用于卤素捕获的材料研究进展

doi:10.6023/A23080392

化学学报 ›› 2024, Vol. 82 ›› Issue (1): 62-74.DOI: 10.6023/A23080392 上一篇下一篇

综述

用于卤素捕获的材料研究进展

林航青^a, 马若茹^a, 江怡蓝^a, 许木榕^a, 林洋彭^a^,^b^,^*(), 杜克钊^a^,^*()

^a福建师范大学化学与材料学院福建福州 350117
^b厦门市环境科学研究院福建厦门 361021

投稿日期:2023-08-27 发布日期:2023-10-31

作者简介:

林航青, 就读于福建师范大学化学与材料学院, 2020级应用化学专业本科生.

马若茹, 就读于福建师范大学化学与材料学院, 2020级应用化学专业本科生.

江怡蓝, 就读于福建师范大学化学与材料学院, 2020级应用化学专业本科生.

许木榕, 就读于福建师范大学化学与材料学院, 2022级化学教育专业本科生.

林洋彭(1995-), 2023年6月于福建师范大学获得理学博士学位, 同年10月入职厦门市环境科学研究院, 主要研究方向为金属卤化物的设计及应用研究. 至今以第一作者身份在J. Phys. Chem. Lett., Chem. Eng. J., Energy Environ. Mater.等期刊发表6篇SCI论文, 以合作者身份在Angew. Chem. Int. Ed., Nano Lett., Adv. Funct. Mater.等期刊发表15篇SCI论文, 授权中国发明专利两项.

杜克钊, 2013年博士毕业于中国科学院大学福建物质结构研究所, 相继在新加坡南洋理工大学和美国杜克大学开展博士后研究, 于2018年入职福建师范大学, 主要研究金属卤化物晶态材料的构效关系, 已在J. Am. Chem. Soc., Angew. Chem. Int. Ed.等国际期刊上发表SCI论文90篇左右, 授权专利3项, h-index 29. 主持(含结题)国家基金三项, 获“闽江学者”特聘教授和福建省杰青项目等省部级项目资助.

基金资助:
项目受国家自然科学基金(22373014); 福建省自然科学基金(2022J06019)

Research Progress of Materials Used for Elemental Halogen Capture

Hangqing Lin^a, Ruoru Ma^a, Yilan Jiang^a, Murong Xu^a, Yangpeng Lin^a^,^b(), Kezhao Du^a()

^aCollege of Chemistry and Materials, Fujian Normal University, Fuzhou, Fujian 350117
^bXiamen Institute of Environmental Science, Xiamen, Fujian 361021

Received:2023-08-27 Published:2023-10-31
Contact: * E-mail: lyp.fjnu@outlook.com; duke@fjnu.edu.cn
About author:
^†These authors contributed equally to this work
Supported by:
National Natural Science Foundation of China(22373014); Natural Science Foundation of Fujian Province(2022J06019)

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摘要/Abstract

卤素单质氟(F₂)、氯(Cl₂)、溴(Br₂)和碘(I₂), 在化学工业中发挥重要作用. 但是由于F₂、Cl₂和Br₂的毒性、腐蚀性和挥发性使得它们的安全储存和运输形成了严峻的挑战, 而将这些卤素单质进行吸附预固化可以有效提高它们使用的安全性. 理想的卤素单质预固化材料须满足多种性能要求, 如对卤素单质的稳定性、选择性、吸脱附可逆性和可加工性等, 这给预固化材料的设计和合成带来了很大的挑战. 目前为止, Cl₂和Br₂的预固化材料已经有不少报道(F₂暂时还未有), 对这类材料进行总结和回顾, 有助于为后续的材料优化和设计提供参考. 然而, 截至本文撰写之前, 还未有人对Cl₂和Br₂预固化材料的研究做过综述报道. 因此, 通过本文综述了多孔有机聚合物(POPs)、金属有机框架(MOFs)、多孔有机笼(POCs)以及金属卤化物等在Cl₂和Br₂吸附预固化上的研究现状, 从材料结构和性能的角度详细讨论了不同材料在卤素单质预固化上的机理和构效关系, 旨在为卤素单质预固化材料的后续研究提供有益的借鉴, 最终开发出有实际应用前景的卤素单质预固化材料, 从而提高卤素单质实际应用的安全性, 降低卤素单质泄露的风险, 对环境保护和实现相关工业的可持续发展具有重要意义.

关键词: 卤素单质, 吸附, 多孔材料, 金属卤化物, 氧化还原

Elemental halogen, that is fluorine (F₂), chlorine (Cl₂), bromine (Br₂) and iodine (I₂), plays an important role in the chemical industry. However, the toxicity, corrosiveness and volatility of elemental halogen pose serious challenges for their safe storage and transportation. Thus, the precuring of these elemental halogen can effectively improve the safety of their usage. Ideal precuring materials for elemental halogen need to meet a variety of requirements, such as stability, selectivity, recyclability, processability, etc., which brings great challenges to the design and synthesis of desired materials. So far, some precuring materials for Cl₂ and Br₂ have been reported (F₂ is not available yet). The summary and review of these materials will help to provide reference for the follow-up materials optimization and design. However, as far as we know, the related review has not been reported yet. Therefore, we give a comprehensive overview of the precuring materials for Cl₂ and Br₂ including porous organic polymers (POPs), metal-organic frameworks (MOFs), porous organic cages (POCs) and metal halides. The corresponding mechanism and structure-property relationship are discussed in detail. The purpose of this paper is to provide a useful insight into the follow-up materials design for the elemental halogen precuring, and finally get an ideal precuring materials with practical application prospects, so as to improve the usage safety of elemental halogen and reduce the risk of halogen leakage. It is of great significance to environmental protection and sustainable development.

Key words: halogen, adsorption, porous materials, metal halide, redox

引用此文

林航青, 马若茹, 江怡蓝, 许木榕, 林洋彭, 杜克钊. 用于卤素捕获的材料研究进展[J]. 化学学报, 2024, 82(1): 62-74.

Hangqing Lin, Ruoru Ma, Yilan Jiang, Murong Xu, Yangpeng Lin, Kezhao Du. Research Progress of Materials Used for Elemental Halogen Capture[J]. Acta Chimica Sinica, 2024, 82(1): 62-74.

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图/表 11

图1. F2、Cl2、Br2和I2的年产量和使用量

Figure 1. Yearly production and use of the halogens fluorine, chlorine, bromine, and iodine[1????-6]

吸附单质	材料类别	材料名称	分解温度/℃	释放卤素温度/℃	最大捕获量/ (g•g^-1)	释放效率/%	储存方式	参考文献
Cl₂	MOF	Co₂Cl₂X₂BTDD	400	275	0.140^a	≈80	化学储存	[30]
	MHP	Cs₂PbCl₆	300	300	0.111^a	≈100	化学储存	[33]
	MHP	Rb₂PbCl₆	350	350	0.136^a	≈100	化学储存	[33]
	MHP	(NH₄)₂PbCl₆	320	320	0.190^a	≈100	化学储存	[33]
	MHP	Cs₄Sb₂Cl₁₂	240	240	0.0627^a	≈100	化学储存	[33]
Br₂	MOF	Co₂Cl₂X₂BTDD	400	195	0.260^a	≈80	化学储存	[30]
	FMOF	PCN-605-H	N.A.^b	室温	4.2	≈20	物理储存	[35]
	FMOF	PCN606-OMe	N.A.	室温	3.7	≈20	物理储存	[35]
	FMOF	PCN-700	N.A.	室温	2.6	≈20	物理储存	[35]
	POP	C4P-POP	295	N.A.	3.6	≈100	化学储存	[36]
	MHP	Cs₂PdBr₆	340	340	0.232^a	≈100	化学储存	[32]
	MHP	Cs₄Sb₂Br₁₂	265	265	0.103^a	≈100	化学储存	[32]
	MHP	Rb₄Sb₂Br₁₂	225	225	0.115^a	≈100	化学储存	[32]
	多卤晶体	CsBr₃	181	181	0.751^a	≈100	化学储存	[34]
	多卤晶体	Et₄NBr₃	N.A.	N.A.	N.A.	0	化学储存	[34]
	多卤晶体	Bu₄NBr₃	N.A.	N.A.	N.A.	0	化学储存	[34]
	POC	CC3-R	N.A.	>100~200	1.761^a	>70	化学储存	[31]
	POC	FT-RCC3	N.A.	N.A.	1.860^a	<10	化学储存	[31]
	树脂聚合物	RF NPs	N.A.	N.A.	7.441	0	化学储存	[37]

表1. 本文所涉及材料的部分性质

Table 1. Some properties of the materials involved in this paper

图2. 筛选的材料对Br2和Cl2的最大捕获量与释放效率

Figure 2. The maximum capture capacity and release efficiency of Br2 and Cl2 for the selected materials[30?????-36]

图3. 1, 2和3的结构数据. (A)沿c轴方向的Co(II) MOF晶体Co2Cl2BTDD (1)的结构图. (B~D) NPD测定的1、2和3中Co中心的SBU结构和局部配位环境

Figure 3. Structural data of 1, 2 and 3. (A) A portion of the structure of the parent Co(II) MOF Co2Cl2BTDD (1) projected along the c axis. (B~D) SBU structures and local coordination environments of the Co centers in 1, 2, and 3, respectively, as determined by NPD (Neutron powder diffraction)[30]

图4. 简单钙钛矿中的B位取代衍生出空位有序的双重和四重钙钛矿. (a)阳离子取代示意图. (b)简单钙钛矿ABX3(如CsPbⅡCl3). (c) ABX3钙钛矿的B位阳离子取代衍生出空位有序的双重钙钛矿A2BX6(如Cs2PbⅣCl6). (d) A2BX6钙钛矿的B位阳离子取代衍生出空位有序的四重钙钛矿A4B2X12(如Cs4Sb2Cl12)

Figure 4. The B-site replacement in simple perovskites results in vacancy-ordered double and quadruple perovskites. (a) Schematic of the cation mutation. (b) The simple perovskite ABX3 (e.g., CsPbIICl3). (c) The vacancy-ordered double-perovskite A2BX6 (e.g., Cs2PbIVCl6) derived from the B-cation mutation of ABX3 perovskite. (d) The vacancy-ordered quadruple-perovskite A4B2X12 (e.g., Cs4Sb2Cl12) derived from the B-cation mutation of A2BX6 perovskite[33]

图5. DFT理论计算. 计算空位有序氯基钙钛矿的化学势能相图: (a) APC, (b) RPC和(c) CPC. (d)沿着氧化还原(青色条)和非氧化还原(金色条)路径所计算的空位有序氯基钙钛矿的分解焓

Figure 5. DFT calculations. Calculated chemical potential diagrams of vacancy-ordered chloride perovskites: (a) APC, (b) RPC and (c) CPC. (d) Calculated decomposition energies of vacancy-ordered chloride perovskites along the redox (cyan bars) and non-redox (golden bars) pathways[33]

图6. UiO-67、PCN-700、PCN-605、PCN-606结构的比较. (a)具有fcu拓扑结构的UiO-67由12连接的Zr6团簇和线性配体组成, 而具有bcu拓扑结构的PCN-700由8连接的Zr6团簇和二甲基化线性配体组成. (b)各种取代基的四配体以Td或D2h对称性, 进一步桥联8连接的Zr6簇, 形成flu或scu拓扑的PCN-605和PCN-606系列

Figure 6. Structural comparison of UiO-67, PCN-700, PCN-605, and PCN-606. (a) UiO-67 with fcu topology is composed of 12-connected Zr6 clusters and linear ligands while PCN-700 with bcu topology is composed of 8-connected Zr6 clusters and dimethylated linear ligands. (b) The tetratopic ligand with various substituents adopt a Td or D2h symmetry and further bridges the 8-connected Zr6 clusters to form PCN-605 and PCN-606 series with flu or scu topologies[35]

图7. (a) C4P-POP的合成和(b) C4P-POP选择性吸附溴的卡通插图

Figure 7. (a) Synthesis of C4P-POP and (b) cartoon illustration showing selective bromine adsorption by C4P-POP[36]

图8. (a) CC3-R和FT-RCC3的合成流程. (b) CC3-R(左)和FT-RCC3(右)的笼结构. 碳用灰色表示; 亚胺和叔胺分别用紫色和淡蓝色表示; 为清楚起见, 省略了氢原子. (c) POCs晶体结构中的窗口-窗口堆积示意图

Figure 8. (a) Synthetic procedure of CC3-R and FT-RCC3. (b) Cage structures of CC3-R (left) and FT-RCC3 (right). Carbons are shown in grey; imine and tertiary amine are shown in purple and light blue; hydrogen atoms are omitted for clarity. (c) Schematic illustration of window-to-window packing in the crystal structure of POCs[31]

图9. (a) Cs2SnBr6、Cs4Sb2Br12和Cs2PdBr6沿氧化还原(青色条)和非氧化还原(金色条)路径的分解焓. (b)从含溴钙钛矿中提取元素溴的方法

Figure 9. (a) Calculated decomposition energies of Cs2SnBr6, Cs4Sb2Br12, and Cs2PdBr6 along the redox (cyan bars) and non-redox (golden bars) pathways. (b) The methods for elemental bromine extraction from the bromide perovskites[32]

图10. RF NPs固定Br2、升级改造和生产. (a) RF NPs固定Br2、回收循环和富集银离子示意图. (b) RF树脂的芳香基的结构式. (c) RF NPs的溴化路线. (d) RF NPs的合成工艺示意图. (e) RF NPs的透射电子显微镜图像. 插图显示了单个RF NPs的图像

Figure 10. Br2 fixation by RF NPs, upcycling, and fabrication. (a) Schematic showing the recycling-coupled Br2 fixation on RF NPs and the tandem upcycling for silver recovery. (b) Structural formula of the aromatic groups of RF resin. (c) Proposed possible bromination routes for RF NPs. (d) Schematic of the fabrication process of RF NPs. (e) TEM images of RF NPs. Inset shows the image of an individual RF NP[37]

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用于卤素捕获的材料研究进展

Research Progress of Materials Used for Elemental Halogen Capture

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