Low Catalyst Loading Enhances Charge Accumulation for Photoelectrochemical Water Splitting

Liu, Tianying; Li, Wei; Wang, David Z.; Luo, Tongtong; Fei, Muchun; Shin, Dongyoon; Waegele, Matthias M.; Wang, Dunwei

doi:10.1002/ange.202307909

Title: Low Catalyst Loading Enhances Charge Accumulation for Photoelectrochemical Water Splitting

Journal Article · 12 July 2023 · Angewandte Chemie

DOI: https://doi.org/10.1002/ange.202307909 · OSTI ID:1989401

^[1]; Li, Wei ^[1]; Wang, David Z. ^[1]; Luo, Tongtong ^[1]; Fei, Muchun ^[1]; Shin, Dongyoon ^[1]; Waegele, Matthias M. ^[1];

^[1]

Department of Chemistry, Merkert Chemistry Center Boston College Chestnut Hill MA 02467 USA

Abstract Solar water oxidation is a critical step in artificial photosynthesis. Successful completion of the process requires four holes and releases four protons. It depends on the consecutive accumulation of charges at the active site. While recent research has shown an obvious dependence of the reaction kinetics on the hole concentrations on the surface of heterogeneous (photo)electrodes, little is known about how the catalyst density impacts the reaction rate. Using atomically dispersed Ir catalysts on hematite, we report a study on how the interplay between the catalyst density and the surface hole concentration influences the reaction kinetics. At low photon flux, where surface hole concentrations are low, faster charge transfer was observed on photoelectrodes with low catalyst density compared to high catalyst density; at high photon flux and high applied potentials, where surface hole concentrations are moderate or high, slower surface charge recombination was afforded by low‐density catalysts. The results support that charge transfer between the light absorber and the catalyst is reversible; they reveal the unexpected benefits of low‐density catalyst loading in facilitating forward charge transfer for desired chemical reactions. It is implied that for practical solar water splitting devices, a suitable catalyst loading is important for maximized performance.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0020261

OSTI ID:: 1989401

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 34 Vol. 135; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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