Deciphering nanoconfinement effects on molecular orientation and reaction intermediate by single molecule imaging

被引：62

作者：

Dong, Bin ^{[1
]}

Pei, Yuchen ^{[2
,3
]}

Mansour, Nourhan ^{[1
]}

Lu, Xuemei ^{[4
,5
]}

Yang, Kai ^{[4
,5
]}

Huang, Wenyu ^{[2
,3
]}

Fang, Ning ^{[1
]}

机构：

[1] Georgia State Univ, Dept Chem, Atlanta, GA 30303 USA

[2] Iowa State Univ, Dept Chem, Ames, IA 50011 USA

[3] US DOE, Ames Lab, Ames, IA 50011 USA

[4] Soochow Univ, Ctr Soft Condensed Matter Phys & Interdisciplinar, Suzhou 215006, Peoples R China

[5] Soochow Univ, Sch Phys Sci & Technol, Suzhou 215006, Peoples R China

来源：

NATURE COMMUNICATIONS | 2019年 / 10卷 / 1期

基金：

美国国家科学基金会;

关键词：

MESOPOROUS SILICA; FLUORESCENCE; DIFFUSION; ADSORPTION; CATALYSIS; CONFINEMENT; HYDROGENATION; DIFFRACTION; ELECTRON; PATHWAYS;

D O I：

10.1038/s41467-019-12799-x

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Nanoconfinement could dramatically change molecular transport and reaction kinetics in heterogeneous catalysis. Here we specifically design a core-shell nanocatalyst with aligned linear nanopores for single-molecule studies of the nanoconfinement effects. The quantitative single-molecule measurements reveal unusual lower adsorption strength and higher catalytic activity on the confined metal reaction centres within the nanoporous structure. More surprisingly, the nanoconfinement effects on enhanced catalytic activity are larger for catalysts with longer and narrower nanopores. Experimental evidences, including molecular orientation, activation energy, and intermediate reactive species, have been gathered to provide a molecular level explanation on how the nanoconfinement effects enhance the catalyst activity, which is essential for the rational design of highly-efficient catalysts.

引用

页数：6

共 61 条

[1] Single-Molecule Catalysis Mapping Quantifies Site-Specific Activity and Uncovers Radial Activity Gradient on Single 2D Nanocrystals [J].