Electrocatalytic CO2 Conversion to Oxalate by a Copper Complex

被引:474
作者
Angamuthu, Raja [1 ]
Byers, Philip [1 ]
Lutz, Martin [2 ]
Spek, Anthony L. [2 ]
Bouwman, Elisabeth [1 ]
机构
[1] Leiden Univ, Leiden Inst Chem, Gorlaeus Labs, NL-2300 RA Leiden, Netherlands
[2] Univ Utrecht, Bijvoet Ctr Biomol Res Crystal & Struct Chem, NL-3584 CH Utrecht, Netherlands
关键词
CARBON-DIOXIDE; FIXATION; TRANSFORMATION; SPECTROSCOPY; REDUCTION; CATALYSIS; BINDING; ZINC;
D O I
10.1126/science.1177981
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
Global warming concern has dramatically increased interest in using CO2 as a feedstock for preparation of value-added compounds, thereby helping to reduce its atmospheric concentration. Here, we describe a dinuclear copper(I) complex that is oxidized in air by CO2 rather than O-2; the product is a tetranuclear copper(II) complex containing two bridging CO2-derived oxalate groups. Treatment of the copper(II) oxalate complex in acetonitrile with a soluble lithium salt results in quantitative precipitation of lithium oxalate. The copper(II) complex can then be nearly quantitatively electrochemically reduced at a relatively accessible potential, regenerating the initial dinuclear copper(I) compound. Preliminary results demonstrate six turnovers (producing 12 equivalents of oxalate) during 7 hours of catalysis at an applied potential of -0.03 volts versus the normal hydrogen electrode.
引用
收藏
页码:313 / 315
页数:3
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