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Over the past few decades, the design and construction of high-efficiency artificial light-harvesting systems (LHSs) involving multistep fluorescence-resonance energy transfer (FRET) processes have gradually received considerable attention within wide fields ranging from supramolecular chemistry to chemical biology and even materials science. Herein, through coordination-driven self-assembly, a novel tetragonal prismatic metallacage featuring a FRET process using tetraphenylethene (TPE) units as donors and BODIPY units as acceptors has been conveniently synthesized. Subsequently, taking advantage of supramolecular hydrophobic interactions, a promising artificial LHS involving two-step FRET processes from TPE to BODIPY and then to Nile Red (NiR) has been successfully fabricated in an aqueous solution using the FRET-featuring metallacage, NiR, and an amphiphilic polymer (mPEG-DSPE). Notably, this obtained aqueous LHS exhibits highly efficient photocatalytic activity in the dehalogenation of a bromoacetophenone derivate. This study provides a unique strategy for fabricating artificial LHSs in aqueous solutions with multistep FRET processes and further promotes the future development of mimicking the photosynthesis process.

During past few years, the construction of fluorescent metallacycles featuring the fluorescence-resonance energy transfer behavior has attracted extensive attention due to their diverse applications such as real-time monitoring the dynamics of coordination-driven self-assembly, photoswitching fluorescence-resonance energy transfer, and light-controlled generation of singlet oxygen for cancer therapy. This review focuses on the recent advances on the design principles, preparation methods, optical properties, and the wide applications of fluorescent metallacycles with the FRET property.

During the past few years, the construction of naphthalene diimide (NDI)- and perylene diimide (PDI)-based cages has attracted increasing attention due to the unique photo- and electrochemical properties and widespread applications of these materials in catalysis, chemical separation, sensing, etc. Thus, it is the right time to summarize the recent development of NDI-/PDI-based cages. In this review, the preparations, properties, and applications of NDI-/PDI-based cages in catalysis, chemical separation, and sensing will be discussed.

Attributed to their synthetic accessibility, unique structural and intriguing photophysical features, pyrene moieties have recently been introduced into supramolecular coordination complexes (SCCs) such as metallocycles and metallocages as either functional groups or key panels. The resultant pyrene-based SCCs displayed not only attractive emission properties but also impressive binding abilities towards diverse guests, endowing them with wide applications in sensing, host–guest chemistry, light harvesting etc. In this review, a comprehensive summary of pyrene-based metallocycles and metallocages is presented, and the emphasis will be on the intriguing photophysical features and unique host–guest chemistry that the pyrene moieties bring to the SCCs.

During the past few decades, fabrication of multistep fluorescence-resonance energy transfer (FRET) systems has become one of the most attractive topics within supramolecular chemistry, chemical biology, and materials science. However, it is challenging to efficiently prepare multistep FRET systems with precise control of the distances between locations and the numbers of fluorophores. Herein we present the successful fabrication of a two-step FRET system bearing specific numbers of anthracene, coumarin, and BODIPY moieties at precise distances and locations through an efficient and controllable orthogonal self-assembly approach based on metal-ligand coordination and host-guest interactions. Notably, the photosensitization efficiency and photooxidation activity of the two-step FRET system gradually increased with the number of energy transfer steps. For example, the two-step FRET system exhibited 1.5-fold higher 1O2 generation efficiency and 1.2-fold higher photooxidation activity than that of its corresponding one-step FRET system. This research not only provides the first successful example of the efficient preparation of multistep FRET systems through orthogonal self-assembly involving coordination and host-guest interactions but also pushes multistep FRET systems toward the application of photosensitized oxidation of a sulfur mustard simulant.

In the past few decades, the construction of discrete supramolecular double-metallacycles has attracted wide interest because of their unique structures and their potential applications in photoelectric materials. Since some progress has been made in this area, it is time to summarize the progress of discrete supramolecular double-metallacycles. In this review, we will briefly introduce the synthetic strategy of discrete supramolecular double-metallacycles. In addition, we will discuss the design principles, preparation methods, optical properties, and functions of these discrete supramolecular double-metallacycles.