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Published December 1, 2022 | Supplemental Material
Journal Article Open

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


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 VRHE, 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.

Additional Information

© 2022 Elsevier. 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). Data availability. Data will be made available on request. The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

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August 22, 2023
October 25, 2023