High nitrogen carbon material with rich defects as a highly efficient metal-free catalyst for excellent catalytic performance of acetylene hydrochlorination

doi:10.1016/j.cjche.2020.06.008

Abstract

Abstract: In this work, we developed a simple strategy to synthesize a carbon material with high nitrogen and rich carbon defects. Our approach polymerized diaminopyridine (DAP) and ammonium persulfate (APS). Following a range of different temperature pyrolysis approaches, the resulting rough surface was shown to exhibit edge defects due to N-doping on graphite carbon. A series of catalysts were evaluated using a variety of characterization techniques and tested for catalytic performance. The catalytic performance of the N-doped carbon material enhanced alongside an increment in carbon defects. The NC-800 catalyst exhibited outstanding catalytic activity and stability in acetylene hydrochlorination (C₂H₂ GHSV=30 h^-1, at 220 ℃, the acetylene conversion rate was 98%), with its stability reaching up to 450 h. Due to NC-800 having a nitrogen content of up to 13.46%, it had the largest specific surface area and a high defect amount, as well as strong C₂H₂ and HCl adsorption. NC-800 has excellent catalytic activity and stability to reflect its unlimited potential as a carbon material.

Key words: Carbon defects material, High nitrogen content, Acetylene hydrochlorination, Catalyst, Chemical reaction, Nanomaterials

Fangjie Lu, Dong Xu, Yusheng Lu, Bin Dai, Mingyuan Zhu. High nitrogen carbon material with rich defects as a highly efficient metal-free catalyst for excellent catalytic performance of acetylene hydrochlorination[J]. Chinese Journal of Chemical Engineering, 2021, 29(1): 196-203.

References

[1] R. Lin, A.P. Amrute, J. Pérez-Ramírez, Halogen-mediated conversion of hydrocarbons to commodities, Chem. Rev. 117(2017) 4182-4247.
[2] M.Y. Zhu, Q.Q. Wang, K. Chen, Y. W, C.F. Huang, H. Dai, F. Yu, L.H. Kang, B. Dai, Development of a heterogeneous non-mercury catalyst for acetylene hydrochlorination, ACS. Catal. 5(2015) 5306-5316.
[3] G.J. Hutchings, Vapor phase hydrochlorination of acetylene:Correlation of catalytic activity of supported metal chloride catalysts, J. Catal. 96(1985) 292-295.
[4] J.L. Zhang, N. Liu, W. Li, B. Dai, Progress on cleaner production of vinyl chloride monomers over non-mercury catalysts, Front. Chem. Sci. Eng. 5(2011) 514-520.
[5] G.J. Hutchings, Gold catalysis in chemical processing, Catal. Today 72(2002) 11-17.
[6] M. Cont, A.F. Carley, C. Heirene, D.J. Willock, P. Johnston, A.A. Herzing, C.J. Kiely, G.J. Hutchings, Hydrochlorination of acetylene using a supported gold catalyst:A study of the reaction mechanism, J. Catal. 250(2007) 231-239.
[7] X.M. Wang, M.Y. Zhu, B. Dai, Effect of phosphorus ligand on Cu-based catalysts for acetylene hydrochlorination, ACS Sustain. Chem. Eng. 7(2019) 6170-6177.
[8] F. Wang, L. Wang, J.D. Wang, Y.L. Zhao, Y.L. Wang, D. Yang, Bimetallic Pd-K/Y-zeolite catalyst in acetylene hydrochlorination for PVC production, React. Kinet. Mech. 114(2015) 725-734.
[9] L. Wang, F. Wang, J.D. Wang, Non-mercury catalytic acetylene hydrochlorination over a NH₄F-urea-modified Pd/HY catalyst for vinyl chloride monomer production, New J. Chem. 40(2016) 3019-3023.
[10] S.A. Mitchenko, T.V. Krasnyakova, R.S. Mitchenko, A.N. Korduban, Acetylene catalytic hydrochlorination over powder catalyst prepared by pre-milling of K₂PtCl₄ salt, J. Mol. Catal. A-Chem. 275(2007) 101-108.
[11] K. Zhou, J.C. Jia, X.G. Li, X.D. Pang, C.H. Li, J. Zhou, G.H. Luo, F. Wei, Continuous vinyl chloride monomer production by acetylene hydrochlorination on Hg-free bismuth catalyst:From lab-scale catalyst characterization, catalytic evaluation to a pilotscale trial by circulating regeneration in coupled fluidized beds, Fuel Process. Technol. 108(2013) 12-18.
[12] L.J. Hou, J.L. Zhang, Y.F. Pu, W. Li, Effects of nitrogen-dopants on Ru-supported catalysts for acetylene hydrochlorination, RSC Adv. 6(2016) 18026-18032.
[13] B.C. Man, H.Y. Zhang, J.L. Zhang, X. Li, N. Xu, H. Dai, M.Y. Zhu, B. Dai, Oxidation modification of Ru-based catalyst for acetylene hydrochlorination, RSC Adv. 7(2017) 23742-23750.
[14] X.Y. Li, Y. Wang, L.H. Kang, M.Y. Zhu, B. Dai, A novel, non-metallic graphitic carbon nitride catalyst for acetylene hydrochlorination, J. Catal. 311(2014) 288-294.
[15] C.L. Zhang, L.H. Kang, M.Y. Zhu, B. Dai, Nitrogen-doped active carbon as a metal-free catalyst for acetylene hydrochlorination, RSC Adv. 5(2015) 7461-7468.
[16] X.Y. Li, C.L. Zhang, Y. Han, M.Y. Zhu, S.S. Shang, W. Li, Email author MOF-derived various morphologies of N-doped carbon composites for acetylene hydrochlorination, J. Mater. Sci. 53(2018) 4913-4926.
[17] X.B. Dong, S.L. Chao, F.F. Wan, Q.X. Guan, G.C. Wang, W. Li, Sulfur and nitrogen codoped mesoporous carbon with enhanced performance for acetylene hydrochlorination, J. Catal. 359(2018) 161-170.
[18] J. Wang, F. Zhao, C.L. Zhang, L.H. Kang, M.Y. Zhu, A novel S, N dual doped carbon catalyst for acetylene hydrochlorination, Appl. Catal. A-Gen. 549(2018) 68-75.
[19] J. Zhao, B.L. Wang, Y. Yue, G.F. Sheng, H.X. Lai, S.S. Wang, L. Yu, Q.F. Zhang, F. Feng, Z.-T. Hu, X.N. Li, Nitrogen-and phosphorus-co-doped carbon-based catalyst for acetylene hydrochlorination, J. Catal. 373(2019) 240-249.
[20] P. Li, H.B. Li, X.L. Pan, K. Tie, T.T. Cui, M.Z. Ding, X.H. Bao, Catalytically active boron nitride in acetylene hydrochlorination, ACS Catal. 7(2017) 8572-8577.
[21] R.H. Lin, S.K. Kaiser, R. Hauert, J. Pérez-Ramírez, Descriptors for high-performance nitrogen-doped carbon catalysts in acetylene hydrochlorination, ACS Catal. 8(2018) 1114-1121.
[22] X.Y. Li, P. Li, X.L. Pan, H. Ma, X. Bao, Deactivation mechanism and regeneration of carbon nanocomposite catalyst for acetylene hydrochlorination, Appl. Catal., B-Environ. 210(2017) 116-120.
[23] F. Zhao, L.H. Kang, The neglected significant role for graphene-based acetylene hydrochlorination catalysts-intrinsic graphene defects, Chemistryselect 2(2017) 6016-6022.
[24] X.J. Zhao, X.Q. Zou, X.C. Yan, C.L. Brown, Z.G. Chen, G.S. Zhu, X.D. Yao, Defect-driven oxygen reduction reaction (ORR) of carbon without any element doping, Inorg. Chem. Front. 3(2016) 417-421.
[25] C.G. Hu, L.M. Dai, Carbon-based metal-free catalysts for electrocatalysis beyond the ORR, Angew. Chem. Int. Edit. 55(2016) 11736-11758.
[26] Y.F. Jiang, L.J. Yang, T. Sun, J. Zhao, Z.Y. Lyu, O. Zhuo, X.Z. Wang, Q. Wu, J. Ma, Z. Hu, Significant contribution of intrinsic carbon defects to oxygen reduction activity, ACS Catal. 5(2015) 6707-6712.
[27] J. Wang, W.Q. Gong, M.Y. Zhu, B. Dai, Effect of carbon defects on the nitrogen-doped carbon catalytic performance for acetylene hydrochlorination, Appl. Catal. A-Gen. 564(2018) 72-78.
[28] X.L. Qiao, Z.Q. Zhou, X.Y. Liu, C.Y. Zhao, Q.X. Guan, W. Li, Constructing of fragmentary g-C₃N₄ framework with rich nitrogen defects as highly efficient metal-free catalyst for acetylene hydrochlorination, Catal. Sci. Technol. 9(2019) 3753-3762.
[29] H. Zhao, C. Sun, Z. Jin, D.W. Wang, X. Yan, Z. Chen, G. Zhu, X. Yao, Carbon for the oxygen reduction reaction:a defect mechanism, J. Mate. Chem. A-Chem. 3(22) (2015) 11736-11739.
[30] Y. Kim, J. Ihm, E. Yoon, G.D. Lee, Thickness-dependent bulk properties and weak antilocalization effect in topological insulator Bi₂Se₃, Phys. Rev. B-Condens Matter. 84(7) (2011) 2789.
[31] X. Yan, Y. Jia, T. Odedairo, X. Zhao, Z. Jin, Z. Zhu, X. Yao, Activated carbon becomes active for oxygen reduction and hydrogen evolution reactions, Chem. Commun. 52(52) (2016) 8156-8159.
[32] T. Najam, S.S.A. Shah, W. Ding, J. Jiang, L. Jia, W. Yao, L. Li, Z.D. Wei, An efficient antipoisoning catalyst against SOx, NOx, and POx:P, N-doped carbon for oxygen reduction in acidic media, Angew. Chem. Int. Edit. 57(2018) 15101-15106.
[33] S.L. Chao, Fang Zou, F.F. Wan, X.B. Dong, Y.L. Wang, Y.X. Wang, Q.X. Guan, G.C. Wang, W. Li, Nitrogen-doped carbon derived from ZIF-8 as a high-performance metal-free catalyst for acetylene hydrochlorination, Sci. Rep. 7(2017) 1-7.
[34] K. Zhou, B. Li, Q. Zhang, J.Q. Huang, G.L. Tian, J.C. Jia, M.Q. Zhao, G.H. Luo, D.S. Su, F. Wei, The catalytic pathways of hydrohalogenation over metal-free nitrogen-doped carbon nanotubes, ChemSusChem 7(2014) 723-728.
[35] X. Wang, B. Dai, Y. Wang, F. Yu, Nitrogen-doped pitch-based spherical active carbon as a nonmetal catalyst for acetylene Hydrochlorination, ChemCatChem 6(2014) 2339-2344.
[36] Y. Yang, G.J. Lan, X.L. Wang, Y. Li, Direct synthesis of nitrogen-doped mesoporous carbons for acetylene hydrochlorination, Chin. J. Catal. 37(2016) 1242-1248.