Atomically Defined Undercoordinated Active Sites for Highly Efficient CO2 Electroreduction

Zheng, Wanzhen1; Yang, Jian1; Chen, Hengquan2; Hou, Yang1; Wang, Qi3; Gu, Meng3; He, Feng4; Xia, Ying5; Xia, Zheng1; Li, Zhongjian1; Yang, Bin1; Lei, Lecheng1; Yuan, Chris6; He, Qinggang2; Qiu, Ming5; Feng, Xinliang7,8

2019-11-04

10.1002/adfm.201907658

ADVANCED FUNCTIONAL MATERIALS   影响因子和分区

1616-301X

1616-3028

Electrocatalytic reduction of carbon dioxide (CO2ER) in rechargeable Zn-CO2 battery still remains a great challenge. Herein, a highly efficient CO2ER electrocatalyst composed of coordinatively unsaturated single-atom copper coordinated with nitrogen sites anchored into graphene matrix (Cu-N-2/GN) is reported. Benefitting from the unsaturated coordination environment and atomic dispersion, the ultrathin Cu-N-2/GN nanosheets exhibit a high CO2ER activity and selectivity for CO production with an onset potential of -0.33 V and the maximum Faradaic efficiency of 81% at a low potential of -0.50 V, superior to the previously reported atomically dispersed Cu-N anchored on carbon materials. Experimental results manifest the highly exposed and atomically dispersed Cu-N-2 active sites in graphene framework where the Cu species are coordinated by two N atoms. Theoretical calculations demonstrate that the optimized reaction free energy for Cu-N-2 sites to capture CO2 promote the adsorption of CO2 molecules on Cu-N-2 sites; meanwhile, the short bond lengths of Cu-N-2 sites accelerate the electron transfer from Cu-N-2 sites to *CO2, thus efficiently boosting the *COOH generation and CO2ER performance. A designed rechargeable Zn-CO2 battery with Cu-N-2/GN nanosheets deliver a peak power density of 0.6 mW cm(-2), and the charge process of battery can be driven by natural solar energy.

active sites atomic dispersion Cu-N-2 CO2 electroreduction unsaturated coordination Zn-CO2 battery

SCI ; EI

英语

ESI高被引 ; NI期刊 ; ESI高被引 ; ESI高被引 ; ESI高被引 ; ESI高被引 ; ESI高被引 ; ESI高被引 ; ESI高被引 ; ESI高被引 ; ESI高被引

其他

Hubei Natural Science Foundation of China[2018CFB531]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:000493827000001

WILEY-V C H VERLAG GMBH

20194607677319

Atoms ; Carbon dioxide ; Dispersions ; Electrocatalysts ; Electrolytic reduction ; Free energy ; Graphene ; Nanosheets ; Secondary batteries ; Solar energy ; Zinc compounds

Ore Treatment:533.1 ; Thermodynamics:641.1 ; Solar Energy and Phenomena:657.1 ; Secondary Batteries:702.1.2 ; Nanotechnology:761 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Atomic and Molecular Physics:931.3 ; Solid State Physics:933 ; Materials Science:951

MATERIALS SCIENCE

Web of Science

1.Zhejiang Univ, Key Lab Biomass Chem Engn, Minist Educ, Coll Chem & Biol Engn, Hangzhou 310027, Zhejiang, Peoples R China
2.Zhejiang Univ, Zhejiang Prov Key Lab Adv Chem Engn Manufacture T, Coll Chem & Biol Engn, Hangzhou 310027, Zhejiang, Peoples R China
3.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Guangdong, Peoples R China
4.Zhejiang Univ Technol, Coll Environm, Hangzhou 310014, Zhejiang, Peoples R China
5.Cent China Normal Univ, Inst Nanosci & Nanotechnol, Coll Phys Sci & Technol, Wuhan 430079, Hubei, Peoples R China
6.Case Western Reserve Univ, Dept Mech & Aerosp Engn, 10900 Euclid Ave, Cleveland, OH 44106 USA
7.Tech Univ Dresden, Ctr Advancing Elect Dresden Cfaed, D-01062 Dresden, Germany
8.Tech Univ Dresden, Dept Chem & Food Chem, D-01062 Dresden, Germany

Zheng, Wanzhen,Yang, Jian,Chen, Hengquan,et al. Atomically Defined Undercoordinated Active Sites for Highly Efficient CO2 Electroreduction[J]. ADVANCED FUNCTIONAL MATERIALS,2019,30(4).

Zheng, Wanzhen.,Yang, Jian.,Chen, Hengquan.,Hou, Yang.,Wang, Qi.,...&Feng, Xinliang.(2019).Atomically Defined Undercoordinated Active Sites for Highly Efficient CO2 Electroreduction.ADVANCED FUNCTIONAL MATERIALS,30(4).

Zheng, Wanzhen,et al."Atomically Defined Undercoordinated Active Sites for Highly Efficient CO2 Electroreduction".ADVANCED FUNCTIONAL MATERIALS 30.4(2019).