Single/dual-atom and cluster metal catalysts, with much higher atom-utilization efficiency, remarkable performance, good recyclability and unique properties, have emerged as a new frontier in energy-related catalysis. In recent years, metal–organic frameworks (MOFs) have demonstrated great potential for the targeted creation of single/dual-atom and cluster catalysts, featuring the distinctive advantages of high metal loadings, porous structures and tailorable catalytic sites. In this review, we discuss the key roles and the critical issues of single/dual-atom and cluster catalysts, and the great opportunities furnished by MOFs for the construction strategy. The accessible characterization techniques for single/dual-atom and cluster catalysts will be showcased. Furthermore, we highlight recent advances in the construction and energy applications of MOF-based single/dual-atom and cluster catalysts by taking advantage of structural features of MOFs. Current issues, promising ideas and future prospects for MOF-based single/dual-atom and cluster catalysts are given.

From metal–organic frameworks to single/dual-atom and cluster metal catalysts for energy applications

Single‐atom catalysts (SACs) have been rising recently as a new frontier in the catalysis field. Due to maximum atom utilization efficiency and tunable electronic structures, SACs exhibit highly distinctive catalytic performance from bulk counterparts. SACs with high metal loading will facilitate practical applications. To that end, this Review focuses on recent strategies to maximize metal loading. An appropriate substrate, mainly heteroatom‐doped carbon materials, is the key to avoiding aggregation or sintering during synthetic procedures. The coordination site construction and spatial confinement strategies are adopted to prepare SACs with high metal loading. Advanced characterization techniques with atomic resolution are indispensable for identification of the exact structure of SACs. This is true, especially for the applications and challenges in developing in situ/operando characterization techniques at the atomic level, which are discussed in this Review. Moreover, it is fundamentally necessary to investigate the active center structure, which facilitates any design of efficient SACs that can maximize single‐atom catalytic activity. Furthermore, this Review highlights challenges and prospects for development of SACs.

Synthesis of High Metal Loading Single Atom Catalysts and Exploration of the Active Center Structure

Interfacial processes in electrochemical energy systems

It has been determined that the exceptional characteristics of MXenes are of great interest in a variety of newly developed applications. MXenes, on the other hand, have a number of drawbacks, the most significant of which is that their general manufacturing in large-scale production requires the use of ecologically hazardous and poisonous compounds, as well as a solid-state reaction at high temperature, which is then followed by selective etching. In this regard, the manner in which MXenes are manufactured is critical to determining their final applications. Thus, it is very necessary to develop strategic ways to synthesize MXenes that are safer, greener, more ecologically friendly, and more sustainable in order to put them on the market at a competitive price. It is very necessary to assemble, review, and synthesize the most recent advancements in the green-related innovation of MXenes since there are a rising number of publications on green synthesis involving technological advances and non-toxic substances. Replacing traditional synthesis methods with green MXenes, physically based rapid generation of MAX phases, molten salt process for the green synthesis of MAX phases, nanoparticulate MAX phase based on the sol-gel process, HF etchant replacement with safer chemicals, electrochemical exfoliation, and nanobioagents can result in more environmentally friendly, efficient, and safer MXenes for future environmental, biomedicine, energy saving, catalysis, and sensors. Our primary focus is on the core synthetic procedure, the mechanism, and the overall benefits, with a particular emphasis on the MXene features that have been passed down from these green synthesis approaches. The growing uses green MXenes in the fields of environmental remediation, energy conversion and storage, and biomedicine are discussed in this article. In conclusion, the remaining obstacles and potential benefits of more environmentally friendly MXene production are reviewed. 

On the horizon of greener pathways to travel into a greener future portal: Green MXenes, environment-friendly synthesis, and their innovative applications

Light energy can be harnessed by photosensitizers or photocatalysts so that some chemical reactions can be carried out under milder conditions compared to the traditional heat-driven processes. To facilitate the photo-driven reactions, a large variety of chromophores that are operated via charge transfer excitations have been reported because of their typically longer excited-state lifetimes, which are the key to the downstream photochemical processes. Although both metal-to-ligand charge transfers and ligand-to-metal charge transfers are well-established light absorption pathways; the former has been widely adopted in photocatalysis, whereas the latter has recently taken on greater importance in photosensitization applications. In this article, we review the latest developments on ligand-to-metal charge transfer photosensitization by molecular complexes across the periodic table by focusing homogeneous photocatalysis and the use of photophysical measurements and computational calculations to understand the electronic structures, photochemical processes, structure–activity relationships, and reaction mechanisms. We also present our perspectives on the possible future developments in the field.

Emergence of ligand-to-metal charge transfer in homogeneous photocatalysis and photosensitization

Non-invasive in situ monitoring of catalyzed chemical reactions can show and probe the stability of the catalyst and ensure a high yield of the desired chemical processes. Infrared in situ measurem...

In Situ Infrared Spectroscopy as a Tool for Monitoring Molecular Catalyst for Hydroformylation in Continuous Processes

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In Situ Infrared Spectroscopy as a Tool for Monitoring Molecular Catalyst for Hydroformylation in Continuous Processes