Photoreduction of N₂ is among the most interesting and challenging methods for N₂ fixation under mild conditions. In this study, we determined that nitrogen vacancies (NVs) could endow graphitic carbon nitride (g-C₃N₄) with the photocatalytic N₂ fixation ability. Photocatalytic N₂ fixation induced by NVs is free from the interference of other gases. The reason is that NVs could selectively adsorb and activate N₂ because NVs have the same shape and size as the nitrogen atom in N₂. In addition to this, NVs could also improve many other properties of g-C₃N₄ to support photocatalytic N₂ fixation. These new findings could elucidate the design of efficient photocatalysts for photocatalytic N₂ fixation.

Selective photocatalytic N₂ fixation dependent on g-C₃N₄ induced by nitrogen vacancies

Ultrathin two-dimensional metal-organic frameworks (2D MOFs) have recently attracted extensive interest in various catalytic fields (e.g., electrocatalysis, photocatalysis, thermocatalysis) due to their ultrathin thickness, large surface area, abundant accessible unsaturated active sites and tunable surface properties. Besides tuning the intrinsic properties of pristine 2D MOFs by changing the metal nodes and organic ligands, one of the hot research trends is to develop 2D MOF hybrids and 2D MOF-derived materials with higher stability and conductivity in order to further increase their activity and durability. Here, the synthesis of 2D MOF nanosheets is briefly summarized and discussed. More attention is focused on summaries and discussions about the applications of these 2D MOFs, their hybrids and their derived materials as electrocatalysts, photocatalysts and thermocatalysts. The superior properties and catalytic performance of these 2D MOF-based catalysts compared to their 3D MOF counterparts in electrocatalysis, photocatalysis and thermocatalysis are highlighted. The enhanced activities of 2D MOFs, their hybrids and derivatives come from abundant accessible active sites, a high density of unsaturated metal nodes, ultrathin thickness, and tunable microenvironments around the MOFs. Views regarding current and future challenges in the field, and new advances in science and technology to meet these challenges, are also presented. Finally, conclusions and outlooks in this field are provided.

2D metal-organic framework-based materials for electrocatalytic, photocatalytic and thermocatalytic applications.

Two-dimensional (2D) transition metal dichalcogenides (TMDs), a rising star in the post-graphene era, are fundamentally and technologically intriguing for photocatalysis. Their extraordinary electronic, optical, and chemical properties endow them as promising materials for effectively harvesting light and catalyzing the redox reaction in photocatalysis. Here, we present a tutorial-style review of the field of 2D TMDs for photocatalysis to educate researchers (especially the new-comers), which begins with a brief introduction of the fundamentals of 2D TMDs and photocatalysis along with the synthesis of this type of material, then look deeply into the merits of 2D TMDs as co-catalysts and active photocatalysts, followed by an overview of the challenges and corresponding strategies of 2D TMDs for photocatalysis, and finally look ahead this topic.

2D Transition Metal Dichalcogenides for Photocatalysis.

Metal-Organic Frameworks Nanocomposites with Different Dimensionalities for Energy Conversion and Storage

Rapid progress on developing smart materials and design of hybrids is motivated by pressing challenges associated with energy crisis and environmental remediation. While emergence of versatile classes of nanomaterials has been fascinating, the real excitement lies in the design of hybrid materials with tunable properties. Metal-organic frameworks (MOFs) are the key materials for gas sorption and electrochemical applications, but their sustainability is challenged by limited chemical stability, poor electrical conductivity, and intricate, inaccessible pores. Despite tremendous efforts towards improving the stability of MOF materials, little progress has made researchers inclined toward developing hybrid materials. MXenes, a family of two-dimensional transition-metal carbides, nitrides and carbonitrides, are known for their compositional versatility and formation of a range of structures with rich surface chemistry. Hybridization of MOFs with functional layered MXene materials may be beneficial if the host structure provides appropriate interactions for stabilizing and improving the desired properties. Recent efforts have focused on integrating Ti3C2Tx and V2CTx MXenes with MOFs to result in hybrid materials with augmented electrochemical and physicochemical properties, widening the scope for emerging applications. This review discusses the potential design strategies of MXene@MOF hybrids, attributes of tunable properties in the resulting hybrids, and their applications in water treatment, sensing, electrochemical energy storage, smart textiles, and electrocatalysis. Comprehensive discussions on the recent efforts on rapidly evolving MXene@MOF materials for various applications and potential future directions are highlighted.

Emerging MXene@Metal-Organic Framework Hybrids: Design Strategies toward Versatile Applications.

To improve the photocatalytic efficiency of the N₂ reduction reaction, MXene quantum dots (Ti₃C₂-QDs) and two-dimensional (2D) nickel metal–organic framework (Ni-MOF) with different ratios were fabricated by a simple self-assembly strategy to form type II heterojunctions. The resultant composites showed enhanced absorption and excellent interfacial charge-transfer capabilities according to the optical and photoelectron properties. The optimal Ti₃C₂-QD/Ni-MOF heterostructure exhibited a considerable ammonia yield rate (88.79 μmol gcₐₜ–¹ h–¹). By means of X-ray absorption near-edge fine structure (XANES) technique, it was found that the interaction of Ti₃C₂-QD and Ni-MOF could accelerate the electron transfer, and Ni site would be the main area to enrich the electron density as well as adsorb and activate N₂. Finally, with the aid of density functional theory (DFT) calculations and in situ Fourier transform infrared spectrometry (FTIR), the reaction pathway and intermediate products were studied.

0D/2D MXene Quantum Dot/Ni-MOF Ultrathin Nanosheets for Enhanced N2 Photoreduction

Solar-driven conversion of nitrogen (N2) to ammonia (NH3) is highly appealing, yet in its infancy, the low photocatalytic efficiency and unclear adsorption and activation mechanisms of N2 are still issues to be addressed In this study, ultrathin alloyed Mo1-xWxS2 nanosheets with tunable hexagonal (2H)/trigonal (1T) phase ratios were proposed to boost photoreduction N2 efficiency, while the mechanisms of N2 adsorption and activation were explored simultaneously The alloyed Mo1-xWxS2 nanosheets for the 1T phase concentration of 336% and Mo/W = 068:032 were proven to reach about 111 μmol gcat-1 h-1 under visible light, which is 37 (or 3)-fold higher than that of pristine MoS2 (or WS2) With the aid of density functional theory calculations and in situ N2 adsorption X-ray absorption near-edge fine structure techniques, the adsorption and activation behaviors of N2 over the interface of Mo1-xWxS2 nanosheets were investigated during the N2 reduction process The results show that the W doping causes a higher electron density state in W 5d orbitals, which can further polarize the adsorbed N2 molecules for adsorption and activation This work provides a new insight into the adsorption and activation mechanisms for the NH3 synthesis

Exploring the N2 Adsorption and Activation Mechanisms over the 2H/1T Mixed-Phase Ultrathin Mo1-xWxS2 Nanosheets for Boosting N2 Photosynthesis.

Defect and Interface Engineering on Two-Dimensional Nanosheets for the Photocatalytic Nitrogen Reduction Reaction

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0D/2D MXene Quantum Dot/Ni-MOF Ultrathin Nanosheets for Enhanced N2 Photoreduction

Exploring the N2 Adsorption and Activation Mechanisms over the 2H/1T Mixed-Phase Ultrathin Mo1-xWxS2 Nanosheets for Boosting N2 Photosynthesis.

Defect and Interface Engineering on Two-Dimensional Nanosheets for the Photocatalytic Nitrogen Reduction Reaction