Copper tetrazolate based metal-organic frameworks as highly efficient catalysts for artificially chemical and electrochemical CO2 conversion

被引:15
作者
Zhong, Haixia [1 ]
Liu, Kaihua [1 ,2 ,3 ]
Zhang, Qi [1 ]
Meng, Fanlu [1 ,2 ,3 ]
Bao, Di [1 ]
Zhang, Xinbo [1 ]
机构
[1] Chinese Acad Sci, State Key Lab Rare Earth Resource Utilizat, Changchun Inst Appl Chem, Changchun 130022, Peoples R China
[2] Jilin Univ, Key Lab Automobile Mat, Minist Educ, Changchun 130022, Jilin, Peoples R China
[3] Jilin Univ, Coll Mat Sci & Engn, Changchun 130022, Jilin, Peoples R China
来源
NANO SELECT | 2020年 / 1卷 / 03期
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
CO2; conversion; copper tetrazolate; cyclic carbonate; electrocatalyst; metal-organic frameworks; COORDINATION POLYMERS; ELECTROREDUCTION; REDUCTION; CAPTURE; DESIGN; SITES; CU;
D O I
10.1002/nano.202000041
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
Development of efficient catalyst for CO2 conversion is highly demanded to alleviate the CO2 related environmental and energy crisis. Here, we develop a series of copper tetrazolate based metal-organic frameworks (MOFs) (Cu-5H, Cu-5M and Cu-5P) to promote the artificial CO2 conversion via chemical and electrochemical route. Featuring with abundant exposed Lewis-acid Cu centers, nitrogen-rich sites, and porous architecture, Cu-5M and Cu-5P exhibit high yield (>99%) toward synthesizing cyclic carbonate via the cycloaddition reaction of CO2 to epoxide at ambient condition. In electrochemical CO2 conversion process, Cu-5H shows high electrocatalytic activity with a large Faradaic efficiency (91%) for formate. The ex situ scanning electron microscopy and x-ray diffraction investigations indicate the in situ generated Cu species in the MOFs structure play vital roles in promoting the high electrocatalytic activity. Our work sheds light on the facile development of metal and nitrogen-rich MOF based catalysts in chemical and electrochemical conversion CO2 to valuable chemical and fuel.
引用
收藏
页码:311 / 319
页数:9
相关论文
共 44 条
[1]   Effective and Reversible Carbon Dioxide Insertion into Cerium Pyrazolates [J].
Bayer, Uwe ;
Werner, Daniel ;
Maichle-Moessmer, Caecilia ;
Anwander, Reiner .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2020, 59 (14) :5830-5836
[2]   A Hafnium-Based Metal Organic Framework as an Efficient and Multifunctional Catalyst for Facile CO2 Fixation and Regioselective and Enantioretentive Epoxide Activation [J].
Beyzavi, M. Hassan ;
Klet, Rachel C. ;
Tussupbayev, Samat ;
Borycz, Joshua ;
Vermeulen, Nicolaas A. ;
Cramer, Christopher J. ;
Stoddart, J. Fraser ;
Hupp, Joseph T. ;
Farha, Omar K. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2014, 136 (45) :15861-15864
[3]   Cr(salophen) Complex Catalyzed Cyclic Carbonate Synthesis at Ambient Temperature And Pressure [J].
Castro-Osma, Jose A. ;
Lamb, Katie J. ;
North, Michael .
ACS CATALYSIS, 2016, 6 (08) :5012-5025
[4]   Ab initio x-ray absorption study of copper K-edge XANES spectra in Cu(II) compounds -: art. no. 134208 [J].
Chaboy, J ;
Muñoz-Páez, A ;
Carrera, F ;
Merkling, P ;
Marcos, ES .
PHYSICAL REVIEW B, 2005, 71 (13)
[5]   Aqueous CO2 Reduction at Very Low Overpotential on Oxide-Derived Au Nanoparticles [J].
Chen, Yihong ;
Li, Christina W. ;
Kanan, Matthew W. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (49) :19969-19972
[6]   Current Issues in Molecular Catalysis Illustrated by Iron Porphyrins as Catalysts of the CO2-to-CO Electrochemical Conversion [J].
Costentin, Cyrille ;
Robert, Marc ;
Saveant, Jean-Michel .
ACCOUNTS OF CHEMICAL RESEARCH, 2015, 48 (12) :2996-3006
[7]   2D Metal-Organic Frameworks as Multifunctional Materials in Heterogeneous Catalysis and Electro/Photocatalysis [J].
Dhakshinamoorth, Amarajothi ;
Asiri, Abdullah M. ;
Garcia, Hermenegildo .
ADVANCED MATERIALS, 2019, 31 (41)
[8]   The role of reticular chemistry in the design of CO2 reduction catalysts [J].
Diercks, Christian S. ;
Liu, Yuzhong ;
Cordova, Kyle E. ;
Yaghi, Omar M. .
NATURE MATERIALS, 2018, 17 (04) :301-307
[9]   Understanding Variability in the Hydrogen Evolution Activity of a Cobalt Anthracenetetrathiolate Coordination Polymer [J].
Downes, Courtney A. ;
Marinescu, Smaranda C. .
ACS CATALYSIS, 2017, 7 (12) :8605-8612
[10]   Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products [J].
Gao, Dunfeng ;
Aran-Ais, Rosa M. ;
Jeon, Hyo Sang ;
Roldan Cuenya, Beatriz .
NATURE CATALYSIS, 2019, 2 (03) :198-210