Citation: Yanming Liu, Haolei Yang, Xinfei Fan, Bing Shan, Thomas J. Meyer. Promoting electrochemical reduction of CO₂ to ethanol by B/N-doped sp³/sp² nanocarbon electrode[J]. Chinese Chemical Letters, ;2022, 33(10): 4691-4694. doi: 10.1016/j.cclet.2021.12.063 shu

Promoting electrochemical reduction of CO₂ to ethanol by B/N-doped sp³/sp² nanocarbon electrode

Yanming Liu ^{a, b, *,} ,
Haolei Yang ^a ,
Xinfei Fan ^c ,
Bing Shan ^b ,
Thomas J. Meyer ^{b, *,}

a.
Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China
b.
Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, United States
c.
College of Environmental Science and Engineering, Dalian Maritime University, Dalian 116026, China

liuyanm@dlut.edu.cn

tjmeyer@unc.edu

Received Date: 6 August 2021
Revised Date: 7 October 2021
Accepted Date: 23 December 2021
Available Online: 27 December 2021

Figures(4)

Electrochemical reduction of CO₂ to value-added chemicals holds promise for carbon utilization and renewable electricity storage. However, selective CO₂ reduction to multi-carbon fuels remains a significant challenge. Here, we report that B/N-doped sp³/sp² hybridized nanocarbon (BNHC), consisting of ultra-small nanoparticles with a sp³ carbon core covered by a sp² carbon shell, is an efficient electrocatalyst for electrochemical reduction of CO₂ to ethanol at relatively low overpotentials. CO₂ reduction occurs with a Faradaic efficiency of 58.8%-69.1% for ethanol and acetate production at -0.5 ~ -0.6 V (vs. RHE), among which 51.6%-56.0% is for ethanol. The high selectivity for ethanol is due to the integrated effect of sp³/sp² carbon and B/N doping. Both sp³ carbon and B/N doping contribute to enhanced ethanol production with sp² carbon reducing the overpotential for CO₂ reduction to ethanol.
- CO₂ reduction,
- Ethanol,
- B/N-doped sp³/sp² hybridized nanocarbon,
- Electrocatalysis,
- multi-carbon product
1. [1]
  H. Wang, Y.K. Tzeng, Y. Ji, et al., Nat. Nanotechnol. 15 (2020) 131-137. doi: 10.1038/s41565-019-0603-y
2. [2]
  X. Yuan, L. Zhang, L. Li, et al., J. Am. Chem. Soc. 141 (2019) 4791-4794. doi: 10.1021/jacs.8b11771
3. [3]
  Z.Z. Niu, F.Y. Gao, X.L. Zhang, et al., J. Am. Chem. Soc. 143 (2021) 8011-8021. doi: 10.1021/jacs.1c01190
4. [4]
  C.T. Dinh, T. Burdyny, M.G. Kibria, et al., Science 360 (2018) 783-787. doi: 10.1126/science.aas9100
5. [5]
  T. Möller, W. Ju, A. Bagger, et al., Energy Environ. Sci. 12 (2019) 640-647. doi: 10.1039/C8EE02662A
6. [6]
  O.S. Bushuyev, P. De Luna, C.T. Dinh, et al., Joule 2 (2018) 825-832. doi: 10.1016/j.joule.2017.09.003
7. [7]
  J.J. Lv, M. Jouny, W. Luc, et al., Adv. Mater. 30 (2018) e1803111. doi: 10.1002/adma.201803111
8. [8]
  K. Jiang, S. Siahrostami, T. Zheng, et al., Energy Environ. Sci. 11 (2018) 893-903. doi: 10.1039/C7EE03245E
9. [9]
  H. Jung, S.Y. Lee, C.W. Lee, et al., J. Am. Chem. Soc. 141 (2019) 4624-4633. doi: 10.1021/jacs.8b11237
10. [10]
  M.D. Sampson, C.P. Kubiak, J. Am. Chem. Soc. 138 (2016) 1386-1393. doi: 10.1021/jacs.5b12215
11. [11]
  Y. Liu, S. Chen, X. Quan, H. Yu, J. Am. Chem. Soc. 137 (2015) 11631-11636. doi: 10.1021/jacs.5b02975
12. [12]
  D. Luo, S. Liu, K. Nakata, A. Fujishima, Chin. Chem. Lett. 30 (2019) 509-512. doi: 10.1016/j.cclet.2018.06.010
13. [13]
  J. Sun, W. Zheng, S. Lyu, et al., Chin. Chem. Lett. 31 (2020) 1415-1421. doi: 10.1016/j.cclet.2020.04.031
14. [14]
  Y. Zheng, A. Vasileff, X. Zhou, et al., J. Am. Chem. Soc. 141 (2019) 7646-7659. doi: 10.1021/jacs.9b02124
15. [15]
  R.M. Arán-Ais, F. Scholten, S. Kunze, R. Rizo, B. Roldan Cuenya, Nat. Energy 5 (2020) 317-325. doi: 10.1038/s41560-020-0594-9
16. [16]
  Q. Zhang, D. Ren, S. Pan, et al., Adv. Funct. Mater. 31 (2021) 2103966. doi: 10.1002/adfm.202103966
17. [17]
  P.P. Yang, X.L. Zhang, F.Y. Gao, et al., J. Am. Chem. Soc. 142 (2020) 6400-6408. doi: 10.1021/jacs.0c01699
18. [18]
  X. Yuan, S. Chen, D. Cheng, et al., Angew. Chem. Int. Ed. 60 (2021) 15344-15347. doi: 10.1002/anie.202105118
19. [19]
  Y. Zhou, F. Che, M. Liu, et al., Nat. Chem. 10 (2018) 974-980. doi: 10.1038/s41557-018-0092-x
20. [20]
  Y. Jiao, Y. Zheng, P. Chen, M. Jaroniec, S.Z. Qiao, J. Am. Chem. Soc. 139 (2017) 18093-18100. doi: 10.1021/jacs.7b10817
21. [21]
  E.L. Clark, C. Hahn, T.F. Jaramillo, A.T. Bell, J. Am. Chem. Soc. 139 (2017) 15848-15857. doi: 10.1021/jacs.7b08607
22. [22]
  J. Wu, T. Sharifi, Y. Gao, T. Zhang, P.M. Ajayan, Adv. Mater. 31 (2019) e1804257. doi: 10.1002/adma.201804257
23. [23]
  Y. Liu, Y. Zhang, K. Cheng, et al., Angew. Chem. Int. Ed. 56 (2017) 15607-15611. doi: 10.1002/anie.201706311
24. [24]
  Y. Lin, X. Sun, D.S. Su, G. Centi, S. Perathoner, Chem. Soc. Rev. 47 (2018) 8438-8473. doi: 10.1039/C8CS00684A
25. [25]
  N. Yang, S. Yu, J.V. Macpherson, et al., Chem. Soc. Rev. 48 (2019) 157-204. doi: 10.1039/C7CS00757D
26. [26]
  Y. Zhu, Y. Lin, B. Zhang, et al., ChemCatChem 7 (2015) 2840-2845. doi: 10.1002/cctc.201402930
27. [27]
  J. Wu, M. Liu, P.P. Sharma, et al., Nano Lett. 16 (2016) 466-470. doi: 10.1021/acs.nanolett.5b04123
28. [28]
  F. Pan, B. Li, X. Xiang, G. Wang, Y. Li, ACS Catal. 9 (2019) 2124-2133. doi: 10.1021/acscatal.9b00016
29. [29]
  W. Luc, X. Fu, J. Shi, et al., Nat. Catal. 2 (2019) 423-430. doi: 10.1038/s41929-019-0269-8
30. [30]
  B. Kumar, M. Asadi, D. Pisasale, et al., Nat. Commun. 4 (2013) 2819. doi: 10.1038/ncomms3819
31. [31]
  E.B. Cole, P.S. Lakkaraju, D.M. Rampulla, et al., J. Am. Chem. Soc. 132 (2010) 11539-11551. doi: 10.1021/ja1023496
32. [32]
  H. Wang, J. Jia, P. Song, et al., Angew. Chem. Int. Ed. 56 (2017) 7847-7852. doi: 10.1002/anie.201703720
33. [33]
  S. Zhang, P. Kang, S. Ubnoske, et al., J. Am. Chem. Soc. 136 (2014) 7845-7848. doi: 10.1021/ja5031529
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通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Promoting electrochemical reduction of CO2 to ethanol by B/N-doped sp3/sp2 nanocarbon electrode

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通讯作者: 陈斌, bchen63@163.com

Promoting electrochemical reduction of CO₂ to ethanol by B/N-doped sp³/sp² nanocarbon electrode