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 and Francesco Ciucci ()
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Zhiqi Zhang: Department of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology
Jiapeng Liu: Department of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology
Jian Wang: Seoul National University
Qi Wang: Southern University of Science and Technology
Yuhao Wang: Department of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology
Kai Wang: South China University of Technology, Guangzhou Higher Education Mega Centre
Zheng Wang: Department of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology
Meng Gu: Southern University of Science and Technology
Zhenghua Tang: South China University of Technology, Guangzhou Higher Education Mega Centre
Jongwoo Lim: Seoul National University
Tianshou Zhao: Department of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology
Francesco Ciucci: Department of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: 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‒1Pt). 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‒O3f (3-fold coordinatively bonded O)‒Rucus (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.

Date: 2021
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DOI: 10.1038/s41467-021-25562-y

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