AI Chat Paper
Note: Please note that the following content is generated by AMiner AI. SciOpen does not take any responsibility related to this content.
{{lang === 'zh_CN' ? '文章概述' : 'Summary'}}
{{lang === 'en_US' ? '中' : 'Eng'}}
Chat more with AI
Powered by AMiner. Clicking this button will take you away from SciOpen.
Home Nano Research Article
Article Link
Cite
EndNote(RIS) BibTeX
Collect
Submit Manuscript
Show Outline
Outline
Show full outline
Hide outline
Outline
Show full outline
Hide outline
Research Article

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

Tai Cao1, Rui Lin1, Shoujie Liu2, Weng-Chon (Max) Cheong3, Zhi Li1( ), Konglin Wu2, Youqi Zhu4, Xiaolu Wang1, Jian Zhang1, Qiheng Li1, Xiao Liang1, Ninghua Fu1, Chen Chen1, Dingsheng Wang1, Qing Peng1, Yadong 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
Show Author Information

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.

Keywords

CO2 reduction reaction Ni-N4 site Ni single atomsself-assembly

Electronic Supplementary Material

Download File(s)
12274_2022_4076_MOESM1_ESM.pdf (2.5 MB)

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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
10

Corbin, N.; Zeng, J.; Williams, K.; Manthiram, K. Heterogeneous molecular catalysts for electrocatalytic CO2 reduction. Nano Res. 2019, 12, 2093–2125.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
14

Sorokin, A. B. Phthalocyanine metal complexes in catalysis. Chem. Rev. 2013, 113, 8152–8191.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
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.
Crossref Google Scholar
Nano Research
Volume 15 Issue 5,
May 2022
Pages 3959-3963
DOI: 10.1007/s12274-022-4076-1
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
Topics:
Electrocatalysis

1020

Views

19

Crossref

20

Web of Science

21

Scopus

9

CSCD

Altmetrics
Received: 30 August 2021
Revised: 11 December 2021
Accepted: 15 December 2021
Published: 15 January 2022
© Tsinghua University Press 2022
Return