Transition-Metal Single Atoms in a Graphene Shell as Active Centers for Highly Efficient Artificial Photosynthesis

被引：392

作者：

Jiang, Kun ^{[1
]}

Siahrostami, Samira ^{[2
]}

Akey, Austin J. ^{[3
]}

Li, Yanbin ^{[4
]}

Lu, Zhiyi ^{[4
]}

Lattimer, Judith ^{[5
]}

Hu, Yongfeng ^{[6
]}

Stokes, Chris ^{[1
]}

Gangishetty, Mahesh ^{[1
]}

Chen, Guangxu ^{[4
]}

Zhou, Yawei ^{[7
]}

Hill, Winfield ^{[1
]}

Cai, Wen-Bin ^{[7
]}

Bell, David ^{[3
,8
]}

Chan, Karen ^{[9
]}

Norskov, Jens K. ^{[2
,9
]}

Cui, Yi ^{[3
,10
]}

Wang, Haotian ^{[1
]}

机构：

[1] Harvard Univ, Rowland Inst, Cambridge, MA 02142 USA

[2] Stanford Univ, SUNCAT Ctr Interface Sci & Catalysis, Dept Chem Engn, Stanford, CA 94305 USA

[3] Harvard Univ, Ctr Nanoscale Syst, Cambridge, MA 02138 USA

[4] Stanford Univ, Dept Mat Sci & Engn, Stanford, CA 94305 USA

[5] Harvard Univ, Dept Chem & Chem Biol, Cambridge, MA 02138 USA

[6] Univ Saskatchewan, Canadian Light Source Inc, 44 Innovat Blvd, Saskatoon, SK S7N 2V3, Canada

[7] Fudan Univ, Collaborat Innovat Ctr Chem Energy Mat, Dept Chem, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai 200433, Peoples R China

[8] Harvard Univ, Sch Engn & Appl Sci, Cambridge, MA 02142 USA

[9] SUNCAT Ctr Interface Sci & Catalysis, SLAC Natl Accelerator Lab, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA

[10] Stanford Inst Mat & Energy Sci, SLAC Natl Accelerator Lab, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA

来源：

CHEM | 2017年 / 3卷 / 06期

基金：

美国国家科学基金会;

关键词：

CO2; REDUCTION; CARBON-DIOXIDE; ELECTROCHEMICAL REDUCTION; HYDROGEN EVOLUTION; ORGANIC FRAMEWORKS; IONIC LIQUID; ELECTROREDUCTION; CONVERSION; OXIDE; CATALYST;

D O I：

10.1016/j.chempr.2017.09.014

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Utilizing solar energy to fix CO2 with water into chemical fuels and oxygen, a mimic process of photosynthesis in nature, is becoming increasingly important but still challenged by low selectivity and activity, especially in CO2 electrocatalytic reduction. Here, we report transition-metal atoms coordinated in a graphene shell as active centers for aqueous CO2 reduction to CO with high faradic efficiencies over 90% under significant currents up to similar to 60 mA/mg. We employed three-dimensional atom probe tomography to directly identify the single Ni atomic sites in graphene vacancies. Theoretical simulations suggest that compared with metallic Ni, the Ni atomic sites present different electronic structures that facilitate CO2-to-CO conversion and suppress the competing hydrogen evolution reaction dramatically. Coupled with Li+-tuned Co3O4 oxygen evolution catalyst and powered by a triple-junction solar cell, our artificial photosynthesis system achieves a peak solar-to-CO efficiency of 12.7% by using earth-abundant transition-metal electrocatalysts in a pH-equal system.

引用

页码：950 / 960

页数：11

共 56 条

[1] Nanostructured transition metal dichalcogenide electrocatalysts for CO2 reduction in ionic liquid [J].