Electrochemical Conversion of CO2 to HCOOH at Tin Cathode: Development of a Theoretical Model and Comparison with Experimental Results

被引:14
作者
Proietto, Federica [1 ]
Galia, Alessandro [1 ]
Scialdone, Onofrio [1 ]
机构
[1] Univ Palermo, DIID, Ingn Chim, Gest,Informat,Meccan, Viale Sci,Ed 6, I-90128 Palermo, Italy
关键词
CO2; reduction; electrochemistry; pressure; theoretical model; tin cathode; CARBON-DIOXIDE; HIGH-PRESSURE; OPERATIVE PARAMETERS; AQUEOUS-SOLUTIONS; METAL-ELECTRODES; FORMIC-ACID; REDUCTION; FORMATE; ELECTROCARBOXYLATION; OXIDE;
D O I
10.1002/celc.201801067
中图分类号
O646 [电化学、电解、磁化学];
学科分类号
081704 ;
摘要
The electrochemical reduction of pressurized carbon dioxide at tin cathode is considered a very promising process for the production of formic acid. Here, the process was studied in an undivided cell with the aim of developing a simple theoretical model. First, a large series of polarization and electrolyses was performed in order to evaluate the kinetic of the process. According to the literature, experimental results can be described by a simple reaction mechanism, which involves the following key stages: (i) mass transfer of CO2 to the cathode; (i) its adsorption described by a Langmuir equation; (iii) the reduction of adsorbed CO2. A simple model was developed based on the cathodic conversion of pressurized CO2 to HCOOH and on its anodic oxidation. The theoretical model was in a good agreement with experimental results collected in this work and in previous ones and well described the effect of several operative parameters, including current density, pressure and kind of reactor.
引用
收藏
页码:162 / 172
页数:11
相关论文
共 51 条
[1]   The Electrochemical Reduction of Carbon Dioxide to Formate/Formic Acid: Engineering and Economic Feasibility [J].
Agarwal, Arun S. ;
Zhai, Yumei ;
Hill, Davion ;
Sridhar, Narasi .
CHEMSUSCHEM, 2011, 4 (09) :1301-1310
[2]   Towards the electrochemical conversion of carbon dioxide into methanol [J].
Albo, J. ;
Alvarez-Guerra, M. ;
Castano, P. ;
Irabien, A. .
GREEN CHEMISTRY, 2015, 17 (04) :2304-2324
[3]   Continuous electrochemical reduction of carbon dioxide into formate using a tin cathode: Comparison with lead cathode [J].
Alvarez-Guerra, Manuel ;
Del Castillo, Andres ;
Irabien, Angel .
CHEMICAL ENGINEERING RESEARCH & DESIGN, 2014, 92 (04) :692-701
[4]   Degradation and deactivation of Sn catalyst used for CO2 reduction as function of overpotential [J].
Anawati ;
Frankel, G. S. ;
Agarwal, Arun ;
Sridhar, Narasi .
ELECTROCHIMICA ACTA, 2014, 133 :188-196
[5]   The investigation of the kinetics and mechanism of hydrogen evolution reaction on tin [J].
Azizi, O. ;
Jafarian, M. ;
Gobal, F. ;
Heli, H. ;
Mahjani, M. G. .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2007, 32 (12) :1755-1761
[6]   ELECTROCHEMICAL REDUCTION OF CARBON-DIOXIDE ON VARIOUS METAL-ELECTRODES IN LOW-TEMPERATURE AQUEOUS KHCO3 MEDIA [J].
AZUMA, M ;
HASHIMOTO, K ;
HIRAMOTO, M ;
WATANABE, M ;
SAKATA, T .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1990, 137 (06) :1772-1778
[7]   Mechanistic Insights into the Reduction of CO2 on Tin Electrodes using in Situ ATR-IR Spectroscopy [J].
Baruch, Maor F. ;
Pander, James E., III ;
White, James L. ;
Bocarsly, Andrew B. .
ACS CATALYSIS, 2015, 5 (05) :3148-3156
[8]   Tinned graphite felt cathodes for scale-up of electrochemical reduction of aqueous CO2 [J].
Bumroongsakulsawat, P. ;
Kelsall, G. H. .
ELECTROCHIMICA ACTA, 2015, 159 :242-251
[9]   Effect of solution pH on CO: formate formation rates during electrochemical reduction of aqueous CO2 at Sn cathodes [J].
Bumroongsakulsawat, P. ;
Kelsall, G. H. .
ELECTROCHIMICA ACTA, 2014, 141 :216-225
[10]   Effects of process conditions and electrode material on reaction pathways for carbon dioxide electroreduction with particular reference to formate formation [J].
Chaplin, RPS ;
Wragg, AA .
JOURNAL OF APPLIED ELECTROCHEMISTRY, 2003, 33 (12) :1107-1123