介孔氧化硅分子筛负载金属氧化物高温煤气脱硫剂结构调控与脱硫过程放硫的研究进展

扫码查看

原文链接

国家科技期刊平台
NETL
NSTL
万方数据

中文摘要：煤气化是煤炭清洁高效利用的核心技术，但气化粗煤气中所含硫化氢(H2S)会腐蚀设备并污染环境，因此需要对煤气进行净化脱硫。介孔氧化硅分子筛具有大比表面积、大孔容和有序的介孔结构等特性，将其作为金属氧化物的载体可促进金属氧化物的分散，并为脱硫反应提供大量的反应活性位点，减少传质阻力。脱硫剂构效关系是煤气脱硫技术的关键科学难题之一，然而对于负载型高温煤气脱硫剂而言，上述关系受介孔氧化硅分子筛、脱硫活性组分种类、脱硫剂改性手段和脱硫条件等多因素叠加影响，因而要明晰其本质极具挑战。为此，首先探讨了不同介孔氧化硅分子筛的孔道结构特性，剖析了介孔氧化硅分子筛负载活性组分后的脱硫行为差异，发现拥有丰富孔结构及较厚孔壁的载体的脱硫剂在高温脱硫过程中表现更优。同时，分析了近年来针对锌基、锰基和铁基等金属氧化物负载型脱硫剂的结构调控策略及其对脱硫性能的影响规律，认为通过金属掺杂复合改性可提高活性组分脱硫活性;并对脱硫过程中的放硫机制、放硫规律及抑制手段进行了探讨，认为在脱硫剂中引入催化羰基硫(COS)氢解助剂可有效抑制放硫行为。本综述内容可为高性能高温脱硫剂结构设计与功能化构筑提供理论依据。

外文标题：Research progress on structure regulation of high-temperature coal gas desulfurizers loaded with metal oxides on mesoporous silica molecular sieves and sulfur release process during desulfurization

外文摘要：Coal gasification is a core technology for the clean and efficient utilization of coal.However,the hydrogen sulfide(H2S)contained in the gasified crude gas will corrode the equipment and pollute the environment,so it is necessary to purify and desulfurize the gas.Mesoporous silica molecular sieves have the characteristics of large specific surface area,large pore volume,and ordered mesoporous structure.As the carrier of the metal oxide,it can promote the dispersion of the metal oxide,provide a large number of reaction active sites for the desulfurization reaction,and reduce mass transfer resistance.The structure-activity relationship of desulfurizer is one of the key scientific problems in gas desulfurization technology.However,for supported high-temperature coal gas desulfurizer,this relationship is superimposed and influenced by multiple factors such as mesoporous silica zeolite,types of desulfurization active components,modification methods of desulfurizers,and desulfurization conditions,so it is extremely challenging to clarify its essence.Firstly,the pore structure characteristics of different mesoporous silica molecular sieves were discussed,and the desulfurization behavior differences of mesoporous silica molecular sieves loaded with active components were analyzed.It is found that desulfurizers with a carrier possessing abundant pore structure and thicker pore walls exhibit better performance in high-temperature desulfurization processes.The structural control strategies of metal oxide supported desulfurizers based on zinc,manganese and iron in recent years and their effects on desulfurization performance were analyzed.It is evident that the desulfurization activity of the active components can be enhanced by metal doping.The sulfur release mechanism,sulfur release pattern and suppression means in the desulfurization process were discussed.The introduction of catalytic carbonyl sulfur(COS)hydrogenolysis agent in the desulfurizer can effectively inhibit the sulfur emission behavior.The review can provide a theoretical basis for the structural design and functional construction of high-performance and high-temperature desulfurizers.

外文关键词：

high-temperature coal gasdesulfurizationmesoporous silica molecular sievesmetal oxidessulfur releasecarbonyl sulfide

作者：

刘佳雯、段新伟、武蒙蒙、米杰、王建成

展开 >

作者单位：

太原理工大学省部共建煤基能源清洁高效利用国家重点实验室,煤科学与技术教育部重点实验室,山西太原 030024

太原理工大学环境科学与工程学院,山西太原 030060

关键词：

高温煤气脱硫介孔氧化硅分子筛金属氧化物放硫羰基硫

基金：

国家自然科学基金国家自然科学基金山西省自然科学基金山西省科技创新人才团队项目山西省环境催化材料技术创新中心项目

项目编号：

222782942197818820210302123191202204051002025202104010911008

出版年：

2024

DOI：

10.12434/j.issn.2097-2547.20230369

天然气化工—C1化学与化工

西南化工研究设计院有限公司全国天然气化工与碳一化工信息中心

天然气化工—C1化学与化工

CSTPCD北大核心

影响因子：0.814

ISSN：1001-9219

年,卷(期)：2024.49(6)