不同金属负载下Al_(2)O_(3)光热催化H_(2)S裂解制氢性能  

Decomposition of H_(2)S for hydrogen production by photothermal catalysis of Al_(2)O_(3) loaded with different metals

作　　者：于姗[1,2] 汪福深 黄靖元 段元刚 付梦瑶 贺桢 周莹[1,2] YU Shan;WANG Fushen;HUANG Jingyuan;DUAN Yuangang;FU Mengyao;HE Zhen;ZHOU Ying(State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation//Southwest Petroleum University,Chengdu,Sichuan 610500,China;School of New Energy and Materials,Southwest Petroleum University,Chengdu,Sichuan 610500,China)

机构地区：[1]油气藏地质及开发工程全国重点实验室·西南石油大学,四川省成都市610500 [2]西南石油大学新能源与材料学院,四川省成都市610500

出　　处：《天然气工业》2025年第2期189-198,共10页Natural Gas Industry

基　　金：国家自然科学基金项目“酸性气藏清洁开发利用”(编号:52325401)、“光解硫化氢制氢活性增强机制及氧化产物资源化利用研究”(编号:22178291);国家自然科学基金项目及成都市国家科技计划项目配套资助项目“无镉量子点用于光催化CO_(2)和H_(2)S协同转化的研究”(编号:22211530070、2023-YF06-0007-HZ);四川省自然科学基金面上项目“太阳能驱动高含硫气藏伴生气高值转化制氢及硫/碳化学品研究”(编号:2024NSFSC0277)。

摘　　要：H_(2)S直接裂解制氢是一种极具前景的H_(2)S处理技术,但现阶段的研究方法大多处于实验室研究阶段,找到一种反应条件温和、能耗低、转化率高的方法是该领域的重点研究方向之一。为此,探索了光热催化H_(2)S裂解制氢的方法,将不同金属Ni、Mo、Co负载到Al_(2)O_(3)上进行光热催化H_(2)S裂解制氢实验,并对比了不同金属负载下Al_(2)O_(3)的活性差异,再通过红外成像测温、X射线衍射、比表面积、紫外可见漫反射光谱、X射线光电子能谱等分析方法与技术对催化剂进行了系统表征分析。研究结果表明:①Ni、Mo、Co的负载显著提升了催化剂的催化活性,其中Mo/Al_(2)O_(3)催化剂表现出相对较好的活性,相同光照(2.85 W/cm^(2))下其H_(2)S转化率高达13.8%,H_(2)产率高达208.5±6.5μmol/(g·h);②Mo的引入提升了催化剂的光热效应,使其在相同光强下表面温度最高,同时Mo减少了表面SO_(4)^(2-)的积累,暴露出更多的活性位点,使得钼硫化物在裂解反应中表现出显著的制氢优势。结论认为:①较之于传统的热催化H_(2)S裂解制氢方法,光热催化H_(2)S裂解制氢具有更好的催化活性;②同等条件下,Mo负载下Al_(2)O_(3)的H_(2)S转化率提高了1.6倍,H_(2)产率提高了2.1倍,认识为H_(2)S裂解制氢方法提供了新的思路和技术参考。Direct decomposition of H_(2)S to produce H_(2) is currently one of the most promising H_(2)S treatment technologies,but existing research methods are mostly in the stage of experimental study.Therefore,one of the main research directions in this field is to find a method with mild reaction conditions,low energy consumption,and high conversion rate.To this end,this paper explores a method of photothermal catalytic H_(2)S decomposition for hydrogen production.Experiments are conducted on photothermal catalytic H_(2)S decomposition for hydrogen production by loading different metals(Ni,Mo,Co)onto Al_(2)O_(3),and the activity differences of Al_(2)O_(3) loaded with different metals are compared.In addition,the catalysts are characterized and analyzed systematically by means of infrared imaging thermometry,X-ray diffraction,specific surface area,UV-visible diffuse reflectance spectroscopy,and X-ray photoelectron spectroscopy analysis methods and technologies.The following results are obtained.First,the loading of Ni,Mo,and Co significantly improves the catalytic activity of the catalyst,among which Mo/Al_(2)O_(3) catalyst shows a relatively good activity,with H_(2)S conversion rate up to 13.8% and H_(2) yield up to 208.5±6.5μmol/(g·h)under the same light intensity(2.85 W/cm^(2)).Second,the introduction of Mo enhances the photothermal effect of the catalyst,maximizing the surface temperature under the same light intensity.And it also reduces the accumulation of SO_(4)^(2-)on the surface,exposing more active sites,so that molybdenum sulfide exhibits remarkable advantages in hydrogen production in the reaction.In conclusion,photothermal catalytic H_(2)S decomposition for hydrogen production has a better catalytic activity than the traditional thermal catalytic H_(2)S decomposition for hydrogen production.What's more,under the same condition,the H_(2)S conversion rate and H_(2) yield of Al_(2)O_(3) loaded with Mo increase by 1.6 times and 2.1 times,respectively.The research results can provide new ideas and technical r

关 键 词：天然气 硫化氢 氢气 裂解制氢 氧化铝 钼硫化物 光热催化 硫酸根 

分 类 号：TQ125.12[化学工程—无机化工]