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Oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER) are three critical reactions for energy-related applications, such as water electrolyzers and metal-air batteries. Graphene-supported single-atom catalysts (SACs) have been widely explored; however, either experiments or density functional theory (DFT) computations cannot screen catalysts at high speed. Herein, based on DFT computations of 104 graphene-supported SACs (M@C3, M@C4, M@pyridine-N4, and M@pyrrole-N4), we built up machine learning (ML) models to describe the underlying pattern of easily obtainable physical properties and limiting potentials (errors = 0.013/0.005/0.020 V for ORR/OER/HER, respectively), and employed these models to predict the catalysis performance of 260 other graphene-supported SACs containing metal-NxCy active sites (M@NxCy). We recomputed the top catalysts recommended by ML towards ORR/OER/HER by DFT, which confirmed the reliability of our ML model, and identified two OER catalysts (Ir@pyridine-N3C1 and Ir@pyridine-N2C2) outperforming noble metal oxides, RuO2 and IrO2. The ML models quantitatively unveiled the significance of various descriptors and fast narrowed down the potential list of graphene-supported single-atom catalysts. This approach can be easily used to screen and design other SACs, and significantly accelerate the catalyst design for many other important reactions.
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Recent Progress of Single‐atom Catalysts in the Electrocatalytic Reduction of Oxygen to Hydrogen Peroxide
Abstract Single‐atom catalysts (SACs) have been attracting extensive interest in the electrocatalytic production of hydrogen peroxide by oxygen reduction reaction (ORR). This is due to the maximal efficiency of atom utilization and intimate interaction of the metal centers with the supporting matrix that may be exploited for deliberate manipulation of the electrocatalytic activity and selectivity, in comparison with the conventional nanoparticle counterparts. Herein, we summarize recent progress of the design and engineering of SACs towards ORR for H2O2generation, based on both noble and non‐noble metals. We conclude the review with a perspective highlighting the promises and challenges involved in future research.
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- PAR ID:
- 10238703
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Electroanalysis
- Volume:
- 32
- Issue:
- 12
- ISSN:
- 1040-0397
- Page Range / eLocation ID:
- p. 2591-2602
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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