Artificial photosynthesis offers a promising strategy to produce hydrogen peroxide (H2O2)—an environmentally friendly oxidant and a clean fuel. However, the low activity and selectivity of the two-electron oxygen reduction reaction (ORR) in the photocatalytic process greatly restricts the H2O2 production efficiency. Here we show a robust antimony single-atom photocatalyst (Sb-SAPC, single Sb atoms dispersed on carbon nitride) for the synthesis of H2O2 in a simple water and oxygen mixture under visible light irradiation. An apparent quantum yield of 17.6% at 420 nm together with a solar-to-chemical conversion efficiency of 0.61% for H2O2 synthesis was achieved. On the basis of time-dependent density function theory calculations, isotopic experiments and advanced spectroscopic characterizations, the photocatalytic performance is ascribed to the notably promoted two-electron ORR by forming μ-peroxide at the Sb sites and highly concentrated holes at the neighbouring N atoms. The in situ generated O2 via water oxidation is rapidly consumed by ORR, leading to boosted overall reaction kinetics.
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We acknowledge the financial support from the Mitsubishi Chemical Corporation, Japan Society for the Promotion of Science (JSPS) Grant-in-Aid for Scientific Research (B, grant no. 20H02847), Grant-in-Aid for JSPS Fellows (DC2, grant no. 20J13064), Project National Natural Science Foundation of China (grant nos. 21805191, 21972094), the Guangdong Basic and Applied Basic Research Foundation (grant no. 2020A1515010982), Shenzhen Pengcheng Scholar Program, Shenzhen Peacock Plan (grant nos. KQJSCX20170727100802505 and KQTD2016053112042971), the Singapore Ministry of Education (Tier 1: RG4/20 and Tier 2: MOET2EP10120-0002) and the Agency for Science, Technology and Research (A*Star IRG: A20E5c0080). We thank X. Huang from the Department of Physics, Southern University of Science and Technology for his help in theoretical calculation and N. Jian from the Electron Microscope Center of the Shenzhen University for his help in HRTEM measurement.
The authors declare no competing interests.
Peer review information Nature Catalysis thanks Wei Lin and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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Supplementary Figs. 1–45, Tables 1–8, Notes 1–8 and references.
Atomic coordinations of optimized models for Vienna ab initio simulation package.
Atomic coordinations of optimized models for Gaussian.
TDDFT calculation data.
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Teng, Z., Zhang, Q., Yang, H. et al. Atomically dispersed antimony on carbon nitride for the artificial photosynthesis of hydrogen peroxide. Nat Catal 4, 374–384 (2021). https://doi.org/10.1038/s41929-021-00605-1
Nature Catalysis (2021)