Volume 59, Issue 3 pp. 1295-1301
Research Article

Engineering the Atomic Interface with Single Platinum Atoms for Enhanced Photocatalytic Hydrogen Production

Yuanjun Chen

Yuanjun Chen

Department of Chemistry, Tsinghua University, Beijing, 100084 China

These authors contributed equally to this work.

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Dr. Shufang Ji

Dr. Shufang Ji

Department of Chemistry, Tsinghua University, Beijing, 100084 China

These authors contributed equally to this work.

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Dr. Wenming Sun

Dr. Wenming Sun

College of Science, China Agricultural University, Beijing, 100193 China

These authors contributed equally to this work.

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Prof. Yongpeng Lei

Corresponding Author

Prof. Yongpeng Lei

State Key Laboratory of Powder Metallurgy & Hunan Provincial Key Laboratory of Chemical Power Sources, College of Chemistry and Chemical Engineering, Central South University, Changsha, 410083 China

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Qichen Wang

Qichen Wang

State Key Laboratory of Powder Metallurgy & Hunan Provincial Key Laboratory of Chemical Power Sources, College of Chemistry and Chemical Engineering, Central South University, Changsha, 410083 China

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Dr. Ang Li

Dr. Ang Li

Beijing Key Laboratory of Microstructure and Property of Advanced Materials, Beijing University of Technology, Beijing, 100024 China

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Dr. Wenxing Chen

Dr. Wenxing Chen

Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 China

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Prof. Gang Zhou

Corresponding Author

Prof. Gang Zhou

School of Science, Hubei University of Technology, Wuhan, 430068 China

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Zedong Zhang

Zedong Zhang

Department of Chemistry, Tsinghua University, Beijing, 100084 China

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Dr. Yu Wang

Dr. Yu Wang

Shanghai Synchrotron Radiation Facilities, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201204 China

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Dr. Lirong Zheng

Dr. Lirong Zheng

Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, China

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Dr. Qinghua Zhang

Dr. Qinghua Zhang

Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190 China

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Prof. Lin Gu

Prof. Lin Gu

Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190 China

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Prof. Xiaodong Han

Prof. Xiaodong Han

Beijing Key Laboratory of Microstructure and Property of Advanced Materials, Beijing University of Technology, Beijing, 100024 China

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Prof. Dingsheng Wang

Corresponding Author

Prof. Dingsheng Wang

Department of Chemistry, Tsinghua University, Beijing, 100084 China

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Prof. Yadong Li

Corresponding Author

Prof. Yadong Li

Department of Chemistry, Tsinghua University, Beijing, 100084 China

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First published: 26 October 2019
Citations: 428

Graphical Abstract

Single Pt atoms assembled on a defective TiO2 support (Pt1/def-TiO2) as a highly efficient photocatalyst serve as proton reduction sites and promote the neighboring TiO2 units to generate surface oxygen vacancies, leading to the formation of an atomic interface between the isolated Pt atom and Ti3+ defects. This unique structure endows Pt1/def-TiO2 with excellent photocatalytic hydrogen production performance.

Abstract

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 (Pt1/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 Pt1/def-TiO2 exhibit a record-level photocatalytic hydrogen production performance with an unexpectedly high turnover frequency of 51423 h−1, exceeding the Pt nanoparticle supported TiO2 catalyst by a factor of 591.

Conflict of interest

The authors declare no conflict of interest.

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