A critical bottleneck in photocatalytic H2O2 production lies not only in the severe non-radiative energy losses incurred from enhancing light absorption, but also in a fundamental proton-electron kinetic imbalance. Here we introduce a light-heat-proton coupling strategy that harnesses the dissipated photothermal energy to activate proton dissociation from carboxylic acids, thereby creating a productive driving force for redox catalysis. A hydrogen-bonded organic framework (HOF-FJU-200) incorporating mixed-valence Fe2+/Fe3+ clusters is constructed via a metalloligand approach. The intervalence charge transfer transitions within these clusters generate strong photothermal conversion while extending light absorption to the NIR-II region ( ~ 2500 nm). The resulting thermal energy activates proton dissociation from unpaired carboxylic acid groups, synchronizing proton release with photoinduced electron transfer. This cooperative mechanism effectively channels non-radiative heat into catalytic function, achieving an H2O2 production rate of 10657 μmol·g-1·h-1 without sacrificial agents. By directly coupling light, heat, and proton dynamics within a single framework, this work establishes a general paradigm for utilizing non-radiative energy to regulate proton-driven photocatalytic reactions.

Recent years have witnessed the significant breakthrough in the field of new materials discovery brought about by the artificial intelligence (AI). AI has successfully been applied for predicting the formability, revealing the properties, and guiding the experimental synthesis of materials. Rapid progress has been made in the integration of increasing database and improved computing power. Though some reviews present the development from their unique aspects, reviews from the view of how AI empowered both discovery of new materials and cognition of existing materials that covers the completed contents with two synergistical aspects are few. Here, the newest development is systematically reviewed in the field of AI empowered materials, reflecting advanced design of the intelligent systems for discovery, synthesis, prediction and validation of materials. First, background and mechanisms are briefed, after which the design for the AI systems with data, machine learning and automated laboratory included is illustrated. Next, strategies are summarized to obtain the AI systems for materials with improved performance which comprehensively cover the aspects from the in-depth cognizance of existing material and the rapid discovery of new materials, and then, the design thought for future AI systems in material science is pointed out. Finally, some perspectives are put forward.

Atomically precise coinage metal nanoclusters possess well-defined structures and distinctive optoelectronic properties. However, their assembly through weak van der Waals interactions often results in inefficient charge migration and rapid electron-hole recombination. Hydrogen-bonded organic frameworks (HOFs) offer an alternative strategy to integrate functional clusters into ordered crystalline materials while preserving molecular isolation. Herein, we report the first example of coinage-metal-cluster-based donor-acceptor (D-A) heterojunction engineered into a HOF. A tailored Ag6 cluster serves as the electron-rich donor, and 4,4'-bipyridine (BPY) acts as the electron-deficient acceptor. Directional N─H···N hydrogen bonds guide the assembly into a crystalline Ag6-HOF, which retains the intrinsic structure of the Ag6 clusters while creating hydrogen-bonded channels for enhanced inter-cluster charge transport. Photoelectrochemical studies and density functional theory calculations reveal an S-scheme heterojunction, with the highest occupied molecular orbital (HOMO) localized on the Ag6 cluster and the lowest unoccupied molecular orbital (LUMO) on the BPY linker. This electronic configuration promotes spatial charge separation, extends visible-light absorption, and significantly boosts photocatalytic H2O2 production compared to the individual components. The work demonstrates hydrogen-bond-directed assembly as a precise and versatile approach to design cluster-based heterojunctional materials with tunable electronic structures and enhanced photocatalytic performance.

Scarce investigations have focused on coinage metal clusters possessing fixed cores but varying binding ligands in the context of catalysis. Here in this work, we successfully employed two types of carboxylic acid-based molecular tweezers to selectively capture two Cu6 clusters (Cu6-a and Cu6-b). Cu6-a and Cu6-b have identical cluster cores but different protected ligands, therefore provide accurate platform for investigating ligand effects in cluster catalysis. Notably, Cu6-b represents a rare example of a two-directional rod framework, marking the first instance of such a structure in coinage metal cluster-based MOFs. The integration of oxygen within OBB significantly enhances local spatial polarization, facilitating the charge separation and ROS generation efficiency of Cu6-b under visible-light irradiation. Consequently, the oxygen-containing Cu6-b exhibits superior photocatalytic performance in the aerobic oxidation of sulfide, achieving both high yield and selectivity. This work provides a valuable approach for precisely control the Cu clusters structures to regulate their properties.

Hydrovoltaic technology harnesses the ubiquitous and perpetual hydrologic cycle for solid-liquid interfacial energy conversion. However, contemporary hydrovoltaic systems exhibit multifaceted performance degradation, which includes dopant dissolution, destabilization of the electric double layer, and interfacial recombination. These factors collectively impair operational consistency and commercial viability. To address these limitations, we have developed sunlight-regenerable generators based on p-/n-type carbon nanotube (CNT) organic fabrics fabricated via scalable drop-casting techniques. The doped p-/n-type CNT organic fabrics facilitate photo-triggered recovery effects under AM 1.5 G irradiation (100 mW/cm(2)). Spectral and thermal analyses confirm that the recovery mechanism is primarily photo-triggered and is cooperatively assisted by photothermal effects, thereby restoring interfacial functionality. The system achieves markedly improved sustained voltage/current output, a higher peak power density of 16.46 mu W at a 10 k Omega load resistance, and scalable integration with an output of 8.7 V from 20 serially connected units and 15.5 mA from 40 parallelly connected units. This work establishes a solar-hydro synergistic strategy for resolving the stability-compatibility dilemma in hydrovoltaic energy harvesting.

The photovoltaic performance of perovskite solar cells (PSCs) depends on the crystallization of the perovskite. Achieving a crystalline perovskite with large grains and ordered lattices remains a challenge. Herein, we employ 2-amino-4,6-dichlorotriazine to facilitate grain growth. The molecular dipole passivation reduces the undercoordinated lead (Pb) defects and iodine (I) vacancy defects, and it corrects the PbI6 4- octahedral distortion, thereby leading to the achievement of the microscale grains and ordered (110) lattice arrangement. The rigid PSCs yield a power conversion efficiency (PCE) of 26.58% and an enhanced operational stability. Furthermore, it enables a flexible PSC with a PCE of 24.29%. This work provides a molecular dipole passivation to induce large perovskite grains and ordered lattice arrangements for high-performance PSCs.

ABSTRACT Atomically precise coinage metal nanoclusters possess well‐defined structures and distinctive optoelectronic properties. However, their assembly through weak van der Waals interactions often results in inefficient charge migration and rapid electron–hole recombination. Hydrogen‐bonded organic frameworks (HOFs) offer an alternative strategy to integrate functional clusters into ordered crystalline materials while preserving molecular isolation. Herein, we report the first example of coinage‐metal‐cluster‐based donor–acceptor (D–A) heterojunction engineered into a HOF. A tailored Ag 6 cluster serves as the electron‐rich donor, and 4,4′‐bipyridine (BPY) acts as the electron‐deficient acceptor. Directional N─H···N hydrogen bonds guide the assembly into a crystalline Ag 6 ‐HOF , which retains the intrinsic structure of the Ag 6 clusters while creating hydrogen‐bonded channels for enhanced inter‐cluster charge transport. Photoelectrochemical studies and density functional theory calculations reveal an S‐scheme heterojunction, with the highest occupied molecular orbital (HOMO) localized on the Ag 6 cluster and the lowest unoccupied molecular orbital (LUMO) on the BPY linker. This electronic configuration promotes spatial charge separation, extends visible‐light absorption, and significantly boosts photocatalytic H 2 O 2 production compared to the individual components. The work demonstrates hydrogen‐bond‐directed assembly as a precise and versatile approach to design cluster‐based heterojunctional materials with tunable electronic structures and enhanced photocatalytic performance.

All-inorganic perovskite solar cells (PSCs) are suffered from both moderate power conversion efficiency (PCE) and stability, primarily owing to abundant defects, limited crystallinity, and mismatched energy levels. Herein, we proposed a sequential amine-hydroiodide post-treatment (namely SAHP) strategy for CsPbI2.8Br0.2 modification through synergistically combining the etching function of 1,3-diaminopropane (DAP) and the protecting function of 1,3-diaminopropane dihydroiodide (PDAI(2)). The subsequent PDAI(2) treatment increased the crystallinity of the DAP-treated perovskite, leading to a formation of low-dimensional (LD) phase at the perovskite surface. The LD phase capping induced a hydrophobic surface of the perovskite. The energy level alignment and field-effect passivation were achieved at the interfaces between the perovskite and electron transport layers, suppressing charge recombination and facilitating charge extraction. Consequently, the optimized inverted CsPbI2.8Br0.2 PSCs delivered a PCE of 20.03 % and a high open-circuit voltage of 1.222 V, along with the enhanced stabilities. The devices retained similar to 92 % of the initial PCE in the storage test for as long as 288 days. This work provides an effective method to make efficient and stable inverted all-inorganic PSCs.

The defect passivation of the perovskite and the mitigation of nonradiative recombination losses substantially contribute to the enhancement of power conversion efficiency (PCE) and operational stability of flexible perovskite solar cells (PSCs). In this study, 2,4,6-triphenyl-1,3,5-triazine, characterized by its multifunctional molecular groups, is selected for the perovskite defect passivation. The molecular anchoring suppresses the undercoordinated lead (Pb), iodine (I), and formamidinium defects, and the PbI antisite defects. Consequently, the resulting PSCs achieve a PCE of 24.85%. Under the maximum power point tracking measurement, the T95, T91, and T90 lifetime (time for the device's efficiency that decreases to 95%, 91%, and 90% of its initial efficiency, respectively) of the flexible PSCs is 1423, 1682, and 2181 h, which are the best results among these flexible PSCs reported so far. The work highlights a promising buried interface anchoring strategy to guide the development of high-performance flexible PSCs.

Recent years have witnessed a growing demand for the storage and computation of data in large-scale with the rapid development of artificial intelligence (AI). The brain-inspired computing, which are featured with many advantages, like high-speed and low power consumption, are promising candidates for meeting this demand. Inspirations have been got by learning from various aspects of human brain, with the structures, architectures, processing tactics, functions, and working manner included, to fully realize those computational advantages of the human brain. Since synapses, as one of the basic components in human brain, are featured with softness and deformability, the flexible brain-inspired computing systems have attached a lot of attention. However, reviews in the view of advanced design for the flexible brain-inspired computing are few. Here, the newest development is comprehensively reviewed in this field. First, background and mechanisms are briefed, and then most important considerations for material, structure and model designs are illustrated together with solutions to realize the device flexibilities and high-level brain intelligence. Next, strategies are summarized to obtain brain-inspired computing with high overall performance. After that, the design thoughts for future flexible brain-inspired computing are proposed. Finally, some perspectives are put forward.

The rigorous synthetic methodologies have significantly impeded the progress in developing single-crystal extended organic polymers. Notably, the existence of macroscopic single-crystalline 2D porphyrin-based organic polymers has never been documented in the literature until now. In this study, we present a groundbreaking example of single-crystal 2D porphyrin-based organic polymers that are compatible with single-crystal X-ray diffraction (SXRD) for precise structural elucidation. Their formation is fundamentally dependent on the synergistic assembly facilitated by dative B─N bonds and halogen bonds. These crystals exhibit remarkable stability in both air and aqueous environments. Notably, the formation of the B–N Lewis pairs within these crystals significantly enhances the separation of photogenerated carriers, and their single crystals demonstrate exceptional photocatalytic activity for the production of hydrogen peroxide (H 2 O 2 ) from water and oxygen, without the requirement for sacrificial agents. This pioneering discovery establishes a new approach for crystalline control within the realm of organic polymers.

Molecular passivation reduces the lattice defects and induces large grains for high efficiencies of perovskite solar cells.

Layered manganese selenide (MnSe), a member of manganese chalcogenide family, has emerged as a prospective cathode for Zn-ion energy storage. However, the practical application of MnSe cathodes is often hindered by capacity degradation stemming from structural instability and sluggish Zn-ion storage kinetics, ultimately limiting their cycling life. Herein, we propose a dual mediation strategy involving silver selenide (Ag2Se) hybridization and Fe3+ electrolyte additive to enhance energy density and extend rechargeable cycling life of MnSe cathodes. Ag2Se nanowires within the microenvironment provide additional active sites and expand interlayer spacing, while Fe3+ additive increases conductivity and shortens ion transport time. Theoretical calculation proves the dual-mediated mechanism by considerably increasing the Zn affinity and decreasing the Zn diffusion energy barrier in MnSe. Additionally, Fe3+ as an electron shuttle in the form of Fe3+/Fe2+ binds to AgxMnSe, stabilizing the structure and restraining oxidation dissolution, thus preventing structural collapse and loss of active sites. Consequently, an assembled Zn-ion capacitor reaches a competitive areal energy of 633.9 mu Wh cm- 2 and exceptional cycling stability, with a capacitance retention of 94.7 % after 15,000 cycles. This work provides valuable insights into mediation strategies for designing Zn-ion energy storage systems with stable longevity at high areal energy.

Aluminum-ion batteries (AIBs) are gaining attention for large-scale energy storage due to their low cost and high theoretical capacity. However, the existing cathode materials frequently encounter rapid capacity degradation and sluggish reaction kinetics due to the strong interaction with high-charge Al3+, which limits the utilization of AIBs. Here, the Se-doping strategy is proposed to facilitate the active participation of anions in charge compensation and enhance the anionic redox process of amorphous anion-rich TiS4. A refined amount of Se doping effectively improves reaction kinetics for Al-storage and stabilizes the structure of the material, preventing polysulfide dissolution under high dealumination states. As a result, amorphous TiS3.5Se0.5 delivers unprecedented Al3+ storage performance, with a stable capacity of 210 mAh g-1 at 500 mA g-1 over 400 cycles. Through detailed characterization, we reveal that a-TiS3.5Se0.5 undergoes reversible Al3+ insertion, accompanied by anionic redox processes involving S22-and Sen-species, which lays the foundation for further development of anionic-redox-based cathodes for high-performance AIBs.

Interface molecules with strong adsorption energies on (100) facets coordinate with lead and iodine ions and reduce the ion defects, leading to uniform and crystalline perovskite and efficient perovskite solar cells (PVSCs). Herein, we demonstrate efficient and stable rigid and flexible PVSCs via defect passivation using 1,3-dibromo-1,3,5-triazine-2,4,6-trione hydrochloride. The molecular passivation enabled a crystalline and uniform perovskite with weak lattice shrinkage. The rigid and flexible PVSCs yield high power conversion efficiencies of 25.50% and 24.56%, respectively. Furthermore, both PVSCs exhibit substantial enhancement in operational stability. Under the maximum power point tracking measurement, the T90 lifetime (time for the device's efficiency to decrease to 90% of its initial efficiency) of the flexible PVSCs is 1100 h, which is the best result among these flexible inverted PVSCs reported so far. The work provides a multifunctional passivation strategy and valuable insights into making high-performance PVSCs.

Restructuring of mortise-and-tenon frameworks at the molecular level has never been achieved. We report the first example of restructuring in molecular mortise-and-tenon joints (MTF-4 and MTF-5). The obtained cross-locking mortise-and-tenon framework of MTF-5 exhibits higher stability, better mechanical stiffness, and superior optical limiting (OL) performance.

Precise control over the isomorphic self-assembly of nanocluster superstructures via weak interactions remains a fundamental challenge in materials science, primarily due to the lack of directional guidance. Inspired by the ancient mortise-and-tenon joint, we herein report a series of crystalline nanocluster superstructures (MTC-1 and MTC-2) that were exclusively assembled by such molecular joints, representing the first paradigm of its kind. Despite alterations in functional groups (methyl and ethyl), the supramolecular packing motif remains invariant, underscoring the robustness of this directed assembly strategy. Notably, the ethyl groups in MTC-2 serve as "locking pins", resulting in MTC-2 a fascinating Luban lock-like construction. This ingenious design endows MTC-2 with enhanced photogenerated charge migration and superior O2 adsorption capability, achieving a record-high photocatalytic H2O2 production rate (19,978 mu molg-1h-1) among all isolated crystalline cluster-based materials, an order-of-magnitude enhancement over existing benchmarks. This work not only presents a record-breaking photocatalyst but also establishes a general assembly strategy, the mortise-and-tenon joint, which is expected to guide the rational design of functional superstructures across diverse nanocluster systems. Locking pin Non-covalent interactions i Robust and directional d Promoting pphotocatalytic H2O2 production

The realization of the perovskite with few ionic defects, high crystallinity, and alleviated residual strains is crucial for making efficient rigid and flexible perovskite solar cells (PSCs). Herein, we used a passivating agent of 3-methylthio-1,2,4-triazine with strong anchoring strengths to passivate defects of the perovskite. This buried interface passivation improved the crystallinity of the perovskite with an alleviated residual strain while eliminating the localized deep-level defect states, thereby reducing the nonradiative recombination and minimizing the charge transport losses. The rigid and flexible PSCs delivered power conversion efficiencies of 26.04 and 24.16%, respectively. The rigid PSCs exhibited improved operational stability, and the flexible PSCs showed enhanced bending stability. The research provides insights into the enhancement in efficiency, operational stability, and bending stability of the perovskite photovoltaics.

Isolated single-site catalysts (ISSCs) have emerged as promising materials for energy conversion and storage. However, current approaches for inorganic nanocatalysts are often ineffective in achieving precisely ordered periodic atomic arrangements of active sites, often leading to a random distribution of active-site motifs on an inorganic substrate. In this work, we introduce a novel partial-coverage-assembly strategy, leveraging graphdiyne-derived fragment ligands, to synthesize a unique Cu nanocluster catalyst with an ordered periodic arrangement of isolated single-metal Cu sites [Cu4(TFA)4(DPBD)2, Cu-SMS], while maintaining identical atomicity and a homogeneous coordination microenvironment. This strategic approach significantly enhances the electron transport capability by incorporating graphdiyne-inspired bridging ligands as compared to non-coverage-assembled Cu-MMS (MMS: multiple-metal site). As a result, the Cu-SMS nanocluster catalyst exhibited superior performance in electrocatalytic nitrate reduction to ammonia, achieving a Faradaic efficiency exceeding 99%, surpassing all previously reported atomic precise metal nanocluster catalysts. Through a combination of in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy, electrochemical mass spectrometry and density functional theory calculations, we unraveled a detailed mechanistic pathway of nitrate reduction on Cu-SMS, highlighting the role of key intermediates (*NO2, *NO, *NHO, *NHOH, *NH2OH, *NH2) and identifying the rate-determining step. In all, these findings present a novel methodology for synthesizing periodic SMS catalysts, emphasizing the emergent catalytic behaviors of precisely ordered metal clusters in heterogeneous catalysis.