材料科学
催化作用
氢
物理
量子力学
生物化学
化学
作者
Dileep Kumar,Ankit Mishra,Shubham,Hemant,Sudip Bhattacharjee,Rajashri Urkude,Biplab Ghosh,Asim Bhaumik,Anil K. Sinha,Amit Sinha,Vipin Amoli
标识
DOI:10.1002/aenm.202401964
摘要
Abstract Atomic‐level tailoring of active sites is an efficient strategy for designing high‐performance photocatalysts for clean energy. Asymmetric atomic sites (AAS) like M SA ‐O v ‐M 2 created through hetero‐metal single atoms (M SA ) doping on defect‐rich metal oxides (M 2 ‐O v ‐M 2 ) are favored for better activation of targeted molecules. However, creating AAS typically demands high energy input, hindering their widespread use in photocatalytic H 2 production. Furthermore, precise control over surface defects to create AAS remains challenging. Here, Cu SA ‐O v ‐Ti 3c highly asymmetric atomic sites catalyst (HAASC) is constructed by strategically trapping Cu single atoms on high‐index (111) faceted TiO 2 . This material combines single‐atom catalysis and facet engineering, achieving unprecedented H 2 production rates (8.3 mmol h −1 g −1 in pure water and 784.5 mmol h −1 g −1 in water/methanol mixture). Experimental and theoretical analyses reveal Cu SA substituting five‐coordinated Ti atoms (Ti 5c ) next to three‐coordinated (Ti 3c ) ones, forming Cu SA ‐O v ‐Ti 3c HAAS. HAAS plays multiple roles in i) improving light harvesting, charge‐transfer dynamics, and redox capability of photoexcited electrons; ii) enhanced adsorption and polarization of H 2 O molecules; iii) facilitating electron transfer from Cu SA ‐O v ‐Ti 3c to H 2 O molecules, and iv) raising d‐band center toward Fermi level resulting in ≈250‐fold enhanced H 2 production than Ti 5c ‐O‐Ti 3c AASC. This work opens new avenues for future structural designs in heterogeneous catalysis for energy‐related applications.
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