Electrochemical upgrade of CO2 from amine capture solution

被引:176
作者
Lee, Geonhui [1 ]
Li, Yuguang C. [1 ]
Kim, Ji-Yong [2 ]
Peng, Tao [1 ]
Nam, Dae-Hyun [1 ]
Sedighian Rasouli, Armin [1 ]
Li, Fengwang [1 ]
Luo, Mingchuan [1 ]
Ip, Alexander H. [1 ]
Joo, Young-Chang [2 ]
Sargent, Edward H. [1 ]
机构
[1] Univ Toronto, Dept Elect & Comp Engn, Toronto, ON, Canada
[2] Seoul Natl Univ, Dept Mat Sci & Engn, Seoul, South Korea
基金
新加坡国家研究基金会; 加拿大自然科学与工程研究理事会;
关键词
NORMAL-COORDINATE ANALYSIS; CARBON-DIOXIDE; ELECTROCATALYTIC REDUCTION; INFRARED-SPECTRA; RAMAN-SPECTRA; ELECTROREDUCTION; ADSORPTION; ELECTRODE; INSIGHTS; CATIONS;
D O I
10.1038/s41560-020-00735-z
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
CO2 capture technologies based on chemisorption present the potential to lower net emissions of CO2 into the atmosphere. The electrochemical upgrade of captured CO2 to value-added products would be particularly convenient. Here we find that this goal is curtailed when the adduct of the capture molecule with CO2 fails to place the CO2 sufficiently close to the site of the heterogeneous reaction. We investigate tailoring the electrochemical double layer to achieve the valorization of chemisorbed CO2 in an aqueous monoethanolamine electrolyte. We reveal, using electrochemical studies and in situ surface-enhanced Raman spectroscopy, that a smaller double layer distance correlates with improved activity for CO2 to CO from amine solutions. With the aid of an alkali cation and accelerated mass transport by system design-temperature and concentration-we demonstrate amine-CO2 conversion to CO with 72% Faradaic efficiency at 50 mA cm(-2). Electrochemical conversion of CO2 into high-value products is attractive for lowering net carbon emissions. Lee et al. present the valorization of chemisorbed CO2 to CO in an aqueous monoethanolamine electrolyte via tailoring of the electrochemical double layer, with 72% Faradaic efficiency at 50 mA cm(-2).
引用
收藏
页码:46 / 53
页数:8
相关论文
共 63 条
[21]   Insights into the electrocatalytic reduction of CO2 on metallic silver surfaces [J].
Hatsukade, Toru ;
Kuhl, Kendra P. ;
Cave, Etosha R. ;
Abram, David N. ;
Jaramillo, Thomas F. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2014, 16 (27) :13814-13819
[22]   CO2 Reduction on Cu at Low Overpotentials with Surface-Enhanced in Situ Spectroscopy [J].
Heyes, Jeffrey ;
Dunwell, Marco ;
Xu, Bingjun .
JOURNAL OF PHYSICAL CHEMISTRY C, 2016, 120 (31) :17334-17341
[23]   Achieving highly efficient CO2 to CO electroreduction exceeding 300 mA cm-2 with single-atom nickel electrocatalysts [J].
Jeong, Hui-Yun ;
Balamurugan, Mani ;
Choutipalli, Venkata Surya Kumar ;
Jeong, Eun-suk ;
Subramanian, Venkatesan ;
Sim, Uk ;
Nam, Ki Tae .
JOURNAL OF MATERIALS CHEMISTRY A, 2019, 7 (17) :10651-10661
[24]   Promoting Amine-Activated Electrochemical CO2 Conversion with Alkali Salts [J].
Khurram, Aliza ;
Yan, Lifu ;
Yin, Yuming ;
Zhao, Lingling ;
Gallant, Betar M. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2019, 123 (30) :18222-18231
[25]   Tailoring the Discharge Reaction in Li-CO2 Batteries through Incorporation of CO2 Capture Chemistry [J].
Khurram, Aliza ;
He, Mingfu ;
Gallant, Betar M. .
JOULE, 2018, 2 (12) :2649-2666
[26]   Fluctuations of surface-enhanced Raman spectra of CO adsorbed on gold substrates [J].
Kudelski, A ;
Pettinger, B .
CHEMICAL PHYSICS LETTERS, 2004, 383 (1-2) :76-79
[27]  
Larkin PJ, 2011, INFRARED AND RAMAN SPECTROSCOPY: PRINCIPLES AND SPECTRAL INTERPRETATION, P1
[28]   Hydrogen bonding steers the product selectivity of electrocatalytic CO reduction [J].
Li, Jingyi ;
Li, Xiang ;
Gunathunge, Charuni M. ;
Waegele, Matthias M. .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2019, 116 (19) :9220-9229
[29]   CO2 Electroreduction from Carbonate Electrolyte [J].
Li, Yuguang C. ;
Lee, Geonhui ;
Yuan, Tiange ;
Wang, Ying ;
Nam, Dae-Hyun ;
Wang, Ziyun ;
de Arquer, F. Pelayo Garcia ;
Lum, Yanwei ;
Cao-Thang Dinh ;
Voznyy, Oleksandr ;
Sargent, Edward H. .
ACS ENERGY LETTERS, 2019, 4 (06) :1427-1431
[30]   Bipolar Membranes Inhibit Product Crossover in CO2 Electrolysis Cells [J].
Li, Yuguang C. ;
Yan, Zhifei ;
Hitt, Jeremy ;
Wycisk, Ryszard ;
Pintauro, Peter N. ;
Mallouk, Thomas E. .
ADVANCED SUSTAINABLE SYSTEMS, 2018, 2 (04)