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改性硫化钼催化剂协同低温等离子体转化H2S-CO2酸气制合成气的研究
  • Title

    Combination of modified molybdenum sulfide catalyst and non-thermal plasma for syngas production from H2S-CO2 acid gas

  • 作者

    冯文爽宇文晓萌穆晓亮赵璐房克功

  • Author

    FENG Wenshuang;YUWEN Xiaomeng;MU Xiaoliang;ZHAO Lu;FANG Kegong

  • 单位

    中国科学院山西煤炭化学研究所 煤炭高效低碳利用全国重点实验室中国科学院大学

  • Organization
    State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences
    University of Chinese Academy of Sciences
  • 摘要

    以低温等离子体和催化剂耦合法将H2S和CO2混合酸气一步转化为合成气,既完成了两者清洁化处理,又实现了资源化利用,是一条制备合成气的新路线。本研究采用铜、锌为助剂对硫化钼催化剂改性,显著提升了其催化H2S-CO2制合成气反应性能。结合多种分析表征手段对比两种助剂引入后对硫化钼催化剂结构、组成、形貌、化合价态等物化特征的影响。通过控制低温等离子体放电条件,深入探究了两种助剂对低温等离子体下催化转化H2S和CO2酸气制合成气的反应性能影响规律和关键因素。研究发现,引入铜、锌助剂后,硫化钼活性相粒径减小且分散度高,提供了更多活性位点。同时也增强了对H2S和CO2分子吸附强度,从而更利于H2S和CO2分子的吸附活化,揭示出低温等离子体与改性硫化钼催化剂协同反应的构效关联。有关理论研究丰富拓展了低温等离子体-催化协同理论,并为改性硫化钼材料的合成提供借鉴。

  • Abstract

    The petrochemical, natural gas, and coal chemical industries will produce a large number of hydrogen sulfide (H2S) and carbon dioxide (CO2) mixed acid gas, causing serious damage to the environment and human health. At present, the most widely used treatment technology for H2S-containing mixed acid gas is the Claus process. Nevertheless, the Claus process is unable to achieve the recovery of hydrogen sources and the reduction of CO2 emissions, resulting in a considerable quantity of CO2 being discharged directly into the atmosphere, which has a detrimental impact on the global climate. Carbon, hydrogen, sulfur and other elements play an important role in the field of energy. Therefore, it is of great importance to explore new methods for the utilization of H2S and CO2 mixed acid gas to save energy, protect the environment and achieve green and low-carbon development. A non-thermal plasma-catalysis method is used to convert H2S and CO2 acid gas into syngas in a single step. This method achieves both the clean treatment of waste gas and its resource utilization, making it a novel route for syngas preparation. The non-thermal plasma contains high-energy electrons that can transfer energy to H2S and CO2 molecules in the form of inelastic collisions, thereby exciting them into free radicals, ions, excited molecules and atoms. Concurrently, the catalyst filled in the discharge gap can facilitate the chemical reactions of these active species. However, the stable molecular structure of H2S and CO2 presents a significant challenge to the improvement of energy efficiency, particularly in the context of high conversions of reactive molecule. The development of efficient catalysts is crucial to improve the H2S and CO2 conversion. The existing results demonstrate that electrons, photons and strong electric field generated by non-thermal plasma can be used to excite MoS2 catalyst to generate highly active electron-hole pairs. These in turn catalyze the conversion of H2S and CO2. This study used copper and zinc as promoters to modify the molybdenum sulfide catalyst, and the catalytic performance for the conversion of H2S-CO2 to syngas was effectively improved. A detailed comparison was made between the effects of the two promoters on the structure, composition, morphology, valence state, and other physicochemical characteristics of the molybdenum sulfide catalyst using various characterization methods. Furthermore, the influence factors of two types of promoters on the catalytic H2S-CO2 conversion was investigated by controlling the discharge conditions. The introduction of copper and zinc promoters was found to result in a reduction in the particle size of the molybdenum sulfide active phase, accompanied by a high degree of dispersion, which in turn led to an increase in the number of active sites. Concurrently, the adsorption strength of H2S and CO2 molecules was enhanced, which was conducive to the adsorption and activation of H2S and CO2. It revealed the structure-activity relationship between the modified molybdenum sulfide catalyst and plasma synergistic reaction. In addition, the theoretical research has enriched and expanded the theory of non-thermal plasma-catalysis. It has also provided a reference for the synthesis of modified molybdenum sulfide materials.

  • 关键词

    硫化氢二氧化碳合成气改性MoS2催化剂低温等离子体

  • KeyWords

    hydrogen sulfide;carbon dioxide;syngas;modified MoS2 catalyst;non-thermal plasma

  • 基金项目(Foundation)
    国家自然科学基金(21978313),中国科学院山西煤炭化学研究所创新基金(SCJC-DT-2022-05),煤转化国家重点实验室自主研究课题项目(2020BWZ002)和中国科学院青年创新促进会人才项目(2020181)资助
  • DOI
  • 引用格式
    冯文爽, 宇文晓萌, 穆晓亮, 赵璐, 房克功. 改性硫化钼催化剂协同低温等离子体转化H2S-CO2酸气制合成气的研究[J]. 燃料化学学报(中英文), 2024, 52(10): 1412-1425. DOI: 10.19906/j.cnki.JFCT.2024026
  • Citation
    FENG Wenshuang, YUWEN Xiaomeng, MU Xiaoliang, ZHAO Lu, FANG Kegong. Combination of modified molybdenum sulfide catalyst and non-thermal plasma for syngas production from H2S-CO2 acid gas[J]. Journal of Fuel Chemistry and Technology, 2024, 52(10): 1412-1425. DOI: 10.19906/j.cnki.JFCT.2024026
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  • 图表
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    • 低温等离子体反应系统示意图

    图(12) / 表(1)

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