Single-atom catalyst for high-performance methanol oxidation

Published in Nature Communications, 2021

Recommended citation: 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*. (2021). "Single-atom catalyst for high-performance methanol oxidation." Nature Communications, 12(1), 1-9. https://www.nature.com/articles/s41467-021-25562-y

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.

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Recommended citation: Zhang, Z., Liu, J., Wang, J., Wang, Q., Wang, Y., Wang, K., Wang, Z., Gu, M., Tang, Z., Lim, J., Zhao, T. and Ciucci, F., 2021. Single-atom catalyst for high-performance methanol oxidation. Nature Communications, 12(1), 1-9.