Chemical Industry and Engineering Progress ›› 2023, Vol. 42 ›› Issue (2): 783-793.DOI: 10.16085/j.issn.1000-6613.2022-0630

• Industrial catalysis • Previous Articles     Next Articles

Effects of constant carbon atmosphere on the activity, selectivity and coking of catalysts in hydrodesulfurization of coke oven gas

LI Naizhen1(), SUN Ruijie1, QIN Zhifeng1,2,3(), MIAO Maoqian1, WU Qiongxiao4, CHANG Liping1, SUN Pengcheng2, ZENG Jian2, LIU Yi3   

  1. 1.Provincial and Ministry Jointly Build the State Key Laboratory of Clean and Efficient Utilization of Coal-based Energy, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
    2.Postdoctoral Research Station, Environmental Planning Institute of Shanxi Province, Taiyuan 030002, Shanxi, China
    3.Environmental Science and Engineering Postdoctoral Mobile Station, Tsinghua University, Beijing 100084, China
    4.Daosheng Xinyu Clean Energy Company Limited, Xinzhou 036300, Shanxi, China
  • Received:2022-04-12 Revised:2022-06-19 Online:2023-03-13 Published:2023-02-25
  • Contact: QIN Zhifeng

焦炉煤气常量含碳气氛对加氢脱硫催化剂活性、选择性和积炭的影响

李乃珍1(), 孙瑞洁1, 秦志峰1,2,3(), 苗茂谦1, 吴琼笑4, 常丽萍1, 孙鹏程2, 曾剑2, 刘毅3   

  1. 1.太原理工大学省部共建煤基能源清洁高效利用国家重点实验室,山西 太原 030024
    2.山西省环境规划院 博士后科研工作站,山西 太原 030002
    3.清华大学环境科学与工程博士后流动站,北京 100084
    4.山西道生鑫宇清洁能源有限公司,山西 忻州 036300
  • 通讯作者: 秦志峰
  • 作者简介:李乃珍(1995—),女,硕士研究生,研究方向为气体净化与工业催化。E-mail:lnzlldmmmmd@163.com
  • 基金资助:
    2016年度山西省科技重大专项(MJH2016-03);东莞市能源投资集团有限公司攻关项目(RH2000004464)

Abstract:

Hydrodesulfurization (HDS) evaluation of the industrial Fe-Mo catalyst was carried out by using a micro fixed bed reactor. The influence of constant carbon components (CH4、C2H4、C2H6、CO、CO2) in coke oven gas on the hydrogenation activity, selectivity and carbon deposition were studied. The catalyst was characterized by infrared carbon sulfur analyzer, N2 adsorption desorption, Raman and TPRS-MS. The results showed that the order of COS, CS2 and C4H4S hydrogenation conversion from easy to difficult was COS>CS2>C4H4S under the carbon-free atmosphere, but the hydroconversion of COS was obviously affected by the carbonaceous atmosphere, which made it difficult to completely remove COSs. The atmosphere also had an impact on the hydrogenation selectivity of sulfide, among which C2H4 had the most obvious effect, while CO2 and CO had the most obvious effect on the yield of H2S. After 11h stable reaction at 410℃ in different carbonaceous atmospheres, carbon deposition took place on the catalyst, mainly as graphitized carbon, and carbon deposition was the most serious in C2H4 atmosphere. The influence order of atmosphere on carbon deposition was C2H4>CO2>CO>CH4>N2>C2H6.

Key words: coke oven gas, carbonaceous atmosphere, hydrodesulfurization, reactivity, selectivity, carbon deposition, deactivation

摘要:

利用微型固定床反应装置对工业Fe-Mo预加氢脱硫催化剂进行加氢脱硫(HDS)评价,研究焦炉煤气中不同常量含碳原料组分(CH4、C2H4、C2H6、CO、CO2)对催化剂加氢活性、选择性以及积炭的影响,并采用红外碳硫分析仪、N2吸附-脱附、Raman以及TPRS-MS对催化剂进行表征。结果表明:在N2气氛下,COS、CS2和C4H4S加氢转化由易到难顺序为:COS>CS2>C4H4S,但COS加氢转化受含碳气氛影响最明显,致使焦炉煤气加氢脱硫中COS难以完全脱除;不同气氛对硫化物加氢选择性都会产生影响,其中C2H4气氛对选择性影响最明显,而对H2S收率影响最明显的是CO2和CO;不同含碳气氛在410℃下稳定反应11h后催化剂均发生积炭,主要以石墨化炭为主,其中C2H4气氛下积炭最严重,气氛对积炭影响顺序为:C2H4>CO2>CO>CH4 >N2>C2H6

关键词: 焦炉煤气, 含碳气氛, 加氢脱硫, 活性, 选择性, 积炭, 失活

CLC Number: 

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