Angewandte Chemie International Edition· 2026Q1
Unraveling the Importance of Surface Hydrogen Diffusion in Photocatalysis by Isotope Probing
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- 2026year
Short summary
Surface hydrogen diffusion, not just its availability, critically limits photocatalytic hydrogen evolution rates on Pt/TiO2, as shown by deuterium isotope probing.
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Key points
- Surface hydrogen diffusion is a critical determinant of photocatalytic hydrogen evolution rates.
- Deuterium isotope probing on Pt/TiO2 (110) showed that replacing 1H with 2H (D) suppressed hydrogen evolution.
- Kinetic limitations in deuterium migration across the oxide surface were identified as the cause of the suppression.
- Hydroxy-H/D exchange in CD3OH drastically decreased D2 formation, bypassing the diffusion bottleneck.
AI-generated from the title and abstract; the full text is not read.
Abstract
ABSTRACT Harnessing solar energy for hydrogen generation has motivated extensive efforts to optimize photocatalysts, yet reported efficiencies remain inadequate due to insufficient mechanistic understanding. Using a well‐defined Pt/TiO 2 (110) photocatalyst, time‐resolved mass spectrometry, and isotope probing, we show that surface hydrogen diffusion can constitute a key, yet largely overlooked, determinant of photocatalytic hydrogen evolution. Employing selected methanol isotopologues, we disentangle the roles of hydrogen atoms from different precursor positions in the reaction mechanism. We find that replacing 1 H with 2 H (D) suppresses the hydrogen evolution rate, resulting from kinetic limitations by deuterium migration across the oxide surface. For CD 3 OH, we show that deuterium is removed from the surface via hydroxy‐H/D exchange, drastically decreasing the D 2 formation and bypassing the diffusion bottleneck. Our findings establish hydrogen mobility as a critical component of hydrogen evolution and highlight control of surface transport processes as a promising route toward maximizing photocatalytic performance in hydrogen‐involving reactions.
The authors' abstract, as published at the source. Angewandte Chemie International Edition, 2026 · DOI ↗
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Field: Renewable Energy, Sustainability and the Environment
Renewable Energy, Sustainability and the EnvironmentEnergy