Direct Laser Writing of Multimetal Bifunctional Catalysts for Overall Water Splitting

McGee, Shannon; Fest, Andres; Chandler, Cierra; Nova, Nabila N.; Lei, Yu; Goff, James; Sinnott, Susan B.; Dabo, Ismaila; Terrones, Mauricio; Zarzar, Lauren D.

doi:10.1021/acsaem.2c03973

Title: Direct Laser Writing of Multimetal Bifunctional Catalysts for Overall Water Splitting

Journal Article · Fri Mar 24 00:00:00 EDT 2023 · ACS Applied Energy Materials

DOI:https://doi.org/10.1021/acsaem.2c03973· OSTI ID:1985210

McGee, Shannon ^[1]; Fest, Andres ^[1]; Chandler, Cierra ^[1]; Nova, Nabila N. ^[1];

^[2];

^[1]; Sinnott, Susan B. ^[1];

^[1];

^[3];

^[1]

Pennsylvania State University, University Park, PA (United States)
Pennsylvania State University, University Park, PA (United States); Tsinghua University, Shenzhen (China)
Pennsylvania State University, University Park, PA (United States); Shinshu University, Nagano (Japan)

Water electrolysis is of interest as a sustainable way to produce clean hydrogen and oxygen fuel and help mitigate the rising problems of climate change while meeting global energy demands. High-efficiency, stable, and earth-abundant bifunctional catalysts are needed to enable more effective electrochemical cells for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Here, we investigate the synthesis, composition, performance, and mechanism of multimetal catalysts serving dual functionality in both OER and HER of water electrolysis. Through a laser synthesis method, we synthesized heterogeneous catalysts of nanocrystalline multimetallic alloy pockets embedded within an amorphous oxide matrix. We evaluated the performance and composition of a range of mixed transition-metal oxide materials for both OER and HER, ultimately synthesizing a Cr_0.01Fe_0.27Co_0.34Ni_0.38O_x/C_y catalyst that has a stable, high-rate, and competitive overall water splitting performance of 1.76 V at 100 mA cm^–2 in an alkaline medium. Using density functional theory to gain insight as the active site and mechanism, we propose that the inclusion of a minor amount of Cr increases the degeneracy of energetic states that lowers the cost of forming the O 2 p–d bond and H 1 s–d bond due to the hybridization of s, p, and d orbitals from Cr. Using a two-electrode water electrolysis cell with a constant potential of 1.636 V to mimic the setup for fuel production, we found the catalyst to be stable at 14–15 mA cm^–2 for 40 h. Furthermore, this laser synthesis method allowing for facile and rapid synthesis of complex multimetal systems demonstrates how doping a Fe, Co, and Ni heterogeneous amorphous/nanocrystalline structure with small amounts of Cr is important for bifunctional catalytic behavior, particularly for increasing HER functionality in advancing our understanding for future electrocatalytic design.

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Research Organization:: Pennsylvania State Univ., University Park, PA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Packard Fellowship for Science and Engineering

Grant/Contract Number:: SC0018646; 2019-69664

OSTI ID:: 1985210

Journal Information:: ACS Applied Energy Materials, Vol. 6, Issue 7; ISSN 2574-0962

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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