The high catalytic activity of metal-organic frameworks (MOFs) can be realized by increasing their effective active sites, which prompts us to perform the functionalization on selected linkers by introducing a strong Lewis basic group of fluorine. Herein, the exquisite combination of paddle-wheel [Cu2(CO2)4(H2O)] clusters and meticulously designed fluorine-funtionalized tetratopic 2',3'-difluoro-[p-terphenyl]-3,3″,5,5″-tetracarboxylic acid (F-H4ptta) engenders one peculiar nanocaged {Cu2}-organic framework of {[Cu2(F-ptta)(H2O)2]·5DMF·2H2O}n (NUC-54), which features two types of nanocaged voids (9.8 Å × 17.2 Å and 10.1 Å × 12.4 Å) shaped by 12 paddle-wheel [Cu2(COO)4H2O)2] secondary building units, leaving a calculated solvent-accessible void volume of 60.6%. Because of the introduction of plentifully Lewis base sites of fluorine groups, activated NUC-54a exhibits excellent catalytic performance on the cycloaddition reaction of CO2 with various epoxides under mild conditions. Moreover, to expand the catalytic scope, the deacetalization-Knoevenagel condensation reactions of benzaldehyde dimethyl acetal and malononitrile were performed using the heterogenous catalyst of NUC-54a. Also, NUC-54a features high recyclability and catalytic stability with excellent catalytic performance in subsequent catalytic tests. Therefore, this work not only puts forward a new solution for developing high-efficiency heterogeneous catalysts, but also enriches the functionalization strategies for nanoporous MOFs.

Fluorine-Functionalized NbO-Type {Cu2}-Organic Framework: Enhanced Catalytic Performance on the Cycloaddition Reaction of CO2 with Epoxides and Deacetalization-Knoevenagel Condensation.

Bifunctional {Pb10K2}–Organic Framework for High Catalytic Activity in Cycloaddition of CO2 with Epoxides and Knoevenagel Condensation

Sulfite activation by cobaltosic oxide nanohydrangeas for tetracycline degradation: Performance, degradation pathways and mechanism.

Recent progress of Ni-based catalysts for methanol electrooxidation reaction in alkaline media

Facile interface engineering of hierarchical flower spherical-like Bi-metal–organic framework microsphere/Bi2MoO6 heterostructure for high-performance visible–light photocatalytic tetracycline hydrochloride degradation

Developing efficient metal-organic framework (MOF)-based electrocatalysts with improvable activity and persistence toward the methanol oxidation reaction (MOR) is attracting great research attention but still remains an enormous challenge. Herein, a facile strategy, hydrangea-shaped nickel hydroxide template-directed synthesis of the hierarchically structured Ni-MOF on the Ni(OH)2 heterocomposite (denoted as Ni-Ni) for efficient MOR, is developed. The unique hierarchical structure and synergistic effect of the heterocomposite afford more exposed active sites, a facile ion diffusion path, and improved conductivity, favorable for improving MOR catalytic performance. Remarkably, the optimized Ni-Ni-2 material delivers an excellent activity with a high peak current density (24.6 mA cm-2). Furthermore, to prove the universality of this strategy, NixCu1-x(OH)2 isometallic hydroxide was used as the precursor, and a series of MOF-74/CuxNi1-x(OH)2 (denoted as Ni-NiCu) heterogeneous materials have been prepared and could be used as an effective electrocatalyst to catalyze MOR. The results indicate that this strategy can be used in the synthesis of other new composite materials with specific hierarchical structures for a more efficient electrocatalytic system.

Common Strategy: Mounting the Rod-like Ni-Based MOF on Hydrangea-Shaped Nickel Hydroxide for Superior Electrocatalytic Methanol Oxidation Reaction.

Ni-based materials have emerged as promising anode electrocatalysts that can replace noble metals for the methanol oxidation reaction (MOR). However, the potential applications of Ni-based metal–organic gels (Ni-MOGs) in MOR have rarely been recognized. In this study, using the readily prepared Al-MOG (MIL-53(Al)) without MOR activity as a template, we fabricated AlNi-MOG and AlNi-based trimetallic MOGs (Cu, Co and Fe) by a simple solvothermal method, which could be directly used as electrocatalysts for the MOR. Among them, the as-obtained AlNiCu-MOG exhibited better MOR activity with an area-specific peak current density of 17.1 mA cm−2 than AlNi-MOG (11.46 mA cm−2), which could be attributed to the electron coupling between Ni and Cu. Moreover, the addition of the conductive material acetylene black (AB) could immensely increase the electric conductivity of AlNiCu-MOG, leading to its improved MOR activity with a peak current density of 33.24 mA cm−2. These results represent an important first step towards the application of MOGs in the MOR.

Convenient synthesis of polymetallic metal–organic gels for efficient methanol electro-oxidation

Engineering the heterogeneous interface fusing MOFs and inorganic active component is an effective strategy to improve the electrochemical performance. Herein, we report a new Ni3-based MOF (denoted as CTGU-24) with an infrequent 2-fold interpenetrating 3D (3,8)-connected network constructed from Ni(II) trimer and mixed tripodal tectonics for the electrocatalytic methanol oxidation reaction (MOR). In order to improve its stability and activities, the heterogeneous hybrid CTGU-24@NiOOH has been fabricated successfully via the first preparation of NiOOH nanosphere and then in situ formation of CTGU-24 decorated on NiOOH surface. Moreover, the integration of CTGU-24@NiOOH and different additives (acetylene black (AB) and ketjen black (KB)), resulting in the optimized hybrid sample AB&CTGU-24@NiOOH (4:4). It attains better MOR performance with an area specific peak current density of 34.53mA•cm−2 than pure CTGU-24 (14.99 mA•cm−2) and improved durability in an alkali medium. The new findings indicate that the CTGU-24@NiOOH heterostructure formed in situ and the integration of moderate additives are critical to optimizing and improving electrocatalytic activity of pure MOFs crystalline material.

In Situ Synthesis of Surface-Mounted Novel Nickel(II) Trimer-Based MOF on Nickel Oxide Hydroxide Heterostructures for Enhanced Methanol Electro-Oxidation

Four new isostructural metal-organic frameworks constructed by a new butterfly-typed nitroheterocyclic carboxylic acid: Synthesis, crystal structures and properties

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Common Strategy: Mounting the Rod-like Ni-Based MOF on Hydrangea-Shaped Nickel Hydroxide for Superior Electrocatalytic Methanol Oxidation Reaction.

Convenient synthesis of polymetallic metal–organic gels for efficient methanol electro-oxidation

In Situ Synthesis of Surface-Mounted Novel Nickel(II) Trimer-Based MOF on Nickel Oxide Hydroxide Heterostructures for Enhanced Methanol Electro-Oxidation

Four new isostructural metal-organic frameworks constructed by a new butterfly-typed nitroheterocyclic carboxylic acid: Synthesis, crystal structures and properties