Citation: Xinyuan Li, Zhuozhu Li, Wenzhong Huang, Jiantao Li, Wei Zhang, Shihao Feng, Hao Fan, Zhuo Chen, Sungsik Lee, Congcong Cai, Liang Zhou. Solvent-free synthesis of Co single atom and nanocluster decorated N-doped carbon for efficient oxygen reduction[J]. Chinese Chemical Letters, ;2025, 36(9): 110716. doi: 10.1016/j.cclet.2024.110716 shu

Solvent-free synthesis of Co single atom and nanocluster decorated N-doped carbon for efficient oxygen reduction

Xinyuan Li ^{a, b, 1} ,
Zhuozhu Li ^{b, 1} ,
Wenzhong Huang ^b ,
Jiantao Li ^c ,
Wei Zhang ^b ,
Shihao Feng ^b ,
Hao Fan ^b ,
Zhuo Chen ^b ,
Sungsik Lee ^d ,
Congcong Cai ^{a, b, *,} ,
Liang Zhou ^{a, b, e, *,}

a.
Hubei Longzhong Laboratory, Wuhan University of Technology (Xiangyang Demonstration Zone), Xiangyang 441000, China
b.
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
c.
Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL 60439, United States
d.
X-ray Science Division, Argonne National Laboratory, Lemont, IL 60439, United States
e.
Zhongyu Feima New Material Technology Innovation Center (Zhengzhou) Co., Ltd., High Technology Industrial Development Zone, Zhengzhou 450001, China

congcai0804@163.com

liangzhou@whut.edu.cn

Received Date: 5 September 2024
Revised Date: 8 October 2024
Accepted Date: 3 December 2024
Available Online: 4 December 2024

Figures(5)

The advancement of efficient, cheap, and durable catalysts for oxygen reduction reaction (ORR) to substitute Pt/C in metal-air batteries is of paramount importance. However, traditional solvent-based methods fall short in terms of environmental benign and scalability. Herein, a solvent-free organic-inorganic self-assembly approach is explored to construct cobalt single atom and cobalt nanocluster decorated nitrogen-doped porous carbon spheres (Co-SA/NC@NCS). The solvent-free synthesis demonstrates an impressively high yield (282 g/L) and the resultant Co-SA/NC@NCS possesses a high N content (6.9 wt%). Density functional theory calculations disclose that the Co-SAs and Co-NCs are able to optimize the surface oxygen adsorption capability and enhance the conductivity of the NCS, thereby facilitating the ORR performance. The solvent-free synthesis is also feasible for the synthesis of other non-noble metal element (Fe, Ni, and Zn) decorated nitrogen-doped porous carbon spheres.
- Organic-inorganic self-assembly,
- Nitrogen-doped carbon,
- Oxygen reduction reaction,
- Single atom catalyst,
- Zn-air battery
1. [1]
  W. Sun, F. Wang, B. Zhang, et al., Science 371 (2021) 46–51. doi: 10.1126/science.abb9554
2. [2]
  L. Yang, C. Du, J. Tian, et al., Appl. Catal. B: Environ. 355 (2024) 124190. doi: 10.1016/j.apcatb.2024.124190
3. [3]
  J. Tian, Y. Zhu, X. Yao, et al., J. Mater. Chem. A 11 (2023) 5288–5295. doi: 10.1039/d2ta08943b
4. [4]
  M. Escudero-Escribano, P. Malacrida, M.H. Hansen, et al., Science 352 (2016) 73–76. doi: 10.1126/science.aad8892
5. [5]
  X. Xie, Z. Zhai, L. Peng, et al., Sci. Bull. 68 (2023) 2862–2875. doi: 10.1016/j.scib.2023.10.013
6. [6]
  C. Zhu, J. Yang, J. Zhang, et al., Interdiscip. Mater. 3 (2024) 74–86. doi: 10.1002/idm2.12141
7. [7]
  V. Papa, Y. Cao, A. Spannenberg, et al., Nat. Catal. 3 (2020) 135–142. doi: 10.1038/s41929-019-0404-6
8. [8]
  X. Yao, Y. Zhu, Z. Han, et al., Appl. Catal. B: Environ. 331 (2023) 122675. doi: 10.1016/j.apcatb.2023.122675
9. [9]
  S. Xie, H. Jin, C. Wang, et al., Chin. Chem. Lett. 34 (2023) 107681. doi: 10.1016/j.cclet.2022.07.024
10. [10]
  F. Yu, J. Zhan, D. Chen, et al., Adv. Funct. Mater. 33 (2023) 2214425. doi: 10.1002/adfm.202214425
11. [11]
  H. Liu, L. Jiang, J. Khan, et al., Angew. Chem. Int. Ed. 62 (2023) e202214988. doi: 10.1002/anie.202214988
12. [12]
  J. Song, Y. Chen, H. Huang, et al., Adv. Sci. 9 (2022) 2104522. doi: 10.1002/advs.202104522
13. [13]
  S. Zhao, F. Hu, L. Yin, et al., Sci. Bull. 68 (2023) 1389–1398. doi: 10.1016/j.scib.2023.06.001
14. [14]
  B. Ramulu, S.J. Arbaz, M. Nagaraju, et al., Nanoscale 15 (2023) 13049–13061. doi: 10.1039/d3nr02103c
15. [15]
  M. Song, Q. Zhang, T. Shen, et al., Chin. Chem. Lett. 35 (2024) 109083. doi: 10.1016/j.cclet.2023.109083
16. [16]
  P. Zhang, L. Wang, S. Yang, et al., Nat. Commun. 8 (2017) 15020. doi: 10.1038/ncomms15020
17. [17]
  S. Li, G. Xing, S. Zhao, et al., Nat. Sci. Rev. 11 (2024) nwae193. doi: 10.1093/nsr/nwae193
18. [18]
  X.R. Wang, J.Y. Liu, Z.W. Liu, et al., Adv. Mater. 30 (2018) 1800005. doi: 10.1002/adma.201800005
19. [19]
  Z. Wang, Q.K. Li, C. Zhang, et al., ACS Catal. 11 (2021) 2454–2459. doi: 10.1021/acscatal.0c04735
20. [20]
  Z. Yang, C. Zhao, Y. Qu, et al., Adv. Mater. 31 (2019) 1808043. doi: 10.1002/adma.201808043
21. [21]
  S. Liu, M. Wang, X. Yang, et al., Angew. Chem. Int. Ed. 59 (2020) 21698–21705. doi: 10.1002/anie.202009331
22. [22]
  Z. Zhuang, Y. Li, R. Yu, et al., Nat. Catal. 5 (2022) 300–310. doi: 10.1038/s41929-022-00764-9
23. [23]
  F. Liu, K. Huang, Q. Wu, et al., Adv. Mater. 29 (2017) 1700445. doi: 10.1002/adma.201700445
24. [24]
  S. Feng, K. Li, P. Hu, et al., ACS Nano 17 (2023) 23152–23159. doi: 10.1021/acsnano.3c09328
25. [25]
  R. Chen, X. Li, C. Cai, et al., Small 19 (2023) 2303790. doi: 10.1002/smll.202303790
26. [26]
  T. Wang, F. Okejiri, Z.A. Qiao, et al., Adv. Mater. 32 (2020) 2002475. doi: 10.1002/adma.202002475
27. [27]
  S. Jin, Y. Ni, Z. Hao, et al., Angew. Chem. Int. Ed. 59 (2020) 21885–21889. doi: 10.1002/anie.202008422
28. [28]
  Z. Wang, C. Zhu, H. Tan, et al., Adv. Funct. Mater. 31 (2021) 2104735. doi: 10.1002/adfm.202104735
29. [29]
  J. Meng, J. Li, J. Liu, et al., ACS Cent. Sci. 6 (2020) 1431–1440. doi: 10.1021/acscentsci.0c00458
30. [30]
  J. Yan, Y. Wang, Y. Zhang, et al., Adv. Mater. 33 (2020) 2007525.
31. [31]
  S. Feng, L. Xing, K. Li, et al., Small Methods 7 (2023) 2300150. doi: 10.1002/smtd.202300150
32. [32]
  L. Wang, Y. Hao, L. Deng, et al., Nat. Commun. 13 (2022) 5785. doi: 10.1177/09544062211063130
33. [33]
  Y. Hao, S. Hung, W. Zeng, et al., J. Am. Chem. Soc. 145 (2023) 23659–23669. doi: 10.1021/jacs.3c07777
34. [34]
  K.E. Fritz, Y. Yan, J. Suntivich, et al., Nano Res. 12 (2019) 2307–2312. doi: 10.1007/s12274-019-2440-6
35. [35]
  X. Li, Z. Liu, C. Cai, et al., ChemSusChem 14 (2021) 1756–1762. doi: 10.1002/cssc.202100113
36. [36]
  X. Jia, Y. Zhang, D. Guo, et al., Ionics 26 (2020) 1885–1894 (Kiel). doi: 10.1007/s11581-020-03465-0
37. [37]
  X. Li, C. Cai, P. Hu, et al., Adv. Mater. 36 (2024) 2400184. doi: 10.1002/adma.202400184
38. [38]
  Y. Ren, F. Tian, L. Jin, et al., Environ. Sci. Technol. 57 (2023) 10458–10466. doi: 10.1021/acs.est.3c02520
39. [39]
  L. Jin, X. Duan, M. Sun, et al., ACS Nano 17 (2023) 12875–12883. doi: 10.1021/acsnano.3c04521
40. [40]
  Y. Wang, Y.J. Tang, K. Zhou, et al., J. Am. Chem. Soc. 141 (2019) 14115–14119. doi: 10.1021/jacs.9b07712
41. [41]
  W. Wang, X. Deng, Z. Tian, et al., Chem. Mater. 35 (2023) 6070–6082. doi: 10.1021/acs.chemmater.3c01171
1. [1]
  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
2. [2]
  Yan Wang , Jiaqi Zhang , Xiaofeng Wu , Sibo Wang , Masakazu Anpo , Yuanxing Fang . Elucidating oxygen evolution and reduction mechanisms in nitrogen-doped carbon-based photocatalysts. Chinese Chemical Letters, 2025, 36(2): 110439-. doi: 10.1016/j.cclet.2024.110439
3. [3]
  Yufeng Wu , Mingjun Jing , Juan Li , Wenhui Deng , Mingguang Yi , Zhanpeng Chen , Meixia Yang , Jinyang Wu , Xinkai Xu , Yanson Bai , Xiaoqing Zou , Tianjing Wu , Xianyou Wang . Collaborative integration of Fe-N_x active center into defective sulfur/selenium-doped carbon for efficient oxygen electrocatalysts in liquid and flexible Zn-air batteries. Chinese Chemical Letters, 2024, 35(9): 109269-. doi: 10.1016/j.cclet.2023.109269
4. [4]
  Juhong Zhou , Hui Zhao , Ping Han , Ziyue Wang , Yan Zhang , Xiaoxia Mao , Konglin Wu , Shengjue Deng , Wenxiang He , Binbin Jiang . Strategic modulation of CoFe sites for advanced bifunctional oxygen electrocatalyst. Chinese Journal of Structural Chemistry, 2025, 44(1): 100470-100470. doi: 10.1016/j.cjsc.2024.100470
5. [5]
  Jin Long , Xingqun Zheng , Bin Wang , Chenzhong Wu , Qingmei Wang , Lishan Peng . Improving the electrocatalytic performances of Pt-based catalysts for oxygen reduction reaction via strong interactions with single-CoN₄-rich carbon support. Chinese Chemical Letters, 2024, 35(5): 109354-. doi: 10.1016/j.cclet.2023.109354
6. [6]
  Yi Zhou , Yanzhen Liu , Yani Yan , Zonglin Yi , Yongfeng Li , Cheng-Meng Chen . Enhanced oxygen reduction reaction on La-Fe bimetal in porous N-doped carbon dodecahedra with CNTs wrapping. Chinese Chemical Letters, 2025, 36(1): 109569-. doi: 10.1016/j.cclet.2024.109569
7. [7]
  Guan-Nan Xing , Di-Ye Wei , Hua Zhang , Zhong-Qun Tian , Jian-Feng Li . Pd-based nanocatalysts for oxygen reduction reaction: Preparation, performance, and in-situ characterization. Chinese Journal of Structural Chemistry, 2023, 42(11): 100021-100021. doi: 10.1016/j.cjsc.2023.100021
8. [8]
  Chenhao Zhang , Qian Zhang , Yezhou Hu , Hanyu Hu , Junhao Yang , Chang Yang , Ye Zhu , Zhengkai Tu , Deli Wang . N-doped carbon confined ternary Pt₂NiCo intermetallics for efficient oxygen reduction reaction. Chinese Chemical Letters, 2025, 36(3): 110429-. doi: 10.1016/j.cclet.2024.110429
9. [9]
  Jiayu Huang , Kuan Chang , Qi Liu , Yameng Xie , Zhijia Song , Zhiping Zheng , Qin Kuang . Fe-N-C nanostick derived from 1D Fe-ZIFs for Electrocatalytic oxygen reduction. Chinese Journal of Structural Chemistry, 2023, 42(10): 100097-100097. doi: 10.1016/j.cjsc.2023.100097
10. [10]
  Xue Zhao , Rui Zhao , Qian Liu , Henghui Chen , Jing Wang , Yongfeng Hu , Yan Li , Qiuming Peng , John S Tse . A p-d block synergistic effect enables robust electrocatalytic oxygen evolution. Chinese Chemical Letters, 2024, 35(11): 109496-. doi: 10.1016/j.cclet.2024.109496
11. [11]
  Yanan Zhou , Li Sheng , Lanlan Chen , Wenhua Zhang , Jinlong Yang . Axial coordinated iron-nitrogen-carbon as efficient electrocatalysts for hydrogen evolution and oxygen redox reactions. Chinese Chemical Letters, 2025, 36(1): 109588-. doi: 10.1016/j.cclet.2024.109588
12. [12]
  Jinli Chen , Shouquan Feng , Tianqi Yu , Yongjin Zou , Huan Wen , Shibin Yin . Modulating Metal-Support Interaction Between Pt3Ni and Unsaturated WOx to Selectively Regulate the ORR Performance. Chinese Journal of Structural Chemistry, 2023, 42(10): 100168-100168. doi: 10.1016/j.cjsc.2023.100168
13. [13]
  Yatian Deng , Dao Wang , Jinglan Cheng , Yunkun Zhao , Zongbao Li , Chunyan Zang , Jian Li , Lichao Jia . A new popular transition metal-based catalyst: SmMn₂O₅ mullite-type oxide. Chinese Chemical Letters, 2024, 35(8): 109141-. doi: 10.1016/j.cclet.2023.109141
14. [14]
  Peng Wang , Daijie Deng , Suqin Wu , Li Xu . Cobalt-based deep eutectic solvent modified nitrogen-doped carbon catalyst for boosting oxygen reduction reaction in zinc-air batteries. Chinese Journal of Structural Chemistry, 2024, 43(1): 100199-100199. doi: 10.1016/j.cjsc.2023.100199
15. [15]
  Kunsong Hu , Yulong Zhang , Jiayi Zhu , Jinhua Mai , Gang Liu , Manoj Krishna Sugumar , Xinhua Liu , Feng Zhan , Rui Tan . Nano-engineered catalysts for high-performance oxygen reduction reaction. Chinese Chemical Letters, 2024, 35(10): 109423-. doi: 10.1016/j.cclet.2023.109423
16. [16]
  Jialin Cai , Yizhe Chen , Ruiwen Zhang , Cheng Yuan , Zeyu Jin , Yongting Chen , Shiming Zhang , Jiujun Zhang . Interfacial Pt-N coordination for promoting oxygen reduction reaction. Chinese Chemical Letters, 2025, 36(2): 110255-. doi: 10.1016/j.cclet.2024.110255
17. [17]
  Peng Jia , Yunna Guo , Dongliang Chen , Xuedong Zhang , Jingming Yao , Jianguo Lu , Liqiang Zhang . In-situ imaging electrocatalysis in a solid-state Li-O₂ battery with CuSe nanosheets as air cathode. Chinese Chemical Letters, 2024, 35(5): 108624-. doi: 10.1016/j.cclet.2023.108624
18. [18]
  Min Song , Qian Zhang , Tao Shen , Guanyu Luo , Deli Wang . Surface reconstruction enabled o-PdTe@Pd core-shell electrocatalyst for efficient oxygen reduction reaction. Chinese Chemical Letters, 2024, 35(8): 109083-. doi: 10.1016/j.cclet.2023.109083
19. [19]
  Xiaoya Cui , Yanchang Liu , Qiang Li , He Zhu , Shibo Xi , Jianrong Zeng . Ultrafast crystallinity engineering of PtCo₃ alloy for enhanced oxygen reduction reaction. Chinese Chemical Letters, 2025, 36(5): 110069-. doi: 10.1016/j.cclet.2024.110069
20. [20]
  Quanyou Guo , Yue Yang , Tingting Hu , Hongqi Chu , Lijun Liao , Xuepeng Wang , Zhenzi Li , Liping Guo , Wei Zhou . Regulating local electron transfer environment of covalent triazine frameworks through F, N co-modification towards optimized oxygen reduction reaction. Chinese Chemical Letters, 2025, 36(1): 110235-. doi: 10.1016/j.cclet.2024.110235

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(10)
HTML views(1)

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