Underpotential Deposition of 3D Transition Metals: Versatile Electrosynthesis of Single-Atom Catalysts on Oxidized Carbon Supports

Meese, Aidan Francis; Napier, Cade; Kim, David J.; Rigby, Kali; Hedtke, Tayler; Leshchev, Denis; Stavitski, Eli; Parent, Lucas R.; Kim, Jae‐Hong

doi:10.1002/adma.202311341

Title: Underpotential Deposition of 3D Transition Metals: Versatile Electrosynthesis of Single-Atom Catalysts on Oxidized Carbon Supports

Journal Article · 07 February 2024 · Advanced Materials

DOI: https://doi.org/10.1002/adma.202311341 · OSTI ID:2324876

Meese, Aidan Francis ^[1]; Napier, Cade ^[1]; Kim, David J. ^[1]; Rigby, Kali ^[1]; Hedtke, Tayler ^[1]; Leshchev, Denis ^[2]; Stavitski, Eli ^[2]; Parent, Lucas R. ^[3];

^[1]

Yale Univ., New Haven, CT (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Univ. of Connecticut, Storrs, CT (United States)

Use of single-atom catalysts (SACs) has become a popular strategy for tuning activity and selectivity toward specific pathways. However, conventional SAC synthesis methods require high temperatures and pressures, complicated procedures, and expensive equipment. Recently, underpotential deposition (UPD) has been investigated as a promising alternative, yielding high-loading SAC electrodes under ambient conditions and within minutes. Yet only few studies have employed UPD to synthesize SACs, and all have been limited to UPD of Cu. In this work, a flexible UPD approach for synthesis of mono- and bi-metallic Cu, Fe, Co, and Ni SACs directly on oxidized, commercially available carbon electrodes is reported. The UPD mechanism is investigated using in situ X-ray absorption spectroscopy and, finally, the catalytic performance of a UPD-synthesized Co SAC is assessed for electrochemical nitrate reduction to ammonia. In conclusion, the findings expand upon the usefulness and versatility of UPD for SAC synthesis, with hopes of enabling future research toward realization of fast, reliable, and fully electrified SAC synthesis processes.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 2324876

Report Number(s):: BNL--225402-2024-JAAM

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 19 Vol. 36; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

36 MATERIALS SCIENCE
electrochemical
nitrate reduction
single atom catalyst
synthesis
underpotential deposition

Title: Underpotential Deposition of 3D Transition Metals: Versatile Electrosynthesis of Single-Atom Catalysts on Oxidized Carbon Supports

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