The influence factors of dielectric barrier discharge plasma to production of syngas derived from H2S-CO2 acid gas
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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。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.
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Key words:
- syngas /
- hydrogen sulfide /
- carbon dioxide /
- non-thermal plasma /
- waste treatment
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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
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
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
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
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
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
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
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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