Citation: Yongqi Ren, Ruopeng Chang, Xu Hu, Junjie Guo, Guangping Hao, Anhui Lu. Layer-by-layer enriching active Ni-N₃C sites in nickel-nitrogen-carbon electrocatalysts for enhanced CO₂-to-CO reduction[J]. Chinese Chemical Letters, ;2023, 34(12): 108634. doi: 10.1016/j.cclet.2023.108634 shu

Layer-by-layer enriching active Ni-N₃C sites in nickel-nitrogen-carbon electrocatalysts for enhanced CO₂-to-CO reduction

Yongqi Ren ^a ,
Ruopeng Chang ^a ,
Xu Hu ^a ,
Junjie Guo ^{b, *,} ,
Guangping Hao ^{a, *,} ,
Anhui Lu ^a

a.
State Key Laboratory of Fine Chemicals, Frontier Science Center for Smart Materials, Liaoning Key Laboratory for Catalytic Conversion of Carbon Resources, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
b.
Key Laboratory of Interface Science and Engineering in Advanced Materials, Ministry of Education, Taiyuan University of Technology, Taiyuan 030024, China

guojunjie@tyut.edu.cn

guangpinghao@dlut.edu.cn

Received Date: 19 March 2023
Revised Date: 24 May 2023
Accepted Date: 29 May 2023
Available Online: 1 June 2023

Figures(6)

Transition metal and nitrogen co-doped carbons (M-N-C) have proven to be promising catalysts for CO₂ electroreduction into CO because of the high activity and selectivity. Effective enrichment of the active transition metal coordinated nitrogen sites is desirable but is challenging for a practical volumetric productivity. Herein, we report four kinds of model electrocatalysts to unveil this issue, which include the NC structures with surface N-functionalities, Ni-N-C_I with one layer of surface Ni-N₃C sites, NC@Ni-N-C_I with surface N-functionalities and underneath Ni-N₃C sites as well as Ni-N-C_II with doubled surface Ni-N₃C sites. The X-ray absorption spectroscopy indicates the coordination configuration of Ni-N₃C. For NC catalysts, when N-doping level increased from 3.5 at% to 8.4 at%, the CO partial current density increased from below 0.1 mA/cm² to 3 mA/cm². Introducing one layer of Ni-N₃C onto the NC structures leads to a 54 times higher CO partial current density than that of NC, in the meantime the FE_CO is 66 times higher. Furthermore, doubling the density of surface Ni-N₃C sites by a layer-by-layer method doubles the CO partial current density (j_CO), indicating its potential to achieve a high density of active coordinated sites and current densities.
- Porous carbons,
- Nanocarbons,
- CO₂ electroreduction,
- M-N₃C structure,
- Nonprecious electrocatalysts
1. [1]
  M. Rahimi, A. Khurram, T.A. Hatton, et al., Chem. Soc. Rev. 51 (2022) 8676–8695. doi: 10.1039/D2CS00443G
2. [2]
  J. Liu, C. Chen, K. Zhang, et al., Chin. Chem. Lett. 32 (2021) 649–659. doi: 10.1016/j.cclet.2020.07.040
3. [3]
  S. Jin, Z. Hao, K. Zhang, et al., Angew. Chem. Int. Ed. 60 (2021) 20627–20648. doi: 10.1002/anie.202101818
4. [4]
  Z. Gao, J. Li, Z. Zhang, et al., Chin. Chem. Lett. 33 (2022) 2270–2280. doi: 10.1016/j.cclet.2021.09.037
5. [5]
  T. He, A.R. Puente-Santiago, S. Xia, et al., Adv. Energy Mater. 12 (2022) 2200493. doi: 10.1002/aenm.202200493
6. [6]
  B. Zhang, Y. Jiang, M. Gao, et al., Nano Energy 80 (2021) 105504. doi: 10.1016/j.nanoen.2020.105504
7. [7]
  F. Wang, W. Zhang, H. Wan, et al., Chin. Chem. Lett. 33 (2022) 2259–2269. doi: 10.1016/j.cclet.2021.08.074
8. [8]
  S. Li, A.V. Nagarajan, D.R. Alfonso, et al., Angew. Chem. Int. Ed. 60 (2021) 6351–6356. doi: 10.1002/anie.202016129
9. [9]
  L. Wei, H. Li, J. Chen, et al., ACS Catal. 10 (2020) 1444–1453. doi: 10.1021/acscatal.9b04633
10. [10]
  J. Zhao, Z. Chen, J. Zhao, J. Mater. Chem. A 7 (2019) 4026–4035. doi: 10.1039/C8TA11825F
11. [11]
  P. Yao, Y. Qiu, T. Zhang, et al., ACS Sustain. Chem. Eng. 7 (2019) 5249–5255. doi: 10.1021/acssuschemeng.8b06160
12. [12]
  C. Li, Y. Wang, N. Xiao, et al., Carbon 151 (2019) 46–52. doi: 10.1016/j.carbon.2019.05.042
13. [13]
  T. Liu, S. Ali, Z. Lian, et al., J. Mater. Chem. A 6 (2018) 19998–20004. doi: 10.1039/C8TA06649C
14. [14]
  F. Pan, B. Li, W. Deng, et al., Appl. Catal. B: Environ. 252 (2019) 240–249. doi: 10.1016/j.apcatb.2019.04.025
15. [15]
  J. Gu, C. Hsu, L. Bai, et al., Science 364 (2019) 1091–1094. doi: 10.1126/science.aaw7515
16. [16]
  L. Dong, X. Hu, Y. Du, et al., J. Mater. Chem. A 9 (2021) 17821–17829. doi: 10.1039/D1TA05355H
17. [17]
  W. Ju, A. Bagger, G. Hao, et al., Nat. Commun. 8 (2017) 944. doi: 10.1038/s41467-017-01035-z
18. [18]
  P. Wang, T. Li, Q. Wu, et al., ACS Nano 16 (2022) 17021–17032. doi: 10.1021/acsnano.2c07138
19. [19]
  P. Su, K. Iwase, S. Nakanishi, et al., Small 12 (2016) 6083–6089. doi: 10.1002/smll.201602158
20. [20]
  W. Wang, L. Shang, G. Chang, et al., Adv. Mater. 31 (2019) 1808276. doi: 10.1002/adma.201808276
21. [21]
  S. Shen, C. Han, B. Wang, et al., Chin. Chem. Lett. 33 (2022) 3721–3725. doi: 10.1016/j.cclet.2021.10.063
22. [22]
  H. Cheng, X. Wu, X. Li, et al., Chem. Eng. J. 407 (2021) 126842. doi: 10.1016/j.cej.2020.126842
23. [23]
  B. Lu, Q. Liu, S. Chen, ACS Catal. 10 (2020) 7584–7618. doi: 10.1021/acscatal.0c01950
24. [24]
  H. Li, K. Gan, R. Li, et al., Adv. Funct. Mater. 33 (2023) 2208622. doi: 10.1002/adfm.202208622
25. [25]
  Y. Li, N.M. Adli, W. Shan, et al., Energy Environ. Sci. 15 (2022) 2108–2119. doi: 10.1039/D2EE00318J
26. [26]
  Y. Lu, H. Wang, P. Yu, et al., Nano Energy 77 (2020) 105158. doi: 10.1016/j.nanoen.2020.105158
27. [27]
  F. Pan, H. Zhang, K. Liu, et al., ACS Catal. 8 (2018) 3116–3122. doi: 10.1021/acscatal.8b00398
28. [28]
  X. Zhao, Y. Liu, J. Am. Chem. Soc. 142 (2020) 5773–5777. doi: 10.1021/jacs.9b13872
29. [29]
  X. Fu, P. Zhang, T. Sun, et al., Small 18 (2022) 2107997. doi: 10.1002/smll.202107997
30. [30]
  X. Li, W. Bi, M. Chen, et al., J. Am. Chem. Soc. 139 (2017) 14889–14892. doi: 10.1021/jacs.7b09074
31. [31]
  D.M. Koshy, A.T. Landers, D.A. Cullen, et al., Adv. Energy Mater. 10 (2020) 2001836. doi: 10.1002/aenm.202001836
32. [32]
  Y. Gong, L. Jiao, Y. Qian, et al., Angew. Chem. Int. Ed. 59 (2020) 2705–2709. doi: 10.1002/anie.201914977
33. [33]
  Z. Liu, S. Li, J. Yang, et al., ACS Nano 14 (2020) 11662–11669. doi: 10.1021/acsnano.0c04210
34. [34]
  Y. Qu, L. Wang, Z. Li, et al., Adv. Mater. 31 (2019) 1970316. doi: 10.1002/adma.201970316
35. [35]
  Z. Miao, X. Wang, M. Tsai, et al., Adv. Energy Mater. 8 (2018) 1801226. doi: 10.1002/aenm.201801226
36. [36]
  S. Liu, M. Wang, X. Yang, et al., Angew. Chem. Int. Ed. 59 (2020) 21698–21705. doi: 10.1002/anie.202009331
37. [37]
  D. De Fazio, D.G. Purdie, A.K. Ott, et al., ACS Nano 13 (2019) 8926–8935. doi: 10.1021/acsnano.9b02621
38. [38]
  K. Huang, Z. Wei, J. Liu, et al., Small 18 (2022) 2201139. doi: 10.1002/smll.202201139
39. [39]
  W. Bi, X. Li, R. You, et al., Adv. Mater. 30 (2018) 1706617. doi: 10.1002/adma.201706617
40. [40]
  C. Yan, H. Li, Y. Ye, et al., Energy Environ. Sci. 11 (2018) 1204–1210. doi: 10.1039/C8EE00133B
41. [41]
  Q. Fan, P. Hou, C. Choi, et al., Adv. Energy Mater. 10 (2020) 1903068. doi: 10.1002/aenm.201903068
42. [42]
  K. Mou, Z. Chen, X. Zhang, et al., Small 15 (2019) 1903668. doi: 10.1002/smll.201903668
43. [43]
  R. Daiyan, X. Zhu, Z. Tong, et al., Nano Energy 78 (2020) 105213. doi: 10.1016/j.nanoen.2020.105213
44. [44]
  C. Zhao, X. Dai, T. Yao, et al., J. Am. Chem. Soc. 139 (2017) 8078–8081. doi: 10.1021/jacs.7b02736
45. [45]
  S. Gong, W. Wang, R. Lu, et al., Appl. Catal. B: Environ. 318 (2022) 121813. doi: 10.1016/j.apcatb.2022.121813
46. [46]
  R. Ge, L. Dong, X. Hu, et al., Chem. Eng. J. 438 (2022) 135500. doi: 10.1016/j.cej.2022.135500
47. [47]
  C. Wen, F. Mao, Y. Liu, et al., ACS Catal. 10 (2020) 1086–1093. doi: 10.1021/acscatal.9b02978
48. [48]
  P. Prslja, N. López, ACS Catal. 11 (2021) 88–94. doi: 10.1021/acscatal.0c01909
49. [49]
  T. Asset, S.T. Garcia, S. Herrera, et al., ACS Catal. 9 (2019) 7668–7678. doi: 10.1021/acscatal.9b01513
50. [50]
  R. Daiyan, W.H. Saputera, H. Masood, et al., Adv. Energy Mater. 10 (2020) 1902106. doi: 10.1002/aenm.201902106
51. [51]
  T. Zheng, K. Jiang, N. Ta, et al., Joule 3 (2019) 265–278. doi: 10.1016/j.joule.2018.10.015
52. [52]
  C. Lu, J. Yang, S. Wei, et al., Adv. Funct. Mater. 29 (2019) 1806884. doi: 10.1002/adfm.201806884
53. [53]
  B. Chen, B. Li, Z. Tian, et al., Adv. Energy Mater. 11 (2021) 2102152. doi: 10.1002/aenm.202102152
54. [54]
  R.M. Yadav, Z. Li, T. Zhang, et al., Adv. Mater. 34 (2022) 2105690. doi: 10.1002/adma.202105690
55. [55]
  M. Huang, B. Deng, X. Zhao, ACS Nano 16 (2022) 2110–2119. doi: 10.1021/acsnano.1c07746
56. [56]
  C. Liu, Y. Wu, K. Sun, et al., Chem 7 (2021) 1297–1307. doi: 10.1016/j.chempr.2021.02.001
57. [57]
  A.S. Varela, N. Ranjbar Sahraie, J. Steinberg, et al., Angew. Chem. Int. Ed. 54 (2015) 10758–10762. doi: 10.1002/anie.201502099
58. [58]
  D.M. Koshy, S. Chen, D.U. Lee, et al., Angew. Chem. Int. Ed. 59 (2020) 4043–4050. doi: 10.1002/anie.201912857
59. [59]
  Z. Li, D. He, X. Yan, et al., Angew. Chem. Int. Ed. 59 (2020) 18572–18577. doi: 10.1002/anie.202000318
60. [60]
  X. Wang, Y. Wang, X. Sang, et al., Angew. Chem. Int. Ed. 60 (2021) 4192–4198. doi: 10.1002/anie.202013427
1. [1]
  Qian-Qian Tang , Li-Fang Feng , Zhi-Peng Li , Shi-Hao Wu , Long-Shuai Zhang , Qing Sun , Mei-Feng Wu , Jian-Ping Zou . Single-atom sites regulation by the second-shell doping for efficient electrochemical CO₂ reduction. Chinese Chemical Letters, 2024, 35(9): 109454-. doi: 10.1016/j.cclet.2023.109454
2. [2]
  Uttam Pandurang Patil . Porous carbon catalysis in sustainable synthesis of functional heterocycles: An overview. Chinese Chemical Letters, 2024, 35(8): 109472-. doi: 10.1016/j.cclet.2023.109472
3. [3]
  Liang Ma , Zhou Li , Zhiqiang Jiang , Xiaofeng Wu , Shixin Chang , Sónia A. C. Carabineiro , Kangle Lv . Effect of precursors on the structure and photocatalytic performance of g-C3N4 for NO oxidation and CO2 reduction. Chinese Journal of Structural Chemistry, 2024, 43(11): 100416-100416. doi: 10.1016/j.cjsc.2023.100416
4. [4]
  Qin Cheng , Ming Huang , Qingqing Ye , Bangwei Deng , Fan Dong . Indium-based electrocatalysts for CO₂ reduction to C1 products. Chinese Chemical Letters, 2024, 35(6): 109112-. doi: 10.1016/j.cclet.2023.109112
5. [5]
  Jiajun Wang , Guolin Yi , Shengling Guo , Jianing Wang , Shujuan Li , Ke Xu , Weiyi Wang , Shulai Lei . Computational design of bimetallic TM₂@g-C₉N₄ electrocatalysts for enhanced CO reduction toward C₂ products. Chinese Chemical Letters, 2024, 35(7): 109050-. doi: 10.1016/j.cclet.2023.109050
6. [6]
  Shaojie Ding , Henan Wang , Xiaojing Dai , Yuru Lv , Xinxin Niu , Ruilian Yin , Fangfang Wu , Wenhui Shi , Wenxian Liu , Xiehong Cao . Mn-modulated Co–N–C oxygen electrocatalysts for robust and temperature-adaptative zinc-air batteries. Chinese Journal of Structural Chemistry, 2024, 43(7): 100302-100302. doi: 10.1016/j.cjsc.2024.100302
7. [7]
  Shengkai Li , Yuqin Zou , Chen Chen , Shuangyin Wang , Zhao-Qing Liu . Defect engineered electrocatalysts for C–N coupling reactions toward urea synthesis. Chinese Chemical Letters, 2024, 35(8): 109147-. doi: 10.1016/j.cclet.2023.109147
8. [8]
  Jiao Li , Chenyang Zhang , Chuhan Wu , Yan Liu , Xuejian Zhang , Xiao Li , Yongtao Li , Jing Sun , Zhongmin Su . Defined organic-octamolybdate crystalline superstructures derived Mo₂C@C as efficient hydrogen evolution electrocatalysts. Chinese Chemical Letters, 2024, 35(6): 108782-. doi: 10.1016/j.cclet.2023.108782
9. [9]
  Wenlong LI , Xinyu JIA , Jie LING , Mengdan MA , Anning ZHOU . Photothermal catalytic CO₂ hydrogenation over a Mg-doped In₂O_3-x catalyst. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 919-929. doi: 10.11862/CJIC.20230421
10. [10]
  Yongheng Ren , Yang Chen , Hongwei Chen , Lu Zhang , Jiangfeng Yang , Qi Shi , Lin-Bing Sun , Jinping Li , Libo Li . Electrostatically driven kinetic Inverse CO2/C2H2 separation in LTA-type zeolites. Chinese Journal of Structural Chemistry, 2024, 43(10): 100394-100394. doi: 10.1016/j.cjsc.2024.100394
11. [11]
  Ziyi Zhu , Yang Cao , Jun Zhang . CO2-switched porous metal-organic framework magnets. Chinese Journal of Structural Chemistry, 2024, 43(2): 100241-100241. doi: 10.1016/j.cjsc.2024.100241
12. [12]
  Maomao Liu , Guizeng Liang , Ningce Zhang , Tao Li , Lipeng Diao , Ping Lu , Xiaoliang Zhao , Daohao Li , Dongjiang Yang . Electron-rich Ni2+ in Ni3S2 boosting electrocatalytic CO2 reduction to formate and syngas. Chinese Journal of Structural Chemistry, 2024, 43(8): 100359-100359. doi: 10.1016/j.cjsc.2024.100359
13. [13]
  Xiuzheng Deng , Changhai Liu , Xiaotong Yan , Jingshan Fan , Qian Liang , Zhongyu Li . Carbon dots anchored NiAl-LDH@In₂O₃ hierarchical nanotubes for promoting selective CO₂ photoreduction into CH₄. Chinese Chemical Letters, 2024, 35(6): 108942-. doi: 10.1016/j.cclet.2023.108942
14. [14]
  Yi Liu , Zhe-Hao Wang , Guan-Hua Xue , Lin Chen , Li-Hua Yuan , Yi-Wen Li , Da-Gang Yu , Jian-Heng Ye . Photocatalytic dicarboxylation of strained C–C bonds with CO₂ via consecutive visible-light-induced electron transfer. Chinese Chemical Letters, 2024, 35(6): 109138-. doi: 10.1016/j.cclet.2023.109138
15. [15]
  Xiuzheng Deng , Yi Ke , Jiawen Ding , Yingtang Zhou , Hui Huang , Qian Liang , Zhenhui Kang . Construction of ZnO@CDs@Co₃O₄ sandwich heterostructure with multi-interfacial electron-transfer toward enhanced photocatalytic CO₂ reduction. Chinese Chemical Letters, 2024, 35(4): 109064-. doi: 10.1016/j.cclet.2023.109064
16. [16]
  Tong Li , Leping Pan , Yan Zhang , Jihu Su , Kai Li , Kuiliang Li , Hu Chen , Qi Sun , Zhiyong Wang . Electrochemical construction of 2,5-diaryloxazoles via N–H and C(sp³)-H functionalization. Chinese Chemical Letters, 2024, 35(4): 108897-. doi: 10.1016/j.cclet.2023.108897
17. [17]
  Chao Ma , Cong Lin , Jian Li . MicroED as a powerful technique for the structure determination of complex porous materials. Chinese Journal of Structural Chemistry, 2024, 43(3): 100209-100209. doi: 10.1016/j.cjsc.2023.100209
18. [18]
  Min WANG , Dehua XIN , Yaning SHI , Wenyao ZHU , Yuanqun ZHANG , Wei ZHANG . Construction and full-spectrum catalytic performance of multilevel Ag/Bi/nitrogen vacancy g-C₃N₄/Ti₃C₂T_x Schottky junction. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1123-1134. doi: 10.11862/CJIC.20230477
19. [19]
  Zhi Zhu , Xiaohan Xing , Qi Qi , Wenjing Shen , Hongyue Wu , Dongyi Li , Binrong Li , Jialin Liang , Xu Tang , Jun Zhao , Hongping Li , Pengwei Huo . Fabrication of graphene modified CeO2/g-C3N4 heterostructures for photocatalytic degradation of organic pollutants. Chinese Journal of Structural Chemistry, 2023, 42(12): 100194-100194. doi: 10.1016/j.cjsc.2023.100194
20. [20]
  Kaihui Huang , Boning Feng , Xinghua Wen , Lei Hao , Difa Xu , Guijie Liang , Rongchen Shen , Xin Li . Effective photocatalytic hydrogen evolution by Ti3C2-modified CdS synergized with N-doped C-coated Cu2O in S-scheme heterojunctions. Chinese Journal of Structural Chemistry, 2023, 42(12): 100204-100204. doi: 10.1016/j.cjsc.2023.100204

Get Citation

PDF

XML

Metrics

PDF Downloads(2)
Abstract views(270)
HTML views(25)

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

Layer-by-layer enriching active Ni-N3C sites in nickel-nitrogen-carbon electrocatalysts for enhanced CO2-to-CO reduction

Metrics

通讯作者: 陈斌, bchen63@163.com

Layer-by-layer enriching active Ni-N₃C sites in nickel-nitrogen-carbon electrocatalysts for enhanced CO₂-to-CO reduction