Citation: Yu Yao, Jinqiang Zhang, Yantao Wang, Kunsheng Hu, Yangyang Yang, Zhongshuai Zhu, Shuang Zhong, Huayang Zhang, Shaobin Wang, Xiaoguang Duan. Nitrogen-rich carbon for catalytic activation of peroxymonosulfate towards green synthesis[J]. Chinese Chemical Letters, ;2024, 35(11): 109633. doi: 10.1016/j.cclet.2024.109633 shu

Nitrogen-rich carbon for catalytic activation of peroxymonosulfate towards green synthesis

a.
School of Chemical Engineering, The University of Adelaide, Adelaide, SA 5005, Australia
b.
School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, China

jinqiang.zhang@adelaide.edu.au

xiaoguang.duan@adelaide.edu.au

Received Date: 18 October 2023
Revised Date: 14 January 2024
Accepted Date: 4 February 2024
Available Online: 12 February 2024

Figures(5)

Nitrogen-doped carbon (N–C) materials have demonstrated exceptional performances in activating peroxymonosulfate (PMS) for environmental remediation. However, accommodating higher nitrogen contents remains challenging in N–C due to the thermodynamic instability of C–N skeleton. In this study, we proposed an innovative epitaxial growth approach to synthesize two-dimensional N–C nanosheets. Leveraging the abundant amino groups supplied by the polymer dots as growing sites, we successfully attained a high nitrogen level and spontaneously introduced abundant structural defects in the carbon framework. The resulting N–C nanosheets exhibited outstanding catalytic activity for the activation of PMS toward selective oxidation of diethyl 1,4-dihydro-2,6-dimethyl-3,5-pyridinedicarboxylate (1,4-DHP) into diethyl 2,6-dimethylpyridine-3,5-dicarboxylate, which serves as a valuable intermediate in the synthesis of various pharmaceutical compounds. Comprehensive experimental and characterization investigations verified that the nitrogen sites and defects are the primary active sites for PMS activation and selective oxidation of 1,4-DHP. This work offered an efficient approach for the fabrication of high-nitrogen-loading carbon materials for catalytic oxidation reactions.
- Nitrogen-rich carbon,
- Peroxymonosulfate,
- Selective oxidation,
- Electron transfer process,
- Catalytic synthesis
1. [1]
  Y.F. Huo, M. Yang, M.Y. Lei, et al., Water Environ. J. 38 (2024) 162–168. doi: 10.1111/wej.12895
2. [2]
  B.R. Scanlon, S. Fakhreddine, A. Rateb, et al., Nat. Rev. Earth Env. 4 (2023) 87–101. doi: 10.1038/s43017-022-00378-6
3. [3]
  A. Mukhopadhyay, S. Duttagupta, A. Mukherjee, J. Environ. Chem. Eng. 10 (2022) 107560. doi: 10.1016/j.jece.2022.107560
4. [4]
  X.G. Duan, Z.M. Ao, D.G. Li, et al., Carbon 103 (2016) 404–411. doi: 10.1016/j.carbon.2016.03.034
5. [5]
  X.G. Duan, H.Q. Sun, M. Tade, et al., Catal. Today 307 (2018) 140–146. doi: 10.1016/j.cattod.2017.04.038
6. [6]
  X.G. Duan, C. Su, J. Miao, et al., Appl. Catal. B: Environ. 220 (2018) 626–634. doi: 10.1016/j.apcatb.2017.08.088
7. [7]
  J.L. Wang, S.Z. Wang, Chem. Eng. J. 334 (2018) 1502–1517. doi: 10.1016/j.cej.2017.11.059
8. [8]
  W.Y. Han, D.G. Li, M.Q. Zhang, et al., J. Hazard. Mater. 395 (2020) 122695. doi: 10.1016/j.jhazmat.2020.122695
9. [9]
  A.B. Alayande, S. Hong, Environ. Pollut. 307 (2022) 119513. doi: 10.1016/j.envpol.2022.119513
10. [10]
  G. Nie, L. Xiao, J.X. Bi, et al., Appl. Catal. B: Environ. 315 (2022) 121584. doi: 10.1016/j.apcatb.2022.121584
11. [11]
  X.G. Duan, C. Su, L. Zhou, et al., Appl. Catal. B: Environ. 194 (2016) 7–15. doi: 10.1016/j.apcatb.2016.04.043
12. [12]
  X.G. Duan, S. Indrawirawan, H.Q. Sun, et al., Catal. Today 249 (2015) 184–191. doi: 10.1016/j.cattod.2014.10.005
13. [13]
  X.G. Duan, H.Q. Sun, Z.M. Ao, et al., Carbon 107 (2016) 371–378. doi: 10.1016/j.carbon.2016.06.016
14. [14]
  S.H. Ho, Y.D. Chen, R.X. Li, et al., Water Res. 159 (2019) 77–86. doi: 10.1016/j.watres.2019.05.008
15. [15]
  X.G. Duan, Z.M. Ao, H.Q. Sun, et al., ACS Appl. Mater. Interfaces 7 (2015) 4169–4178. doi: 10.1021/am508416n
16. [16]
  W.J. Tian, H.Y. Zhang, X.G. Duan, et al., Adv. Funct. Mater. 30 (2020) 1909265. doi: 10.1002/adfm.201909265
17. [17]
  H.R. Li, J.Y. Tian, Z.G. Zhu, et al., Chem. Eng. J. 354 (2018) 507–516. doi: 10.1016/j.cej.2018.08.043
18. [18]
  X.J. Wei, L. Wang, W.L. Jia, et al., Chin. J. Chem. 32 (2014) 1245–1250. doi: 10.1002/cjoc.201400521
19. [19]
  K.K. Borowicz, M. Gasior, Z. Kleinrok, et al., Eur. J. Pharmacol. 323 (1997) 45–51. doi: 10.1016/S0014-2999(97)00020-4
20. [20]
  S.D. Dhengale, V.M. Naik, G.B. Kolekar, et al., Res. Chem. Intermed. 47 (2021) 3263–3287. doi: 10.1007/s11164-021-04473-z
21. [21]
  H. Saffarian, F. Karimi, M. Yarie, et al., J. Mol. Struct. 1224 (2021) 129294. doi: 10.1016/j.molstruc.2020.129294
22. [22]
  J.Q. Zhang, X.H. An, N. Lin, et al., Carbon 100 (2016) 450–455. doi: 10.1016/j.carbon.2016.01.027
23. [23]
  S. Indrawirawan, H.Q. Sun, X.G. Duan, et al., J. Mater. Chem. A 3 (2015) 3432–3440. doi: 10.1039/C4TA05940A
24. [24]
  J.Q. Zhang, Y.G. Li, X.L. Zhao, et al., Nano Energy 89 (2021) 106357. doi: 10.1016/j.nanoen.2021.106357
25. [25]
  Y.W. Gao, T. Li, Y. Zhu, et al., J. Hazard. Mater. 393 (2020) 121280. doi: 10.1016/j.jhazmat.2019.121280
26. [26]
  Y.W. Gao, Z.H. Chen, Y. Zhu, et al., Environ. Sci. Technol. 54 (2020) 1232–1241. doi: 10.1021/acs.est.9b05856
27. [27]
  W. Zhang, Y. Li, X.B. Fan, et al., Carbon 155 (2019) 268–278. doi: 10.1016/j.carbon.2019.08.071
28. [28]
  P. Liang, C. Zhang, X.G. Duan, et al., Environ. Sci. Nano 4 (2017) 315–324. doi: 10.1039/C6EN00633G
29. [29]
  J. Li, Y. Zhang, X. Zhang, et al., ACS Appl. Mater. Interfaces 7 (2015) 19626–19634. doi: 10.1021/acsami.5b03845
30. [30]
  F. Li, M.E. Han, Y. Jin, et al., Appl. Catal. B: Environ. 256 (2019) 117705. doi: 10.1016/j.apcatb.2019.05.007
31. [31]
  Q.F. Li, C. Ren, C.T. Qiu, et al., Chin. Chem. Lett. 32 (2021) 3463–3468. doi: 10.1016/j.cclet.2021.05.039
32. [32]
  G.Q. Zhang, Y.S. Xu, G.S. Liu, et al., Chin. Chem. Lett. 34 (2023) 107383. doi: 10.1016/j.cclet.2022.03.106
33. [33]
  Y. Zhang, L. Wu, S. Wang, et al., Chin. Chem. Lett. 35 (2023) 108551. doi: 10.1016/j.cclet.2023.108551
34. [34]
  W.J. Tian, J.K. Lin, H.Y. Zhang, et al., J. Hazard. Mater. 408 (2021) 124459. doi: 10.1016/j.jhazmat.2020.124459
35. [35]
  D.G. Li, X.G. Duan, H.Q. Sun, et al., Carbon 115 (2017) 124459.
36. [36]
  X. Chen, X.G. Duan, W.D. Oh, et al., Appl. Catal. B: Environ. 253 (2019) 419–432. doi: 10.1016/j.apcatb.2019.04.018
37. [37]
  H. Jiang, J.X. Gu, X.S. Zheng, et al., Energ. Environ. Sci. 12 (2019) 322–333. doi: 10.1039/C8EE03276A
38. [38]
  Y. Zheng, Y. Jiao, Y. Zhu, et al., Nat. Commun. 5 (2014) 3783. doi: 10.1038/ncomms4783
39. [39]
  Y. Xu, M. Fan, W. Yang, et al., Adv. Mater. 33 (2021) e2101455. doi: 10.1002/adma.202101455
40. [40]
  T. Wang, Y. Sun, L. Zhang, et al., Adv. Mater. 31 (2019) e1807876. doi: 10.1002/adma.201807876
41. [41]
  S.J. Wang, L. Chen, X.L. Zhao, et al., Appl. Catal. B: Environ. 278 (2020) 119312. doi: 10.1016/j.apcatb.2020.119312
42. [42]
  W. Ren, G. Nie, P. Zhou, et al., Environ. Sci. Technol. 54 (2020) 6438–6447. doi: 10.1021/acs.est.0c01161
43. [43]
  J. Wang, X.G. Duan, J. Gao, et al., Water Res. 185 (2020) 116244. doi: 10.1016/j.watres.2020.116244
44. [44]
  P.P. Zhang, Y.Y. Yang, X.G. Duan, et al., ACS Catal. 11 (2021) 11129–11159. doi: 10.1021/acscatal.1c03099
45. [45]
  W.T. Zheng, Y.B.A. Liu, W. Liu, et al., Water Res. 194 (2021) 116961. doi: 10.1016/j.watres.2021.116961
46. [46]
  Y.Y. Yang, P.P. Zhang, K.S. Hu, et al., Appl. Catal. B: Environ. 286 (2021) 119903. doi: 10.1016/j.apcatb.2021.119903
47. [47]
  H. Wu, X.Y. Xu, L. Shi, et al., Water Res. 167 (2019) 115110. doi: 10.1016/j.watres.2019.115110
48. [48]
  Y.D. Chen, X.G. Duan, X. Zhou, et al., Chem. Eng. J. 409 (2021) 128207. doi: 10.1016/j.cej.2020.128207
49. [49]
  P.H. Shao, Y.P. Jing, X.G. Duan, et al., Environ. Sci. Technol. 55 (2021) 16078–16087. doi: 10.1021/acs.est.1c02042
50. [50]
  Y.B. Xie, Y. Liu, Y.J. Yao, et al., Chin. Chem. Lett. 33 (2022) 1298–1302. doi: 10.1016/j.cclet.2021.07.055
51. [51]
  Y. Liu, F.X. Cun, D.Q. Tian, et al., J. Hazard. Mater. 435 (2022) 128975. doi: 10.1016/j.jhazmat.2022.128975
52. [52]
  W. Ren, C. Cheng, P.H. Shao, et al., Environ. Sci. Technol. 56 (2022) 78–97. doi: 10.1021/acs.est.1c05374
53. [53]
  W. Ren, L.L. Xiong, X.H. Yuan, et al., Environ. Sci. Technol. 53 (2019) 14595–14603. doi: 10.1021/acs.est.9b05475
54. [54]
  Y.X. Wang, X. Li, S.N. Liu, et al., ACS Catal. 12 (2022) 2770–2780. doi: 10.1021/acscatal.1c05447
55. [55]
  W. Han, D. Li, Y. Kong, et al., J. Colloid Interface Sci. 646 (2023) 633–648. doi: 10.1016/j.jcis.2023.05.092
1. [1]
  Weixu Li , Yuexin Wang , Lin Li , Xinyi Huang , Mengdi Liu , Bo Gui , Xianjun Lang , Cheng Wang . Promoting energy transfer pathway in porphyrin-based sp2 carbon-conjugated covalent organic frameworks for selective photocatalytic oxidation of sulfide. Chinese Journal of Structural Chemistry, 2024, 43(7): 100299-100299. doi: 10.1016/j.cjsc.2024.100299
2. [2]
  Yun-Xin Huang , Lin-Qian Yu , Ke-Yu Chen , Hao Wang , Shou-Yan Zhao , Bao-Cheng Huang , Ren-Cun Jin . Biochar with self-doped N to activate peroxymonosulfate for bisphenol-A degradation via electron transfer mechanism: The active edge graphitic N site. Chinese Chemical Letters, 2024, 35(9): 109437-. doi: 10.1016/j.cclet.2023.109437
3. [3]
  Mengmeng Ao , Jian Wei , Chuan-Shu He , Heng Zhang , Zhaokun Xiong , Yonghui Song , Bo Lai . Insight into the activation of peroxymonosulfate by N-doped copper-based carbon for efficient degradation of organic pollutants: Synergy of nonradicals. Chinese Chemical Letters, 2025, 36(1): 109882-. doi: 10.1016/j.cclet.2024.109882
4. [4]
  Kexin Yin , Jingren Yang , Yanwei Li , Qian Li , Xing Xu . Metal-free diatomaceous carbon-based catalyst for ultrafast and anti-interference Fenton-like oxidation. Chinese Chemical Letters, 2024, 35(12): 109847-. doi: 10.1016/j.cclet.2024.109847
5. [5]
  Ming-Zhen Li , Yang Zhang , Kun Li , Ya-Nan Shang , Yi-Zhen Zhang , Yu-Jiao Kan , Zhi-Yang Jiao , Yu-Yuan Han , Xiao-Qiang Cao . In situ regeneration of catalyst for Fenton-like degradation by photogenerated electron transportation: Characterization, performance and mechanism comparison. Chinese Chemical Letters, 2025, 36(1): 109885-. doi: 10.1016/j.cclet.2024.109885
6. [6]
  Yinyin Xu , Yuanyuan Li , Jingbo Feng , Chen Wang , Yan Zhang , Yukun Wang , Xiuwen Cheng . Covalent organic frameworks doped with manganese-metal organic framework for peroxymonosulfate activation. Chinese Chemical Letters, 2024, 35(4): 108838-. doi: 10.1016/j.cclet.2023.108838
7. [7]
  Dong Cheng , Youyou Feng , Bingxi Feng , Ke Wang , Guoxin Song , Gen Wang , Xiaoli Cheng , Yonghui Deng , Jing Wei . Polyphenol-mediated interfacial deposition strategy for supported manganese oxide catalysts with excellent pollutant degradation performance. Chinese Chemical Letters, 2024, 35(5): 108623-. doi: 10.1016/j.cclet.2023.108623
8. [8]
  Ruiying Liu , Li Zhao , Baishan Liu , Jiayuan Yu , Yujie Wang , Wanqiang Yu , Di Xin , Chaoqiong Fang , Xuchuan Jiang , Riming Hu , Hong Liu , Weijia Zhou . Modulating pollutant adsorption and peroxymonosulfate activation sites on Co3O4@N,O doped-carbon shell for boosting catalytic degradation activity. Chinese Journal of Structural Chemistry, 2024, 43(8): 100332-100332. doi: 10.1016/j.cjsc.2023.100332
9. [9]
  Jiaojiao Liang , Youming Peng , Zhichao Xu , Yufei Wang , Menglong Liu , Xin Liu , Di Huang , Yuehua Wei , Zengxi Wei . Boron/phosphorus co-doped nitrogen-rich carbon nanofiber with flexible anode for robust sodium-ion battery. Chinese Chemical Letters, 2025, 36(1): 110452-. doi: 10.1016/j.cclet.2024.110452
10. [10]
  Ruonan Guo , Heng Zhang , Changsheng Guo , Ningqing Lv , Beidou Xi , Jian Xu . Degradation of neonicotinoids with different molecular structures in heterogeneous peroxymonosulfate activation system through different oxidation pathways. Chinese Chemical Letters, 2024, 35(9): 109413-. doi: 10.1016/j.cclet.2023.109413
11. [11]
  Zhuoyan Lv , Yangming Ding , Leilei Kang , Lin Li , Xiao Yan Liu , Aiqin Wang , Tao Zhang . Light-Enhanced Direct Epoxidation of Propylene by Molecular Oxygen over CuO_x/TiO₂ Catalyst. Acta Physico-Chimica Sinica, 2025, 41(4): 100038-. doi: 10.3866/PKU.WHXB202408015
12. [12]
  Yiqian Jiang , Zihan Yang , Xiuru Bi , Nan Yao , Peiqing Zhao , Xu Meng . Mediated electron transfer process in α-MnO₂ catalyzed Fenton-like reaction for oxytetracycline degradation. Chinese Chemical Letters, 2024, 35(8): 109331-. doi: 10.1016/j.cclet.2023.109331
13. [13]
  Rui PAN , Yuting MENG , Ruigang XIE , Daixiang CHEN , Jiefa SHEN , Shenghu YAN , Jianwu LIU , Yue ZHANG . Selective electrocatalytic reduction of Sn(Ⅳ) by carbon nitrogen materials prepared with different precursors. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 1015-1024. doi: 10.11862/CJIC.20230433
14. [14]
  Peng Zhang , Yitao Yang , Tian Qin , Xueqiu Wu , Yuechang Wei , Jing Xiong , Xi Liu , Yu Wang , Zhen Zhao , Jinqing Jiao , Liwei Chen . Interface engineering of Pt/CeO₂-{100} catalysts for enhancing catalytic activity in auto-exhaust carbon particles oxidation. Chinese Chemical Letters, 2025, 36(2): 110396-. doi: 10.1016/j.cclet.2024.110396
15. [15]
  Xiaxia Xing , Xiaoyu Chen , Zhenxu Li , Xinhua Zhao , Yingying Tian , Xiaoyan Lang , Dachi Yang . Polyethylene imine functionalized porous carbon framework for selective nitrogen dioxide sensing with smartphone communication. Chinese Chemical Letters, 2024, 35(9): 109230-. doi: 10.1016/j.cclet.2023.109230
16. [16]
  Zhipeng Wan , Hao Xu , Peng Wu . Selective oxidation using in-situ generated hydrogen peroxide over titanosilicates. Chinese Journal of Structural Chemistry, 2024, 43(6): 100298-100298. doi: 10.1016/j.cjsc.2024.100298
17. [17]
  Gang Hu , Chun Wang , Qinqin Wang , Mingyuan Zhu , Lihua Kang . The controlled oxidation states of the H₄PMo₁₁VO₄₀ catalyst induced by plasma for the selective oxidation of methacrolein. Chinese Chemical Letters, 2025, 36(2): 110298-. doi: 10.1016/j.cclet.2024.110298
18. [18]
  Xiao Li , Wanqiang Yu , Yujie Wang , Ruiying Liu , Qingquan Yu , Riming Hu , Xuchuan Jiang , Qingsheng Gao , Hong Liu , Jiayuan Yu , Weijia Zhou . Metal-encapsulated nitrogen-doped carbon nanotube arrays electrode for enhancing sulfion oxidation reaction and hydrogen evolution reaction by regulating of intermediate adsorption. Chinese Chemical Letters, 2024, 35(8): 109166-. doi: 10.1016/j.cclet.2023.109166
19. [19]
  Fabrice Nelly Habarugira , Ducheng Yao , Wei Miao , Chengcheng Chu , Zhong Chen , Shun Mao . Synergy of sodium doping and nitrogen defects in carbon nitride for promoted photocatalytic synthesis of hydrogen peroxide. Chinese Chemical Letters, 2024, 35(8): 109886-. doi: 10.1016/j.cclet.2024.109886
20. [20]
  Cunjun Li , Wencong Liu , Xianlei Chen , Liang Li , Shenyu Lan , Mingshan Zhu . Adsorption and activation of peroxymonosulfate on BiOCl for carbamazepine degradation: The role of piezoelectric effect. Chinese Chemical Letters, 2024, 35(10): 109652-. doi: 10.1016/j.cclet.2024.109652

Get Citation

PDF

XML

Metrics

PDF Downloads(1)
Abstract views(151)
HTML views(3)

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