Artificial light-harvesting systems based on supramolecular polymers ✩
English
Artificial light-harvesting systems based on supramolecular polymers ✩
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1. Introduction
The depletion of fossil fuels and mounting environmental concerns have intensified the search for sustainable energy alternatives. As an abundant and renewable resource, solar energy holds immense potential for addressing the global energy crisis [1,2]. To efficiently capture and utilize solar energy, researchers have developed artificial light-harvesting systems (LHSs) inspired by natural photosynthesis. These engineered systems are designed to absorb and convert light into usable energy, providing a sustainable route for energy generation. Enhancing the efficiency, stability, and scalability of artificial LHSs remains a key objective in advancing solar energy technologies. In recent years, significant progress has been made in constructing artificial LHSs that replicate the intricate supramolecular organization of their natural counterparts [3–7]. Various supramolecular frameworks, including macrocycles [8–12], cages [13–15], nanoparticles [16–21], biomacromolecules [22–25], and hybrid materials [26–30], have been employed to achieve this goal.
In recent years, numerous reviews have provided comprehensive overviews of various artificial LHSs. For instance, Xing et al. examined artificial LHSs and their applications in photocatalysis and cell labelling [31], while Li et al. focused on self-assembled artificial LHSs, detailing their construction, modulation, and practical uses [32]. Hu et al. reviewed supramolecular artificial LHSs for photocatalytic applications [33], and Matsubara et al. discussed biomimetic light-harvesting antennas formed through the self-assembly of chemically programmed chlorophylls [34]. Additionally, Mukherjee et al. highlighted LHSs based on Pt(Ⅱ)/Pd(Ⅱ)-based metallosupramolecular architectures [35]. Zhang, Luo et al. summarized supramolecular LHSs utilizing cucurbit[n]urils-based assemblies [36]. Despite these extensive reviews, no study has specifically addressed supramolecular polymer-based LHSs, leaving a critical gap in the literature. Supramolecular polymers represent a distinct class of materials that self-assemble through reversible non-covalent interactions, including multiple hydrogen bonding, host-guest interaction, and metal coordination [37–41]. Unlike conventional polymers, which rely on covalent linkages for structural integrity, these dynamic systems can spontaneously form and reorganize, giving rise to complex, hierarchical architectures. This intrinsic adaptability allows for precise control over their optical and electronic properties, making them highly suitable for artificial LHSs. By incorporating diverse chromophores, supramolecular polymers can be tailored to optimize light absorption and energy transfer efficiency. Their modular nature further facilitates the integration of multiple functional components, enabling the design of advanced LHSs with tunable spectral properties and improved stability. Additionally, their ability to mimic the natural organization of photosynthetic systems enhances their potential for sustainable energy applications. The versatility and responsiveness of supramolecular polymers position them as a promising platform for next-generation light-harvesting technologies.
Förster resonance energy transfer (FRET) plays a crucial role in artificial LHSs by enabling efficient energy transfer between chromophores within supramolecular polymers [42–45]. This non-radiative process occurs when an excited donor molecule transfers energy to an acceptor via dipole-dipole interactions. The efficiency of FRET is governed by several factors, including donor-acceptor distance, spectral overlap, and dipole orientation. To further enhance LHS performance, aggregation-induced emission (AIE) [46,47] luminogens such as tetraphenylethylene (TPE) [48,49] and cyanostilbene [50–55] derivatives are commonly employed as donors. These fluorophores exhibit increased emission in aggregated states, improving energy transfer efficiency. In 2020, Xu, Yang et al. summarized supramolecular artificial LHSs based on AIE [56]. Notably, supramolecular polymers not only activate AIE very efficiently [57], but also provide a well-organized molecular framework to optimize FRET by precisely arranging chromophores in close proximity. Through rational design, researchers can fine-tune chromophore positioning to maximize energy transfer, thereby improving light-harvesting efficiency and advancing the development of artificial LHSs.
This review provides a comprehensive examination of supramolecular polymer materials in artificial LHSs driven by FRET, with particular emphasis on their structural design, synthetic strategies, and functional modifications. The discussion is organized according to the principal non-covalent interactions facilitating self-assembly, including hydrogen bonding, metal coordination, host-guest chemistry, and the interplay of multiple supramolecular forces. Specifically, the article is divided into four main sections: (1) Supramolecular polymer-based LHSs driven by quadruple hydrogen bonding, (2) supramolecular polymer-based LHSs driven by host-guest interactions, (3) supramolecular polymer-based LHSs driven by metal coordination, and (4) supramolecular polymer-based LHSs driven by multiple non-covalent interactions. Each section explores how these interactions influence the optical properties of the polymers, focusing on strategies to enhance light absorption, energy transfer efficiency, and photostability. Furthermore, the review discusses the integration of supramolecular polymers with hybrid nanostructures, illustrating their ability to improve LHS performance through cooperative effects. The final section outlines future directions, emphasizing the need for novel molecular motifs, nature-inspired architectures, and sustainable synthesis approaches to drive progress toward real-world applications in solar energy harvesting and conversion.
2. Supramolecular polymer-based LHSs driven by quadruple hydrogen bonding
Quadruple hydrogen bonding, particularly that based on ureidopyrimidinone (UPy) [58], represents a robust and versatile non-covalent interaction with significant potential in supramolecular polymer design [59–62]. These interactions endow the resulting materials with dynamic reversibility and environmental responsiveness, making them ideal candidates for functional applications. In 2011, we introduced a supramolecular polymer featuring UPy-based quadruple hydrogen bonding and investigated its FRET properties (Fig. 1) [63]. The key monomer, M1, incorporates a photochromic dithienylethene core, enabling the formation of linear supramolecular polymers in concentrated solution. To further explore energy transfer behavior, we synthesized a mono-UPy fluorescent dye, F1, which was introduced in small amounts to cap the polymer chains. The resulting mixture was spin-coated to generate a homogeneous thin film. By leveraging spectral overlap between F1 and the closed form of M1, fluorescence quenching was achieved, enabling UV-vis-controlled fluorescence switching. This example is a prototype of a supramolecular polymer-based light-harvesting system.
Figure 1
Figure 1. (a) Chemical structure of monomer M1 and F1. (b) Absorption and fluorescence spectra. (c) FRET process of the thin film spin-coated from solutions of 97:3 M1–F1 under UV–vis irradiation. Reproduced with permission [63]. Copyright 2011, Wiley-VCH.In 2014, Yang et al. synthesized four ditopic UPy compounds that self-assembled into linear supramolecular polymers in chloroform [64]. Using a mini-emulsion technique assisted by cetyltrimethyl ammonium bromide (CTAB), these polymers were converted into water-dispersible nanospheres. To mimic natural LHS, the authors incorporated a mono-functionalized anthracene derivative with green fluorescence, selected for its optimal spectral overlap with the energy donor. By adjusting the donor-to-acceptor (D/A) ratios to 58:1, 88:1, and 176:1, they achieved antenna effects of 13, 20, and 29, respectively.
In 2019, the same group developed AIE materials, including nanoparticles (NPs), microfibers, and thin films, using a light-harvesting approach (Fig. 2) [65]. Supramolecular polymers comprising TPE and BODIPY chromophores facilitated efficient energy transfer, resulting in a sixfold enhancement in fluorescence intensity and a significant narrowing of the emission bandwidth, with the full width at half-maxima (FWHM) reduced from 148 nm to 32 nm (Fig. 2, inset). The fluorescence quantum yield was significantly increased from 12% (TPEH) to 27% (TPEH-RM) after light harvesting. These luminescent NPs have been applied in vitro and in vivo for fluorescence and chemiluminescence imaging. Additionally, high-colour-purity fluorescent fibres and films, spanning blue to deep red and even pure white emissions, were achieved through precise tuning of energy acceptors, expanding their potential for optoelectronic applications.
Figure 2
Figure 2. Schematic illustration of the preparation of AIE materials with light-harvesting properties, and chemical structures of the UPy-modified donors (TPEH, TPEP, and TPEDC) and acceptors (GM, YM, RM, and NIR-M). Inset: fluorescence spectra showing the narrowed emission band after light harvesting. Reproduced with permission [65]. Copyright 2019, American Chemical Society.In 2020, we developed a tunable LHS using supramolecular polymer NPs prepared via a mini-emulsion approach in aqueous media [66]. As depicted in Fig. 3, molecule M2 forms linear supramolecular polymers through quadrupole hydrogen bonding and subsequently assembles into NPs in water through mini-emulsion. Incorporating the hydrophobic dye Nile Red (NiR) yielded a binary chromophore system (M2-NiR) that efficiently facilitated FRET. The self-assembled nature of the NPs allowed precise compositional control while achieving high energy transfer efficiency (ΦET = 53.4%) and an antenna effect (AE = 28), leading to white light emission. This aqueous LHS serves as a versatile platform for artificial photosynthesis and luminescent material applications. Expanding on this strategy, in 2021, we developed another hydrogen bonding-driven LHS using a novel supramolecular monomer [67]. Assisted by surfactants, we fabricated water-dispersible NPs from supramolecular polymers composed of an AIE-active chromophore-bridged ditopic UPy. Introducing the hydrophobic chromophore naphthalene diimide (NDI) derivative as an energy acceptor enabled co-assembly within the nanocarrier, allowing continuous spectral tuning with minimal acceptor content. This system offers promising potential for dynamic luminescent materials.
Figure 3
Figure 3. Schematic illustration of the self-assembly of an artificial LHS based on M2 and NiR. Reproduced with permission [66]. Copyright 2020, Royal Society of Chemistry.In 2017, Guo et al. reported supramolecular color-tunable photoluminescent materials based on two-step FRET [68]. Building on this work and our previous work [66], we developed a two-step energy transfer LHS using the TPE-bridged UPy derivative (M2) as the donor and two hydrophobic dyes, 4,7-di(2-thienyl)-benzo[2,1,3]thiadiazole (DBT) and a synthetic fluorescent dye 2,6-disubstituted naphthalene diimide (NDI), as sequential acceptors [69]. Supramolecular polymeric NPs were fabricated via a mini-emulsion approach in aqueous media using CTAB, yielding a cyan-emissive solution. The quadruple hydrogen bonding interactions not only guided monomer assembly but also enhanced AIE properties. This LHS exhibited tunable fluorescence from blue to near-infrared, with the ability to generate pure white light. Notably, the system achieved a high antenna effect of 63 at a M2/DBT/NDI ratio of 1250:25:1. The cascading energy transfer within these supramolecular NPs offers a promising strategy for mimicking photosynthesis and developing tunable organic fluorescent materials.
Natural photosynthesis transfers excitation energy from antenna chromophores to the reaction center, driving electron transfer and converting light into chemical energy. In contrast, most artificial LHSs rely on FRET to enhance acceptor emission. In 2024, Niu, Yang, and co-workers introduced a supramolecular LHS integrating both excitation energy and electron transfer for photocatalysis [70]. This system utilized a UPy-functionalized TPE derivative as the antenna chromophore and an iodine-substituted boron-dipyrromethene (BODIPY) derivative as the acceptor. Quadruple hydrogen bonding-driven self-assembly yielded supramolecular NPs, where photoexcited donor efficiently transferred energy to the acceptor (ΦET = 95.3%). Simultaneously, the acceptor extracted an electron from the donor, generating radical ions that facilitated H2O2 production. Additionally, the LHS enabled photodynamic therapy by oxidizing 1,4-dihydronicotinamide adenine dinucleotide (NADH) to produce cytotoxic reactive oxygen species (ROS), effectively killing tumor cells. This work provides a blueprint for artificial LHSs with synergistic energy and electron transfer capabilities.
White-light emission in donor-acceptor systems typically requires high acceptor content or multiple acceptors. We addressed this challenge by designing a cyanostilbene-bridged UPy donor (CSU) that self-assembles into well-dispersed NPs [71]. The cyanostilbene core exhibits AIE activity, while UPy units drive supramolecular polymerization via quadruple hydrogen bonding. Using a mini-emulsion strategy, CSU-based supramolecular polymers form AIE-enhanced NPs. Pairing CSU with DBT as an acceptor enables efficient LHS formation in water, achieving white-light emission at an ultralow DBT content (A/D = 1/1000). This strategy offers promising applications in information encryption and white-light-emitting materials. In 2024, we built another two-step LHS system based on CSU NPs (Fig. 4) [72]. The integration of the primary acceptor, Eosin Y (ESY), and the secondary acceptor, NDI, into the NPs to form an efficient, sequential LHS. When CSU/ESY/NDI = 750/10/6, ΦET was determined to be 88.2% and the absolute fluorescence quantum yield was 25.3%, which is higher than that of CSU/ESY (65.4% and 19.1%, respectively). The emission region delineated by the CSU-ESY and CSU-ESY-NDI within the CIE (Commission Internationale de l’Eclairage) chromaticity space forms a triangle, indicating the potential for developing materials capable of emitting white light, which was realized with a molar ratio of CSU to ESY to NDI of 1000:5:1. Consequently, the work successfully demonstrated tuneable emission capabilities, encompassing the generation of white light.
Figure 4
Figure 4. Cartoon representation of the fabrication of a two-step energy transfer LHS from CSU, ESY, and NDI. Reproduced with permission [72]. Copyright 2024, Elsevier.3. Supramolecular polymer-based LHSs driven by host-guest interactions
Supramolecular macrocyclic hosts, including cyclodextrins, calix[n]arenes, cucurbit[n]urils, and pillar[n]arenes, play a crucial role in modulating the photophysical properties of organic dyes. These macrocycles provide well-defined nanocavities that encapsulate guest molecules, suppressing non-radiative decay pathways and enhancing fluorescence efficiency [73–75]. Additionally, host-guest interactions can influence the molecular conformation and aggregation state of the dyes, significantly altering their emission behavior. By tuning intermolecular and intramolecular charge transfer interactions, macrocyclic hosts enable precise fluorescence modulation. Beyond fluorescence enhancement, host-guest complexation promotes intersystem crossing, stabilizes triplet excitons, and enhances room-temperature phosphorescence, expanding the functionality of luminescent systems [76]. Leveraging these properties, artificial LHSs have been developed using macrocyclic host-guest chemistry, providing a versatile strategy for optimizing light-harvesting efficiency and energy transfer processes [77–80]. These supramolecular architectures hold promise for advanced photofunctional materials, particularly in optoelectronic and photocatalytic applications.
3.1 Light-harvesting supramolecular polymers based on CB[n]
Cucurbit[n]urils (CB[n]s), a family of macrocyclic hosts with a distinctive pumpkin-like structure, exhibit exceptional host–guest interactions in aqueous environments, making them valuable in supramolecular chemistry [81,82]. In 2022, Liu and co-workers developed tunable solid-state room-temperature phosphorescent (RTP) materials by incorporating CB[7] into acrylamide-based polymers functionalized with 4-phenylpyridine derivatives (Fig. 5) [83]. These supramolecular RTP assemblies exhibit ultralong phosphorescence lifetimes ranging from 0.9 s to 2.2 s, achieved through precise modulation of intersystem crossing and exciton relaxation pathways. Beyond serving as efficient RTP emitters, these supramolecular polymers enable the construction of ternary systems featuring phosphorescent energy transfer (ET, efficiency up to 68.9%). Upon integration with acceptor dyes such as sulforhodamine 101 (SR101) or ESY, the RTP donors facilitate ultralong RTP-ET, leading to delayed fluorescence emission from the dyes. By varying the acceptor ratio, tunable multicolor persistent luminescence is realized. This study presents a versatile strategy for designing long-lived RTP materials and optimizing phosphorescent ET systems for advanced optical applications.
Figure 5
Figure 5. The schematic illustration of tunable second-level RTP of solid supramolecules between acrylamide–phenylpyridinium copolymers and CB[7]. Reproduced with permission [83]. Copyright 2022, Wiley.Cucurbit[8]uril (CB[8])-based host–guest interactions, characterized by their unique 1:2 binding mode, serve as a powerful driving force for constructing supramolecular organic frameworks (SOFs). These SOF materials provide a robust platform for designing artificial LHSs [84]. To investigate their potential in photocatalysis, Xing and co-workers reported a CB[8]-templated SOF-based LHS in 2023, leveraging TPE-derived guests to enhance aerobic cross-dehydrogenative coupling (CDC) reactions in aqueous media (Fig. 6) [85]. Two TPE derivatives, MV-TPE (bearing four methylated viologen units) and NA-TPE (functionalized with four methoxynaphthyl groups), were synthesized and self-assembled into SOFs via CB[8]-mediated host–guest interactions. The incorporation of fluorescent dyes DBT and SR101 as sequential energy acceptors enabled efficient two-step energy transfer within the SOF framework. The ΦET and the antenna effect of the energy transfer process from the SOF to DBT were calculated to be 70.2% and 12.3, respectively. Moreover, the ΦET of the second energy transfer was 44.5% and the antenna effect was 1.8. This system functioned as a photocatalyst, achieving an 87% yield in the aerobic CDC reaction. The study highlights the potential of SOF-based LHSs for photocatalytic applications, offering a new strategy for supramolecular catalysis.
Figure 6
Figure 6. Schematic illustration of the construction of artificial LHS based on MV-TPE, NA-TPE and CB[8] and its photocatalytic CDC coupling reaction. Reproduced with permission [85]. Copyright 2023, Royal Society of Chemistry.Most SOFs rely on high-energy ultraviolet or blue light for photocatalytic reactions [85,86]. In 2023, Xing and co-workers utilized host-guest interactions between a triphenylamine derivative (TP-3Py) and CB[8] to fabricate a water-soluble, two-dimensional (2D) SOF (TP-SOF) [87]. The 2D structure forms due to the synergistic effect of head-to-tail stacking between the vinylpyridine groups of TP-3Py and CB[8], resulting in strong green light absorption. This system efficiently generates singlet oxygen (1O2) and promotes the photocatalytic oxidation of thioanisole in water. Compared to the TP-3Py monomer, the confinement within CB[8] enhances the production of superoxide anion radicals (O2•−), boosting the oxidative hydroxylation of arylboronic acids. This reaction under green light achieved a high yield of 91%. This study demonstrates the potential of triphenylamine-based SOFs in low-energy photocatalysis, offering new insights into their application in oxidation reactions under green light.
3.2 Light-harvesting supramolecular polymers based on pillar[n]arene
Pillar[n]arenes are a class of supramolecular macrocycles composed of dialkoxybenzene units interconnected by methylene bridges at the para-positions [88,89]. Their unique dynamic structure provides exceptional host–guest complexation properties, making them versatile for a range of applications in supramolecular chemistry [90]. Our group was among the first to explore light-harvesting supramolecular polymers based on pillar[n]arenes. In 2015, we developed a novel system consisting of BODIPY-bridged guests and BODIPY-derived pillar[5]arene dimers. This system was designed to mimic natural LHS in organic media, marking a significant advancement in the development of artificial LHS for energy capture and conversion [91]. In 2016, Diao and co-workers reported stimulus-responsive light-harvesting complexes formed through the pillar[5]arene-induced co-assembly of β-carotene and chlorophyll. This work highlighted the potential of supramolecular strategies to modulate light-harvesting efficiency in response to external stimuli [92]. In 2018, Yang and co-workers reported the creation of water-dispersible artificial light-harvesting NPs using pillar[5]arene-based supramolecular polymers [93]. The system exhibited efficient energy transfer, aided by steric bulk preventing chromophore self-quenching.
Given the desirable properties of supramolecular chemistry and the inherent stability of covalent polymers, both of which are essential for the development of functional materials, the incorporation of polymer hosts bearing multiple synthetic macrocycles on their side chains offers potential advantages. In 2019, Tang, Yang and co-workers synthesized a novel class of linear copolymer hosts (Fig. 7) [94]. Pillar[5]arene units are incorporated into the long chains of linear copolymers as host sites (poly-P[5]A), while a multifunctional TPE derivative (TPE-(TA-CN)4) serves as the guest molecule. Through host-guest interactions, a supramolecular polymer network (SPN) is formed, leading to the construction of an efficient and tunable artificial LHS. The SPN increases the density of pillar[5]arene macrocycles, allowing closer binding of the TPE derivatives within the polymer network. The resulting supramolecular assemblies exhibit strong fluorescence with a quantum yield of 98.22%. By introducing a yellow-emitting fluorescent molecule, DSA-(TA-CN)2, into the SPN, spherical supramolecular NPs with tunable colors, from cold to warm tones, were obtained. This approach not only introduces a novel concept of polymer hosts but also enables the fabrication of color-tunable LHSs, offering potential applications in sensing, bio-probing, and optoelectronics.
Figure 7
Figure 7. Schematic illustration of the fabrication of LHS by using polymer host materials. Reproduced with permission [94]. Copyright 2019, Wiley-VCH.In 2020, Tang, Cao, Tang, and colleagues reported an artificial LHS with unprecedented antenna effects based on a conjugated polymeric supramolecular network (CPSN) [95]. As depicted in Fig. 8a, they constructed the CPSN via the self-assembly of a conjugated polymeric host (CPH) containing pillar[5]arenes and TPE units with ditopic guest molecules (GR, GB, GY). The TPE moieties served as both antennae and donors, while the guests acted as acceptors. Notably, the absorption spectra of GR and GY displayed strong overlap with the emission profile of the CPH, enabling favorable spectral conditions for energy transfer. In contrast, the spectral mismatch between the CPH emission and GB absorption suggested limited energy transfer efficiency in that case (Fig. 8b). Consequently, efficient donor-to-acceptor energy transfer was anticipated for the GR- and GY-containing systems, provided spatial proximity between host and guest units was achieved within the CPSN framework. The resulting network enabled efficient energy transfer, yielding tunable multicolor fluorescence that covered 96% of the CIE chromaticity diagram, including pure white-light emission at (0.33, 0.33). Notably, the LHS demonstrated exceptional antenna effects, reaching 35.9 in solution and 90.4 in solid films. This study presents a viable approach for engineering highly luminescent materials. Ongoing research aims to enhance artificial LHSs using conjugated frameworks, which facilitate energy transfer but suffer from aggregation-caused quenching (ACQ). To address this, the same group developed an assembly-induced-emission orthogonal supramolecular network (AOSN) [96]. Comprising a tetratopic conjugated host with pillar[5]arene units and a spirobifluorene core, along with ditopic guests, AOSN achieves efficient sequential energy transfer. Notably, its antenna effect exceeds 60, attributed to host-guest interactions, spirobifluorene rigidity, and donor-acceptor spectral overlap.
Figure 8
Figure 8. (a) Schematic illustration of LHS based on conjugated polymer host (CPH). (b) Normalized fluorescence spectra (dashed curves) of CPH, GY, GR and GB, and their normalized absorbance spectra (solid curves). Reproduced with permission [95]. Copyright 2020, Wiley-VCH.4. Supramolecular polymer-based LHSs driven by metal coordination
Metal-coordination bonds exhibit high directionality and controllability [97,98], making them valuable for constructing metallosupramolecular architectures in artificial LHSs [35,99]. Metalloporphyrins assemble into ordered structures via axial coordination. In 2015, Lee, Jang, and co-workers reported artificial light-harvesting dendrimers with zinc porphyrin units linked to a freebase porphyrin core [100]. These dendrimers exhibited efficient energy transfer, while their assembly with pyridine-functionalized porphyrins enabled a transition from energy to electron transfer, offering tunable optical and electronic properties.
Metal-coordinated supramolecular polymers offer high surface area, ordered porosity, and stability, making them ideal for artificial LHSs. Mukherjee and colleagues synthesized a TPE-based Pt(Ⅱ) coordination polymer via self-assembly between a TPE-tetraimidazole donor (M3) and a trans-[Pt-(PEt3)2(OTf)2] acceptor (Fig. 9a) [101]. The donor exhibited strong fluorescence in water/DMSO (fw = 90%) and formed NPs capable of encapsulating organic dyes for LHS construction. Using ESY (Fig. 9b) and NiR (Fig. 9c) as acceptors enabled two-step sequential FRET, shifting fluorescence from blue to yellow (λem = 553 nm) and then pink. Energy transfer efficiencies reached 58.8% and 68.5%, respectively. This study highlights the potential of coordinated supramolecular polymers in designing efficient LHSs.
Figure 9
Figure 9. (a) Schematic representation of supramolecular coordination polymer-based artificial LHS with two-step energy transfer. (b) Fluorescence spectra of the polymer with gradual addition of ESY. (c) Fluorescence spectra of (polymer + ESY) with gradual addition of NiR. Reproduced with permission [101]. Copyright 2022, American Chemical Society.5. Supramolecular polymer-based LHSs driven by multiple non-covalent interactions
Light-harvesting supramolecular polymers typically rely on a single non-covalent interaction for self-assembly. However, some systems incorporate multiple interactions. For instance, in 2016, Zhou, Yan et al. synthesized dandelion-like supramolecular polymers by coupling β-cyclodextrin-functionalized hyperbranched polymers with adamantane-functionalized guests [102]. These polymers self-assembled into nanotubes in water, forming a bilayer structure with hydrophobic-hyperbranched-hydrophilic layers. The hydrophobic donors within the nanotube core and hydrophilic acceptors on the surface offer significant potential for aqueous LHSs. In 2019, Ouyang, Liu et al. introduced a supramolecular light-harvesting nanotube constructed from a cyanostilbene-functionalized glutamate derivative [103]. This system exhibited cooperative chirality and facilitated sequential FRET, demonstrating the potential of rational molecular design in enhancing light-harvesting efficiency. This section explores artificial LHSs constructed via multiple supramolecular interactions in recent years.
Rotaxane-based dendrimers represent a fascinating class of supramolecular polymers characterized by interlocked molecular architectures, where a macrocyclic component encircles a linear thread. This unique structure imparts dynamic properties, such as restricted motion and enhanced stability, making rotaxane dendrimers highly attractive for functional materials. Recently, Wang, Yang, and co-workers synthesized a novel series of AIEgen-branched rotaxane dendrimers using a controlled divergence strategy based on metal coordination (Fig. 10) [104]. These dendrimers served as efficient platforms for constructing artificial LHSs. The first-generation dendrimer (TG1) was synthesized from 1,3,5-triethynylbenzene and a TPE-based rotaxane featuring a pillar[5]arene macrocycle. Further expansion yielded the third-generation dendrimer (TG3), incorporating 21 TPE units at the dendritic periphery. The addition of MeOH as a poor solvent induced molecular backbone movement and aggregation, enhancing emission and promoting energy transfer. Incorporating ESY as an acceptor enabled efficient energy harvesting. Notably, the antenna effect values for the TGn-ESY systems (n = 1, 2, 3) were determined to be 1.1 for TG1-ESY, 2.3 for TG2-ESY, and 4.1 for TG3-ESY. These results clearly demonstrate a progressive enhancement in light-harvesting efficiency with increasing dendrimer generation of the TPE-branched rotaxane structure. The resulting LHS demonstrated high photocatalytic activity in aerobic CDC and photooxidation reactions. This study establishes AIEgen-branched rotaxane dendrimers as promising candidates for artificial LHSs in photocatalysis.
Figure 10
Figure 10. Schematic illustration of a LHS based on a TPE-branched rotaxane dendrimer and its photocatalytic oxidation and CDC reaction. Reproduced with permission [104]. Copyright 2021, Wiley-VCH.Cyclopeptide-polymer conjugates form supramolecular polymers through strong hydrogen bonding between cyclic peptide rings. Conjugating hydrophilic polymers enhances solubility and prevents aggregation, leading to stable nanotube assemblies. Inspired by this, Perrier and colleagues (2021) developed an artificial LHS using cyclic peptide-polymer conjugates with hydrophobic chromophores [105]. Three fluorophore-attached conjugates enabled a two-step sequential FRET process in water. By tuning their ratios, emission was modulated from blue to orange, including white light with a 29.9% quantum yield. This system offers a promising strategy for luminescent applications.
In 2024, Song and co-workers introduced a cyclic peptide (CP)-based supramolecular scaffold enabling multi-step sequential FRET in water [106]. As illustrated in Fig. 11, five fluorophores were rationally selected and conjugated to CP to obtain the corresponding fluorophore-CP polymer conjugates (denoted as DPA-CP-PEG) or fluorophore-CP conjugates (denoted as Cou343-CP, Cy3-CP, Cy5-CP, Cy7-CP). Co-assembly of these units positioned the fluorophores along nanotubes, ensuring efficient spectral overlap for up to four consecutive FRET steps. The resulting LHS exhibited remarkable energy transfer efficiencies (≥90%) and fluorescence quantum yields (17.6%–58.4%). In-depth studies of these artificial LHS elucidated the associated energy transfer pathways and indicated the presence of additional energy transfer processes beyond the targeted sequential energy transfer. This comprehensive analysis highlights the potential of CP-based supramolecular scaffolds as a powerful platform for developing high-performance cascaded LHS.
Figure 11
Figure 11. Cartoon representation of an artificial LHS with multi-step FRET constructed from cyclic peptides. Reproduced with permission [106]. Copyright 2024, Wiley-VCH.In photosynthetic organisms, rigid protein scaffolds precisely arrange pigments to optimize excitation energy transfer. However, most artificial LHSs exhibit an overall energy transfer efficiency (Φoverall) below 70%, far lower than the nearly 100% efficiency in purple photosynthetic bacteria. This inefficiency stems from disordered donor-acceptor (D/A) arrangements. Inspired by bacterial chlorophyll packing, Wang and co-workers designed a two-step LHS using π-stacked σ-platinum-complexed (hetero)acenes [107]. These monomers self-assemble in apolar solvents via strong π-stacking interactions, reinforced by hydrogen bonding from amide groups (Fig. 12). The Pt(Ⅱ) centers prevent ACQ by maintaining intermolecular spacing, preserving fluorescence. Due to their structural compatibility, donor and acceptor monomers co-aggregate into supramolecular copolymers, enabling efficient D/A energy transfer. This system achieves an extended exciton diffusion length, enhanced migration rates, and a Φoverall of 87.4%. This work demonstrates the power of supramolecular design in constructing high-performance LHSs and provides a blueprint for advancing artificial photosynthetic materials.
Figure 12
Figure 12. Supramolecular copolymerization of 1, 2, and 3 with the sequential FRET behaviours. Reproduced with permission [107]. Copyright 2022, Nature Publishing Group.Lanthanide complexes exhibit excellent photophysical properties, including large Stokes shifts, sharp emission bands, and long-lived excited states. However, their excited states are easily quenched by water molecules and chelating ligands, limiting their tunability in aqueous environments. Achieving full-color emission from a single lanthanide ion in water remains challenging. To address this, Zhang, Liu, and co-workers developed a supramolecular lanthanide assembly integrating host-guest phosphorescence with intrinsic lanthanide luminescence [108]. As shown in Fig. 13a, bromobenzylpyridinium-based guests (PY-DPA) form stable pseudorotaxanes with CB[8], shifting fluorescence from blue to green phosphorescence in water. Additionally, europium ion (Eu3+) coordination triggers intramolecular energy transfer, significantly enhancing Eu3+ luminescence. By adjusting Eu3+/CB[8] ratios, the system achieves tunable full-color emission, including white light, and enables multicolor cellular imaging (Figs. 13b and c). This work provides a novel strategy for designing versatile luminescent materials and advanced bioimaging probes.
Figure 13
Figure 13. (a) Schematic illustration of a lanthanide noncovalent SP for tuneable full-colour emission. (b) 1.0 equiv. of CB[8] upon gradual addition 1/3 equiv. of Eu3+ in H2O. (c) The 1931 CIE chromaticity diagram illustrating the luminescent color changes of PY-DPA with the addition of Eu3+ and CB[8]. Reproduced with permission [108]. Copyright 2022, Royal Society of Chemistry.In 2024, Li, Yang, Yao and co-workers designed a recyclable artificial light-harvesting supramolecular polymer based on pillar[5]arene for photocatalytic applications (Fig. 14) [109]. The fluorescent supramolecular polymer, (P5Py2/Zn/Gen)n, was constructed via orthogonal self-assembly using pillar[5]arene-based host-guest interactions and metal ion coordination. In this system, the Gen unit functions as the light-harvesting chromophore, stabilized against ACQ by the rigid pillar[5]arene cavity, while the (Py)2/Zn complex serves as the catalytic site. This cooperative assembly enhances donor-acceptor stability, facilitating efficient photocatalytic reduction of p-nitrophenol to p-aminophenol. Notably, the catalyst retained high activity after five reuse cycles. Additionally, its performance was evaluated across various nitroaromatic substrates, highlighting its broad applicability. This work presents a promising strategy for developing recyclable artificial light-harvesting systems that emulate key aspects of natural photosynthesis, offering insights into supramolecular approaches for sustainable photocatalysis.
Figure 14
Figure 14. Schematic illustration of the construction of light-harvesting supramolecular polymers and their application in the photocatalytic reduction of nitroaromatics. Reproduced with permission [109]. Copyright 2024, Elsevier.Bacteriochlorophyll (BChl) α naturally assembles into curved columns along a ring-shaped axis with the aid of polypeptides and carotenoids. This arrangement enables strong intermolecular interactions, promoting exciton delocalization and enhancing energy diffusion for efficient Förster resonance energy transfer (FRET) to the reaction center. Inspired by this biological architecture, Tian and co-workers developed a discotic columnar liquid crystalline polymer (PTCS) that functions as a donor within a supramolecular columnar assembly (Fig. 15) [110]. By incorporating the acceptor NiR, they achieved an exceptionally high donor-to-acceptor (D/A) ratio of 20,000:1 and an antenna effect surpassing 100, demonstrating remarkable light-harvesting efficiency. The liquid crystalline state and polymerization-induced intercolumnar interactions optimize energy migration, effectively replicating the hierarchical organization of purple photosynthetic bacteria. Furthermore, the modular donor-acceptor assembly enables dynamic full-color tuning, supporting multi-level information encryption with spatiotemporal control. This system offers a promising platform for advanced photonic applications, particularly in secure data storage and encryption technologies.
Figure 15
Figure 15. Schematic diagram of the preparation and regulation of discotic columnar liquid crystalline polymer (PTCS) for light harvesting. Reproduced with permission [110]. Copyright 2024, Springer Nature.When combined with polyelectrolytes, AIE molecules can form supramolecular polymer networks that enhance emission properties. Polyelectrolytes like poly(sodium 4-styrenesulfonate) (PSS) offer a flexible platform for co-assembling with charged luminophores, improving both the stability and fluorescence of the system. Such assemblies are ideal for developing artificial LHSs due to their cost-effectiveness and environmentally friendly processing methods. Xing and co-workers recently reported polyelectrolyte-based supramolecular LHSs [111–113], while our own research led to the development of a system based on polyacrylic acid and a cyanostilbene derivative [114]. In a subsequent study (Fig. 16), a novel TPE derivative, TPEN, was synthesized and co-assembled with PSS to enhance fluorescence [115]. This PSS⊃TPEN network increased blue emission, which, when combined with the energy-matched dye DBT, generated a yellow-emitting LHS. This LHS showed remarkable antenna effect (16.9) and energy transfer efficiency (74.8%). This system was further successfully applied to color-tunable LED devices, offering a promising and sustainable approach for the development of advanced luminescent materials and energy-efficient lighting technologies.
Figure 16
Figure 16. (a) Schematic illustration of the construction of an artificial LHS based on TPEN, PSS, and DBT. (b) Normalized absorption spectrum of DBT and emission spectrum of PSS⊃TPEN. (c) Fluorescence spectra of PSS⊃TPEN in water with varying concentrations of DBT. Reproduced with permission [115]. Copyright 2025, Wiley-VCH.6. Conclusions
In summary, this review highlights the pivotal role of supramolecular polymers in advancing artificial light-harvesting systems by leveraging their dynamic self-assembly and modular design. Three key advantages underscore their superiority: (1) The inherent tunability of non-covalent interactions enables precise control over chromophore arrangement, facilitating broad-spectrum light absorption and directional energy transfer. (2) Their self-healing and adaptive properties enhance photostability and fault tolerance under continuous irradiation, addressing common degradation issues in static systems. (3) Integration with nanomaterials (e.g., NPs, frameworks) allows hybrid architectures to synergistically combine multiple energy conversion pathways, achieving excellent energy transfer efficiencies. These features position supramolecular polymers as versatile platforms for mimicking natural photosynthesis while enabling tailored functionalities.
Despite progress, challenges persist in translating laboratory-scale success to practical applications. First, achieving long-term stability in diverse environments remains hindered by the labile nature of non-covalent bonds. Second, scalability is limited by the difficulty in controlling hierarchical assembly across multiple length scales reproducibly. Third, quantitative models linking molecular design to macroscopic photophysical outcomes are underdeveloped, complicating rational optimization. Future efforts should prioritize bio-inspired motifs (e.g., excitonically coupled arrays) and sustainable synthesis routes, coupled with advanced characterization tools to unravel assembly-energy transfer correlations. By addressing these gaps, supramolecular LHSs could revolutionize solar energy conversion, photocatalysis, photonic devices, and beyond.
Declaration of competing interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
CRediT authorship contribution statement
Qunpeng Duan: Writing – original draft, Funding acquisition, Conceptualization. Qiaona Zhang: Writing – original draft. Jiayuan Zhang: Writing – original draft. Shihao Lin: Writing – original draft. Tangxin Xiao: Writing – review & editing, Supervision, Project administration, Conceptualization. Leyong Wang: Writing – review & editing, Supervision, Funding acquisition.
Acknowledgments
This work was supported by Henan Province Science and Technology Research Program (No. 252102320064) and the Innovation Support Program of Jiangsu Province (No. BZ2023055). We also acknowledge the Postgraduate Research & Practice Innovation Program of Jiangsu Province (No. KYCX24_3184).
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Figure 1 (a) Chemical structure of monomer M1 and F1. (b) Absorption and fluorescence spectra. (c) FRET process of the thin film spin-coated from solutions of 97:3 M1–F1 under UV–vis irradiation. Reproduced with permission [63]. Copyright 2011, Wiley-VCH.
Figure 2 Schematic illustration of the preparation of AIE materials with light-harvesting properties, and chemical structures of the UPy-modified donors (TPEH, TPEP, and TPEDC) and acceptors (GM, YM, RM, and NIR-M). Inset: fluorescence spectra showing the narrowed emission band after light harvesting. Reproduced with permission [65]. Copyright 2019, American Chemical Society.
Figure 3 Schematic illustration of the self-assembly of an artificial LHS based on M2 and NiR. Reproduced with permission [66]. Copyright 2020, Royal Society of Chemistry.
Figure 4 Cartoon representation of the fabrication of a two-step energy transfer LHS from CSU, ESY, and NDI. Reproduced with permission [72]. Copyright 2024, Elsevier.
Figure 5 The schematic illustration of tunable second-level RTP of solid supramolecules between acrylamide–phenylpyridinium copolymers and CB[7]. Reproduced with permission [83]. Copyright 2022, Wiley.
Figure 6 Schematic illustration of the construction of artificial LHS based on MV-TPE, NA-TPE and CB[8] and its photocatalytic CDC coupling reaction. Reproduced with permission [85]. Copyright 2023, Royal Society of Chemistry.
Figure 7 Schematic illustration of the fabrication of LHS by using polymer host materials. Reproduced with permission [94]. Copyright 2019, Wiley-VCH.
Figure 8 (a) Schematic illustration of LHS based on conjugated polymer host (CPH). (b) Normalized fluorescence spectra (dashed curves) of CPH, GY, GR and GB, and their normalized absorbance spectra (solid curves). Reproduced with permission [95]. Copyright 2020, Wiley-VCH.
Figure 9 (a) Schematic representation of supramolecular coordination polymer-based artificial LHS with two-step energy transfer. (b) Fluorescence spectra of the polymer with gradual addition of ESY. (c) Fluorescence spectra of (polymer + ESY) with gradual addition of NiR. Reproduced with permission [101]. Copyright 2022, American Chemical Society.
Figure 10 Schematic illustration of a LHS based on a TPE-branched rotaxane dendrimer and its photocatalytic oxidation and CDC reaction. Reproduced with permission [104]. Copyright 2021, Wiley-VCH.
Figure 11 Cartoon representation of an artificial LHS with multi-step FRET constructed from cyclic peptides. Reproduced with permission [106]. Copyright 2024, Wiley-VCH.
Figure 12 Supramolecular copolymerization of 1, 2, and 3 with the sequential FRET behaviours. Reproduced with permission [107]. Copyright 2022, Nature Publishing Group.
Figure 13 (a) Schematic illustration of a lanthanide noncovalent SP for tuneable full-colour emission. (b) 1.0 equiv. of CB[8] upon gradual addition 1/3 equiv. of Eu3+ in H2O. (c) The 1931 CIE chromaticity diagram illustrating the luminescent color changes of PY-DPA with the addition of Eu3+ and CB[8]. Reproduced with permission [108]. Copyright 2022, Royal Society of Chemistry.
Figure 14 Schematic illustration of the construction of light-harvesting supramolecular polymers and their application in the photocatalytic reduction of nitroaromatics. Reproduced with permission [109]. Copyright 2024, Elsevier.
Figure 15 Schematic diagram of the preparation and regulation of discotic columnar liquid crystalline polymer (PTCS) for light harvesting. Reproduced with permission [110]. Copyright 2024, Springer Nature.
Figure 16 (a) Schematic illustration of the construction of an artificial LHS based on TPEN, PSS, and DBT. (b) Normalized absorption spectrum of DBT and emission spectrum of PSS⊃TPEN. (c) Fluorescence spectra of PSS⊃TPEN in water with varying concentrations of DBT. Reproduced with permission [115]. Copyright 2025, Wiley-VCH.
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