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Frontiers of Chemical Science and Engineering

ISSN 2095-0179

ISSN 2095-0187(Online)

CN 11-5981/TQ

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Front Chem Sci Eng    2012, Vol. 6 Issue (4) : 381-388    https://doi.org/10.1007/s11705-012-1216-2
RESEARCH ARTICLE
Preparation of a Pb loaded gas diffusion electrode and its application to CO2 electroreduction
Ang LI, Hua WANG(), Jinyu HAN, Li LIU
Key Laboratory for Green Chemical Technology (Ministry of Education), School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China
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Abstract

A Pb loaded gas diffusion electrode was fabricated and used for the electroreduction of CO2 to formic acid. The Pb/C catalyst was prepared by isometric impregnation. The crystal structure and morphology of the Pb/C catalyst were characterized by X-ray diffraction (XRD) and transmission electron microscope (TEM). The preparation conditions of the gas diffusion electrode were optimized by adjusting the amounts of polytetrafluoroethylene (PTFE) in the gas diffusion layer and acetylene black in the catalytic layer. The electrochemical performance of the as-prepared gas diffusion electrode was studied by chronoamperometry and cyclic voltammetry. The optimized gas diffusion electrode showed good catalytic performance for the electroreduction of CO2. The current efficiency of formic acid after 1 h of operation reached a maximum of 22% at -2.0 V versus saturated calomel electrode (SCE).
Keywords electroreduction      carbon dioxide      lead catalyst      gas diffusion electrode      formic acid     
Corresponding Author(s): WANG Hua,Email:tjuwanghua@tju.edu.cn   
Issue Date: 05 December 2012
 Cite this article:   
Ang LI,Hua WANG,Jinyu HAN, et al. Preparation of a Pb loaded gas diffusion electrode and its application to CO2 electroreduction[J]. Front Chem Sci Eng, 2012, 6(4): 381-388.
 URL:  
https://academic.hep.com.cn/fcse/EN/10.1007/s11705-012-1216-2
https://academic.hep.com.cn/fcse/EN/Y2012/V6/I4/381
Fig.1  Schematic diagram of the self-made electrolytic cell
Fig.1  Schematic diagram of the self-made electrolytic cell
Fig.1  Schematic diagram of the self-made electrolytic cell
Fig.1  Schematic diagram of the self-made electrolytic cell
Fig.1  Schematic diagram of the self-made electrolytic cell
Fig.1  Schematic diagram of the self-made electrolytic cell
Fig.2  XRD patterns of the active carbon carrier and Pb/C catalyst
Fig.2  XRD patterns of the active carbon carrier and Pb/C catalyst
Fig.2  XRD patterns of the active carbon carrier and Pb/C catalyst
Fig.2  XRD patterns of the active carbon carrier and Pb/C catalyst
Fig.2  XRD patterns of the active carbon carrier and Pb/C catalyst
Fig.2  XRD patterns of the active carbon carrier and Pb/C catalyst
Fig.3  TEM image of Pb/C catalyst with different particles sizes
Fig.3  TEM image of Pb/C catalyst with different particles sizes
Fig.3  TEM image of Pb/C catalyst with different particles sizes
Fig.3  TEM image of Pb/C catalyst with different particles sizes
Fig.3  TEM image of Pb/C catalyst with different particles sizes
Fig.3  TEM image of Pb/C catalyst with different particles sizes
SampleAcetylene black:PTFE/(g:g)a)Acetylene black:Na2SO4/(g:g)Thickness /mmCO2 permeability /(103cm3(STP)·cm-2·s-1·cm-1 Hg)
GDL-11:12.5:10.383.90
GDL-23:22.5:10.385.21
GDL-37:32.5:10.385.88
Tab.1  Compositions and permeability evaluation of GDL samples
Fig.4  SEM images of GDLs (a) GDL-1, (b) GDL-2, and (c) GDL-3
Fig.4  SEM images of GDLs (a) GDL-1, (b) GDL-2, and (c) GDL-3
Fig.4  SEM images of GDLs (a) GDL-1, (b) GDL-2, and (c) GDL-3
Fig.4  SEM images of GDLs (a) GDL-1, (b) GDL-2, and (c) GDL-3
Fig.4  SEM images of GDLs (a) GDL-1, (b) GDL-2, and (c) GDL-3
Fig.4  SEM images of GDLs (a) GDL-1, (b) GDL-2, and (c) GDL-3
Fig.5  CA measurements of GDEs with different proportions of acetylene black at -1.0 V
Fig.5  CA measurements of GDEs with different proportions of acetylene black at -1.0 V
Fig.5  CA measurements of GDEs with different proportions of acetylene black at -1.0 V
Fig.5  CA measurements of GDEs with different proportions of acetylene black at -1.0 V
Fig.5  CA measurements of GDEs with different proportions of acetylene black at -1.0 V
Fig.5  CA measurements of GDEs with different proportions of acetylene black at -1.0 V
Fig.6  The relationship between the proportion of acetylene black and the amount of formic acid produced. Reaction conditions: room temperature, -1.8 V, 1 h; cathode fed with CO at 40 mL·min
Fig.6  The relationship between the proportion of acetylene black and the amount of formic acid produced. Reaction conditions: room temperature, -1.8 V, 1 h; cathode fed with CO at 40 mL·min
Fig.6  The relationship between the proportion of acetylene black and the amount of formic acid produced. Reaction conditions: room temperature, -1.8 V, 1 h; cathode fed with CO at 40 mL·min
Fig.6  The relationship between the proportion of acetylene black and the amount of formic acid produced. Reaction conditions: room temperature, -1.8 V, 1 h; cathode fed with CO at 40 mL·min
Fig.6  The relationship between the proportion of acetylene black and the amount of formic acid produced. Reaction conditions: room temperature, -1.8 V, 1 h; cathode fed with CO at 40 mL·min
Fig.6  The relationship between the proportion of acetylene black and the amount of formic acid produced. Reaction conditions: room temperature, -1.8 V, 1 h; cathode fed with CO at 40 mL·min
Fig.7  CV test of optimized GDE in 0.5 mol·L KHCO solution. Scan rate was 10 mV·s
Fig.7  CV test of optimized GDE in 0.5 mol·L KHCO solution. Scan rate was 10 mV·s
Fig.7  CV test of optimized GDE in 0.5 mol·L KHCO solution. Scan rate was 10 mV·s
Fig.7  CV test of optimized GDE in 0.5 mol·L KHCO solution. Scan rate was 10 mV·s
Fig.7  CV test of optimized GDE in 0.5 mol·L KHCO solution. Scan rate was 10 mV·s
Fig.7  CV test of optimized GDE in 0.5 mol·L KHCO solution. Scan rate was 10 mV·s
Fig.8  Accumulated product concentration over the course of GDE operation. Reaction conditions: operated at room temperature and -1.8 V for 1 h; cathode fed with CO at 40 mL·min
Fig.8  Accumulated product concentration over the course of GDE operation. Reaction conditions: operated at room temperature and -1.8 V for 1 h; cathode fed with CO at 40 mL·min
Fig.8  Accumulated product concentration over the course of GDE operation. Reaction conditions: operated at room temperature and -1.8 V for 1 h; cathode fed with CO at 40 mL·min
Fig.8  Accumulated product concentration over the course of GDE operation. Reaction conditions: operated at room temperature and -1.8 V for 1 h; cathode fed with CO at 40 mL·min
Fig.8  Accumulated product concentration over the course of GDE operation. Reaction conditions: operated at room temperature and -1.8 V for 1 h; cathode fed with CO at 40 mL·min
Fig.8  Accumulated product concentration over the course of GDE operation. Reaction conditions: operated at room temperature and -1.8 V for 1 h; cathode fed with CO at 40 mL·min
Time interval/min5–1010–2020–3030–4040–5050–60
Average reaction rate/(mg·L-1·min-1)0.061.440.161.380.840.25
Tab.2  Average reaction rates at different time intervals
Fig.9  (a) Final formic acid concentrations at different potentials (b) Final current efficiency at different potentials Reaction conditions: room temperature for 1 h; cathode fed with CO at 40?mL·min
Fig.9  (a) Final formic acid concentrations at different potentials (b) Final current efficiency at different potentials Reaction conditions: room temperature for 1 h; cathode fed with CO at 40?mL·min
Fig.9  (a) Final formic acid concentrations at different potentials (b) Final current efficiency at different potentials Reaction conditions: room temperature for 1 h; cathode fed with CO at 40?mL·min
Fig.9  (a) Final formic acid concentrations at different potentials (b) Final current efficiency at different potentials Reaction conditions: room temperature for 1 h; cathode fed with CO at 40?mL·min
Fig.9  (a) Final formic acid concentrations at different potentials (b) Final current efficiency at different potentials Reaction conditions: room temperature for 1 h; cathode fed with CO at 40?mL·min
Fig.9  (a) Final formic acid concentrations at different potentials (b) Final current efficiency at different potentials Reaction conditions: room temperature for 1 h; cathode fed with CO at 40?mL·min
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