Challenge, Advance and Emerging Opportunities for Metal-Organic Framework Glasses: from Dynamic Chemistry to Material Science and Noncrystalline Physics

doi:10.6023/A22120508

Acta Chimica Sinica ›› 2023, Vol. 81 ›› Issue (3): 246-252.DOI: 10.6023/A22120508 Previous Articles Next Articles

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动态化学与材料和非晶物理新关联——金属有机框架玻璃的挑战、进展与新机遇

殷政^a^,^b^,^*(), 赵英博^c^,^*(), 曾明华^a^,^*()

a 广西师范大学化学与药学学院药用资源化学与药物分子工程省部共建国家重点实验室桂林 541004
b 陕西科技大学化学与化工学院西安 710021
c 上海科技大学物质科学与技术学院上海 201210

投稿日期:2022-12-23 发布日期:2023-02-16

作者简介:

殷政, 博士、副教授、硕士生导师. 2015年博士毕业于广西师范大学, 导师曾明华教授, 随后进入陕西科技大学工作. 主要从事功能配位聚合物材料的晶态、固态及玻璃态结构转变、后合成修饰及功能调变相关研究.

赵英博, 博士, 上海科技大学助理教授、研究员、博士生导师. 2017年博士毕业于加州大学伯克利分校, 导师Omar Yaghi教授. 2017至2021年在加州大学伯克利分校电子工程系从事博士后研究, 合作导师Ali Javey教授. 2021年8月加入上海科技大学. 主要开展分子框架结构设计合成、界面生长控制和功能器件构筑的相关研究.

曾明华, 博士, 广西师范大学教授、博士生导师, 国家自然科学基金杰出青年科学基金获得者(2015), 国家“万人计划”科技创新领军人才(2017). 2004年博士毕业于中山大学, 导师陈小明教授. 在功能配位化学及溶液配位领域, 系统性开展基于固-液结构关联、固-固结构对应性的配位导向序列化串联反应过程与机理、多级结构演变及其物化性能效应研究.

基金资助:
国家自然科学基金(22171075); 广西八桂英才项目(2019AC26001); 霍英东教育基金会高等院校青年教师基金(171110); 上海市科学技术委员会项目(22QC1401500); 上海市科学技术委员会项目(21DZ2260400)

Challenge, Advance and Emerging Opportunities for Metal-Organic Framework Glasses: from Dynamic Chemistry to Material Science and Noncrystalline Physics

Zheng Yin^a^,^b(), Yingbo Zhao^c(), Minghua Zeng^a()

a Chemistry and Pharmaceutical Sciences, State Key Laboratory for the Chemistry and Molecular Engineering of Medicinal Resources, Guangxi Normal University, Guilin 541004
b College of Chemistry and Chemical Engineering, Shaanxi University of Science and Technology, Xi’an 710021
c School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210

Received:2022-12-23 Published:2023-02-16
Contact: *E-mail: yinzheng@sust.edu.cn; zhaoyb2@shanghaitech.edu.cn; zmh@mailbox.gxnu.edu.cn
Supported by:
National Natural Science Foundation of China(22171075); BaGui Talent Program of Guangxi Province(2019AC26001); Young Teachers Grants from the Fok Ying-Tong Education Foundation(171110); Science and Technology Commission of Shanghai Municipality(22QC1401500); Science and Technology Commission of Shanghai Municipality(21DZ2260400)

The emerging metal-organic framework (MOF) glass, that is brand-new comer to the traditional glass and noncrystalline physics world, was viewed as the Holy Grail of future porous chemistry and the key direction of MOF derived functional materials. The known examples of MOF glass are extremely scarce, prepared mainly through the traditional melt-quenching method. As porous framework constructed from metal ions/clusters and organic linkers through coordinative bonds, the majority of MOFs can not reach high-temperature melt state, which prevents MOF glass formation. Facing these challenges, here we summarized the development history and latest advance of MOF glass. A new strategy of sequential perturbation based on dynamic chemistry was presented to widely prepare MOF glass. How to discover more MOF glasses, expand their properties and functions, and clarify their nature, is the new interdisciplinary frontier from dynamic chemistry to material science and noncrystalline physics. This topic also provides a range of new research opportunities, including the design and regulation of MOF glass based on reticular and dynamic chemistry, exploring new functions of MOF glass beyond its crystalline counterpart, and effectively responding to the scientific challenges in noncrystalline physics including the glass nature, based on the solid-solid structure transformation and relevance between crystalline and glassy MOFs.

Key words: metal-organic framework, glass transition, sequential perturbation, dynamic chemistry, noncrystalline physics

Cite this article

Zheng Yin, Yingbo Zhao, Minghua Zeng. Challenge, Advance and Emerging Opportunities for Metal-Organic Framework Glasses: from Dynamic Chemistry to Material Science and Noncrystalline Physics[J]. Acta Chimica Sinica, 2023, 81(3): 246-252.

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MOFs	Formula	T_m/K	Vitrification	T_g/K	Glass Properties and Functions
ZIF-4	[Zn(Im)₂]	863	MQ, MM	570	Strong/fragile liquid change, fragility index of 39, E=8.2 GPa, H=0.92 GPa, solid-state electrolyte for LMB
GIS	[Zn(Im)₂]	857	MQ	564	Fragility index of 39, E=8.5 GPa, H=0.9 GPa
ZIF-62	[Zn(Im)_1.75(bIm)_0.25] [Zn(Im)_2-_x(bIm)_x] (x=0.03~0.35) [Co(Im)_1.7(bIm)_0.3] [Zn_1-_xCo_x(Im)_1.7(bIm)_0.3] (x=0.007~0.5)	708 643~721 705 672~725	MQ MQ MQ MQ	595 565~602 563 604~607	Properties for family: (i) ultrahigh glass-forming ability, fragility index of 23, viscosity of 10⁵ Pa•s at T_m, Poisson’s ratio of 0.45; mixed metal and ligand ratio modified T_m and T_g; (ii) fracture toughness of 0.1 MPa•m^0.5, anomalous brittle-to-ductile transition, creep resistance, low strain-rate sensitivity, (iii) CO₂ uptake of 0.75 mmol•g^-1(273 K, 95 kPa) for a_gZIF-62(Co), selective sorption to n-butane, propane and propylene; glass membrane for H₂/CH₄, CO₂/N₂ and CO₂/CH₄ separation; (iv) transmittance up to 90% for visible and near-infrared wave, 1.5~4.8 μm mid-infrared luminescence, strong NLO response with modulation depth of 63.85%; (v) anode with exceptional cycling-induced capacity enhancement for lithium-ion batteries, flexible electrodes for oxygen evolution reaction
ZIF-76	[Zn(Im)_1.33(5-mbIm)_0.67]	724	MQ	583	Permanent gas accessible porosity with CO₂ adsorption of 4% (w) at 273 K
ZIF-8	[Zn(mIm)₂] (Ionic liquid incorporated)	654	MQ	595	High T_g/T_m of 0.91, E=5.42 GPa, H=0.73 GPa, a four-fold increase of glass’ porosity after ionic liquid washing
Others	[Ag(pL₂)(CF₃SO₃)] [Ti₁₆O₁₆₍BPA)_x(OR)₃₂₋_x] [Co(pybz)₂]₄_n	544	MQ, MM VE SP	434 — 568	Adsorption capacity of 9.2 cm³/g (CO₂, 195 K) and 160 cm³/g (benzene vapor) 77 K N₂ accessible internal surface area of 267 m²/g Fragility index of 83, supercooled liquid range of 26 K, thermal stable for 10⁴ s at T_g, CH₃OH and CO₂ accessible porosity
		—
		—

MOFs	Formula	T_m/K	Vitrification	T_g/K	Glass Properties and Functions
ZIF-4	[Zn(Im)₂]	863	MQ, MM	570	Strong/fragile liquid change, fragility index of 39, E=8.2 GPa, H=0.92 GPa, solid-state electrolyte for LMB
GIS	[Zn(Im)₂]	857	MQ	564	Fragility index of 39, E=8.5 GPa, H=0.9 GPa
ZIF-62	[Zn(Im)_1.75(bIm)_0.25] [Zn(Im)_2-_x(bIm)_x] (x=0.03~0.35) [Co(Im)_1.7(bIm)_0.3] [Zn_1-_xCo_x(Im)_1.7(bIm)_0.3] (x=0.007~0.5)	708 643~721 705 672~725	MQ MQ MQ MQ	595 565~602 563 604~607	Properties for family: (i) ultrahigh glass-forming ability, fragility index of 23, viscosity of 10⁵ Pa•s at T_m, Poisson’s ratio of 0.45; mixed metal and ligand ratio modified T_m and T_g; (ii) fracture toughness of 0.1 MPa•m^0.5, anomalous brittle-to-ductile transition, creep resistance, low strain-rate sensitivity, (iii) CO₂ uptake of 0.75 mmol•g^-1(273 K, 95 kPa) for a_gZIF-62(Co), selective sorption to n-butane, propane and propylene; glass membrane for H₂/CH₄, CO₂/N₂ and CO₂/CH₄ separation; (iv) transmittance up to 90% for visible and near-infrared wave, 1.5~4.8 μm mid-infrared luminescence, strong NLO response with modulation depth of 63.85%; (v) anode with exceptional cycling-induced capacity enhancement for lithium-ion batteries, flexible electrodes for oxygen evolution reaction
ZIF-76	[Zn(Im)_1.33(5-mbIm)_0.67]	724	MQ	583	Permanent gas accessible porosity with CO₂ adsorption of 4% (w) at 273 K
ZIF-8	[Zn(mIm)₂] (Ionic liquid incorporated)	654	MQ	595	High T_g/T_m of 0.91, E=5.42 GPa, H=0.73 GPa, a four-fold increase of glass’ porosity after ionic liquid washing
Others	[Ag(pL₂)(CF₃SO₃)] [Ti₁₆O₁₆₍BPA)_x(OR)₃₂₋_x] [Co(pybz)₂]₄_n	544	MQ, MM VE SP	434 — 568	Adsorption capacity of 9.2 cm³/g (CO₂, 195 K) and 160 cm³/g (benzene vapor) 77 K N₂ accessible internal surface area of 267 m²/g Fragility index of 83, supercooled liquid range of 26 K, thermal stable for 10⁴ s at T_g, CH₃OH and CO₂ accessible porosity
		—
		—

动态化学与材料和非晶物理新关联——金属有机框架玻璃的挑战、进展与新机遇

Challenge, Advance and Emerging Opportunities for Metal-Organic Framework Glasses: from Dynamic Chemistry to Material Science and Noncrystalline Physics

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