介质阻挡放电等离子体转化H<sub>2</sub>S-CO<sub>2</sub>酸气制合成气的影响因素研究

余康; 李民; 孙高攀; 周鹏; 谭金浪; 王斌; 王涛; 穆晓亮; 赵璐; 房克功

doi:10.1016/S1872-5813(23)60365-2

介质阻挡放电等离子体转化H₂S-CO₂酸气制合成气的影响因素研究

doi: 10.1016/S1872-5813(23)60365-2

余康^{1, 2,},
李民^3,,
孙高攀^3,,
周鹏^3,,
谭金浪^3,,
王斌^3,,
王涛^3,,
穆晓亮^1,,
赵璐^1, ,,
房克功^1,

1.
中国科学院山西煤炭化学研究所煤转化国家重点实验室, 山西太原 030001
2.
中国科学院大学, 北京 100049
3.
国能包头煤化工有限责任公司, 内蒙古包头 014060

基金项目: 国家自然科学基金（21978313, 21603255），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（2020BWZ002），中国科学院青年创新促进会人才项目(2020181)和国家能源集团科技创新项目（SBCCC-CO-[2021]16）资助

详细信息

通讯作者:
Tel: + 86-0351-4041153, E-mail: zhaolu@sxicc.ac.cn

中图分类号: TQ110.9; X701.7
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- 文章访问数: 151
- HTML全文浏览量: 37
- PDF下载量: 28
- 被引次数: 0
出版历程
- 收稿日期: 2023-03-19
- 修回日期: 2023-04-10
- 录用日期: 2023-04-10
- 网络出版日期: 2023-05-06

The influence factors of dielectric barrier discharge plasma to production of syngas derived from H₂S-CO₂ acid gas

YU Kang^{1, 2
,},
LI Min^3
,,
SUN Gao-pan^3
,,
ZHOU Peng^3
,,
TAN Jin-lang^3
,,
WANG Bin^3
,,
WANG Tao^3
,,
MU Xiao-liang^1
,,
ZHAO Lu^{1
, ,},
FANG Ke-gong^1
,

1.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001 China
2.
University of Chinese Academy of Sciences, Beijing 100049, China
3.
China Energy Baotou Coal Chemical Co., Ltd., Baotou 014060, China

Funds: The project was supported by the National Natural Science Foundation of China (21978313, 21603255), the Innovation Foundation of ICC-CAS (SCJC-DT-2022-05), the Autonomous Research Project of SKLCC (2020BWZ002), the Youth Innovation Promotion Association of CAS (2020181) and the Science and Technology Innovation Project of China Energy Investment Corporation (SBCCC-CO-[2021]16).

摘要

摘要: H₂S和CO₂两种有害酸性废气常共存于煤化工、天然气化工及石油化工等重要化工生产中，造成了工业设备及管线腐蚀，必须就地进行无害化处理。采用介质阻挡放电等离子体催化实现一步转化H₂S-CO₂混合酸气制合成气，将具有强腐蚀性、毒性的H₂S和温室气体CO₂无害化，又产出合成气，完成了以废治废的酸性废气资源化再利用。研究了用于H₂S-CO₂一步转化制合成气的介质阻挡放电等离子体反应各参数对转化反应的影响，进行了不同参数的对比研究，考察并揭示了比能量密度（SEI）、放电结构、放电频率、放电间隙以及放电区域长度等与H₂S-CO₂转化制合成气反应性能的内在关联。在此基础上设计并构建了多管并联介质阻挡放电等离子体反应系统。
- 合成气 /
- 硫化氢 /
- 二氧化碳 /
- 低温等离子体 /
- 废物处理
Abstract: H₂S and CO₂, two harmful acid waste gases, often co-exist in important chemical production such as coal-chemical industry, natural gas chemical industry and petrochemical industry, causing corrosion of industrial equipment and pipelines, and must be treated innocuously. Co-conversion of H₂S‒CO₂ mixed acid gas to syngas has been carried out using dielectric barrier discharge (DBD) plasma-catalysis, which renders the highly corrosive and toxic H₂S and greenhouse gas CO₂ harmless, and produces syngas. The effects of various parameters of the DBD plasma on the reaction of one-step conversion of H₂S‒CO₂ to syngas were studied. Moreover, a comparative study of the different parameters of DBD plasma was carried out. The intrinsic correlation between the reaction performance of syngas production via H₂S-CO₂ conversion and these parameters, including specific energy input (SEI), discharge shape, discharge frequency, discharge gap and discharge length, was investigated and revealed. On this basis, a multi-tube parallel DBD plasma reaction system was designed and constructed.
- syngas /
- hydrogen sulfide /
- carbon dioxide /
- non-thermal plasma /
- waste treatment

HTML全文

图 1 低温等离子体系统示意图

1：质量流量计；2：高压电极；3：等离子体发生器；4：数字示波器；5：油浴；6：等离子体反应器；7：接地极；8：积硫槽；9：冷阱；10：气相色谱分析仪；11：碱液处理

Figure 1 Schematic diagram of non-thermal plasma system

1: mass flow meter; 2: high-voltage electrode; 3: AC power supply; 4: digital oscilloscope; 5: oil bath; 6: non-thermal plasma reactor; 7: grounding electrode; 8: sulphur tank; 9: cold trap; 10: gas chromatograph; 11: lye treatment

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图 2 单、双介质阻挡放电低温等离子体单管反应器中H₂S转化率(a)及CO₂转化率(b)随SEI的变化

Figure 2 H₂S (a) and CO₂ (b) conversions as a function of SEI with single and double dielectric barrier discharge

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图 3 低温等离子体下H₂S-CO₂转化反应网络示意图

Figure 3 Schematic diagram of the reaction network for H₂S-CO₂ conversion under non-thermal plasma

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图 4 单、双介质阻挡放电低温等离子体单管反应器的放电反应照片

Figure 4 Discharge reaction photos of single (a) and double (b) dielectric barrier discharge in non-thermal plasma reactor

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图 5 低温等离子体单管放电反应器在不同放电频率下H₂S转化率(a)及CO₂转化率(b)随SEI的变化

Figure 5 H₂S (a) and CO₂ (b) conversions for various discharge frequencies as a function of SEI

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图 6 不同放电间隙的低温等离子体单管放电反应器中H₂S转化率及CO₂转化率随SEI的变化

Figure 6 H₂S and CO₂ conversions for various discharge gaps as a function of SEI

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图 7 低温等离子体单管放电反应器不同放电区域长度下H₂S转化率(a)及CO₂转化率(b)随SEI的变化

Figure 7 H₂S (a) and CO₂ (b) conversions for various discharge lengths as a function of SEI Feed flow rate: 400 mL/min

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图 8 低温等离子体单管放电反应器不同放电区域长度下H₂S-CO₂转化反应产物分布(a)及合成气H₂/CO比(b)

Figure 8 Gaseous product distributions (a) and H₂/CO ratio (b) for various discharge lengths as a function of SEI in H₂S-CO₂ conversion Feed flow rate: 400 mL/min

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图 9 多管并联低温等离子体放电反应器（三支）在不同SEI下H₂S及CO₂转化率对比

Figure 9 H₂S and CO₂ conversions for multi-tube parallel non-thermal plasma system as a function of SEI Discharge length: 0.90 m; feed flow rate: 600 mL/min

Discharge length: 0.90 m; feed flow rate: 600 mL/min

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