Cu/Cu2O Interconnected Porous Aerogel Catalyst for Highly Productive Electrosynthesis of Ethanol from CO2

被引:149
作者
Kim, Chansol [1 ,2 ]
Cho, Kyeong Min [1 ,2 ,3 ]
Park, Kangho [1 ,2 ,4 ]
Kim, Ju Ye [1 ,2 ,5 ]
Yun, Geun-Tae [1 ,2 ]
Toma, Francesca M. [6 ,7 ]
Gereige, Issam [8 ]
Jung, Hee-Tae [1 ,2 ]
机构
[1] Korea Adv Inst Sci & Technol KAIST, Dept Chem & Biomol Engn BK21 Plus, 291 Daehak Ro, Daejeon 34141, South Korea
[2] KAIST Inst Nanocentury, 291 Daehak Ro, Daejeon 34141, South Korea
[3] Agcy Def Dev ADD, CBR Def Technol Directorate, Daejeon 34186, South Korea
[4] Samsung Elect Co Ltd, 1 Samsungjeonja Ro, Hwasung City 18448, Gyeonggi Do, South Korea
[5] Korea Res Inst Chem Technol KRICT, Chem & Proc Technol Div, Daejeon 34114, South Korea
[6] Lawrence Berkeley Natl Lab, Chem Sci Div, 1 Cyclotron Rd, Berkeley, CA 94720 USA
[7] Lawrence Berkeley Natl Lab, Joint Ctr Artificial Photosynth, 1 Cyclotron Rd, Berkeley, CA 94720 USA
[8] Saudi Aramco, Res & Dev Ctr, Dhahran 31311, Saudi Arabia
基金
新加坡国家研究基金会;
关键词
aerogels; carbon dioxide; copper oxide; electrocatalysts; electrosynthesis; CARBON-DIOXIDE REDUCTION; ELECTROCHEMICAL REDUCTION; COPPER-CATALYSTS; ELECTROREDUCTION; ETHYLENE; SELECTIVITY; CONVERSION; HYDROCARBONS; EFFICIENT; INSIGHTS;
D O I
10.1002/adfm.202102142
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Use of Cu and Cu+ is one of the most promising approaches for the production of C-2 products by the electrocatalytic CO2 reduction reaction (CO2RR) because it can facilitate CO2 activation and C-C dimerization. However, the selective electrosynthesis of C2+ products on Cu-0-Cu+ interfaces is critically limited due to the low electrocatalytic production of ethanol relative to ethylene. In this study, a novel porous Cu/Cu2O aerogel network is introduced to afford high ethanol productivity by the electrocatalytic CO2RR. The aerogel is synthesized by a simple chemical redox reaction of a precursor and a reducing agent. CO2RR results reveal that the Cu/Cu2O aerogel produces ethanol as the major product, exhibiting a Faradaic efficiency (FEEtOH) of 41.2% and a partial current density (J(EtOH)) of 32.55 mA cm(-2) in an H-cell reactor. This is the best electrosynthesis performance for ethanol production reported thus far. Electron microscopy and electrochemical analysis results reveal that this dramatic increase in the electrosynthesis performance for ethanol can be attributed to a large number of Cu-0-Cu+ interfaces and an increase of the local pH in the confined porous aerogel network structure with a high-surface-area.
引用
收藏
页数:9
相关论文
共 43 条
[1]   Tuning Cu/Cu2O Interfaces for the Reduction of Carbon Dioxide to Methanol in Aqueous Solutions [J].
Chang, Xiaoxia ;
Wang, Tuo ;
Zhao, Zhi-Jian ;
Yang, Piaoping ;
Greeley, Jeffrey ;
Mu, Rentao ;
Zhang, Gong ;
Gong, Zhongmiao ;
Luo, Zhibin ;
Chen, Jun ;
Cui, Yi ;
Ozin, Geoffrey A. ;
Gong, Jinlong .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2018, 57 (47) :15415-15419
[2]   Confined cavity on a mass-producible wrinkle film promotes selective CO2reduction [J].
Cho, Kyeong Min ;
Jung, Woo-Bin ;
Kim, Donggyu ;
Kim, Ju Ye ;
Kim, Yesol ;
Yun, Geun-Tae ;
Ryu, Seunghwa ;
Al-Saggaf, Ahmed ;
Gereige, Issam ;
Jung, Hee-Tae .
JOURNAL OF MATERIALS CHEMISTRY A, 2020, 8 (29) :14592-14599
[3]   CO2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface [J].
Dinh, Cao-Thang ;
Burdyny, Thomas ;
Kibria, Md Golam ;
Seifitokaldani, Ali ;
Gabardo, Christine M. ;
de Arquer, F. Pelayo Garcia ;
Kiani, Amirreza ;
Edwards, Jonathan P. ;
De Luna, Phil ;
Bushuyev, Oleksandr S. ;
Zou, Chengqin ;
Quintero-Bermudez, Rafael ;
Pang, Yuanjie ;
Sinton, David ;
Sargent, Edward H. .
SCIENCE, 2018, 360 (6390) :783-787
[4]   Continuous-flow electroreduction of carbon dioxide [J].
Endrodi, B. ;
Bencsik, G. ;
Darvas, F. ;
Jones, R. ;
Rajeshwar, K. ;
Janaky, C. .
PROGRESS IN ENERGY AND COMBUSTION SCIENCE, 2017, 62 :133-154
[5]   Plasma-Activated Copper Nanocube Catalysts for Efficient Carbon Dioxide Electroreduction to Hydrocarbons and Alcohols [J].
Gao, Dunfeng ;
Zegkinoglou, Ioannis ;
Divins, Nuria J. ;
Scholten, Fabian ;
Sinev, Ilya ;
Grosse, Philipp ;
Roldan Cuenya, Beatriz .
ACS NANO, 2017, 11 (05) :4825-4831
[6]   Mesostructure-Induced Selectivity in CO2 Reduction Catalysis [J].
Hall, Anthony Shoji ;
Yoon, Youngmin ;
Wuttig, Anna ;
Surendranath, Yogesh .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (47) :14834-14837
[7]   CO2 Reduction Selective for C≥2 Products on Polycrystalline Copper with N-Substituted Pyridinium Additives [J].
Han, Zhiji ;
Kortlever, Ruud ;
Chen, Hsiang-Yun ;
Peters, Jonas C. ;
Agapie, Theodor .
ACS CENTRAL SCIENCE, 2017, 3 (08) :853-859
[8]   Mechanistic Insights into the Selective Electroreduction of Carbon Dioxide to Ethylene on Cu2O-Derived Copper Catalysts [J].
Handoko, Albertus D. ;
Ong, Cheng Wai ;
Huang, Yun ;
Lee, Zheng Guang ;
Lin, Liyi ;
Panetti, Grace B. ;
Yeo, Boon Siang .
JOURNAL OF PHYSICAL CHEMISTRY C, 2016, 120 (36) :20058-20067
[9]   The Effects of Ethanol and Propanol Additions Into Unleaded Gasoline on Exhaust and Noise Emissions of a Spark Ignition Engine [J].
Keskin, A. ;
Guru, M. .
ENERGY SOURCES PART A-RECOVERY UTILIZATION AND ENVIRONMENTAL EFFECTS, 2011, 33 (23) :2194-2205
[10]   Ternary Hybrid Aerogels of g-C3N4/α-Fe2O3 on a 3D Graphene Network: An Efficient and Recyclable Z-Scheme Photocatalyst [J].
Kim, Chansol ;
Cho, Kyeong Min ;
Park, Kangho ;
Kim, Kyoung Hwan ;
Gereige, Issam ;
Jung, Hee-Tae .
CHEMPLUSCHEM, 2020, 85 (01) :169-175