Single-atom catalyst for high-performance methanol oxidation

Zhiqi Zhang(Hong Kong University of Science and Technology), Jiapeng Liu(Hong Kong University of Science and Technology), Jian Wang(Seoul National University), Qi Wang(Southern University of Science and Technology), Yuhao Wang(Hong Kong University of Science and Technology), Kai Wang(Energy Research Institute), Zheng Wang(Hong Kong University of Science and Technology), Meng Gu(Southern University of Science and Technology), Zhenghua Tang(Energy Research Institute), Jongwoo Lim(Seoul National University), Tianshou Zhao(Hong Kong University of Science and Technology), Francesco Ciucci(Hong Kong University of Science and Technology)
Nature Communications
September 2, 2021
Cited by 251Open Access
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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 (Pt 1 /RuO 2 ) using a simple impregnation-adsorption method. We find that Pt 1 /RuO 2 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 Pt 1 /RuO 2 is superior to that of most Pt-based catalysts previously developed. Moreover, Pt 1 /RuO 2 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 Pt 1 /RuO 2 favors the electrochemical dehydrogenation of methanol with lower energy barriers and onset potential than those encountered for Pt‒C and Pt‒Ru.


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