The crystal-liquid-glass phase transition of coordination polymers (CPs) and metal-organic frameworks (MOFs) offers attractive opportunities as a new class of amorphous materials. Unlike conventional glasses, coordination chemistry allows the utilization of rational design concepts to fine-tune the desired properties. Although the glassy state has been rare in CPs/MOFs, it exhibits diverse advantages complementary to their crystalline counterparts, including improved mass transport, optical properties, mechanical properties, and the ability to form grain-boundary-free monoliths. This Review discusses the current achievements in improving the understanding of anomalous phase transitions in CPs/MOFs. We elaborate on the criteria for classifying CP/MOF glasses and comprehensively discuss the three common strategies employed to obtain a glassy state. We include all CP/MOF glass research progress since its inception, discuss the current challenges, and express our perspective on future research directions. 

https://pubs.acs.org/doi/pdf/10.1021/acs.chemrev.1c00826

Metal–Organic Network-Forming Glasses

https://onlinelibrary.wiley.com/doi/pdf/10.1002/adfm.202104300

Glassy Metal–Organic-Framework-Based Quasi-Solid-State Electrolyte for High-Performance Lithium-Metal Batteries

Metal-organic framework (MOF)-based materials, including pristine MOFs, MOF composites, and MOF derivatives, have become a research focus in energy storage and conversion applications due to their customizability, large specific surface area, and tunable pore size. However, MOF-based materials are currently in their infancy, and more efforts need to be dedicated to enable them to perform competitively in large-scale practical applications. This updated review provides an overview of the advances in MOF-based materials in energy storage and conversion applications, including gas storage, batteries, supercapacitors, and photo/electrochemical energy conversion, highlighting the advantages of different materials in various scenarios. Finally, we summarize the current challenges and status of MOF-based materials for energy storage and conversion and provide an outlook for future research directions. 

Metal-organic framework-based materials as platforms for energy applications

Metal-organic frameworks (MOFs) with diverse composition, tunable structure, and unique physicochemical properties have emerged as promising materials in various fields. The tunable pore structure, abundant active sites, and ultrahigh specific surface area can facilitate mass transport and provide outstanding capacity, making MOFs an ideal active material for electrochemical energy storage and conversion. However, the poor electrical conductivity of pristine MOFs severely limits their applications in electrochemistry. Developing conductive MOFs has proved to be an effective solution to this problem. This review focuses on the design and synthesis of conductive MOF composites with judiciously chosen conducting materials, pristine MOFs, and assembly methods, as well as the preparation of intrinsically conductive MOFs based on building 2D π-conjugated structures, introducing mixed-valence metal ions/redox-active ligands, designing π-π stacked pathways, and constructing infinite metal-sulfur chains (-M-S-)∞ . Furthermore, recent progress and challenges of conductive MOFs for energy storage and conversion (supercapacitors, Li-ion batteries, Li-S batteries, and electrochemical water splitting) are summarized.

Recent Progress of Advanced Conductive Metal-Organic Frameworks: Precise Synthesis, Electrochemical Energy Storage Applications, and Future Challenges.

Metal-organic frameworks (MOFs) are emerging as attractive electrode materials for lithium-ion batteries, owing to their fascinating features of sustainable resources, tunable chemical components, flexible molecular skeletons, and renewability. However, they are faced with a limited number of redox-active sites and unstable molecular frameworks during electrochemical processes. Herein, we design a novel two-dimensional (2D) iron(III)-tetraamino-benzoquinone (Fe-TABQ) with dual redox centers of Fe cations and TABQ ligands for high-capacity and stable lithium storage. It is constructed of square-planar Fe-N2O2 linkages and phenylenediamine building blocks, between which the Fe-TABQ chains are connected by multiple hydrogen bonds, and then featured as an extended π-d-conjugated 2D structure. The redox chemistry of both Fe3+ cations and TABQ anions is revealed to render its remarkable specific capacity of 251.1 mAh g-1. Benefiting from the intrinsic robust Fe-N(O) bonds and reinforced Li-N(O) bonds during cycling, Fe-TABQ delivers high capacity retentions over 95% after 200 cycles at various current densities. This work will enlighten more investigations for the molecular designs of advanced MOF-based electrode materials.

Reversible Metal and Ligand Redox Chemistry in Two-Dimensional Iron-Organic Framework for Sustainable Lithium-Ion Batteries.

Metal organic frameworks (MOFs) hold
great promise as high-energy anode materials for next-generation lithium ion
batteries (LIBs) due to their tuneable pore structure and abundant reaction
sites. However, since the pore structure of crystalline MOFs tends to collapse
during lithium ion insertion and extraction, it has been a challenge to develop
crystalline MOF-based anodes for high performance lithium ion batteries. Here
we report a breakthrough in developing the high-performance MOF anodes. In
detail, we have developed the first MOF glass anode, i.e., melt-quenched
Cobalt-ZIF-62 glass anode with exceptional electrochemical performances. Compared
with its crystalline counterpart, the Co-ZIF-62 glass anode exhibits
significantly higher lithium storage capacity (306 mAh g-1 after
1000 cycles at the current density of 2 A g-1), outstanding cycling
stability and superior rate performance. Amazingly, the Li-ion storage capacity
of the MOF glass anode continuously rises with increasing the number of
charge-discharge cycles and even tripled
after 1000 cycles. We revealed the possible origin of the unusual
cycling-enhanced performances of the MOF glass anode. These superior
performances make MOF glasses ideal candidates for anode materials for LIBs.

/pdf/metal-organic-framework-glass-anode-with-an-exceptional-o75bj4vxwu.pdf

Metal-Organic Framework Glass Anode with an Exceptional Cycling-Induced Capacity Enhancement for Lithium Ion Batteries

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Metal-Organic Framework Glass Anode with an Exceptional Cycling-Induced Capacity Enhancement for Lithium Ion Batteries