Designing a Bifunctional Brønsted Acid–Base Heterogeneous Catalyst Through Precise Installation of Ligands on Metal–Organic Frameworks

Hu, Xiaoqing; Li, Zixuan; Xue, Huan; Huang, Xinfang; Cao, Rong; Liu, Tian‐Fu

doi:10.31635/ccschem.019.201900040

Cited by 38 publications

(24 citation statements)

References 49 publications

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“…Postsynthetic linker functionalization has also been widely studied. [67][68][69][70] On the one hand, desirable linkers can be chemically bonded into parent MOFs to realize certain functions. In a recent study, Hu et al elegantly have installed Brønsted acid and base functionalities in a Zr-based MOFs.…”

Section: Design Of Pore Chemistrymentioning

confidence: 99%

“…In a recent study, Hu et al elegantly have installed Brønsted acid and base functionalities in a Zr-based MOFs. [68] In brief, PCN-700 has been fabricated by coordinating Zr 6 clusters (Zr 6 O 4 (OH) 8 (H 2 O) 4 ) with H 2 Me 2 -BPDC linkers (H 2 Me 2 -BPDC = 2,2′-dimethylbiphenyl-4,4′-dicarboxylic acid) to serve as parent MOFs. In light of two-type pockets presented in the structure of PCN-700 (see Figure 3d), Brønsted basic (2-aminoterephthalic acid) and acidic linkers ([(1,1′:4′,1″-terphenyl)-2,2″,4,4″tetracarboxylic acid]) have been sequentially bonded into a network structure and thus yielded PCN-700-AB.…”

Section: Design Of Pore Chemistrymentioning

confidence: 99%

Section: Porosity Engineering Of Mof‐based Materialsmentioning

confidence: 99%

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Porosity Engineering of MOF‐Based Materials for Electrochemical Energy Storage

Yang

et al. 2021

Advanced Energy Materials

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energy storage (EES)-primarily supercapacitors and metal-ion batteries (MIBs, e.g., lithium-ion batteries (LIBs), sodiumion batteries (SIBs), and potassium-ion batteries (PIBs)).Both supercapacitors and batteries typically consist of current collectors, electrodes, electrolyte, and a separator. By applying a suitable potential between current collectors, the charge/discharge process takes place mediated by the electrode materials, and the electrolyte ions (i.e., the charge carriers) are accordingly driven to travel across the separator so as to connect the circuit. In recent years, solidstate electrolytes (SSEs) are also under popular development to enhance cell voltage (energy density) and safety of the devices. [1] Upon charging, electrical energy is converted to electrostatic potential for supercapacitors and to chemical energy for batteries, and vice versa. Therefore, each device has pros and cons. Supercapacitors usually provide a high power density (i.e., a fast charge/ discharge velocity) due to the fast physical charge-discharge process across the interfaces between electrode materials and the electrolyte solutions, while the energy density is usually small (≈5 Wh kg −1 ). In comparison, batteries often offer a large energy density (i.e., a large specific energy capacity of ≈200 Wh kg −1 ) attributed to the chemical redox reactions which take place throughout the whole volume of electrode materials, while the operation rate is relatively slow. [2] To construct desirable energy storage devices, porous materials have been widely adopted, particularly for electrodes and SSEs. These materials typically feature a large fraction of interconnected or reticulated porosity with a high specific surface area (SSA), offering numerous potential active sites and mass transfer channels. For example, porous materials based on nanocarbons (e.g., carbon nanotubes, graphene), conducting polymers, and conjugated microporous polymers with high electrical conductivity and large SSAs have been frequently adopted for supercapacitors, [3] while porous carbons, MoS 2 , and metal oxides have been used for LIBs because of the theoretically large stoichiometric lithium content in the respectively lithiated compound and an accelerated Li diffusion rate inside the pores. [4][5][6] Despite considerable progress made so far, these porous materials fall short of sufficiently large SSAs and readily tunable pores, which constrain the upper limit for the performance optimization and affect an accurate investigation of the structure-performance relationship.Metal-organic frameworks (MOFs) feature rich chemistry, ordered micro-/ mesoporous structure and uniformly distributed active sites, offering great scope for electrochemical energy storage (EES) applications. Given the particular importance of porosity for charge transport and catalysis, a critical assessment of its design, formation, and engineering is needed for the development and optimization of EES devices. Such efforts can be realized via the design of reticular chemistry, multiscale...

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Section: Design Of Pore Chemistrymentioning

confidence: 99%

Section: Design Of Pore Chemistrymentioning

confidence: 99%

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Porosity Engineering of MOF‐Based Materials for Electrochemical Energy Storage

Yang

et al. 2021

Advanced Energy Materials

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“…Pore B can be rationally designed to extend into the mesoporous region by expanding the size of Pore A. The resultant materials are desirable for potential applications that have been systematically demonstrated in other mesoporous materials, [19][20][21] such as metal-organic frameworks (MOFs). However, due to the high porosity and weak intermolecular interactions between the MOCs, the resulting supramolecular frameworks are prone to collapse upon activation, 22 leading to pore blockage and limitations of their potential applicability in areas requiring solid-state porosity.…”

Section: Introductionmentioning

confidence: 99%

Stabilizing the Extrinsic Porosity in Metal–Organic Cages-Based Supramolecular Framework by In Situ Catalytic Polymerization

Liu

Zhou

et al. 2021

CCS Chem

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Porous supramolecular frameworks based on metal-organic cages (MOCs) usually have poor structural stability after activation. This issue narrows the scope of their potential applications, particularly for the inclusion of guest molecules that demand high porosity. Herein, the authors have reported the stabilization of a mesoporous zirconium MOC-based supramolecular framework with an in situ catalytic polymerization strategy. Due to the passivation effect imparted by this strategy, the introduced polymer is primarily distributed on the surface of the crystals, which results in the hybrid material retaining its crystallinity and permanent porosity. A preliminary application of this type of stabilized mesoporous supramolecular framework shows that among MOC-based supramolecular frameworks, it has the highest high-pressure methane uptake. Such a facile strategy may provide a general way to stabilize fragile porous materials and facilitate exploration of their potential applications.

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“…Metal-organic polyhedra (MOPs), or supramolecular coordination cages, are an emerging class of discrete nanostructure constructed by organic linkers and metal ions/clusters. [1][2][3][4][5] By virtue of designable structure, tunable porosity, and diverse chemical/physical properties, [6][7][8] MOPs show potential in various applications like separation, [9][10][11][12][13] catalysis, [14][15][16][17][18] drug delivery, [19][20][21] and sensing. [22][23][24] More interestingly, unlike metal-organic frameworks (MOFs) with infinite networks, MOPs are discrete molecules with particular geometries and sizes, which can be adopted as artificial models to simulate certain biological architectures and processes.…”

Section: Introductionmentioning

confidence: 99%

Breathing Metal–Organic Polyhedra Controlled by Light for Carbon Dioxide Capture and Liberation

Jiang

Tan

et al. 2021

CCS Chem

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Metal-organic polyhedra (MOPs) have emerged as versatile platforms for artificial models of biological systems due to their discrete structure and modular nature. However, the design and fabrication of MOPs with special functionality for mimicking biological processes are challenging. Inspired by the breathing mechanism of lungs, we developed a new type of MOP (a breathing MOP, denoted as NUT-101) by directly using azobenzene units as the pillars of the polyhedra to coordinate with Zr-based metal clusters. In addition to considerable thermal and chemical stability, the obtained MOP exhibits photocontrollable breathing behavior. Upon irradiation with visible or UV light, the configuration of azobenzene units transforms, leading to reversible expansion or contraction of the cages and, correspondingly, capture or liberation of CO 2 molecules. Such a breathing behavior of NUT-101 is further confirmed by density functional theory (DFT) calculation. This system might establish an avenue for the construction of new materials with particular functionality that mimic biological processes.

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Designing a Bifunctional Brønsted Acid–Base Heterogeneous Catalyst Through Precise Installation of Ligands on Metal–Organic Frameworks

Cited by 38 publications

References 49 publications

Porosity Engineering of MOF‐Based Materials for Electrochemical Energy Storage

Porosity Engineering of MOF‐Based Materials for Electrochemical Energy Storage

Stabilizing the Extrinsic Porosity in Metal–Organic Cages-Based Supramolecular Framework by In Situ Catalytic Polymerization

Breathing Metal–Organic Polyhedra Controlled by Light for Carbon Dioxide Capture and Liberation

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