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Spectroscopic and Theoretical Insights Into High-Entropy-Alloy Surfaces and Their Interfaces with Semiconductors for Enhanced Photocatalytic Hydrogen Production

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Τίτλος: Spectroscopic and Theoretical Insights Into High-Entropy-Alloy Surfaces and Their Interfaces with Semiconductors for Enhanced Photocatalytic Hydrogen Production
Συγγραφείς: Lin, Jui-Tai, Hsiao, Yueh-Chun, Li, Chao, Tseng, Ching-Yuan, He, Zong-Ying, Gardner, Adrian M, Chen, Yi, Yang, Chueh-Cheng, Wang, Chia-Hsin, Lin, Shang-Cheng, Lin, Xin-Xuan, Lin, Chih-Yi, Lin, Kun-Han, Cowan, Alexander J, Yang, Tung-Han
Στοιχεία εκδότη: Wiley
Έτος έκδοσης: 2025
Συλλογή: The University of Liverpool Repository
Περιγραφή: Recently, high-entropy alloy (HEA) nanocatalysts have shown outstanding catalytic performance. However, their integration with semiconductors for photocatalytic reactions remains largely unexplored. Here, Pd@HEA core–shell nanocrystals with controlled compositions and facets on TiO 2 supports are synthesized, achieving significantly enhanced photocatalytic hydrogen production. Compared to Pd@Pt/TiO 2 , Pd@Pt 0.4 Pd 0.15 Ir 0.15 Ru 0.15 Rh 0.15 core–shell nanocubes/TiO 2 exhibit superior photoactivity, driven by optimized Schottky junctions and synergistic multimetallic interactions that enhance photocatalysis. UV photoelectron spectroscopy reveals a high work function of 4.81 eV for Pd@Pt 0.4 Pd 0.15 Ir 0.15 Ru 0.15 Rh 0.15 , enabling efficient charge separation between Pd@HEA and TiO₂. Meanwhile, transient absorption spectroscopy confirms a significantly prolonged carrier lifetime of 4 ms, far surpassing that of pure TiO 2 ; (65 µs). In addition, in situ X-ray photoelectron spectroscopy confirms that photo-induced electrons preferentially accumulate on Ir and Pt sites, increasing their electron density and identifying them as primary adsorption sites. Furthermore, density functional theory calculations further reveal that Pt-based bridge sites exhibit a more optimal hydrogen binding free energy than Ir-based sites, suggesting that Pt serves as the dominant active site in photocatalysis. This study establishes a framework for the rational design of HEA-semiconductor photocatalysts, providing fundamental insights for solar-driven hydrogen production.
Τύπος εγγράφου: article in journal/newspaper
Περιγραφή αρχείου: text
Γλώσσα: English
ISSN: 1613-6810
Relation: https://livrepository.liverpool.ac.uk/3191524/1/accepted%20version-2025-04-22.pdf; https://livrepository.liverpool.ac.uk/3191524/2/Supporting%20Information-2025-04-22.pdf; Collapse authors list. Lin, Jui-Tai, Hsiao, Yueh-Chun, Li, Chao, Tseng, Ching-Yuan, He, Zong-Ying, Gardner, Adrian M orcid:0000-0002-2423-8799 , Chen, Yi, Yang, Chueh-Cheng, Wang, Chia-Hsin, Lin, Shang-Cheng et al (show 5 more authors) , Lin, Xin-Xuan, Lin, Chih-Yi, Lin, Kun-Han, Cowan, Alexander J orcid:0000-0001-9032-3548 and Yang, Tung-Han (2025) Spectroscopic and Theoretical Insights Into High-Entropy-Alloy Surfaces and Their Interfaces with Semiconductors for Enhanced Photocatalytic Hydrogen Production SMALL, 21 (25). e2503512-. ISSN 1613-6810, 1613-6829
DOI: 10.1002/smll.202503512
Διαθεσιμότητα: https://livrepository.liverpool.ac.uk/3191524/
https://doi.org/10.1002/smll.202503512
Rights: cc_by_4
Αριθμός Καταχώρησης: edsbas.10D802BA
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  Data: Recently, high-entropy alloy (HEA) nanocatalysts have shown outstanding catalytic performance. However, their integration with semiconductors for photocatalytic reactions remains largely unexplored. Here, Pd@HEA core–shell nanocrystals with controlled compositions and facets on TiO 2 supports are synthesized, achieving significantly enhanced photocatalytic hydrogen production. Compared to Pd@Pt/TiO 2 , Pd@Pt 0.4 Pd 0.15 Ir 0.15 Ru 0.15 Rh 0.15 core–shell nanocubes/TiO 2 exhibit superior photoactivity, driven by optimized Schottky junctions and synergistic multimetallic interactions that enhance photocatalysis. UV photoelectron spectroscopy reveals a high work function of 4.81 eV for Pd@Pt 0.4 Pd 0.15 Ir 0.15 Ru 0.15 Rh 0.15 , enabling efficient charge separation between Pd@HEA and TiO₂. Meanwhile, transient absorption spectroscopy confirms a significantly prolonged carrier lifetime of 4 ms, far surpassing that of pure TiO 2 ; (65 µs). In addition, in situ X-ray photoelectron spectroscopy confirms that photo-induced electrons preferentially accumulate on Ir and Pt sites, increasing their electron density and identifying them as primary adsorption sites. Furthermore, density functional theory calculations further reveal that Pt-based bridge sites exhibit a more optimal hydrogen binding free energy than Ir-based sites, suggesting that Pt serves as the dominant active site in photocatalysis. This study establishes a framework for the rational design of HEA-semiconductor photocatalysts, providing fundamental insights for solar-driven hydrogen production.
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  Data: https://livrepository.liverpool.ac.uk/3191524/1/accepted%20version-2025-04-22.pdf; https://livrepository.liverpool.ac.uk/3191524/2/Supporting%20Information-2025-04-22.pdf; Collapse authors list. Lin, Jui-Tai, Hsiao, Yueh-Chun, Li, Chao, Tseng, Ching-Yuan, He, Zong-Ying, Gardner, Adrian M orcid:0000-0002-2423-8799 , Chen, Yi, Yang, Chueh-Cheng, Wang, Chia-Hsin, Lin, Shang-Cheng et al (show 5 more authors) , Lin, Xin-Xuan, Lin, Chih-Yi, Lin, Kun-Han, Cowan, Alexander J orcid:0000-0001-9032-3548 and Yang, Tung-Han (2025) Spectroscopic and Theoretical Insights Into High-Entropy-Alloy Surfaces and Their Interfaces with Semiconductors for Enhanced Photocatalytic Hydrogen Production SMALL, 21 (25). e2503512-. ISSN 1613-6810, 1613-6829
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