pt₁/RuO₂ favors the electrochemical dehydrogenation of methanol with lower energy barriers and onset potential than those encountered for Pt‒C and Pt‒Ru.

Grants and funding

201807010074/Guangzhou Science and Technology Program key projects