Single-atom catalyst for high-performance methanol oxidation

被引：212

作者：

Zhang, Zhiqi ^{[1
]}

Liu, Jiapeng ^{[1
]}

Wang, Jian ^{[2
]}

Wang, Qi ^{[3
]}

Wang, Yuhao ^{[1
]}

Wang, Kai ^{[4
]}

Wang, Zheng ^{[1
]}

Gu, Meng ^{[3
]}

Tang, Zhenghua ^{[4
]}

Lim, Jongwoo ^{[2
]}

Zhao, Tianshou ^{[1
]}

Ciucci, Francesco ^{[1
,5
]}

机构：

[1] Hong Kong Univ Sci & Technol, Dept Mech & Aerosp Engn, Hong Kong, Peoples R China

[2] Seoul Natl Univ, Coll Sci, Dept Chem, Seoul, South Korea

[3] Southern Univ Sci & Technol, Dept Mat Sci & Engn, Guangdong Prov Key Lab Energy Mat Elect Power, Shenzhen, Peoples R China

[4] South China Univ Technol, Guangzhou Higher Educ Mega Ctr, Sch Environm & Energy, Guangzhou Key Lab Surface Chem Energy Mat & New E, Guangzhou, Peoples R China

[5] Hong Kong Univ Sci & Technol, Dept Chem & Biol Engn, Hong Kong, Peoples R China

来源：

NATURE COMMUNICATIONS | 2021年 / 12卷 / 01期

关键词：

TOTAL-ENERGY CALCULATIONS; FINDING SADDLE-POINTS; ELASTIC BAND METHOD; OXYGEN REDUCTION; COORDINATION ENVIRONMENT; ELECTROOXIDATION; PLATINUM; HYDROGEN; ACHIEVE; ORIGIN;

D O I：

10.1038/s41467-021-25562-y

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：

It is still challenging to engineer single-atom catalysts for electrocatalytic methanol oxidation. Here, the authors design Pt single atom supported on RuO2 for highly active methanol oxidation in contrast to the inert Pt single atom supported on carbon. Single-atom catalysts have been widely investigated for several electrocatalytic reactions except electrochemical alcohol oxidation. Herein, we synthesize atomically dispersed platinum on ruthenium oxide (Pt-1/RuO2) using a simple impregnation-adsorption method. We find that Pt-1/RuO2 has good electrocatalytic activity towards methanol oxidation in an alkaline media with a mass activity that is 15.3-times higher than that of commercial Pt/C (6766 vs. 441 mA mg(Pt)(-1)). In contrast, single atom Pt on carbon black is inert. Further, the mass activity of Pt-1/RuO2 is superior to that of most Pt-based catalysts previously developed. Moreover, Pt-1/RuO2 has a high tolerance towards CO poisoning, resulting in excellent catalytic stability. Ab initio simulations and experiments reveal that the presence of Pt-O-3f (3-fold coordinatively bonded O)-Ru-cus (coordinatively unsaturated Ru) bonds with the undercoordinated bridging O in Pt-1/RuO2 favors the electrochemical dehydrogenation of methanol with lower energy barriers and onset potential than those encountered for Pt-C and Pt-Ru.

引用

页数：9

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