Citation: Yusheng Lu, Chaofeng Huang, Zhigang Lei, Mingyuan Zhu. Catalytic effects of structural design in N-modified carbon materials for the hydrochlorination of acetylene[J]. Chinese Chemical Letters, ;2025, 36(8): 110583. doi: 10.1016/j.cclet.2024.110583 shu

Catalytic effects of structural design in N-modified carbon materials for the hydrochlorination of acetylene

Yusheng Lu ^a ,
Chaofeng Huang ^a ,
Zhigang Lei ^{a, b, *,} ,
Mingyuan Zhu ^{c, *,}

a.
School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering, Shihezi 832000, China
b.
State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China
c.
College of Chemistry & Chemical Engineering, Yantai University, Yantai 264010, China

leizhg@mail.buct.edu.cn

zhuminyuan@shzu.edu.cn

Received Date: 1 July 2024
Revised Date: 23 September 2024
Accepted Date: 26 October 2024
Available Online: 28 October 2024

Figures(4)

Polyvinyl chloride is the most widely used general-purpose plastic and plays a vital role in various industries. Mercury-based catalysts severely limit the green sustainability of industry. Non-metallic carbon materials are very promising alternatives in acetylene hydrochlorination, but their stability remains a challenge of major concern at present. Based on the principle of green chemistry, structurally tunable and defect-rich carbon materials were synthesized by hydrothermal carbonization and pyrolysis using glucose as carbon source and m-phenylenediamine as nitrogen source and cross-linking agent. Experimental characterization and density functional theory confirmed that pyridinic N was the main active site. The introduction of N not only regulated the formation of the hierarchically porous structure of the carbon material, but also increased the adsorption of HCl and decreased the adsorption strength of C₂H₂. The synergistic effect of high N content and porous structure significantly enhanced the catalytic performance of the catalysts in acetylene hydrochlorination. The C₂H₂ conversion was maintained at around 98% after 100 h under the reaction conditions (T = 220 ℃, GHSV(C₂H₂) = 30 h^-1, V_HCl/V_C₂H₂ = 1.15). Thus, the one-pot synthesis process used here is a good benchmark for future catalyst research.
- Acetylene hydrochlorination,
- Hierarchically porous structure,
- Structure modulation,
- N-Modified carbon materials,
- Pyridinic N,
- One-pot hydrothermal process
1. [1]
  M. Safarpour, A. Safikhani, V. Vatanpour, Sep. Purif. Technol. 279 (2021) 119678.
2. [2]
  R. Lin, A.P. Amrute, J. Pérez-Ramírez, Chem. Rev. 117 (2017) 4182–4247. doi: 10.1021/acs.chemrev.6b00551
3. [3]
  K.H. Kim, E. Kabir, S.A. Jahan, J. Hazard. Mater. 306 (2016) 376–385.
4. [4]
  G. Wang, Y. Liu, X. Dong, et al., J. Hazard. Mater. 437 (2022) 129357.
5. [5]
  B. Dai, K. Chen, Y. Wang, et al., ACS Catal. 5 (2015) 2541–2547. doi: 10.1021/acscatal.5b00199
6. [6]
  K. Zhou, B. Li, Q. Zhang, et al., ChemSusChem 7 (2014) 723–728. doi: 10.1002/cssc.201300793
7. [7]
  R. Lin, S.K. Kaiser, R. Hauert, et al., ACS Catal. 8 (2018) 1114–1121. doi: 10.1021/acscatal.7b03031
8. [8]
  Z. Shen, Y. Liu, Y. Han, et al., RSC Adv. 10 (2020) 14556–14569. doi: 10.1039/d0ra00475h
9. [9]
  Y. Lu, F. Lu, M. Zhu, J. Taiwan Inst. Chem. Eng. 113 (2020) 198–203.
10. [10]
  G. Lan, Y. Wang, Y. Qiu, et al., Chem. Commun. 54 (2018) 623–626. doi: 10.1039/c7cc09370e
11. [11]
  X. Li, J. Zhang, W. Li, J. Ind. Eng. Chem. 44 (2016) 146–154.
12. [12]
  S. Chao, F. Zou, F. Wan, et al., Sci. Rep. 7 (2017) 39789.
13. [13]
  B. Wang, Y. Yue, X. Pang, et al., Phys. Chem. Chem. Phys. 22 (2020) 20995–20999. doi: 10.1039/d0cp04043f
14. [14]
  F. Li, H. Zhang, M. Zhang, et al., ACS Sustain. Chem. Eng. 10 (2022) 194–203. doi: 10.1021/acssuschemeng.1c05661
15. [15]
  X. Li, P. Li, X. Pan, et al., Appl. Catal. B: Environ. 210 (2017) 116–120. doi: 10.3901/JME.2017.05.116
16. [16]
  D. Xu, Y. Lu, L. Liu, et al., ChemistrySelect 7 (2022) e202104556.
17. [17]
  S. Wang, Z. Liu, D. Xu, et al., Mol. Catal. 563 (2024) 114240.
18. [18]
  X. Dong, S. Chao, F. Wan, et al., J. Catal. 359 (2018) 161–170.
19. [19]
  X. Li, X. Pan, X. Bao, J. Energy Chem. 23 (2014) 131–135.
20. [20]
  X. Tao, F. Chen, Y. Xie, et al., J. Taiwan Inst. Chem. Eng. 126 (2021) 80–87.
21. [21]
  S.K. Kaiser, K.S. Song, S. Mitchell, et al., ChemCatChem 12 (2020) 1922–1925. doi: 10.1002/cctc.201902331
22. [22]
  H. Liang, Q. Guan, L. Chen, et al., Angew. Chem. Int. Ed. 51 (2012) 5101–5105. doi: 10.1002/anie.201200710
23. [23]
  L. Liang, M. Zhou, K. Li, et al., Microporous Mesoporous Mater. 265 (2018) 26–34.
24. [24]
  J. Gao, Y. Wang, H. Wu, et al., Angew. Chem. Int. Ed. 58 (2019) 15089–15097. doi: 10.1002/anie.201907915
25. [25]
  S. Balou, S.E. Babak, A. Priye, A.C.S. Appl. Mater. Inter. 12 (2020) 42711–42722. doi: 10.1021/acsami.0c10218
26. [26]
  X. Zhao, X. Yu, S. Xin, et al., Appl. Catal. B: Environ. 301 (2022) 120785.
27. [27]
  Y. Zhou, L. Luo, W. Yan, et al., Energy 246 (2022) 123367.
28. [28]
  H. Cui, H. Chen, Z. Guo, et al., Microporous Mesoporous Mater. 309 (2020) 110591.
29. [29]
  K. Li, M. Zhou, L. Liang, et al., J. Colloid Interface Sci. 546 (2019) 333–343.
30. [30]
  S. Mezzavilla, C. Zanella, P.R. Aravind, et al., J. Mater. Sci. 47 (2012) 7175–7180. doi: 10.1007/s10853-012-6662-1
31. [31]
  S. Mei, J. Gu, T. Ma, et al., Chem. Eng. J. 371 (2019) 118–129.
32. [32]
  X. Jin, Y. Hao, C. Liu, et al., New J. Chem. 45 (2021) 19358–19363. doi: 10.1039/d1nj03858c
33. [33]
  Z. Li, Y. Zhou, W. Yan, et al., ACS Appl. Mater. Inter. 12 (2020) 21748–21760. doi: 10.1021/acsami.0c04015
34. [34]
  Q. Zhang, H. Zhang, M. Huang, et al., ACS Sustain. Chem. Eng. 11 (2023) 3103–3113. doi: 10.1021/acssuschemeng.2c07478
35. [35]
  C. Zhang, H. Zhang, Y. Li, et al., ChemCatChem 11 (2019) 3441–3450. doi: 10.1002/cctc.201900624
36. [36]
  X. Dong, G. Liu, Z. Chen, et al., Mol. Catal. 525 (2022) 112366.
37. [37]
  X. Qiao, X. Liu, Z. Zhou, et al., Catal. Sci. Technol. 11 (2021) 2327–2339. doi: 10.1039/d0cy01950j
38. [38]
  X. Liu, X. Qiao, Z. Zhou, et al., Catal. Commun. 147 (2020) 106147.
39. [39]
  X. Li, X. Pan, L. Yu, et al., Nat. Commun. 5 (2014) 3688.
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