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High-throughput screening to predict highly active dual-atom catalysts for electrocatalytic reduction of nitrate to ammonia

Rehman, Faisal and Kwon, Soonho and Musgrave, Charles B., III and Tamtaji, Mohsen and Goddard, William A., III and Luo, Zhengtang (2022) High-throughput screening to predict highly active dual-atom catalysts for electrocatalytic reduction of nitrate to ammonia. Nano Energy, 103 (Part B). Art. No. 107866. ISSN 2211-2855. doi:10.1016/j.nanoen.2022.107866. https://resolver.caltech.edu/CaltechAUTHORS:20221011-984640000.3

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Abstract

Ammonia is an essential chemical owing to its importance in fertilizer production and other industrial applications. Electrocatalytic nitrate reduction to ammonia (NO₃RR) holds great promise for low-temperature ammonia production while simultaneously addressing nitrate-based environmental concerns. To provide the mechanistic understanding needed to design an effective electrocatalyst, we systematically investigated the catalytic performance of metal-based dual-atom catalysts (DACs) anchored on two-dimensional (2D) expanded phthalocyanine (Pc) for NO₃RR. We found that NO₃RR can efficiently produce ammonia on Cr₂-Pc, V₂-Pc, Ti₂-Pc, and Mn₂-Pc surfaces with low limiting potentials of − 0.02, − 0.25, − 0.34, and − 0.41 V_(RHE), respectively. Moreover, using the free energy difference of *NO₃⁻ and *H as a descriptor, we found that the hydrogen evolution reaction is significantly suppressed on the DAC surface due to an ensemble effect in which the two metal atoms cooperate to selectively form ammonia. We performed high-throughput screening to develop an efficient metal-based DAC for NO₃⁻ reduction, followed by a mechanistic study to elucidate the NO₃RR pathway on the DAC. This work provides design information for advancing sustainable ammonia synthesis under ambient conditions.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1016/j.nanoen.2022.107866DOIArticle
https://ars.els-cdn.com/content/image/1-s2.0-S2211285522009430-mmc1.docxRelated ItemSupplementary material
ORCID:
AuthorORCID
Kwon, Soonho0000-0002-9225-3018
Musgrave, Charles B., III0000-0002-3432-0817
Tamtaji, Mohsen0000-0001-9118-5474
Goddard, William A., III0000-0003-0097-5716
Luo, Zhengtang0000-0002-5134-9240
Additional Information:Z.L. acknowledge supports by the RGC (16304421), the Innovation and Technology Commission (ITC-CNERC14SC01), Guangdong Science and Technology Department (Project#: 2020A0505090003), Research Fund of Guangdong-Hong Kong-Macao Joint Laboratory for Intelligent Micro-Nano Optoelectronic Technology (No. 2020B1212030010), IER Foundation (HT-JD-CXY-201907), and Shenzhen Special Fund for Central Guiding the Local Science and Technology Development (2021Szvup136). F.R. appreciates financial support from the Higher Education Commission (HEC) of Pakistan. WAG acknowledges support from the Liquid Sunlight Alliance, which is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Fuels from Sunlight Hub under Award Number DE-SC0021266. SK acknowledges support from the Resnick Sustainability Institute (RSI).
Group:Resnick Sustainability Institute, Liquid Sunlight Alliance
Funders:
Funding AgencyGrant Number
Higher Education Commission (Pakistan)UNSPECIFIED
Department of Energy (DOE)DE-SC0021266
Resnick Sustainability InstituteUNSPECIFIED
Research Grants Council of Hong Kong16304421
Innovation and Technology Commission (Hong Kong)ITC-CNERC14SC01
Guangdong Science and Technology Department2020A0505090003
Research Fund of Guangdong-Hong Kong-Macao Joint Laboratory for Intelligent Micro-Nano Optoelectronic Technology2020B1212030010
IER FoundationHT-JD-CXY-201907
Shenzhen Special Fund for Central Guiding the Local Science and Technology Development2021Szvup136
Subject Keywords:Dual-atom electrocatalyst; Nitrate reduction; Ammonia synthesis; In silico catalyst design; Electrocatalysis
Other Numbering System:
Other Numbering System NameOther Numbering System ID
WAG1540
Issue or Number:Part B
DOI:10.1016/j.nanoen.2022.107866
Record Number:CaltechAUTHORS:20221011-984640000.3
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20221011-984640000.3
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:117365
Collection:CaltechAUTHORS
Deposited By: Donna Wrublewski
Deposited On:12 Oct 2022 17:57
Last Modified:12 Oct 2022 22:22

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