DataVXACS Applied Materials & InterfacesPaper
journal article·2023-03-01Open access

External-Shell Oxygen Enabling the Local Environment Modulation of Unsaturated NbN3 for Efficient Electrosynthesis of Hydrogen Peroxide

Dingding Li, Run-Xi Zhu, Zheng Han, Lei Bai, Jianting Zhang, Ruixin Xu, Weilong Ma, Liangpeng Nie, Yi Wang, Jinbo Bai, Hang Zhao, Ji-Quan Liu, Kunyue Leng, Ya-Qiong Su, Yunteng Qu

ACS Applied Materials & Interfaces· Volume 15· Issue 8
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Source abstract

Abstract

Single-atom catalysts with a tunable coordination structure have shown grand potential in flexibly altering the selectivity of oxygen reduction reaction (ORR) toward the desired pathway. However, rationally mediating the ORR pathway by modulating the local coordination number of the single-metal sites is still challenging. Herein, we prepare the Nb single-atom catalysts (SACs) with an external-shell oxygen-modulated unsaturated NbN 3 site in carbon nitride and the NbN 4 site anchored in nitrogen-doped carbon carriers, respectively. Compared with typical NbN 4 moieties for 4e – ORR, the as-prepared NbN 3 SACs exhibit excellent 2e – ORR activity in 0.1 M KOH, with the onset overpotential close to zero (9 mV) and the H 2 O 2 selectivity above 95%, making it one of the state-of-the-art catalysts in the electrosynthesis of hydrogen peroxide. Density functional theory (DFT) theoretical calculations indicate the unsaturated Nb–N 3 moieties and the adjacent oxygen groups optimize the interface bond strength of pivotal intermediates (OOH*) for producing H 2 O 2, thus accelerating the 2e – ORR pathway. Our findings may provide a novel platform for developing SACs with high activity and tunable selectivity.
Source: openalex_inverted_index · Quality: baseline

Research context

Catalysis & surfaces

OpenAlex topics: Electrocatalysts for Energy Conversion · Fuel Cells and Related Materials · Advanced Photocatalysis Techniques

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

State Key Laboratory of Photoelectric Technology and Functional Materials, International Collaborative Center on Photoelectric Technology and Nano Functional Materials, Institute of Photonics & Photon-Technology, Northwest University, Xi’an 710069, P. R. China

Xi’an Key Laboratory of Sustainable Energy Materials Chemistry, State Key Laboratory of Electrical Insulation and Power Equipment, School of Chemistry, Xi’an Jiaotong University, Xi’an 710049, P. R. China

Key Laboratory of Synthetic and Natural Functional Molecule Chemistry, College of Chemistry & Materials Science, Northwest University, 1 Xuefu Avenue, Xi’an 710127, P. R. China

LMPS − Laboratoire de Mécanique Paris-Saclay, CentraleSupélec, ENS Paris-Saclay, Université Paris-Saclay, CNRS, 8-10 rue Joliot-Curie, Gif-sur-Yvette 91190, France

Funding

China Postdoctoral Science Foundation · National Natural Science Foundation of China · Natural Science Basic Research Program of Shaanxi

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