Metal-organic framework (MOF) nanoparticles, also called porous coordination polymers, are a major part of nanomaterials science, and their role in catalysis is becoming central. The extraordinary variability and richness of their structures afford engineering synergies between the metal nodes, functional linkers, encapsulated substrates, or nanoparticles for multiple and selective heterogeneous interactions and activations in these MOF-based nanocatalysts. Pyrolysis of MOF-nanoparticle composites forms highly porous N- or P-doped graphitized MOF-derived nanomaterials that are increasingly used as efficient catalysts especially in electro- and photocatalysis. This review first briefly summarizes this background of MOF nanoparticle catalysis and then comprehensively reviews the fast-growing literature reported during the last years. The major parts are catalysis of organic and molecular reactions, electrocatalysis, photocatalysis, and views of prospects. Major challenges of our society are addressed using these well-defined heterogeneous catalysts in the fields of synthesis, energy, and environment. In spite of the many achievements, enormous progress is still necessary to improve our understanding of the processes involved beyond the proof-of-concept, particularly for selective methane oxidation, hydrogen production, water splitting, CO2 reduction to methanol, nitrogen fixation, and water depollution.

State of the Art and Prospects in Metal-Organic Framework (MOF)-Based and MOF-Derived Nanocatalysis.

Herein, ZnO/CdS hierarchical composite was prepared through a hydrothermal and chemical bath deposition (CBD) process. Its photocatalytic H2-production performance was tested. Mass ratio of CdS acted a pivotal part in light absorption and photocatalytic properties. Noticeably, promoted photocatalytic H2-production activity of 4134 μmol g−1 h-1 was achieved by the sample with optimal CdS content. Significantly, the photoluminescence (PL) detection of hydroxyl radicals, as well as the in-situ XPS measurements was selected to verify the direct Z-scheme charge migration mechanism. This mechanism endowed the composite with strong capability for hydrogen evolution and elucidated the improved photocatalytic performance. The improvement of photocatalytic activity was due to hierarchical structure, extended visible light response and direct Z-scheme mechanism. This work will give an innovative vision in constructing direct Z-scheme photocatalytic system with great photocatalytic H2-production activity.

Direct Z-scheme ZnO/CdS hierarchical photocatalyst for enhanced photocatalytic H2-production activity

Visible light-induced photocatalysis is a promising way for environmental remediation due to efficient utilization of solar energy. Recently, metal–organic frameworks (MOFs) have attracted increasing attention in the field of photocatalysis. In comparison with traditional metal oxide semiconductors, MOFs have many advantages, such as high specific surface area, rich topology and easily tunable porous structure. In this review, we aim to summarize and illustrate recent advances in MOF-based photocatalysis for environmental remediation under visible light, including wastewater treatment, air purification and disinfection. A series of strategies have been designed to modify and regulate pristine MOFs for enhanced photocatalytic performance, such as ligand functionalization, mixed-metal/linker strategy, metal ion/ligand immobilization, dye sensitization, metal nanoparticle loading, carbon material decoration, semiconductor coupling, MOF/COF coupling, carrier loading and magnetic recycling. The above modifications may result in extended visible light absorption, efficient generation, separation and transfer of photogenerated charges, as well as good recyclability. However, there are still many challenges and obstacles. In order to meet the requirements of using MOF photocatalysis as a friendly and stable technology for low-cost practical applications, its future development prospects are also discussed.

/pdf/recent-advances-in-mof-based-photocatalysis-environmental-3m7z4g349c.pdf

Recent advances in MOF-based photocatalysis: environmental remediation under visible light

A Review of MOFs and Their Composites-Based Photocatalysts: Synthesis and Applications

Photocatalytic water splitting for H2 production becomes one of the most favorable pathways for solar energy utilization, while the charge-separation dynamics in composite photocatalysts is largely elusive. In the present work, CdS-decorated metal–organic framework (MOF) composites, namely, CdS/UiO-66, have been synthesized and exhibit high H2 production activity from photocatalytic water splitting, far surpassing the MOF and CdS counterparts, under visible light irradiation. Transient absorption (TA) spectroscopy has been adopted in this report to unveil the charge-separation dynamics in CdS/UiO-66 composites, a key process that dictates their function in photocatalysis. We show that, in addition to the preferable formation of fine CdS particles assisted by the MOF, effective electron transfer, which occurs from excited CdS to UiO-66, significantly inhibits the recombination of photogenerated charge carriers, ultimately boosting the photocatalytic activity for H2 generation. This report on charge-separat...

Unveiling Charge-Separation Dynamics in CdS/Metal–Organic Framework Composites for Enhanced Photocatalysis

Through the labile coordination sites of a robust phosphonate-stabilized titanium-oxo cluster, 14 O-donor ligands have been successfully introduced without changing the cluster core. The increasing electron-withdrawing effect of the organic species allows the gradual reduction of the bandgaps of the {Ti6 } complexes. Transition-metal ions are then incorporated by the use of bifunctional O/N-donor ligands, organizing these {Ti6 } clusters into polymeric structures. The coordination environments of the applied metal ions show significant influence on their visible-light adsorption. Both the above structural functionalizations also tune the photocatalytic H2 production activities of these clusters. This work provides a systematic bandgap engineering study of titanium-oxo clusters, which is important not only for their future photocatalytic applications, also for the better understanding of the structure-property relationships.

https://onlinelibrary.wiley.com/doi/pdf/10.1002/anie.201681761

Bandgap Engineering of Titanium–Oxo Clusters: Labile Surface Sites Used for Ligand Substitution and Metal Incorporation

A new Cd-doped titanium–oxo cluster (TOC) stabilized by tert-butylacetic acid ligands has been prepared through an easily handled solvothermal reaction; photocatalytic studies indicate that it displays good H2 evolution ability (3.15 μmol h−1), and moreover preserves high catalytic stability.

A new cadmium-doped titanium–oxo cluster with stable photocatalytic H2 evolution properties

Four rectangular molecular architectures have been successfully constructed using {Ti5O7} clusters as inorganic vertical edges and bridging aromatic carboxylates as horizontal edges. The introduced organic ligands show a strong influence on the light absorption behaviors of the obtained hybrid complexes.

/pdf/construction-of-molecular-rectangles-with-titanium-oxo-4y34pbhugu.pdf

Construction of molecular rectangles with titanium–oxo clusters and rigid aromatic carboxylate ligands

Polyoxo-titanium clusters (PTCs) are applied to construct highly efficient ternary PTC/CdS/MIL-101 visible-light-range H2 -evolution photocatalysts. The application of PTCs not only increases the photocatalytic activities but also provides a molecular tool to tune them.

Assembling Polyoxo‐Titanium Clusters and CdS Nanoparticles to a Porous Matrix for Efficient and Tunable H2‐Evolution Activities with Visible Light

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Bandgap Engineering of Titanium–Oxo Clusters: Labile Surface Sites Used for Ligand Substitution and Metal Incorporation

A new cadmium-doped titanium–oxo cluster with stable photocatalytic H2 evolution properties

Construction of molecular rectangles with titanium–oxo clusters and rigid aromatic carboxylate ligands

Assembling Polyoxo‐Titanium Clusters and CdS Nanoparticles to a Porous Matrix for Efficient and Tunable H2‐Evolution Activities with Visible Light