Anchoring Pt Single Atoms on Te Nanowires for Plasmon-Enhanced Dehydrogenation of Formic Acid at Room Temperature

被引：66

作者：

Han, Lei ^{[1
]}

Zhang, Leijie ^{[2
]}

Wu, Hong ^{[2
]}

Zu, Hualu ^{[1
]}

Cui, Peixin ^{[3
]}

Guo, Jiasheng ^{[1
]}

Guo, Ruihan ^{[1
]}

Ye, Jian ^{[2
]}

Zhu, Junfa ^{[2
]}

Zheng, Xusheng ^{[2
]}

Yang, Liuqing ^{[1
]}

Zhong, Yici ^{[1
]}

Liang, Shuquan ^{[1
]}

Wang, Liangbing ^{[1
]}

机构：

[1] Cent South Univ, Sch Mat Sci & Engn, Minist Educ, Key Lab Nonferrous Met Mat Sci & Engn, Changsha 410083, Hunan, Peoples R China

[2] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China

[3] Chinese Acad Sci, Inst Soil Sci, Key Lab Soil Environm & Pollut Remediat, Nanjing 210008, Jiangsu, Peoples R China

来源：

ADVANCED SCIENCE | 2019年 / 6卷 / 12期

基金：

国家重点研发计划;

关键词：

dehydrogenation of formic acid; plasmonic catalysis; platinum; single atoms; tellurium; HYDROGEN-PRODUCTION; EFFICIENT CATALYST; NANOPARTICLES; CONVERSION; ENERGY; DECOMPOSITION; OXIDATION; PD; NANOCRYSTALS; INTEGRATION;

D O I：

10.1002/advs.201900006

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Formic acid (HCOOH), as a promising hydrogen carrier, is renewable, safe, and nontoxic. However, the catalytic dehydrogenation of HCOOH is typically conducted at elevated temperature. Here, HCOOH decomposition is successfully achieved for hydrogen production on the developed Pt single atoms modified Te nanowires with the Pt mass loading of 1.1% (1.1%Pt/Te) at room temperature via a plasmon-enhanced catalytic process. Impressively, 1.1%Pt/Te delivers 100% selectivity for hydrogen and the highest turnover frequency number of 3070 h(-1) at 25 degrees C, which is significantly higher than that of Pt single atoms and Pt nanoclusters coloaded Te nanowires, Pt nanocrystals decorated Te nanowires, and commercial Pt/C. A plasmonic hot-electron driven mechanism rather than photothermal effect domains the enhancement of catalytic activity for 1.1%Pt/Te under light. The transformation of HCOO* to CO2 delta (-)* on Pt atoms is proved to be the rate-determining step by further mechanistic studies. 1.1%Pt/Te exhibits tremendous catalytic activity toward the decomposition of HCOOH owing to its plasmonic hot-electron driven mechanism, which efficiently stimulates the rate-determining step. In addition, hot electrons generated by the Te atoms nearby Pt single atoms are regarded to directly inject into the reactants adsorbed and activated on Pt single atoms.

引用

页数：8

共 51 条

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