Ionic Exchange of Metal Organic Frameworks to Access Single Nickel Sites for Efficient Electroreduction of CO2

被引：1262

作者：

Zhao, Changming ^{[1
]}

Dai, Xinyao ^{[1
]}

Yao, Tao ^{[4
]}

Chen, Wenxing ^{[2
,3
]}

Wang, Xiaoqian ^{[1
]}

Wang, Jing ^{[1
]}

Yang, Jian ^{[1
]}

Wei, Shiqiang ^{[4
]}

Wu, Yuen ^{[1
]}

Li, Yadong ^{[2
,3
]}

机构：

[1] Univ Sci & Technol China, Dept Chem, Collaborat Innovat Ctr Chem Energy Mat iChEM, Hefei 230026, Peoples R China

[2] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China

[3] Tsinghua Univ, Collaborat Innovat Ctr Nanomat Sci & Engn, Beijing 100084, Peoples R China

[4] Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2017年 / 139卷 / 24期

基金：

中国国家自然科学基金;

关键词：

CARBON-DIOXIDE; OXYGEN REDUCTION; CATALYST; CONVERSION; ELECTRODE; METHANE;

D O I：

10.1021/jacs.7b02736

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Single-atom catalysts often exhibit unexpected catalytic activity for many important chemical reactions because of their unique electronic and geometric structures with respect to their bulk counterparts. Herein we adopt metal-organic frameworks (MOFs) to assist the preparation of a catalyst containing single Ni sites for efficient electroreduction of CO2. The synthesis is based on ionic exchange between Zn nodes and adsorbed Ni ions within the cavities of the MOF. This single-atom catalyst exhibited an excellent turnover, frequency for electroreduction of CO2 (5273 h(-1)), with a Faradaic efficiency for CO production of over 71.9% and a current density of 10.48 mA cm(-2) at an overpotential of 0.89 V. Our findings present some guidelines for the rational design and accurate modulation of nanostructured catalysts at the atomic scale.

引用

页码：8078 / 8081

页数：4

共 30 条

[1] Copper-Based Metal-Organic Porous Materials for CO2 Electrocatalytic Reduction to Alcohols [J].

Albo, Jonathan ;

Vallejo, Daniel ;

Beobide, Garikoitz ;

Castillo, Oscar ;

Castano, Pedro ;

Irabien, Angel .

CHEMSUSCHEM, 2017, 10 (06) :1100-1109

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

Asadi, Mohammad ;

Kim, Kibum ;

Liu, Cong ;

Addepalli, Aditya Venkata ;

Abbasi, Pedram ;

Yasaei, Poya ;

Phillips, Patrick ;

Behranginia, Amirhossein ;

Cerrato, Jose M. ;

Haasch, Richard ;

Zapol, Peter ;

Kumar, Bijandra ;

Klie, Robert F. ;

Abiade, Jeremiah ;

Curtiss, Larry A. ;

Salehi-Khojin, Amin .

SCIENCE, 2016, 353 (6298) :467-470

[3] Single-atom catalysts for CO2 electroreduction with significant activity and selectivity improvements [J].

Back, Seoin ;

Lim, Juhyung ;

Kim, Na-Young ;

Kim, Yong-Hyun ;

Jung, Yousung .

CHEMICAL SCIENCE, 2017, 8 (02) :1090-1096

[4] Confinement of Ionic Liquids in Nanocages: Tailoring the Molecular Sieving Properties of ZIF-8 for Membrane-Based CO2 Capture [J].

Ban, Yujie ;

Li, Zhengjie ;

Li, Yanshuo ;

Peng, Yuan ;

Jin, Hua ;

Jiao, Wenmei ;

Guo, Ang ;

Wang, Po ;

Yang, Qingyuan ;

Zhong, Chongli ;

Yang, Weishen .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2015, 54 (51) :15483-15487

[5] High-throughput synthesis of zeolitic imidazolate frameworks and application to CO2 capture [J].

Banerjee, Rahul ;

Phan, Anh ;

Wang, Bo ;

Knobler, Carolyn ;

Furukawa, Hiroyasu ;

O'Keeffe, Michael ;

Yaghi, Omar M. .

SCIENCE, 2008, 319 (5865) :939-943

[6] A Local Proton Source Enhances CO2 Electroreduction to CO by a Molecular Fe Catalyst [J].

Costentin, Cyrille ;

Drouet, Samuel ;

Robert, Marc ;

Saveant, Jean-Michel .

SCIENCE, 2012, 338 (6103) :90-94

[7] A single iron site confined in a graphene matrix for the catalytic oxidation of benzene at room temperature [J].

Deng, Dehui ;

Chen, Xiaoqi ;

Yu, Liang ;

Wu, Xing ;

Liu, Qingfei ;

Liu, Yun ;

Yang, Huaixin ;

Tian, Huanfang ;

Hu, Yongfeng ;

Du, Peipei ;

Si, Rui ;

Wang, Junhu ;

Cui, Xiaoju ;

Li, Haobo ;

Xiao, Jianping ;

Xu, Tao ;

Deng, Jiao ;

Yang, Fan ;

Duchesne, Paul N. ;

Zhang, Peng ;

Zhou, Jigang ;

Sun, Litao ;

Li, Jianqi ;

Pan, Xiulian ;

Bao, Xinhe .

SCIENCE ADVANCES, 2015, 1 (11)

[8] The Central Role of Bicarbonate in the Electrochemical Reduction of Carbon Dioxide on Gold [J].

Dunwell, Marco ;

Lu, Qi ;

Heyes, Jeffrey M. ;

Rosen, Jonathan ;

Chen, Jingguang G. ;

Yan, Yushan ;

Jiao, Feng ;

Xu, Bingjun .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2017, 139 (10) :3774-3783

[9] Atomically isolated nickel species anchored on graphitized carbon for efficient hydrogen evolution electrocatalysis [J].

Fan, Lili ;

Liu, Peng Fei ;

Yan, Xuecheng ;

Gu, Lin ;

Yang, Zhen Zhong ;

Yang, Hua Gui ;

Qiu, Shilun ;

Yao, Xiangdong .

NATURE COMMUNICATIONS, 2016, 7

[10] Grain-Boundary-Dependent CO2 Electroreduction Activity [J].

Feng, Xiaofeng ;

Jiang, Kaili ;

Fan, Shoushan ;

Kanan, Matthew W. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (14) :4606-4609

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