Main-group metal elements as promising active centers for single-atom catalyst toward nitric oxide reduction reaction

Qian Wu; Baibiao Huang; Ying Dai; Thomas Heine; Yandong Ma

doi:10.1038/s41699-022-00326-4

Main-group metal elements as promising active centers for single-atom catalyst toward nitric oxide reduction reaction

Qian Wu, Baibiao Huang, Ying Dai, Thomas Heine, Yandong Ma

Department of Chemistry

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1 Citation (Scopus)

Abstract

Current research efforts on single-atom catalysts (SACs) exclusively focus on nonmetal or transition-metal atoms as active centers, while employing main-group metal elements is seemingly excluded because their delocalized s/p-bands are prone to yield a broadened resonance for the interaction with adsorbates. Here, we use high-throughput first-principles calculations to investigate the possible incorporation of Mg, Al, and Ga to form graphene-based SACs for NO reduction reaction (NORR) toward NH₃. 51 SAC candidates with different metal coordination environments have been computationally screened employing a rationally designed four-step process, yielding six SACs with high catalytic activity and NORR selectivity. The performance is rationalized by the modulation of s/p-band filling of the main-group metals. The adsorption free energy of NO is identified as an efficient descriptor for such SACs. The underlying physical mechanism is revealed and generally applicable to other main group metal SACs. These fundamental insights extend NORR SACs to main-group metal elements.

Original language	English
Article number	52
Journal	npj 2D Materials and Applications
Volume	6
Issue number	1
DOIs	https://doi.org/10.1038/s41699-022-00326-4
Publication status	Published - 2022 Dec

Bibliographical note

Funding Information:
This work is supported by the National Natural Science Foundation of China (Nos. 11804190, 12074217), Shandong Provincial Natural Science Foundation (Nos. ZR2019QA011 and ZR2019MEM013), Shandong Provincial Key Research and Development Program (Major Scientific and Technological Innovation Project) (No. 2019JZZY010302), Shandong Provincial Key Research and Development Program (No. 2019RKE27004), Shandong Provincial Science Foundation for Excellent Young Scholars (No. ZR2020YQ04), Qilu Young Scholar Program of Shandong University, and Taishan Scholar Program of Shandong Province. Deutsche Forschungsgemeinschaft is thanked for continuous support via CRC 1415, Shandong Provincial QingChuang Technology Support Plan (No. 2021KJ002).

Publisher Copyright:
© 2022, The Author(s).

All Science Journal Classification (ASJC) codes

Chemistry(all)
Materials Science(all)
Condensed Matter Physics
Mechanics of Materials
Mechanical Engineering

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10.1038/s41699-022-00326-4

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abstract = "Current research efforts on single-atom catalysts (SACs) exclusively focus on nonmetal or transition-metal atoms as active centers, while employing main-group metal elements is seemingly excluded because their delocalized s/p-bands are prone to yield a broadened resonance for the interaction with adsorbates. Here, we use high-throughput first-principles calculations to investigate the possible incorporation of Mg, Al, and Ga to form graphene-based SACs for NO reduction reaction (NORR) toward NH3. 51 SAC candidates with different metal coordination environments have been computationally screened employing a rationally designed four-step process, yielding six SACs with high catalytic activity and NORR selectivity. The performance is rationalized by the modulation of s/p-band filling of the main-group metals. The adsorption free energy of NO is identified as an efficient descriptor for such SACs. The underlying physical mechanism is revealed and generally applicable to other main group metal SACs. These fundamental insights extend NORR SACs to main-group metal elements.",

author = "Qian Wu and Baibiao Huang and Ying Dai and Thomas Heine and Yandong Ma",

note = "Funding Information: This work is supported by the National Natural Science Foundation of China (Nos. 11804190, 12074217), Shandong Provincial Natural Science Foundation (Nos. ZR2019QA011 and ZR2019MEM013), Shandong Provincial Key Research and Development Program (Major Scientific and Technological Innovation Project) (No. 2019JZZY010302), Shandong Provincial Key Research and Development Program (No. 2019RKE27004), Shandong Provincial Science Foundation for Excellent Young Scholars (No. ZR2020YQ04), Qilu Young Scholar Program of Shandong University, and Taishan Scholar Program of Shandong Province. Deutsche Forschungsgemeinschaft is thanked for continuous support via CRC 1415, Shandong Provincial QingChuang Technology Support Plan (No. 2021KJ002). Publisher Copyright: {\textcopyright} 2022, The Author(s).",

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Main-group metal elements as promising active centers for single-atom catalyst toward nitric oxide reduction reaction

Abstract

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