Chemical Industry and Engineering Progress ›› 2023, Vol. 42 ›› Issue (4): 2130-2141.DOI: 10.16085/j.issn.1000-6613.2022-1108

• Resources and environmental engineering • Previous Articles     Next Articles

Effects of tungsten decoration on the performance of a Ni-based oxygen carrier during chemical looping reforming of biogas for hydrogen generation

GONG Chenjun1,2(), MEI Daofeng1,2,3()   

  1. 1.Key Laboratory of Agricultural Equipment in Mid-lower Yangtze River, Ministry of Agriculture and Rural Affairs (Huazhong Agricultural University), Wuhan 430070, Hubei, China
    2.College of Engineering, Huazhong Agricultural University, Wuhan 430070, Hubei, China
    3.Department of Energy Technology, Chalmers University of Technology, Gothenburg 41296, Sweden
  • Received:2022-06-13 Revised:2022-08-22 Online:2023-05-08 Published:2023-04-25
  • Contact: MEI Daofeng

钨修饰对镍载氧体的沼气化学链重整制氢性能影响

龚陈俊1,2(), 梅道锋1,2,3()   

  1. 1.华中农业大学农业农村部长江中下游农业装备重点实验室,湖北 武汉 430070
    2.华中农业大学工学院,湖北 武汉 430070
    3.查尔姆斯理工大学能源技术系,瑞典 哥德堡 41296
  • 通讯作者: 梅道锋
  • 作者简介:龚陈俊(1997—),男,硕士研究生,研究方向为化学链技术。E-mail:gcjifuli@126.com
  • 基金资助:
    国家自然科学基金(51906083);国家重点研发计划(2018YFB0605402)

Abstract:

Biogas, typically containing around 60% CH4 and 40% CO2, can be used as feedstock in chemical looping reforming (CLR) process. In our previous work, a Ni-based oxygen carrier (OC) using high-alumina firebrick as support has shown excellent performance of complete CH4 and CO2 conversion of biogas, thus resulting in high H2 and CO yield in CLR. Nonetheless, that work also found that the presence of H2S in biogas can poison the OC and then leads to decrease of the OC reactivity. Based on some literatures, tungsten is promising of lessening the sulfur poisoning on catalysts. In the present work, tungsten was used to decorate the Ni oxygen carrier and the impregnating sequence of Ni and W in the firebrick was changed to study the effects on the OC performance. An 1000μL/L H2S was mixed with the biogas (the ratio of CH4/CO2 was 3/2) and experiments were carried out in a batch fluidized bed reactor under various reacting conditions. It is found that the W-decoration can lower catalytic activity of the oxygen carrier, and the sequence of Ni and W impregnation can also impact the reforming performance. In the case of no H2S mixing, the OC-Ni-W (first with Ni impregnation, then W impregnation) oxygen carrier has better catalytic performance as compared to OC-Ni=W (Ni, W simultaneous impregnation) and OC-W-Ni (first W then Ni). With the presence of 1000μL/L H2S, the OC-Ni-W has higher CO and H2 yield as compared to OC-W-Ni and OC-Ni=W.

Key words: chemical looping reforming, biogas, Ni-based oxygen carrier, tungsten decoration, hydrogen sulfide

摘要:

沼气中含有约60% CH4和40% CO2,可以作为化学链重整(chemical looping reforming,CLR)的原料。以高铝耐火砖为惰性载体负载Ni作为载氧体(oxygen carrier,OC),在无H2S的条件H2产率和CO产率较高,且沼气中的CH4和CO2能够完全转化。前期的研究显示沼气中含有的少量H2S会对载氧体(OC)活性产生负面影响,导致载氧体失活。根据已有文献,钨元素能够抑制H2S对催化剂的毒化作用。本文以高铝耐火砖为惰性载体,制备了同时含有W和Ni的载氧体、改变Ni和W的浸渍顺序,探究W对化学链重整制氢特性的影响。将1000μL/L H2S和CH4/CO2为3/2的气氛混合来模拟含硫沼气,在批次进料流化床反应器中开展多种工况下的实验。结果显示,经钨修饰后载氧体的催化性能均有一定的降低,而不同的钨修饰顺序对重整性能也具有一定的影响。对于不掺杂H2S的沼气,相对于OC-Ni=W(镍和钨同时负载)和OC-W-Ni(先负载钨后负载镍)而言,OC-Ni-W(先负载镍后负载钨)具有更高的催化性能。在沼气中掺杂1000μL/L H2S后,相对于其他两种载氧体,OC-Ni-W载氧体具有更高的CO产率和H2产率。

关键词: 化学链重整, 沼气, 镍载氧体, 钨修饰, 硫化氢

CLC Number: 

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