Synergetic effect of nitrogen-doped carbon catalysts for high-efficiency electrochemical CO2 reduction

doi:10.1016/S1872-2067(21)64006-8

Chinese Journal of Catalysis ›› 2022, Vol. 43 ›› Issue (7): 1697-1702.DOI: 10.1016/S1872-2067(21)64006-8

• Special column on catalytic conversion of CO₂ • Previous Articles Next Articles

Synergetic effect of nitrogen-doped carbon catalysts for high-efficiency electrochemical CO₂ reduction

Chuhao Liu^a^,^†, Yue Wu^a^,^†, Jinjie Fang^c, Ke Yu^a, Hui Li^a, Wenjun He^b, Weng-Chon Cheong^d, Shoujie Liu^a, Zheng Chen^e, Jing Dong^b^,^*(), Chen Chen^a^,^#()

^aDepartment of Chemistry, Tsinghua University, Beijing 100084, China
^bScientific Research Department, Nanjing Tech University, Nanjing 211816, Jiangsu, China
^cBeijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
^dDepartment of Physics and Chemistry, Faculty of Science and Technology, University of Macau, Macau, China
^eKey Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Normal University, Wuhu 241000, Anhui, China

Received:2021-09-21 Accepted:2021-11-12 Online:2022-07-18 Published:2022-05-20
Contact: Jing Dong, Chen Chen
About author:First author contact:
^†Contributed equally to this work.
Supported by:
National Key R&D Program of China(2016YFA0202801);National Natural Science Foundation of China(21925202);National Natural Science Foundation of China(21872076);Beijing Natural Science Foundation(JQ18007);Tsinghua University Initiative Scientific Research Program

Abstract

Abstract:

The use of carbon-based materials is an appealing strategy to solve the issue of excessive CO₂ emissions. In particular, metal-free nitrogen-doped carbon materials (mf-NCs) have the advantages of convenient synthesis, cost-effectiveness, and high conductivity and are ideal electrocatalysts for the CO₂ reduction reaction (CO₂RR). However, the unclear identification of the active N sites and the low intrinsic activity of mf-NCs hinder the further development of high-performance CO₂RR electrocatalysts. Achieving precise control over the synthesis of mf-NC catalysts with well-defined active N-species sites is still challenging. To this end, we adopted a facile synthesis method to construct a set of mf-NCs as robust catalysts for CO₂RR. The resulting best-performing catalyst obtained a Faradaic efficiency of CO of approximately 90% at -0.55 V (vs. reversible hydrogen electrode) and good stability. The electrocatalytic performance and in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy measurements collectively revealed that graphitic and pyridinic N can synergistically adsorb CO₂ and H₂O and thus promote CO₂ activation and protonation.

Key words: CO₂ reduction reaction, Nitrogen-doped carbon material, Pyridinic N, Graphitic N, Synergetic effect

Chuhao Liu, Yue Wu, Jinjie Fang, Ke Yu, Hui Li, Wenjun He, Weng-Chon Cheong, Shoujie Liu, Zheng Chen, Jing Dong, Chen Chen. Synergetic effect of nitrogen-doped carbon catalysts for high-efficiency electrochemical CO₂ reduction[J]. Chinese Journal of Catalysis, 2022, 43(7): 1697-1702.

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Figures/Tables 5

Fig. 1. Schematic representation of the mf-NCs synthesis process.

Fig. 2. (a) Thermogravimetric analysis in Ar atmosphere. (b) XRD patterns. (c) Raman spectra of mf-NCs. SEM (d), TEM (e), HRTEM (f), and HAADF-STEM images (g) and corresponding elemental mapping of C (h), N (i), and overlapped (j) images of mf-NC-1000.

Fig. 3. C K-edge XANES of mf-NC-800 (a), mf-NC-1000 (b), and mf-NC-1200 (c). High-resolution N 1s XPS profiles of mf-NC-800 (d), mf-NC-1000 (e), and mf-NC-1200 (f).

Fig. 4. LSV curves (a), FECO (b), and JCO (c) of the catalysts. (d) Stability of mf-NC-1000 at -0.55 V.

Fig. 5. (a) Proposed reaction pathway of CO2RR. In situ ATR-SEIRAS spectra of mf-NC-1000 (b,c) and mf-NC-1200 (d,e).

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Synergetic effect of nitrogen-doped carbon catalysts for high-efficiency electrochemical CO₂ reduction

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