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In-Silico Screening the Nitrogen Reduction Reaction on Single-Atom Electrocatalysts Anchored on MoS₂

Xu, Liang and Xie, Miao and Yang, Hao and Yu, Peiping and Ma, Bingyun and Cheng, Tao and Goddard, William A., III (2022) In-Silico Screening the Nitrogen Reduction Reaction on Single-Atom Electrocatalysts Anchored on MoS₂. Topics in Catalysis, 65 (1-4). pp. 234-241. ISSN 1572-9028. doi:10.1007/s11244-021-01546-6. https://resolver.caltech.edu/CaltechAUTHORS:20220118-011418400

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Abstract

We show that a Single-Atom Electrocatalyst (SAC) for the Nitrogen Reduction Reaction (NRR) can provide an environmentally green alternative to the Haber–Bosch high-temperature high-pressure process, replacing the water gas shift production of H₂ with H extracted from water. Anchoring the single atom on a two-dimensional substrate provides control to tune NRR catalytic performance toward a SAC possessing high utilization, high activity, and high selectivity. Experimental results suggest that this can significantly improve the activity and selectivity of NRR, but the specific reaction mechanism remains uncertain. This makes it difficult to select new catalytic materials for further optimization. Here we use Density Functional Theory to study the NRR catalytic mechanism on a catalytic model using a MoS₂ substrate to support a single atom site. We correct for solvation effects on the electrochemical reactions. We started with Fe@MoS₂, for which there are promising experimental reports, and conducted a systematic study of the NRR reaction mechanisms. These results show that N₂ adsorption, hydrogenation of N₂, desorption of NH₃, and Hydrogen Evolution are all critical steps affecting the reaction rates. Based on these steps, we scanned 23 transition metal elements to find improved catalysts. We identified Ir@MoS₂ (Mo top site) as the best candidate, predicted to have good catalytic activity and selectivity with 64.11% Faraday Efficiency. These results on the mechanism for NRR and the in silico search for alternative catalysts provide new promising targets for synthesizing novel and efficient SAC@MoS₂ NRR catalysts.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1007/s11244-021-01546-6DOIArticle
https://rdcu.be/cFep0PublisherFree ReadCube access
ORCID:
AuthorORCID
Xie, Miao0000-0002-9797-1449
Yang, Hao0000-0002-8241-6231
Yu, Peiping0000-0002-7269-9709
Cheng, Tao0000-0003-4830-177X
Goddard, William A., III0000-0003-0097-5716
Alternate Title:In-Silico Screening the Nitrogen Reduction Reaction on Single-Atom Electrocatalysts Anchored on MoS2
Additional Information:© The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature 2021. Accepted 25 November 2021. Published 08 January 2022. TC thanks to the National Natural Science Foundation of China (21903058), the Natural Science Foundation of Jiangsu Higher Education Institutions (SBK20190810), the Jiangsu Province High-Level Talents (JNHB-106), the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD) for financial support. HY thanks China Postdoctoral Science Foundation (2019M660128) for financial support. This work was partly supported by the Collaborative Innovation Center of Suzhou Nano Science & Technology. WAG thanks NSF (CBET-2005250) for support. The authors declare no conflict of interest.
Funders:
Funding AgencyGrant Number
National Natural Science Foundation of China21903058
Natural Science Foundation of Jiangsu Higher Education InstitutionsSBK20190810
Jiangsu Province High-Level TalentsJNHB-106
Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)UNSPECIFIED
China Postdoctoral Science Foundation2019M660128
Suzhou Nano Science and TechnologyUNSPECIFIED
NSFCBET-2005250
Subject Keywords:Density Functional Theory; Implicit solvation; Electrochemical catalysis; Rational catalysis design; Computational modeling
Other Numbering System:
Other Numbering System NameOther Numbering System ID
WAG1507
Issue or Number:1-4
DOI:10.1007/s11244-021-01546-6
Record Number:CaltechAUTHORS:20220118-011418400
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20220118-011418400
Official Citation:Xu, L., Xie, M., Yang, H. et al. In-Silico Screening the Nitrogen Reduction Reaction on Single-Atom Electrocatalysts Anchored on MoS2. Top Catal 65, 234–241 (2022). https://doi.org/10.1007/s11244-021-01546-6
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:112937
Collection:CaltechAUTHORS
Deposited By: Donna Wrublewski
Deposited On:18 Jan 2022 16:18
Last Modified:09 Feb 2022 17:38

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