锆基金属-有机骨架呼吸道防护材料研究进展

doi:10.11896/cldb.19090073

材料导报

2020, Vol. 34

Issue (23): 23121-23130 https://doi.org/10.11896/cldb.19090073

金属与金属基复合材料

锆基金属-有机骨架呼吸道防护材料研究进展

王馨博¹, 苏茹月¹, 栗丽^1,2, 梁国杰^1,2, 赵越¹, 栾志强^1,2, 李凯¹, 习海玲^1,2

1 防化研究院,北京 100191
2 国民核生化灾害防护国家重点实验室,北京 102205

Research Progress on Zirconium-based Metal-organic Frameworks Respiratory Protection Materials

WANG Xinbo¹, SU Ruyue¹, LI Li^1,2, LIANG Guojie^1,2, ZHAO Yue¹, LUAN Zhiqiang^1,2, LI Kai¹, XI Hailing^1,2

1 Research Institute of Chemical Defense, Beijing 100191, China
2 State Key Laboratory of NBC Protection for Civilian, Beijing 102205, China

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摘要在执行作战、应急救援及事故处理等任务的过程中,经典化学战剂(Chemical warfare agents,CWAs)和有毒工业化学品(Toxic industrial chemicals,TICs)扩散均会对人员呼吸安全造成严重威胁,从而要求防毒面具必须能够同时对CWAs和TICs提供广谱有效的防护。目前,国内外过滤式防毒面具主要使用ASZM-TEDA型浸渍活性炭作为防护材料,该材料对TICs防护性能较差,且表面物理吸附的有毒物质分子室温下易发生解吸。因此,需要设计开发新型呼吸道防护材料,在对CWAs和TICs进行广谱防护的同时,实现有毒物质的原位降解。
金属-有机骨架(Metal-organic frameworks,MOFs)材料比表面积高、结构多样,其模块化的构筑方式使人们可以灵活地对MOFs性质进行按需设计,因而被认为是最有潜力实现有毒物质广谱防护和原位消毒的新型呼吸道防护材料。其中,锆基金属-有机骨架(Zr-MOFs)材料具有丰富的表面活性中心与良好的稳定性,并表现出优异的CWAs和TICs吸附与催化降解性能,近年来受到各国研究者的关注。
就用于CWAs和TICs吸附消除的Zr-MOFs材料而言,目前的研究工作主要集中于UiO-66-NH₂体系。研究人员分别对其粉体和成型颗粒的吸附性能进行了系统研究,发现UiO-66-NH₂粉体对NH₃、Cl₂和NO₂等多种TICs具有优异的本征吸附能力,并进一步探索通过构筑等级孔隙结构改善有毒物质分子在UiO-66-NH₂成型颗粒孔道内的扩散性质。针对用于CWAs和TICs催化降解的Zr-MOFs材料,目前的研究工作主要围绕具有不同节点连接数的一系列Zr-MOFs展开。研究人员通过优化孔径尺寸、节点连接数以及有机配体种类,实现了对Zr-MOFs有毒物质催化降解性能的有效调控,并拓展研究了Zr-MOFs在多相缓冲介质及纯液体环境中对有毒物质的催化降解能力,以推进其作为防护材料的实际应用。
本文围绕Zr-MOFs呼吸道防护材料,在分析其结构与表面酸碱性质特点的基础上,综述了Zr-MOFs材料在有毒物质吸附与催化降解方面的研究进展,探讨了Zr-MOFs结构与其性能间的构效关系,并展望了未来研究工作的重点方向。

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	王馨博
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	李凯
	习海玲

关键词: 锆金属-有机骨架化学战剂有毒工业化学品呼吸道防护吸附催化降解

Abstract: During the process of combat, emergency rescue and accident handling, both chemical warfare agents (CWAs) and toxic industrial chemicals (TICs) diffusion will pose a serious threat to the breathing safety of personnel. Therefore, the respirators are required to provide broad-spectrum protection against CWAs and TICs at the same time. The activated carbon impregnated with copper, silver, zinc, molybdenum, and triethy-lenediamine, known as the ASZM-TEDA carbon, is the main protection material used in current gas masks for military and emergency response personnel. Although a variety of chemicals are added, the ASZM-TEDA carbon still has some limitations such as poor protection performance against TICs and a high risk of physically adsorbed toxic molecules releasing at room temperature. It is thus urgent to develop novel respiratory protection materials with broad-spectrum protection and in-situ degradation capabilities against both CWAs and TICs.
Metal-organic frameworks (MOFs), characterized by their huge specific surface areas, diverse structures and on-demand modular design, are considered as the novel respiratory protection materials with the greatest potential to achieve broad-spectrum protection and in-situ degradation against toxic chemicals. In recent years, the zirconium-based metal-organic frameworks (Zr-MOFs) have been extensively studied due to their high specific surface areas, various surface active sites, remarkable stabilities, as well as excellent CWAs/TICs adsorption and catalytic degradation performance.
In terms of Zr-MOFs used for the adsorption removal of CWAs and TICs, current research work mainly focuses on UiO-66-NH₂. Researchers have systematically studied the adsorption properties of UiO-66-NH₂ powders and granules. They found that UiO-66-NH₂ powders shows excellent intrinsic adsorption capacities for many TICs, such as NH₃, Cl₂, and NO₂. The hierarchical structure was further developed in UiO-66-NH₂ to increase the diffusion rates of toxic molecules through the pores of UiO-66-NH₂ granules. In terms of Zr-MOFs used for the catalytic degradation of CWAs and TICs, current research work mainly focuses on a series of Zr-MOFs with different node connectivity. By optimizing the pore size, node connectivity and types of organic ligands, researchers have effectively regulated the catalytic degradation performance of Zr-MOFs against toxic chemicals. They further investigated the catalytic degradation behavior of toxic chemicals in heterogeneous buffer and pure liquid environment, so as to promote the practical application of Zr-MOFs as protection materials.
This review focuses on the Zr-MOFs respiratory protection materials. Based on analysis of the structures and surface chemistry of Zr-MOFs, this paper summarized the research progress on the application of Zr-MOFs in toxic chemicals adsorption and degradation. The structure-activity relationship of Zr-MOFs respiratory protection materials was discussed and the future research trend was also prospected.

Key words: zirconium metal-organic frameworks chemical warfare agents toxic industrial chemicals respiratory protection adsorption catalytic degradation

出版日期: 2020-12-10 发布日期: 2020-12-24

ZTFLH:	TB34
	TJ92

基金资助: 国家重点研发计划项目(2016YFC0204205);国家自然科学基金(21876204);国民核生化灾害防护国家重点实验室基金(SKLNBC2018-04)

通讯作者: 750455@sohu.com; fhxhl@163.com

作者简介: 王馨博,2015年6月本科毕业于中国科学技术大学化学系,2018年6月于军事科学院防化研究院环境工程专业取得硕士学位。现为军事科学院防化研究院博士研究生,在习海玲研究员和李凯副研究员的指导下进行研究。目前主要研究方向为金属-有机骨架呼吸道防护材料。
李凯,军事科学院防化研究院副研究员、硕士研究生导师。核生化防护材料与技术、特种多孔材料专家,长期从事活性炭、碳泡沫、分子筛、气凝胶、金属-有机骨架等微纳多孔材料的研究和应用技术开发工作。先后主持或参加国家重点研发计划、军队重点科研项目等20余项,获军队科技进步二等奖1项、三等奖3项,发表论文40余篇,授权国家或国防发明专利10余项。
习海玲,军事科学院防化研究院研究员、博士研究生导师,享受国务院政府特殊津贴,现任国民核生化灾害防护国家重点实验室主任。长期从事核生化防护材料与技术、军事环境科学与工程技术研究,先后主持或参加国家重点研发计划、国家自然科学基金、军队重点科研项目等30余项,获国家科技进步二等奖1项、军队科技进步一等奖3项、二等奖9项,发表SCI论文30余篇,授权国家或国防发明专利27项。

引用本文:

王馨博, 苏茹月, 栗丽, 梁国杰, 赵越, 栾志强, 李凯, 习海玲. 锆基金属-有机骨架呼吸道防护材料研究进展[J]. 材料导报, 2020, 34(23): 23121-23130.
WANG Xinbo, SU Ruyue, LI Li, LIANG Guojie, ZHAO Yue, LUAN Zhiqiang, LI Kai, XI Hailing. Research Progress on Zirconium-based Metal-organic Frameworks Respiratory Protection Materials. Materials Reports, 2020, 34(23): 23121-23130.

链接本文:

http://www.mater-rep.com/CN/10.11896/cldb.19090073 或 http://www.mater-rep.com/CN/Y2020/V34/I23/23121

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