Progress in Preparation of Carbon Materials by Electrochemical Reduction of Carbon Dioxide in Molten Salt

doi:10.19894/j.issn.1000-0518.210313

Chinese Journal of Applied Chemistry ›› 2022, Vol. 39 ›› Issue (7): 1026-1038.DOI: 10.19894/j.issn.1000-0518.210313

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Progress in Preparation of Carbon Materials by Electrochemical Reduction of Carbon Dioxide in Molten Salt

Zhi-Qiang QIAO, De-Qiang JI, Peng WANG, Ying-Ming HE, Zhi-Da LI, De-Bin JI, Hong-Jun WU()

College of Chemistry & Chemical Engineering，Northeast Petroleum University，Daqing 163318，China

Received:2021-06-25 Accepted:2021-10-19 Published:2022-07-01 Online:2022-07-11
Contact: Hong-Jun WU
About author:hjw@nepu.edu.cn
Supported by:
the Excellent Youth Foundation of Heilongjiang Scientific Committee(JC2017002)

Abstract

Abstract:

The greenhouse effect caused by the continuous increase of carbon dioxide concentration has caused a series of ecological and environmental problems such as extreme weather and melting of glaciers around the world. In order to reduce carbon dioxide content and improve the adverse impact of climate warming， it is urgent to develop efficient， green and safe processing technologies and promote the sustainable development of carbon resource cycle. Molten salt ionic liquid， as a good electrochemical conversion medium， provides a promising technical route for carbon dioxide reduction. The research on the capture and electrochemical reduction of carbon dioxide in high-temperature molten salt at home and abroad in recent years is reviewed， and the electrochemical and thermodynamic mechanisms of molten salt electrodeposited carbon are briefly described. The preparation of high value-added carbon materials with different morphologies： amorphous carbon， carbon spheres and carbon nanotubes are summarized， and finally the future development direction is prospected.

Key words: Molten salt electrochemistry, Carbon dioxide, Carbon material, High value utilization

CLC Number:

O646

Zhi-Qiang QIAO, De-Qiang JI, Peng WANG, Ying-Ming HE, Zhi-Da LI, De-Bin JI, Hong-Jun WU. Progress in Preparation of Carbon Materials by Electrochemical Reduction of Carbon Dioxide in Molten Salt[J]. Chinese Journal of Applied Chemistry, 2022, 39(7): 1026-1038.

Figures/Tables 9

Table 1 Carbon dioxide absorption capacity of oxides in different molten carbonate at 450 ℃［29］

熔盐 Molten salt	CO₂平衡分压（Pa， a（M _y O）=0.001 mol/L） Equilibrium partial pressure of CO₂（Pa， a（M _y O）=0.001 mol/L）
Li₂CO₃	1.039
Na₂CO₃	2.462 × 10^-8
K₂CO₃	2.054 × 10^-1
CaCO₃	2.309 × 10³
BaCO₃	1.793 × 10^-3

Fig.1 Internal reaction mechanism of CO2 atmosphere molten carbonate electrolytic cell［45］

Table 2 Gibbs free energy and corresponding standard reduction potential of the electrochemical reduction reaction of alkali metal carbonate［59-60］

温度 Temperature/℃	金属 Metal	还原为碱金属的吉布斯自由能 $Δ G M 2 C O 3 / M °$ /（kJ·mol^-1）	还原为碱金属的电解电势 $E M °$ /V	还原为单质碳的吉布斯自由能 $Δ G M 2 C O 3 / M °$ /（kJ·mol^-1）	还原为单质碳的电解电势 $E M 2 O °$ /V
	Li	581.3	-3.01	661.4	-1.71
540	Na	500.3	-2.59	978.1	-2.53
	K	511.0	-2.65	1181.8	-3.06
	Li	562.5	-2.91	638.4	-1.65
620	Na	480.5	-2.49	952.1	-2.47
	K	489.7	-2.54	1150.1	-2.98
	Li	543.6	-2.82	615.3	-1.59
700	Na	460.7	-2.39	926.2	-2.40
	K	468.5	-2.43	1118.4	-2.90
	Li	531.8	-2.76	599.6	-1.55
750	Na	451.8	-2.34	917.1	-2.38
	K	459.3	-2.38	1110.7	-2.88

Table 2 Gibbs free energy and corresponding standard reduction potential of the electrochemical reduction reaction of alkali metal carbonate［59-60］

温度 Temperature/℃	金属 Metal	还原为碱金属的吉布斯自由能 $Δ G M 2 C O 3 / M °$ /（kJ·mol^-1）	还原为碱金属的电解电势 $E M °$ /V	还原为单质碳的吉布斯自由能 $Δ G M 2 C O 3 / M °$ /（kJ·mol^-1）	还原为单质碳的电解电势 $E M 2 O °$ /V
	Li	581.3	-3.01	661.4	-1.71
540	Na	500.3	-2.59	978.1	-2.53
	K	511.0	-2.65	1181.8	-3.06
	Li	562.5	-2.91	638.4	-1.65
620	Na	480.5	-2.49	952.1	-2.47
	K	489.7	-2.54	1150.1	-2.98
	Li	543.6	-2.82	615.3	-1.59
700	Na	460.7	-2.39	926.2	-2.40
	K	468.5	-2.43	1118.4	-2.90
	Li	531.8	-2.76	599.6	-1.55
750	Na	451.8	-2.34	917.1	-2.38
	K	459.3	-2.38	1110.7	-2.88

Fig.2 SEM images of amorphous carbon prepared by salt mixture system Li2-Na2-K2CO3（mass fraction 33.3%， 33.3%， 33.3%） at different magnification［65］

Fig.3 SEM images of carbon spheres prepared by the salt mixture system （A） Li2-Ca-Na2CO3（mass fraction 66.7%， 20%， 13.3%） and （B） Li2-Ca-K2CO3（mass fraction 66.7%， 20%， 13.3%）［67］

Fig.4 （A） The shape of the cathode before the reaction；（B－E） The shape of product precipitated in the cathode after reaction；（F－H） The scanning electron microscope image of carbon nanofibers prepared by Li2CO3 system at different magnification；（H） The red arrow indicates the nucleation site of Ni， and the blue arrow represents a segment of carbon nanofiber growing from the nucleation site；（I） EOS spectrum of carbon snarofiber shownon blue arrow.［81］

Fig.5 Low（A，C，E） and high（B，D，F） magnification SEM images of carbon sphere prepared by salt mixture system，（A，B）Na2CO3-Li2CO3（mass fraction 8.9%，91.1%），（C，D）Na2CO3-Li2CO3（mass fraction 50%，50%） and （E，F）BaCO3-Li2CO3（mass fraction 20%，80%）［44］

Fig.6 Polarization curves of different metal anodes （A） and cathodes （B）［49］

Fig.7 （A） SEM image of Fe cathode after small current electrolysis，（B－F） EDS spetrum distributions of C， O， Ni， Fe and Zn at the Fe cathode［49］

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Progress in Preparation of Carbon Materials by Electrochemical Reduction of Carbon Dioxide in Molten Salt

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