Domino electroreduction of CO2 to methanol on a molecular catalyst

Wu, Yueshen1,2; Jiang, Zhan3; Lu, Xu1,2; Liang, Yongye3; Wang, Hailiang1,2

2019-11-28

10.1038/s41586-019-1760-8

NATURE   影响因子和分区

0028-0836

1476-4687

Electrochemical carbon dioxide (CO2) reduction can in principle convert carbon emissions to fuels and value-added chemicals, such as hydrocarbons and alcohols, using renewable energy, but the efficiency of the process is limited by its sluggish kinetics(1,2). Molecular catalysts have well defined active sites and accurately tailorable structures that allow mechanism-based performance optimization, and transition-metal complexes have been extensively explored in this regard. However, these catalysts generally lack the ability to promote CO2 reduction beyond the two-electron process to generate more valuable products(1,3). Here we show that when immobilized on carbon nanotubes, cobalt phthalocyanine-used previously to reduce CO2 to primarily CO-catalyses the six-electron reduction of CO2 to methanol with appreciable activity and selectivity. We find that the conversion, which proceeds via a distinct domino process with CO as an intermediate, generates methanol with a Faradaic efficiency higher than 40 per cent and a partial current density greater than 10 milliamperes per square centimetre at -0.94 volts with respect to the reversible hydrogen electrode in a near-neutral electrolyte. The catalytic activity decreases over time owing to the detrimental reduction of the phthalocyanine ligand, which can be suppressed by appending electron-donating amino substituents to the phthalocyanine ring. The improved molecule-based electrocatalyst converts CO2 to methanol with considerable activity and selectivity and with stable performance over at least 12 hours.

SCI

英语

NI期刊 ; NI论文 ; ESI高被引

通讯

Guangdong Provincial Key Laboratory[2018B030322001]

Science & Technology - Other Topics

Multidisciplinary Sciences

WOS:000500036800054

NATURE PUBLISHING GROUP

BIOLOGY & BIOCHEMISTRY;CLINICAL MEDICINE;MULTIDISCIPLINARY;PLANT & ANIMAL SCIENCE;ENVIRONMENT/ECOLOGY;SOCIAL SCIENCES, GENERAL;MICROBIOLOGY;ECONOMICS BUSINESS;IMMUNOLOGY;MATERIALS SCIENCE;COMPUTER SCIENCE;SPACE SCIENCE;MOLECULAR BIOLOGY & GENETICS;CHEMISTRY;NEUROSCIENCE & BEHAVIOR;PHYSICS;GEOSCIENCES;ENGINEERING

Web of Science

1.Yale Univ, Dept Chem, 225 Prospect St, New Haven, CT 06520 USA
2.Yale Univ, Energy Sci Inst, West Haven, CT 06516 USA
3.Southern Univ Sci & Technol, Guangdong Prov Key Lab Energy Mat Elect Power, Dept Mat Sci & Engn, Shenzhen, Peoples R China

Wu, Yueshen,Jiang, Zhan,Lu, Xu,et al. Domino electroreduction of CO2 to methanol on a molecular catalyst[J]. NATURE,2019,575(7784):639-+.

Wu, Yueshen,Jiang, Zhan,Lu, Xu,Liang, Yongye,&Wang, Hailiang.(2019).Domino electroreduction of CO2 to methanol on a molecular catalyst.NATURE,575(7784),639-+.

Wu, Yueshen,et al."Domino electroreduction of CO2 to methanol on a molecular catalyst".NATURE 575.7784(2019):639-+.