Journal Article

PUBDB-2025-03681

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Cation Vacancies in Ti‐Deficient TiO$_2$ Nanosheets Enable Highly Stable Trapping of Pt Single Atoms for Persistent Photocatalytic Hydrogen Evolution

Jung, H. ; Cha, G. ; Kim, H. ; Will, J.Extern* ; Zhou, X. ; Bad'ura, Z. ; Zoppellaro, G. ; Dobrota, A. S. ; Skorodumova, N. V. ; Pašti, I. A. ; Sarma, B. B.Extern* ; Schmidt, J.Extern* ; Spiecker, E.Extern* ; Breu, J. ; Schmuki, P. (Corresponding author)Extern*

2025
Wiley-VCH Weinheim

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Please use a persistent id in citations: doi:10.1002/smll.202502428  doi:10.3204/PUBDB-2025-03681

Abstract: The stabilization of single-atom catalysts on semiconductor substrates is pivotal for advancing photocatalysis. TiO$_2$, a widely employed photocatalyst, typically stabilizes single atoms at oxygen vacancies—sites that are accessible but prone to agglomeration under illumination. Here, we demonstrate that cation vacancies in Ti-deficient TiO$_2$ nanosheets provide highly stable anchoring sites for Pt single atoms, enabling persistent photocatalytic hydrogen evolution. Ultrathin TiO$_2$ nanosheets with intrinsic Ti$^{4+}$ vacancies are synthesized via lepidocrocite-type titanate delamination and Pt single atoms are selectively trapped within these vacancies through a simple immersion process. The resulting Pt-decorated nanosheets exhibit superior photocatalytic hydrogen evolution performance, outperforming both Pt nanoparticle-loaded nanosheets and benchmarked Pt single-atom catalysts on P25. Crucially, Pt atoms anchored at Ti$^{4+}$ vacancies display remarkable resistance to light-induced agglomeration, a key limitation of conventional single-atom photocatalysts. Density functional theory calculations reveal that Pt incorporation into Ti$^{4+}$ vacancies is highly thermodynamically favorable and optimizes hydrogen adsorption energetics for enhanced catalytic activity. This work highlights the critical role of cation defect engineering in stabilizing single-atom co-catalysts and advancing the efficiency and durability of photocatalytic hydrogen evolution.

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Contributing Institute(s):

1. DOOR-User (DOOR ; HAS-User)

Research Program(s):

1. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
2. DFG project G:(GEPRIS)431791331 - SFB 1452: Katalyse an flüssigen Grenzflächen (CLINT) (431791331) (431791331)
3. SAN4Fuel - Single atom based nanohybrid photocatalyts for green fuels (101079384) (101079384)

Experiment(s):

1. PETRA Beamline P65 (PETRA III)

Appears in the scientific report 2025

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Database coverage:
; ; ; Clarivate Analytics Master Journal List ; Current Contents - Physical, Chemical and Earth Sciences ; DEAL Wiley ; Essential Science Indicators ; IF >= 10 ; JCR ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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