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Research Article

Atomically dispersed Ni anchored on polymer-derived mesh-like N-doped carbon nanofibers as an efficient CO2 electrocatalytic reduction catalyst

Tai Cao1Rui Lin1Shoujie Liu2Weng-Chon (Max) Cheong3Zhi Li1( )Konglin Wu2Youqi Zhu4Xiaolu Wang1Jian Zhang1Qiheng Li1Xiao Liang1Ninghua Fu1Chen Chen1Dingsheng Wang1Qing Peng1Yadong Li1( )
Department of Chemistry, Tsinghua University, Beijing 100084, China
College of Chemistry and Materials Science, Anhui Normal University, Wuhu 241000, China
Department of Physics and Chemistry, Faculty of Science and Technology, University of Macau, Macao SAR, China
Research Center of Materials Science, Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, Beijing Institute of Technology, Beijing 100081, China
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Graphical Abstract

A self-assembly strategy was developed to synthesize a highly efficient CO2 reduction electrocatalyst with atomically dispersed Ni active centers anchored on polymer-derived mesh-like N-doped carbon nanofibers.

Abstract

Efficient electroreduction of CO2 into CO and other chemicals turns greenhouse gases into fuels and value-added chemicals, holding great promise for a closed carbon cycle and the alleviation of climate changes. However, there are still challenges in the large-scale application of CO2 electroreduction due to the sluggish kinetics. Herein we develop a self-assembly strategy to synthesize a highly efficient CO2 reduction electrocatalyst with atomically dispersed Ni-N4 active centers anchored on polymer-derived mesh-like N-doped carbon nanofibers (Ni-N4/NC). The Ni-N4/NC exhibits high selectivity for CO2 reduction reaction with CO Faradaic efficiency (CO FE) above 90% over a wide potential range from −0.6 to −1.0 V vs. RHE. The catalyst reaches a maximum CO FE up to 98.4% at −0.8 V with a TOF of 1.28 x 105 h–1 and Tafel slope of 113 mV·dec–1. The catalyst also exhibits remarkable stability, with little change in current density and CO FE over a 10-hour durability test at –0.8 V vs. RHE. This method provides a new route for the synthesis of highly efficient CO2 reduction electrocatalyst.

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References

1

Gu, J.; Hsu, C. S.; Bai, L. C.; Chen, H. M.; Hu, X. L. Atomically dispersed Fe3+ sites catalyze efficient CO2 electroreduction to CO. Science 2019, 364, 1091–1094.

2

Nitopi, S.; Bertheussen, E.; Scott, S. B.; Liu, X. Y.; Engstfeld, A. K.; Horch, S.; Seger, B.; Stephens, I. E. L.; Chan, K.; Hahn, C. et al. Progress and perspectives of electrochemical CO2 reduction on copper in aqueous electrolyte. Chem. Rev. 2019, 119, 7610–7672.

3

Zheng, T. T.; Jiang, K.; Wang, H. T. Recent advances in electrochemical CO2-to-CO conversion on heterogeneous catalysts. Adv. Mater. 2018, 30, 1802066.

4

Birdja, Y. Y.; Pérez-Gallent, E.; Figueiredo, M. C.; Göttle, A. J.; Calle-Vallejo, F.; Koper, M. T. M. Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels. Nat. Energy 2019, 4, 732–745.

5

Su, X.; Yang, X. F.; Huang, Y. Q.; Liu, B.; Zhang, T. Single-atom catalysis toward efficient CO2 conversion to CO and formate products. Acc. Chem. Res. 2019, 52, 656–664.

6

Chen, W. Y.; Liu, X. M.; Han, B.; Liang, S. J.; Deng, H.; Lin, Z. Boosted photoreduction of diluted CO2 through oxygen vacancy engineering in NiO nanoplatelets. Nano Res. 2020, 14, 730–737.

7

Liang, S. J.; Liu, X. M.; Zhong, Z. Q.; Han, B.; Zhong, X. H.; Chen, W. Y.; Song, K. N.; Deng, H.; Lin, Z. Lattice-strained nanotubes facilitate efficient natural sunlight-driven CO2 photoreduction. Nano Res. 2020, 14, 2558–2567.

8

Lin, R.; Ma, X. L.; Cheong, W. C.; Zhang, C.; Zhu, W.; Pei, J. J.; Zhang, K. Y.; Wang, B.; Liang, S. Y.; Liu, Y. X. et al. PdAg bimetallic electrocatalyst for highly selective reduction of CO2 with low COOH* formation energy and facile CO desorption. Nano Res. 2019, 12, 2866–2871.

9

Zhang, N. Q.; Zhang, X. X.; Tao, L.; Jiang, P.; Ye, C. L.; Lin, R.; Huang, Z. W.; Li, A.; Pang, D. W.; Yan, H. et al. Silver single-atom catalyst for efficient electrochemical 2 reduction synthesized from thermal transformation and surface reconstruction. Angew. Chem., Int. Ed. 2021, 60, 6170–6176.

10

Corbin, N.; Zeng, J.; Williams, K.; Manthiram, K. Heterogeneous molecular catalysts for electrocatalytic CO2 reduction. Nano Res. 2019, 12, 2093–2125.

11

Jiang, Z. L.; Wang, T.; Pei, J. J.; Shang, H. S.; Zhou, D. N.; Li, H. J.; Dong, J. C.; Wang, Y.; Cao, R.; Zhuang, Z. B. et al. Discovery of main group single Sb-N4 active sites for CO2 electroreduction to formate with high efficiency. Energy Environ. Sci. 2020, 13, 2856–2863.

12

Cheng, Y.; Veder, J. P.; Thomsen, L.; Zhao, S. Y.; Saunders, M.; Demichelis, R.; Liu, C.; De Marco, R.; Jiang, S. P. Electrochemically substituted metal phthalocyanines, e-MPc (M = Co, Ni), as highly active and selective catalysts for CO2 reduction. J. Mater. Chem. A 2018, 6, 1370–1375.

13

Chen, J. Y.; Wang, T. T.; Li, Z. J.; Yang, B.; Zhang, Q. H.; Lei, L. C.; Feng, P. Y.; Hou, Y. Recent progress and perspective of electrochemical CO2 reduction towards C2-C5 products over non-precious metal heterogeneous electrocatalysts. Nano Res. 2021, 14, 3188–3207.

14

Sorokin, A. B. Phthalocyanine metal complexes in catalysis. Chem. Rev. 2013, 113, 8152–8191.

15

Zhang, X.; Wang, Y.; Gu, M.; Wang, M. Y.; Zhang, Z. S.; Pan, W. Y.; Jiang, Z.; Zheng, H. Z.; Lucero, M.; Wang, H. L. et al. Molecular engineering of dispersed nickel phthalocyanines on carbon nanotubes for selective CO2 reduction. Nat. Energy 2020, 5, 684–692.

16

Ma, Z. J.; Zhang, X. L.; Han, X. Y.; Wu, D. P.; Wang, H. J.; Gao, Z. Y.; Xu, F.; Jiang, K. Synergistic adsorption and activation of nickel phthalocyanine anchored onto ketjenblack for CO2 electrochemical reduction. Appl. Surf. Sci. 2021, 538, 148134.

17

Pan, Y.; Lin, R.; Chen, Y. J.; Liu, S. J.; Zhu, W.; Cao, X.; Chen, W. X.; Wu, K. L.; Cheong, W. C.; Wang, Y. et al. Design of single-atom Co-N5 catalytic site: A robust electrocatalyst for CO2 reduction with nearly 100% CO selectivity and remarkable stability. J. Am. Chem. Soc. 2018, 140, 4218–4221.

18

Pan, Y.; Liu, S. J.; Sun, K. A.; Chen, X.; Wang, B.; Wu, K. L.; Cao, X.; Cheong, W. C.; Shen, R. A.; Han, A. J. et al. A bimetallic Zn/Fe polyphthalocyanine-derived single-atom Fe-N4 catalytic site: A superior trifunctional catalyst for overall water splitting and Zn-air batteries. Angew. Chem., Int. Ed. 2018, 57, 8614–8618.

19

Yang, X.; Cheng, J.; Fang, B. Z.; Xuan, X. X.; Liu, N.; Yang, X.; Zhou, J. H. Single Ni atoms with higher positive charges induced by hydroxyls for electrocatalytic CO2 reduction. Nanoscale 2020, 12, 18437–18445.

20

Zhang, Y.; Jiao, L.; Yang, W. J.; Xie, C. F.; Jiang, H. L. Rational fabrication of low-coordinate single-atom Ni electrocatalysts by mofs for highly selective CO2 reduction. Angew. Chem., Int. Ed. 2021, 133, 7686–7689.

21

Fan, Q.; Hou, P. F.; Choi, C.; Wu, T. S.; Hong, S.; Li, F.; Soo, Y. L.; Kang, P.; Jung, Y.; Sun, Z. Y. Activation of Ni particles into single Ni-N atoms for efficient electrochemical reduction of CO2. Adv. Energy Mater. 2020, 10, 1903068.

22

Zheng, T. T.; Jiang, K.; Ta, N.; Hu, Y. F.; Zeng, J.; Liu, J. Y.; Wang, H. T. Large-scale and highly selective CO2 electrocatalytic reduction on nickel single-atom catalyst. Joule 2019, 3, 265–278.

23

Prslja, P.; López, N. Stability and redispersion of Ni nanoparticles supported on N-doped carbons for the CO2 electrochemical reduction. ACS Catal. 2021, 11, 88–94.

24

Cheng, Y.; Zhao, S. Y.; Johannessen, B.; Veder, J. P.; Saunders, M.; Rowles, M. R.; Cheng, M.; Liu, C.; Chisholm, M. F.; De Marco, R. et al. Atomically dispersed transition metals on carbon nanotubes with ultrahigh loading for selective electrochemical carbon dioxide reduction. Adv. Mater. 2018, 30, 1706287.

25

Li, X. G.; Bi, W. T.; Chen, M. L.; Sun, Y. X.; Ju, H. X.; Yan, W. S.; Zhu, J. F.; Wu, X. J.; Chu, W. S.; Wu, C. Z. et al. Exclusive Ni-N4 sites realize near-unity CO selectivity for electrochemical CO2 reduction. J. Am. Chem. Soc. 2017, 139, 14889–14892.

26

Tan, D. X.; Zhang, J. L.; Yao, L.; Tan, X. N.; Cheng, X.; Wan, Q.; Han, B. X.; Zheng, L. R.; Zhang, J. Multi-shelled CuO microboxes for carbon dioxide reduction to ethylene. Nano Res. 2020, 13, 768–774.

27

Jiang, K.; Siahrostami, S.; Zheng, T. T.; Hu, Y. F.; Hwang, S.; Stavitski, E.; Peng, Y. D.; Dynes, J.; Gangisetty, M.; Su, D. et al. Isolated Ni single atoms in graphene nanosheets for high-performance CO2 reduction. Energy Environ. Sci. 2018, 11, 893–903.

28

Xiong, W. F.; Li, H. F.; Wang, H. M.; Yi, J. D.; You, H. H.; Zhang, S. Y.; Hou, Y.; Cao, M. N.; Zhang, T.; Cao, R. Hollow mesoporous carbon sphere loaded Ni-N4 single-atom: Support structure study for CO2 electrocatalytic reduction catalyst. Small 2020, 16, 2003943.

29

Cao, T.; Wang, D. S.; Zhang, J. T.; Cao, C. B.; Li, Y. D. Bamboo-like nitrogen-doped carbon nanotubes with Co nanoparticles encapsulated at the tips: Uniform and large-scale synthesis and high-performance electrocatalysts for oxygen reduction. Chemistry 2015, 21, 14022–14029.

30

Rong, X.; Wang, H. J.; Lu, X. L.; Si, R.; Lu, T. B. Controlled synthesis of a vacancy-defect single-atom catalyst for boosting CO2 electroreduction. Angew. Chem., Int. Ed. 2020, 59, 1961–1965.

Nano Research
Pages 3959-3963
Cite this article:
Cao T, Lin R, Liu S, et al. Atomically dispersed Ni anchored on polymer-derived mesh-like N-doped carbon nanofibers as an efficient CO2 electrocatalytic reduction catalyst. Nano Research, 2022, 15(5): 3959-3963. https://doi.org/10.1007/s12274-022-4076-1
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Received: 30 August 2021
Revised: 11 December 2021
Accepted: 15 December 2021
Published: 15 January 2022
© Tsinghua University Press 2022
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