Octahedral gold-silver nanoframes with rich crystalline defects for efficient methanol oxidation manifesting a CO-promoting effect

被引：105

作者：

Xiong, Likun ^{[1
,2
]}

Sun, Zhongti ^{[1
,2
]}

Zhang, Xiang ^{[1
,2
]}

Zhao, Liang ^{[1
,2
]}

Huang, Peng ^{[1
,2
]}

Chen, Xiwen ^{[1
,2
]}

Jin, Huidong ^{[1
,2
]}

Sun, Hao ^{[1
,2
]}

Lian, Yuebin ^{[1
,2
]}

Deng, Zhao ^{[1
,2
]}

Rummerli, Mark H. ^{[1
,2
]}

Yin, Wanjian ^{[1
,2
]}

Zhang, Duo ^{[3
,4
]}

Wang, Shuao ^{[3
,4
]}

Peng, Yang ^{[1
,2
]}

机构：

[1] Soochow Univ, Coll Energy, Soochow Inst Energy & Mat Innovat, Suzhou 215006, Peoples R China

[2] Key Lab Adv Carbon Mat & Wearable Energy Technol, Suzhou, Peoples R China

[3] Soochow Univ, Sch Radiat Med & Protect, State Key Lab Radiat Med & Protect, Suzhou 215123, Peoples R China

[4] Collaborat Innovat Ctr Radiol Med Jiangsu Higher, Suzhou, Peoples R China

来源：

NATURE COMMUNICATIONS | 2019年 / 10卷 / 1期

关键词：

ENHANCED ELECTROCATALYTIC ACTIVITY; ELECTRONIC BEHAVIOR; CATALYTIC-ACTIVITY; NANOPOROUS GOLD; SHAPE-CONTROL; AG NANOCUBES; ACTIVE-SITE; AU; NANOCRYSTALS; NANOPARTICLES;

D O I：

10.1038/s41467-019-11766-w

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：

Three-dimensional bimetallic nanoframes with high spatial diffusivity and surface heterogeneity possess remarkable catalytic activities owing to their highly exposed active surfaces and tunable electronic structure. Here we report a general one-pot strategy to prepare ultrathin octahedral Au3Ag nanoframes, with the formation mechanism explicitly elucidated through well-monitored temporal nanostructure evolution. Rich crystalline defects lead to lowered atomic coordination and varied electronic states of the metal atoms as evidenced by extensive structural characterizations. When used for electrocatalytic methanol oxidation, the Au3Ag nanoframes demonstrate superior performance with a high specific activity of 3.38 mA cm(-2), 3.9 times that of the commercial Pt/C. More intriguingly, the kinetics of methanol oxidation on the Au3Ag nanoframes is counter-intuitively promoted by carbon monoxide. The enhancement is ascribed to the altered reaction pathway and enhanced OH- co-adsorption on the defect-rich surfaces, which can be well understood from the d-band model and comprehensive density functional theory simulations.

引用

页数：11

共 69 条

[1] Long-Range Segregation Phenomena in Shape-Selected Bimetallic Nanoparticles: Chemical State Effects [J].