天然气藏中酸气H2S与CO2协同转化研究进展

doi:10.16085/j.issn.1000-6613.2023-0180

摘要/Abstract

摘要：

为保障国家能源安全，减少我国对国外油气资源的依存度，必须加大对国内天然气等资源的开发。在天然气的开采净化过程中，往往会产生酸气H₂S与CO₂等。现有酸气处理技术主要通过克劳斯工艺回收得到H₂S中的硫黄，并未对CO₂进行处理，造成了氢资源的浪费和严重的碳排放。如果能将H₂S与CO₂协同转化，则有望在减少碳排放的同时得到氢气、合成气和硫黄高值化学品。本文基于国内外30多年相关领域的实验研究和理论模拟，总结阐述了H₂S与CO₂协同转化的发展历史，并分别从热反应（直接热反应、工艺流程和经济性评估、催化热分解）、光催化、电催化和等离子体催化角度详细综述了H₂S与CO₂协同转化的研究进展。从催化剂、反应条件和反应产物分布等方面展开了细致的分析，对比了各种技术的优缺点。展望了H₂S与CO₂协同转化的发展趋势，近期可考虑使用绿电进行电催化技术的小规模应用示范；同时可以考虑通过太阳光储热的方式减小热催化技术的碳排放，或通过太阳能聚光等方式提升光催化技术的催化效率等。此外，在后续研究中，必须结合酸性气藏的特点，考虑不同的H₂S/CO₂比例或是H₂O等杂质分子对反应过程的影响。

关键词: 催化, 硫化氢, 二氧化碳, 化学反应, 活性

Abstract:

In order to ensure national energy security and reduce our dependence on foreign oil and gas resources, it is necessary to enhance the exploration of domestic natural gas and other resources. During the exploitation and purification of natural gas, acid gas H₂S and CO₂ are often produced. Existing acid gas treatment technologies mainly recover the sulfur in H₂S through the Claus process, which leaves CO₂ untreated and results in the waste of hydrogen and serious carbon emissions. If H₂S and CO₂ can be synergistically converted, it is expected to reduce carbon emissions and obtain high-value chemicals such as hydrogen, syngas and sulfur simultaneously. Based on the experimental and theoretical researches of more than 30 years in related fields worldwide, this paper reviews the development history of synergistic conversion of H₂S and CO₂, and summarizes the relevant research progress from the perspectives of thermal reaction (direct thermal reaction, process flow and economic evaluation, catalytic thermal decomposition), photocatalysis, electrocatalysis and plasma catalysis. Detailed information on catalysts, reaction conditions and distribution of reaction products is presented, and the advantages and disadvantages of various technologies are compared. The development trend of the synergistic conversion of H₂S and CO₂ is prospected and the use of green electricity for small-scale application of electrocatalysis technology in the near future is suggested. At the same time, it is feasible to reduce the carbon emission of thermal catalytic technology through solar heat storage and improve the photocatalytic efficiency through concentration of solar energy. In addition, it is necessary to consider the characteristics of acid gas reservoirs in future studies, including the influence of different H₂S/CO₂ ratios and impurities such as H₂O on the reaction process.

Key words: catalysis, hydrogen sulfide, carbon dioxide, chemical reaction, reactivity

中图分类号:

TE99

于姗, 张洪华, 付梦瑶, 段元刚, 段超, 黄靖元, 唐春, 黄泽皑, 周莹. 天然气藏中酸气H₂S与CO₂协同转化研究进展[J]. 化工进展, 2023, 42(12): 6507-6517.

YU Shan, ZHANG Honghua, FU Mengyao, DUAN Yuangang, DUAN Chao, HUANG Jingyuan, TANG Chun, HUANG Ze’ai, ZHOU Ying. Research progress on synergistic conversion of acid gas H₂S and CO₂ in natural gas[J]. Chemical Industry and Engineering Progress, 2023, 42(12): 6507-6517.

图/表 8

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反应体系	CO₂转化率 /%	H₂S转化率 /%	CO选择性 /%	S₂选择性 /%	H₂选择性 /%
热力学平衡值	26.5	33.9	69.7	76.1	21.5
空白实验	1.7	2.2	15.1	18.2	1.4
SiO₂	4.6	4.8	42.7	42.8	4.0
CaO	26.0	26.4	53.9	57.4	14.6
γ-Al₂O₃	24.3	24.8	51.1	56.6	14.5
NiO/γ-Al₂O₃	24.8	27.6	52.7	56.7	22.1
NiO/MgO	25.6	27.9	53.3	58.1	16.6
MgO	25.2	25.4	50.2	51.5	8.2

反应体系	CO₂转化率 /%	H₂S转化率 /%	CO选择性 /%	S₂选择性 /%	H₂选择性 /%
热力学平衡值	26.5	33.9	69.7	76.1	21.5
空白实验	1.7	2.2	15.1	18.2	1.4
SiO₂	4.6	4.8	42.7	42.8	4.0
CaO	26.0	26.4	53.9	57.4	14.6
γ-Al₂O₃	24.3	24.8	51.1	56.6	14.5
NiO/γ-Al₂O₃	24.8	27.6	52.7	56.7	22.1
NiO/MgO	25.6	27.9	53.3	58.1	16.6
MgO	25.2	25.4	50.2	51.5	8.2

催化剂	反应产物生成速率（以催化剂面积计）/mmol·m^-2
催化剂	H₂	CO	SO₂	S₂
FeS	0.889	0.027	0.025	0.252
RuO₂	0.009	0.001	0.007	0.003
MoS₂	0.014	0.070	0.004	0.014
Nb₂O₅	0.011	0.093	0.028	0.074
IrO₂	0.027	0.003	0.001	0.012
V₂O₅	0.141	0.210	0.013	0.730
CdS	0.005	0.017	0.001	0.017
PbS	0.037	0.054	0.023	0.001
Mn₃O₄	0.038	0.065	0.011	0.199
CoS	0.217	0.143	0.069	0.001
NiS	1.502	0.285	0.051	0.001
WS₂	0.032	0.019	0.005	0.001

催化剂	反应产物生成速率（以催化剂面积计）/mmol·m^-2
催化剂	H₂	CO	SO₂	S₂
FeS	0.889	0.027	0.025	0.252
RuO₂	0.009	0.001	0.007	0.003
MoS₂	0.014	0.070	0.004	0.014
Nb₂O₅	0.011	0.093	0.028	0.074
IrO₂	0.027	0.003	0.001	0.012
V₂O₅	0.141	0.210	0.013	0.730
CdS	0.005	0.017	0.001	0.017
PbS	0.037	0.054	0.023	0.001
Mn₃O₄	0.038	0.065	0.011	0.199
CoS	0.217	0.143	0.069	0.001
NiS	1.502	0.285	0.051	0.001
WS₂	0.032	0.019	0.005	0.001

反应体系	产率/µmol·g^-1·h^-1
	气相产物			液相产物
	CH₄	CO	H₂	HCOOH
纯水溶液无CO₂	—	—	—	—
纯水溶液	0.3	0.3	0.6	—
NaOH（100mmol/L）	—	0.3	—	—
NaCl（500mmol/L）	—	0.8	1.8	—
NaBr（500mmol/L）	—	0.5	0.7	—
Na₂S（100mmol/L）	—	2.8	209.4	25.7

天然气藏中酸气H₂S与CO₂协同转化研究进展

Research progress on synergistic conversion of acid gas H₂S and CO₂ in natural gas

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处理工艺	碳税/每吨CO₂
处理工艺	0	10	25	50	100
MDEA + LO-CAT	0.00948	0.0124	0.0168	0.0242	0.0389
双塔络合法脱硫	0.01103	0.0140	0.0184	0.0258	0.0405
干法脱硫	0.06636	0.0693	0.0737	0.0811	0.0958
电催化系统（50mA/cm²，商用电）	0.01123	0.01123	0.01123	0.01123	0.01123
电催化系统（50mA/cm²，绿电）	-0.02285	-0.02285	-0.02285	-0.02285	-0.02285

处理工艺	优势	劣势
直接热转化技术	经济性评估体系完善，工艺改造成本低	能耗高
热催化技术	处理量大，工艺改造成本低	能耗较高，反应过程认识不明确
光催化技术	能量来源广，绿色无污染	转化效率低，产物复杂，机理研究不充分
电催化技术	反应条件温和，活性高	电极材料成本高，工艺开发不够完善，机理研究不充分
等离子体催化技术	操作简单，装置体积小，能量效率高	湿度、反应气体纯度影响大、能耗较高

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