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Formic acid oxidation (FAO) is a typical anode reaction in fuel cells that can be facilitated by modulating its direct and indirect reaction pathways. Herein, PtAu bimetallic nanoparticles loaded onto Co and N co-doping carbon nanoframes (CoNC NFs) were designed to improve the selectivity of the direct reaction pathway for efficient FAO. Based on these subtle nanomaterials, the influences of elemental composition and carbon-support materials on the two pathways of FAO were investigated in detail. The results of fuel cell tests verified that the appropriate amount of Au in PtAu/CoNC can promote a direct reaction pathway for FAO, which is crucial for enhancing the oxidation efficiency of formic acid. In particular, the obtained PtAu/CoNC with an optimal Pt/Au atomic ratio of 1:1 (PtAu/CoNC-3) manifests the best catalytic performance among the analogous obtained Pt-based electrocatalysts. The FAO mass activity of the PtAu/CoNC-3 sample reached 0.88 A·mgPt−1, which is 26.0 times higher than that of Pt/C. The results of first-principles calculation and CO stripping jointly demonstrate that the CO adsorption of PtAu/CoNC is considerably lower than that of Pt/CoNC and PtAu/C, which indicates that the synergistic effect of Pt, Au, and CoNC NFs is critical for the resistance of Pt to CO poisoning. This work is of great significance for a deeper understanding of the oxidation mechanism of formic acid and provides a feasible and promising strategy for enhancing the catalytic performance of the catalyst by improving the direct reaction pathway for FAO.

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Publication history

Received: 23 February 2021
Revised: 18 May 2021
Accepted: 30 May 2021
Published: 01 July 2021
Issue date: February 2022

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© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021

Acknowledgements

Acknowledgements

Thanks for the financial support from the National Natural Science Foundation of China (Nos. 51801188, 12034002, and 51971025), the China Postdoctoral Science Foundation (No. 2018M632792), program for the Innovation Team of Science and Technology in University of Henan (No. 20IRTSTHN014), Excellent Youth Foundation of He'nan Scientific Committee (No. 202300410356), the CAS Interdisciplinary Innovation Team (No. JCTD-2019-01), and Beijing Natural Science Foundation (No. 2204085). The Center of Advanced Analysis & Gene Sequencing of Zhengzhou University is acknowledged for providing characterization facilities. Shanghai Synchrotron Radiation Facility (SSRF) is acknowledged for providing X-ray absorption near edge structure (XANES) test at the BL11B beamline.

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Email: nanores@tup.tsinghua.edu.cn

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