Non−noble single−atom alloy for electrocatalytic nitrate reduction using hierarchical high−throughput screening

Wang, Shuo, Li, Lei, Hui, Kwan San ORCID:, Dinh, Duc Anh, Lu, Zhiyi, Zhang, Qiuju and Hui, Kwun Nam (2023) Non−noble single−atom alloy for electrocatalytic nitrate reduction using hierarchical high−throughput screening. Nano Energy, 113. ISSN 2211-2855

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Electrochemical nitrate reduction reaction (NO3RR) holds promise for the management of wastewater contamination and synthesis of carbon−neutral ammonia (NH3). However, high−quality catalysts with controllable reaction pathways and high activity and selectivity are still lacking. The emerging single atom alloys (SAAs) offer attractive possibilities in nitrate reduction due to their unique atomic and electronic structures. By high−throughput first−principles calculations, we explore the possible incorporation of a series of transition−metal alloyed Cu−based SAAs, referred to as TM/Cu(111), for NO3RR toward NH3. A hierarchical four−step screening strategy have been employed to evaluate twenty−seven SAA catalysts yielding three alloying elements (Ti, Ni and Nb) with high catalytic activity and NO3RR selectivity. Finally, only Ni/Cu(111) possess the best activity among these three candidates because of its lowest limiting potential of −0.29 V. After further analysis, we found that the adsorption free energy of *NO3 can be recognized as efficient descriptor to design and predict the NO3RR performance of SAA. Furthermore, the Cu−based SAAs were revealed to exhibit pH dependent properties, which influence the competition between the hydrogen evolution reaction (HER) and NO3RR. This work not only indicates the significant potential of SAA in electrocatalysis for NO3RR to NH3, but also highlights the important influence of pH on the activity and selectivity of catalysts under reaction conditions.

Item Type: Article
Additional Information: Data availability: Data will be made available on request. Acknowledgements: This work was funded by the Science and Technology Development Fund, Macau SAR (File no. 0046/2019/AFJ, 0007/2021/AGJ, 006/2022/ALC), University of Macau (File no., MYRG2020 −00187 −IAPME and MYRG2022 −00223 −IAPME), the UEA funding, the Strategic Priority Research Program of the Chinese Academy of Sciences, (Grant No. XDB0450401), and Natural Science Foundation of Zhejiang Province (LY21B030006). The DFT calculations are performed at High Performance Computing Cluster (HPCC) of Information and Communication Technology Office (ICTO) at University of Macau.
Faculty \ School: Faculty of Science > School of Engineering
University of East Anglia Research Groups/Centres > Theme - ClimateUEA
UEA Research Groups: Faculty of Science > Research Groups > Emerging Technologies for Electric Vehicles (EV)
Faculty of Science > Research Groups > Energy Materials Laboratory
Depositing User: LivePure Connector
Date Deposited: 25 May 2023 09:34
Last Modified: 22 May 2024 01:38
DOI: 10.1016/j.nanoen.2023.108543


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