Electrochemical Reduction of Carbon Dioxide to Carbon Materials for Two⁃Electron Oxygen Reduction Reaction

doi:10.19894/j.issn.1000-0518.210320

Chinese Journal of Applied Chemistry ›› 2022, Vol. 39 ›› Issue (4): 657-665.DOI: 10.19894/j.issn.1000-0518.210320

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Electrochemical Reduction of Carbon Dioxide to Carbon Materials for Two⁃Electron Oxygen Reduction Reaction

Ao YU, Guo-Ming MA, Long-Tao ZHU, Ping PENG(), Fang-Fang LI()

State Key Laboratory of Materials Processing and Die & Mould Technology，School of Materials Science and Engineering，Huazhong University of Science and Technology，Wuhan 430074，China

Received:2021-06-30 Accepted:2021-09-26 Published:2022-04-01 Online:2022-04-19
Contact: Ping PENG,Fang-Fang LI
About author:ffli@hust.edu.cn
Supported by:
the National Natural Science Foundation of China(21971077)

1. .pdf(830KB)

Abstract

Abstract:

In this paper， the effects of three different anodic materials （copper wire， galvanized steel and nickel wire） on the structure and morphology of carbon materials prepared by electrochemical reduction of CO₂ in molten salt were studied. Three carbon structures， e.g.， hollow quadrilateral carbon （HQC，the product with Cu as an anode）， carbon nanosheet （CNS， the product with galvanized steel as an anode） and sponge porous carbon （SPC， the product with Ni as an anode）， were prepared， and their electrocatalytic properties towards the two-electron oxygen reduction reaction （2e^-ORR） were explored. The results show that the CNS prepared by using galvanized steel as the anode material is composed of a large number of carbon nanosheets， in which there are abundant pore structure defects. Compared with HQC and SPC， CNS shows the highest 2e^-ORR electrocatalytic activity and H₂O₂ selectivity （close to 90%）. The high activity and selectivity of CNS are attributed to its high I_D/I_G （I_D/I_G is the ratio of the intensity of D peak and G peak in Raman spectrum， and its ratio reflects the defective degree of the material） value and high C—O/CO ratio， indicating that structural defects and C—O/CO functional groups are crucial to the catalytic performance of CNS. In addition， CNS exhibits excellent electrocatalytic stability， and the ring current almost does not decay after 14 hours potentiostatic test. The use of CO₂ as the carbon source to synthesize electrocatalytic carbon materials not only can be used as a potential option to mitigate the greenhouse effect， but also provide a new idea for the practical application of CO₂ derived carbons.

Key words: Electrochemical reduction, Carbon dioxide, Carbon materials, Hydrogen peroxide

CLC Number:

O646

Ao YU, Guo-Ming MA, Long-Tao ZHU, Ping PENG, Fang-Fang LI. Electrochemical Reduction of Carbon Dioxide to Carbon Materials for Two⁃Electron Oxygen Reduction Reaction[J]. Chinese Journal of Applied Chemistry, 2022, 39(4): 657-665.

Figures/Tables 5

Fig.1 Schematic diagram of preparation of solid carbon materials with carbon dioxide as the carbon source

Fig.2 TEM images （A - D） of SPC； HAADF images （E） and mapping images （F - H） of SPC

Fig.3 （A） XRD patterns of HQC （a）， CNS （b） and SPC （c）；（B） Normalized Raman spectra

Fig.4 High resolution XPS spectra of C 1s （A）， O 1s （B） and the relative content of C—O and CO （C） of HQC，CNS and SPC

Fig.5 （A - C） Cyclic voltammetry curves of HQC， CNS and SPC in N2 （a） and O2 （b） saturated 0.1 mol/L KOH solution， respectively；（D） Polarization curves of the catalysts at 1600 r/min （solid lines） and simultaneous H2O2 detection currents at the ring electrode （dashed lines）， a， b and c represent the disk current of HQC， CNS and SPC， respectively； d， e and f represent the ring current of HQC， CNS and SPC， respectively；（E） Calculated selectivity of HQC （a）， CNS （b） and SPC （c） at various potentials in 0.1 mol/L KOH；（F） Electron transfer numbers of HQC （a）， CNS （b） and SPC （c） at various potentials in 0.1 mol/L KOH；（G） The catalytic stability of CNS， and the a and b represent the disc current and ring current， respectively；（H） Relationship between the average H2O2 selectivity and ID/IG values；（I） Relationship between the average H2O2 selectivity and the ratios of C—O/CO

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Electrochemical Reduction of Carbon Dioxide to Carbon Materials for Two⁃Electron Oxygen Reduction Reaction

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