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

被引:487
作者
Chen, Yuanjun [1 ]
Ji, Shufang [1 ]
Sun, Wenming [2 ]
Lei, Yongpeng [3 ,4 ]
Wang, Qichen [3 ,4 ]
Li, Ang [5 ]
Chen, Wenxing [6 ]
Zhou, Gang [7 ]
Zhang, Zedong [1 ]
Wang, Yu [8 ]
Zheng, Lirong [9 ]
Zhang, Qinghua [10 ]
Gu, Lin [10 ]
Han, Xiaodong [5 ]
Wang, Dingsheng [1 ]
Li, Yadong [1 ]
机构
[1] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
[2] China Agr Univ, Coll Sci, Beijing 100193, Peoples R China
[3] Cent South Univ, Coll Chem & Chem Engn, State Key Lab Powder Met, Changsha 410083, Peoples R China
[4] Cent South Univ, Coll Chem & Chem Engn, Hunan Prov Key Lab Chem Power Sources, Changsha 410083, Peoples R China
[5] Beijing Univ Technol, Beijing Key Lab Microstruct & Property Adv Mat, Beijing 100024, Peoples R China
[6] Beijing Inst Technol, Sch Mat Sci & Engn, Mat & Green Applicat, Beijing 100081, Peoples R China
[7] Hubei Univ Technol, Sch Sci, Wuhan 430068, Peoples R China
[8] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
[9] Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing, Peoples R China
[10] Chinese Acad Sci, Inst Phys, Beijing Natl Lab Condensed Matter Phys, Beijing 100190, Peoples R China
基金
中国博士后科学基金; 国家重点研发计划; 北京市自然科学基金; 中国国家自然科学基金;
关键词
atomic interfaces; photocatalytic hydrogen production; platinum; single atoms; surface defect engineering; OXYGEN VACANCIES; TIO2; SEPARATION; ANATASE; SURFACE; WATER; STRATEGIES; REACTIVITY; CLUSTERS; PROGRESS;
D O I
10.1002/anie.201912439
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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.
引用
收藏
页码:1295 / 1301
页数:7
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