期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 3, 页码 1295-1301出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201912439
关键词
atomic interfaces; photocatalytic hydrogen production; platinum; single atoms; surface defect engineering
资金
- China Postdoctoral Science Foundation [2018M640113] Funding Source: Medline
- National Natural Science Foundation of China [21890383, 21703219, 21671117, 21871159, 51872008] Funding Source: Medline
- the Beijing Natural Science Foundation [1182005] Funding Source: Medline
- National Key R&D Program of China [2018YFB0704100, 2018YFA0702003] Funding Source: Medline
- National Postdoctoral Program for Innovative Talents [BX20180160] Funding Source: Medline
It is highly desirable but challenging to optimize the structure of photocatalysts at the atomic scale to facilitate the separation of electron-hole pairs for enhanced performance. Now, a highly efficient photocatalyst is formed by assembling single Pt atoms on a defective TiO2 support (Pt-1/def-TiO2). Apart from being proton reduction sites, single Pt atoms promote the neighboring TiO2 units to generate surface oxygen vacancies and form a Pt-O-Ti3+ atomic interface. Experimental results and density functional theory calculations demonstrate that the Pt-O-Ti3+ atomic interface effectively facilitates photogenerated electrons to transfer from Ti3+ defective sites to single Pt atoms, thereby enhancing the separation of electron-hole pairs. This unique structure makes Pt-1/def-TiO2 exhibit a record-level photocatalytic hydrogen production performance with an unexpectedly high turnover frequency of 51423h(-1), exceeding the Pt nanoparticle supported TiO2 catalyst by a factor of 591.
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