Atomically dispersed Lewis acid sites boost 2-electron oxygen reduction activity of carbon-based catalysts

Qihao Yang, Wenwen Xu, Shun Gong, Guokui Zheng, Ziqi Tian (), Yujie Wen, Luming Peng, Linjuan Zhang, Zhiyi Lu () and Liang Chen ()
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Qihao Yang: Chinese Academy of Sciences
Wenwen Xu: Chinese Academy of Sciences
Shun Gong: Chinese Academy of Sciences
Guokui Zheng: Chinese Academy of Sciences
Ziqi Tian: Chinese Academy of Sciences
Yujie Wen: Nanjing University
Luming Peng: Nanjing University
Linjuan Zhang: Chinese Academy of Sciences
Zhiyi Lu: Chinese Academy of Sciences
Liang Chen: Chinese Academy of Sciences

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: Abstract Elucidating the structure-property relationship is crucial for the design of advanced electrocatalysts towards the production of hydrogen peroxide (H2O2). In this work, we theoretically and experimentally discovered that atomically dispersed Lewis acid sites (octahedral M–O species, M = aluminum (Al), gallium (Ga)) regulate the electronic structure of adjacent carbon catalyst sites. Density functional theory calculation predicts that the octahedral M–O with strong Lewis acidity regulates the electronic distribution of the adjacent carbon site and thus optimizes the adsorption and desorption strength of reaction intermediate (*OOH). Experimentally, the optimal catalyst (oxygen-rich carbon with atomically dispersed Al, denoted as O-C(Al)) with the strongest Lewis acidity exhibited excellent onset potential (0.822 and 0.526 V versus reversible hydrogen electrode at 0.1 mA cm−2 H2O2 current in alkaline and neutral media, respectively) and high H2O2 selectivity over a wide voltage range. This study provides a highly efficient and low-cost electrocatalyst for electrochemical H2O2 production.

Date: 2020
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DOI: 10.1038/s41467-020-19309-4

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