氯化氢催化氧化制氯气的研究进展
Recent Progress in Catalytic Oxidation of Hydrogen Chloride into Chlorine
DOI: 10.12677/japc.2021.101001, PDF,    科研立项经费支持
作者: 辛 旭, 黄雅琦, 刘佳慧, 卢信清, 马 睿, 朱伟东, 傅仰河*:先进催化材料教育部重点实验室,浙江师范大学含氟新材料研究所,浙江 金华;周黎旸:巨化集团有限公司,浙江 衢州
关键词: Deacon反应氯化氢催化氧化氯气反应机理Deacon Reaction Hydrogen Chloride Catalytic Oxidation Chlorine Reaction Mechanism
摘要: 在众多涉氯化工过程中,氯原子利用率较低,导致产生大量副产氯化氢制约行业发展。氯化氢催化氧化循环制氯气,是一个低能耗、高效率、环境友好可解决大量副产氯化氢的有效途径。本文综述了Deacon催化剂的发展历程,以及不同Deacon催化剂的作用机理。虽然Ru基催化剂已在工业上实现大规模应用,但是如何提高催化剂稳定性,和降低催化剂成本,仍是未来需要重点研究的方向。
Abstract: In many chlorine-related chemical processes, the low utilization of chlorine atoms with a large amount of hydrogen chloride as the by-product restricts the development of the chemical industry. Therefore, how to efficiently recover chlorine resources is an urgent issue for the chlorine-related industry. The catalytic oxidation of hydrogen chloride into chlorine, as the Deacon process, is an ef-fective way to solve this issue with low energy consumption, high efficiency and environmental friendliness. In this paper, the development of Deacon catalysts is reviewed, and their reaction mechanisms are also discussed. Ru-based catalysts have been used on a large scale in industry, but how to improve catalyst stability and reduce catalyst cost is still the key research direction for the future.
文章引用:辛旭, 黄雅琦, 刘佳慧, 卢信清, 马睿, 朱伟东, 周黎旸, 傅仰河. 氯化氢催化氧化制氯气的研究进展[J]. 物理化学进展, 2021, 10(1): 1-8. https://doi.org/10.12677/japc.2021.101001

参考文献

[1] Teschner, D., Farra, R., Yao, L., Schlögl, R., Soerijanto, H., Schomäcker, R., Schmidt, T., Szentmiklósi, L., Amrute, A.P., Mondelli, C., Pérez-Ramírez, J., Novell-Leruth, G. and López, N. (2012) An Integrated Approach to Deacon Chemistry on RuO2-Based Catalysts. Journal of Catalysis, 285, 273-284. [Google Scholar] [CrossRef
[2] Till, Z., Varga, T., Réti, J. and Chován, T. (2017) Optimization Strategies in a Fixed-Bed Reactor for HCl Oxidation. Industrial & Engineering Chemistry Research, 56, 5352-5359. [Google Scholar] [CrossRef
[3] López, N., Gómez-Segura, J., Marín, R.P. and Pérez-Ramírez, J. (2008) Mechanism of HCl Oxidation (Deacon Process) over RuO2. Journal of Catalysis, 255, 29-39. [Google Scholar] [CrossRef
[4] Pérez-Ramírez, J., Mondelli, C., Schmidt, T., Schlüter, O.F.K., Wolf, A., Mleczko, L. and Dreier, T. (2011) Sustainable Chlorine Recycling via Catalysed HCl Oxidation: From Fundamentals to Implementation. Energy & Environmental Science, 4, 4786-4799. [Google Scholar] [CrossRef
[5] Zhang, J. (1998) Technology Progress of Hydrogen Chloride Catalytic Oxidation. China Chlor-Alkali, 5, 6-10.
[6] Motupally, S., Mah, D.T., Freire, F.J. and Weidner, J.W. (1998) Recycling Chlorine from Hydrogen Chloride: A New and Economical Electrolytic Process. Electrochemical Society Interface, 7, 32-36.
[7] Davy, H. (1811) On a Combination of Oxymuriatic Gas and Oxygene Gas. Philosophical Transactions of the Royal Society of London, 101, 155-162. [Google Scholar] [CrossRef
[8] 常培廷, 胡刚石, 韩明汉, 吴勤, 魏飞, 金涌. 两段循环流化床中氯化氢催化氧化制氯气[J]. 过程工程学报, 2006, 6(1): 47-50.
[9] Tseng, H.H., Wey, M.Y. and Liang, Y.S. (2003) Catalytic Removal of SO2, NO and HCl from Incineration Flue Gas over Activated Carbon-Supportde Metal Oxides. Carbon, 41, 1079-1085. [Google Scholar] [CrossRef
[10] Seki, K. (2010) Development of RuO2/Rutile-TiO2 Catalyst for Industrial HCl Oxidation Process. Catalysis Surveys from Asia, 14, 168-175. [Google Scholar] [CrossRef
[11] Hisham, M.W.M. and Benson, S.W. (1995) Thermochemistry of the Deacon Process. Journal of Physical Chemistry, 99, 6194-6198. [Google Scholar] [CrossRef
[12] Over, H. (2012) Atomic-Scale Understanding of the HCl Oxidation over RuO2, a Novel Deacon Process. The Journal of Physical Chemistry C, 116, 6779-6792. [Google Scholar] [CrossRef
[13] Tian, X., Wang, S., Wang, Z.J., Wang, H., Zhou, Y., Zhong, H. and Mao, Y. (2020) Sustainable Utilization of Chlorine via Converting HCl to Cl2 over a Robust Copper Catalyst. Molecular Catalysis, 492, Article ID: 110977. [Google Scholar] [CrossRef
[14] Pan, H.Y., Minet, R.G., Benson, S.W. and Tsotsis, T.T. (1994) Process for Converting Hydrogen Chloride to Chlorine. Industrial & Engineering Chemistry Research, 33, 2996-3003. [Google Scholar] [CrossRef
[15] Wattimena, F. and Sachtler, W.M.H. (1981) Catalyst Research for the Shell Chlorine Process. Studay Surface Science Catalysis, 7, 816-827. [Google Scholar] [CrossRef
[16] Hammes, M., Soerijanto, H., Schomäcker, R., Valtchev, M., Stöwe, K. and Maier, W.F. (2014) Niobium: Activator and Stabilizer for a Copper-Based Deacon Catalyst. ChemCatChem, 6, 245-254. [Google Scholar] [CrossRef
[17] Mondelli, C., Amrute, A.P., Schmidt, T. and Perez-Ramirez, J. (2011) A Delafossite-Based Copper Catalyst for Sustainable Cl2 Production by HCl Oxidation. Chemical Communications, 47, 7173-7175. [Google Scholar] [CrossRef] [PubMed]
[18] Amrute, A.P., Mondelli, C. and Pérez-Ramírez, J. (2012) Kinetic Aspects and Deactivation Behaviour of Chromia-Based Catalysts in Hydrogen Chloride Oxidation. Catalysis Science & Technology, 2, 2057-2065. [Google Scholar] [CrossRef
[19] Weckhuysen, B.M. and Wachs, I.E. (1996) In Situ Raman Spectroscopy of Supported Chromium Oxide Catalysts: Reactivity Studies with Methanol and Butane. The Journal of Physical Chemistry, 100, 14437-14442. [Google Scholar] [CrossRef
[20] Uhm, J.H., Shin, M.Y., Jiang, Z.D. and Chung, J.S. (1999) Selective Oxidation of H2S to Elemental Sulfur over Chromium Oxide Catalysts. Applied Catalysis B: Environmental, 22, 293-303. [Google Scholar] [CrossRef
[21] Hsieh, M.C., Ge, Y., Kahn, H., Michal, G.M., Ernst, F. and Heuer, A.H. (2012) Volatility Diagrams for the Cr-O and Cr-Cl Systems: Application to Removal of Cr2O3-Rich Passive Films Onstainless Steel. Metallurgical and Materials Transactions B, 43, 1187-1201. [Google Scholar] [CrossRef
[22] Amrute, A., Mondelli, C., Schmidt, T., Hauert, R. and Pérez-Ramírez, J. (2013) Industrial RuO2-Based Deacon Catalysts: Carrier Stabilization and Active Phase Content Optimization. ChemCatChem, 5, 748-756. [Google Scholar] [CrossRef
[23] Yao, Z. and Reuter, K. (2018) First-Principles Computational Screening of Dopants to Improve the Deacon Process over RuO2. ChemCatChem, 10, 465-469. [Google Scholar] [CrossRef
[24] Mondelli, C., Amrute, A.P., Krumeich, F., Schmidt, T. and Pérez-Ramírez, J. (2011) Shaped RuO2/SnO2-Al2O3 Catalyst for Large-Scale Stable Cl2 Production by HCl Oxidation. ChemCatChem, 3, 657-660. [Google Scholar] [CrossRef
[25] Hevia, M.A.G., Amrute, A.P., Schmidt, T. and Pérez-Ramírez, J. (2010) Transient Mechanistic Study of the Gas-Phase HCl Oxidation to Cl2 on Bulk and Supported RuO2 Catalysts. Journal of Catalysis, 276, 141-151. [Google Scholar] [CrossRef
[26] Teschner, D., Novell-Leruth, G., Farra, R., Knop-Gericke, A., Schlogl, R., Szentmiklosi, L., Gonzalez Hevia, M., Soerijanto, H., Schomacker, R., Perez-Ramirez, J. and Lopez, N. (2012) In Situ Surface Coverage Analysis of RuO2-Catalysed HCl Oxidation Reveals the Entropic Origin of Compensation in Heterogeneous Catalysis. Nature Chemistry, 4, 739-745. [Google Scholar] [CrossRef] [PubMed]
[27] Sun, Y., Hess, F., Djerdj, I., Wang, Z., Weber, T., Guo, Y., Smarsly, B.M. and Over, H. (2020) sReactivation of CeO2-Based Catalysts in the HCl Oxidation Reaction: In Situ Quantification of the Degree of Chlorination and Kinetic Modeling. ChemCatChem, 12, 5511-5522. [Google Scholar] [CrossRef
[28] Tian, X., Lin, B., Li, Y., Wang, S., Zhou, Y. and Zhong, H. (2020) CeO2-MnOx Composite Loaded on Al2O3 as a Catalyst for HCl Oxidation. Catalysis Science & Technology, 10, 4553-4561. [Google Scholar] [CrossRef
[29] Whittaker, E.J.W. (1964) Simple Procedures to a Hexagonal Unit Cell with a Volume Approximating 9000Å3(Ettringite) Demonstrates Tts Great Usefulness. Mineralogical Magazine, 35, 554-555. [Google Scholar] [CrossRef
[30] Zhou, F., Zhao, X., Xu, H. and Yuan, C. (2007) CeO2 Spherical Crystallites: Synthesis, Formation Mechanism, Size Control, and Electrochemical Property Study. Journal of Physical Chemistry C, 111, 1651-1657. [Google Scholar] [CrossRef
[31] Moser, M., Mondelli, C., Schmidt, T., Girgsdies, F., Schuster, M.E., Farra, R., Szentmiklósi, L., Teschner, D. and Pérez-Ramírez, J. (2013) Supported CeO2 Catalysts in Technical Form for Sustainable Chlorine Production. Applied Catalysis B: Environmental, 132-133, 123-131. [Google Scholar] [CrossRef
[32] Amrute, A.P., Mondelli, C., Moser, M., Novell-Leruth, G., López, N., Rosenthal, D., Farra, R., Schuster, M.E., Teschner, D., Schmidt, T. and Pérez-Ramírez, J. (2012) Performance, Structure, and Mechanism of CeO2 in HCl Oxidation to Cl2. Journal of Catalysis, 286, 287-297. [Google Scholar] [CrossRef