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Spin-based sensors have attracted considerable attention owing to their high sensitivities. Herein, we developed a metallofullerene-based nano spin sensor to probe gas adsorption within porous organic frameworks. For this, spin-active metallofullerene, Sc 3 C 2 @C 80, was selected and embedded into a nanopore of a pyrene-based covalent organic framework (Py-COF). Electron paramagnetic resonance (EPR) spectroscopy recorded the EPR signals of Sc 3 C 2 @C 80 within Py-COF after adsorbing N 2 , CO, CH 4 , CO 2 , C 3 H 6 , and C 3 H 8 . Results indicated that the regularly changing EPR signals of embedded Sc 3 C 2 @C 80 were associated with the gas adsorption performance of Py-COF. In contrast to traditional adsorption isotherm measurements, this implantable nano spin sensor could probe gas adsorption and desorption with in situ, real-time monitoring. The proposed nano spin sensor was also employed to probe the gas adsorption performance of a metal–organic framework (MOF-177), demonstrating its versatility. The nano spin sensor is thus applicable for quantum sensing and precision measurements. Spin-based sensors have attracted attention due to their high sensitivities. Here authors present a fullerene-based nano spin sensor for in-situ sensing of gas adsorption in porous organic frameworks, demonstrating the potential applications of molecular spin systems in quantum sensing.

Spin-active materials with sensitive electron spin centers have drawn significant attention in quantum sensing due to their unique quantum characteristics. Herein, we report a molecular spin sensor based on metallofullerene Y 2 @C 79 N for in-situ monitoring of crystallization behavior and phase transitions in aromatic materials with high precision. Temperature-dependent spin resonance signals of Y 2 @C 79 N dissolved in aromatic materials are analyzed using electron paramagnetic resonance (EPR) spectroscopy. Two functional aromatic materials, 1-chloronaphthalene and a liquid crystal material of 5CB, are selected based on their significant crystallization-related technological applications. For Y 2 @C 79 N in 1-chloronaphthalene, a distinct EPR signal transition attributed to the crystallization of 1-chloronaphthalene. For Y 2 @C 79 N in 5CB, three EPR signal transitions correspond to the phase transitions of crystalline 5CB. Theoretical calculations reveal that the sensing mechanism originates from crystallization-induced alignment of fullerene molecular orientation. This work establishes metallofullerene-based spin probes as a powerful analytical tool for detecting the crystallization processes in materials. Spin-active materials with sensitive electron spin centers have drawn significant attention in quantum sensing due to their unique quantum characteristics. Herein, the authors report a molecular spin sensor based on metallofullerene Y 2 @C 79 N for in-situ monitoring of crystallization behavior and phase transitions in aromatic materials with high precision.

The design and fabrication of intricate hollow architectures as cost-effective and dual-function electrocatalyst for water and urea electrolysis is of vital importance to the energy and environment issues. Herein, a facile solvothermal strategy for construction of Prussian-blue analogue (PBA) hollow cages with an open framework was developed. The as-obtained CoFe and NiFe hollow cages (CFHC and NFHC) can be directly utilized as electrocatalysts towards oxygen evolution reaction (OER) and urea oxidation reaction (UOR) with superior catalytic performance (lower electrolysis potential, faster reaction kinetics and long-term durability) compared to their parent solid precursors (CFC and NFC) and even the commercial noble metal-based catalyst. Impressively, to drive a current density of 10 mA cm −2 in alkaline solution, the CFHC catalyst required an overpotential of merely 330 mV, 21.99% lower than that of the solid CFC precursor (423 mV) at the same condition. Meanwhile, the NFHC catalyst could deliver a current density as high as 100 mA cm −2 for the urea oxidation electrolysis at a potential of only 1.40 V, 24.32% lower than that of the solid NFC precursor (1.85 V). This work provides a new platform to construct intricate hollow structures as promising nano-materials for the application in energy conversion and storage.

Modulating hot carrier dynamics is crucial in tin halide perovskite photovoltaics, particularly under indoor illumination with limited photon flux. Herein, a fullerene derivative bearing four piperazine groups (denoted as TPPC) is synthesized to engineer the perovskite/C 60 interface. The TPPC molecule exhibits a dipole moment of 1.97 Debye, leading to enhanced adsorption energy on perovskite surface and robust interfacial interaction. The newly formed surface dipole optimizes the interfacial energy level alignment via a cascade gradient, enabling modulation of interfacial hot carrier dynamics. Consequently, TPPC-treated photovoltaic devices achieve a champion power conversion efficiency (PCE) of 22.49% and a maximum output power density ( P out ) of 64.1 μW cm -2 under white light-emitting diode illumination (3000 K, 1000 lux, 285 μW cm -2 ). Large-area (1.21 cm 2 ) devices attain a PCE of 17.94% (certified: 15.93%) and a maximum P out of 51.2 μW cm -2 under the same illumination conditions. Xiao et al. report the synthesis of a fullerene derivative bearing four piperazidine groups to engineer the tin halide perovskite/C60 interface, enabling the photovoltaic devices with a power conversion efficiency of 22.49% and an output power density of 64.1 μW cm-2 under 1,000 lux white light illuminance.

Fast photoinduced charge separation (CS) and long-lived charge-separated state (CSS) in small-molecules facilitate light-energy conversion, while simultaneous attainment of both remains challenging. Here we accomplish this through aggregation based on fullerene-indacenodithiophene dyads. Transient absorption spectroscopy reveals that, compared to solution, the CS time in aggregates is accelerated from 41.5 ps to 0.4 ps, and the CSS lifetime is prolonged from 311.4 ps to 40 μs, indicating that aggregation concomitantly promotes fast CS and long-lived CSS. Fast CS arises from the hot charge-transfer states dissociation, opening up additional resonant channels to free carriers (FCs); subsequently, charge recombination into intramolecular triplet CSS becomes favorable mediated by spin-uncorrelated FCs. Different from fullerene/indacenodithiophene blends, the unique CS mechanism in dyad aggregates reduces the long-lived CSS dependence on molecular order, resulting in a CSS lifetime 200 times longer than blends. This endows the dyad aggregates to exhibit both photoelectronic switch properties and superior photocatalytic capabilities. Light-harvesting applications require dyes with efficiently formed long-lived charge separated electronic states. Here the authors achieve this through aggregation in fullerene dyads and reveal their excited-state dynamics mechanism.

The endohedral fullerenes lead to well-protected internal species by the fullerene cages, and even highly reactive radicals can be stabilized. However, the manipulation of the magnetic properties of these radicals from outside remains challenging. Here we report a system of a paramagnetic metallofullerene Sc 3 C 2 @C 80 connected to a nitroxide radical, to achieve the remote control of the magnetic properties of the metallofullerene. The remote nitroxide group serves as a magnetic switch for the electronic spin resonance (ESR) signals of Sc 3 C 2 @C 80 via spin–spin interactions. Briefly, the nitroxide radical group can ‘switch off’ the ESR signals of the Sc 3 C 2 @C 80 moiety. Moreover, the strength of spin–spin interactions between Sc 3 C 2 @C 80 and the nitroxide group can be manipulated by changing the distance between these two spin centres. In addition, the ESR signals of the Sc 3 C 2 @C 80 moiety can be switched on at low temperatures through weakened spin–lattice interactions. Endohedral fullerenes are known to stabilize reactive radicals; however, the external magnetic manipulation of these species’ remains challenging. Here, the authors link a nitroxide radical to a paramagnetic fullerene system and are able to alter the spin behaviour of the fullerene via spin–spin interactions.

Efficient energy conversion and environmental protection are still constrained by rapid carrier recombination, unstable interfaces, limited active site, and so on. Owing to the unique electronic structure and tunable physicochemical properties, fullerenes offer a powerful platform to address these bottlenecks in photocatalysis, electrocatalysis, and energy storage. This review systematically summarizes recent advances in the classification and design strategies of fullerene–based functional materials, as well as their innovative applications in photo‐/electro‐/thermo‐catalysis and energy storage. From the perspective of material system design, we emphasize the construction strategies of inorganic hybrids such as fullerene–metal nanoparticle and fullerene–semiconductor composites, as well as fullerene–organic hybrid materials. In catalytic applications, the review analyzes activity enhancement mechanisms of fullerene‐based materials in photocatalytic pollutant degradation, photo‐/electro‐catalytic water splitting, CO2 conversion, and highlights their innovative roles in traditional thermal catalytic processes such as ammonia synthesis. In the field of energy storage devices, we focus on the essential function of fullerene derivatives in crucial segments like the electron transport layer, interfacial modification/passivation layers of solar cells. Finally, the challenges and opportunities faced by fullerene–based functional materials are discussed. Overall, this review not only highlights advances in fullerene–based functional materials but also outlines a roadmap for harnessing their structural and electronic advantages to guide the rational design of next‐generation strategies for energy conversion and environmental remediation. A schematic illustration summarizing the classification, and photo‐/electro‐‐/thermo‐catalysis and energy storage applications of C60 and derivatives.

This fundamental understanding of molecular structure–NLO property relationships provides critical design principles for next-generation optical limiting materials, quantum photonic devices, and ultrafast nonlinear optical switches, addressing the growing demand for high-performance organic optoelectronic materials in laser protection and photonic computing applications. In this study, it was observed that selenophene-incorporated fused D-A-D architectures exhibit a remarkable enhancement in two-photon absorption characteristics. By strategically modifying the heteroatomic composition of the Y6-derived fused-ring core, replacing thiophene (BDS) with selenophene (BDSe), the optimized system achieves unprecedented NLO performance. BDSe displays a nonlinear absorption coefficient (β) of 3.32 × 10−10 m/W and an effective two-photon absorption cross-section (σTPA) of 2428.2 GM under 532 nm with ns pulse excitation. Comprehensive characterization combining Z-scan measurements, transient absorption spectroscopy, and DFT calculations reveals that the heavy atom effect of selenium induces enhanced spin–orbit coupling, optimized intramolecular charge transfer dynamics and stabilized excited states, collectively contributing to the superior reverse saturable absorption behavior. It is believed that this molecular engineering strategy establishes critical structure–property relationships for the rational design of organic NLO materials.

Spin-based interdisciplinary research has attracted considerable attention, and various applications in magnetic memory, quantum science, and precision measuring technology have been reported. In this study, we induced a fluorescence property in a spin-active molecule by supramolecular assembly and realized a synergistic modulation of its spin and fluorescence properties. A Saturn-shaped supramolecular complex was synthesized using a spin-active metallofullerene Sc 3 C 2 @C 80 with a fluorescent nanohoop of tetra-benzothiadiazole-based [12]cycloparaphenylene (TB[12]CPP), and its spin and fluorescence properties were comprehensively investigated. Temperature-dependent electron paramagnetic resonance (EPR) spectroscopy and fluorescence analyses were conducted. Synchronous changes in the EPR signals and fluorescence peaks were discovered in the temperature range of 170–290 K. Based on nuclear magnetic resonance observations and theoretical calculations, a temperature-dependent host—guest interaction between Sc 3 C 2 @C 80 and a nanohoop was demonstrated, which explained the synchronous changes in the EPR signals and fluorescence peaks for Sc 3 C 2 @C 80 ⊂TB[12]CPP. The application of Sc 3 C 2 @C 80 as a molecular spin system to probe the host—guest interaction was also evaluated. These results show that the supramolecular assembly can be used to design advanced spin systems coupled with optical and magnetic behaviors based on paramagnetic and luminescent molecules.