Redox flow batteries, by virtue of their advantages in power/capacity decoupling, high safety, and long cycle life, have become a strategic support for long-duration energy storage systems; however, capacity degradation remains a bottleneck for their commercialization. This review systematically identifies the multi-dimensional mechanisms of capacity degradation: including volume imbalance caused by transmembrane migration, inactivation and decomposition of active species, electrode degradation, and valence imbalance induced by side reactions. Targeting these challenges, the review deeply explores recovery strategies from physical repair to intelligent scheduling: covering the research and development of high-selectivity membranes, precise regulation of valence states, functionalized repair of electrodes, and model-driven predictive pathways integrating digital twins. Finally, current challenges such as characterization limitations and incomplete recovery rates are summarized, and future development directions for capacity recovery are envisioned. This review aims to provide a theoretical basis and technical guidance for extending the system cycle life of flow batteries and improving capacity recovery efficiency.
Hard carbon anodes for sodium-ion batteries suffer from unstable solid-electrolyte interphase formation, leading to low initial Coulombic efficiency and poor cycle stability. Herein, we demonstrate a molecular-level surface design that actively orchestrates an anionic bottom-up flux from the electrolyte bulk to the hard carbon interface. By engineering a synergistic pair of pyridinic-N and carbonyl groups on the carbon surface, we create a functional-differentiation microenvironment where pyridinic-N selectively anchors PF6− anions, while the cooperative carbonyl repels solvent molecules. This dual functionality establishes a sustained concentration gradient that drives a continuous reverse flux of anions toward the interface, fundamentally redirecting the electrolyte decomposition pathway from solvent-dominated to anion-preferential. The tailored surface lowers the PF6− decomposition barrier by over 70
All-optical control of synaptic weights offers a promising route toward low-power and massively parallel neuromorphic hardware. However, existing optoelectronic memristors often require electrical assistance or exhibit nonlinear and asymmetric conductance updates, limiting their energy efficiency and scalability. Herein, we report a spectrally partitioned all-optical memristor based on a PbS/PEDOT:PSS/VOx heterostructure, in which near-infrared and visible light are coupled to opposite defect-state filling and depletion pathways. Near-infrared illumination selectively excites PbS quantum dots and drives gradual electron transfer into oxygen-vacancy-related defect states in VOx through the PEDOT:PSS-regulated interface, producing continuous conductance potentiation. By contrast, visible illumination activates VOx and promotes interfacial hole-assisted recombination, leading to reversible depletion of defect-state electrons and conductance depression. This wavelength-selective carrier-transfer process enables highly linear and symmetric all-optical weight updates, achieving a linearity of 0.9994 and an effective 8-bit conductance resolution. The electrical energy consumption per optically induced synaptic event is calculated to be as low as 0.63 fJ under an ultralow probing bias. By integrating the devices into a 32 × 32 all-optically programmed array, we further demonstrate hardware-based BloodMNIST microscopic blood-cell image classification with an accuracy of 96.5
The common-ion effect of SO42− limits the solubility of MnSO4 to ≤ 1 M in conventional H2SO4 electrolytes, resulting in low specific capacity of manganese (Mn)-based redox flow batteries (RFBs). Although MnO2 semi-solid RFBs are expected to improve the specific capacity, the sluggish electrochemical reaction kinetics leads to low operating current densities (≤ 1 mA cm−2). Herein, we employ a reverse-design strategy by introducing additional high-concentration MnO2 into the conventional Mn-based electrolyte. Leveraging the MnO2/Mn2+ electrochemical reaction successfully circumvents the common-ion effect, raising the concentration of soluble Mn species in the electrolyte to 3.76 M and achieving a specific capacity of 156.2 Ah L_Catholyte^ - 1 —a 409
The common-ion effect of SO42- limits the solubility of MnSO4 to ≤ 1 M in conventional H2SO4 electrolytes, resulting in low specific capacity of manganese (Mn)-based redox flow batteries (RFBs). Although MnO2 semi-solid RFBs are expected to improve the specific capacity, the sluggish electrochemical reaction kinetics leads to low operating current densities (≤ 1 mA cm-2). Herein, we employ a reverse-design strategy by introducing additional high-concentration MnO2 into the conventional Mn-based electrolyte. Leveraging the MnO2/Mn2+ electrochemical reaction successfully circumvents the common-ion effect, raising the concentration of soluble Mn species in the electrolyte to 3.76 M and achieving a specific capacity of 156.2 Ah L Catholyte - 1 -a 409% increment over reported MnSO4-based electrolytes. Subsequently, the reverse disproportionation of electrolytic MnO2 generated during the second charging cycle shifts the redox mechanism from the MnO2(s)/Mn2+ couple to the solution-phase Mn3+(aq)/Mn2+ pair. This transformation not only elevates the discharge voltage but also enables stable operation at 30 mA cm-2, representing a current density 30-fold higher than reported Mn-based semi-solid RFBs. This work demonstrates a rational design strategy for semi-solid slurry electrolytes to enhance the specific capacity of RFBs, thereby advancing their applicability in grid-scale renewable energy storage.
Perylene diimide (PDI)-based electron-transport layers (ETLs) are fundamental in governing charge extraction, interfacial recombination, and the operational longevity of organic solar cells (OSCs), yet their molecular design still lacks transferable principles. Here we present a PDI-ETL molecular design framework that couples bay-position engineering with polar, bulky side-chain modulation to improve additive-free alcohol solubility, suppress over-crystallization, and mitigate oxidative degradation. With this framework, H75-DMA suppresses reactive-oxygen-driven chemical evolution and interfacial trap accumulation, thereby stabilizing interfacial energetics and electron transport. Binary OSCs based on H75-DMA achieve a power conversion efficiency (PCE) above 20
The quality of the buried interface between the self-assembled molecules (SAM) and the perovskite layer directly governs the processes of charge carrier transport and non-radiative recombination, which ultimately dictates the efficiency and stability of the inverted perovskite solar cells. However, the simultaneous mitigation of poor SAM layer adhesion and perovskite substrate interface defects remains a significant challenge. Herein, low-cost and readily available 2‑formylbenzenesulfonic acid sodium salt (2‑FAS) is employed as a bifunctional interlayer to molecularly bridge the SAM and perovskite. The benzene ring of 2‑FAS interacts via π–π stacking with the SAM, strengthening adhesion and promoting hole transfer, while its sulfonate group (-SO3−) coordinates with Pb2+ to regulate crystallization and passivate surface defects. As a result, the 2-FAS-modified devices deliver a champion power conversion efficiency of 26.21
Transition metal dichalcogenide (TMD) nanolaminate membranes hold great promise for molecular sieving due to their two-dimensional capillary structures, which facilitate size-restricted diffusion. However, many transition metal sulfides exhibit intrinsic instability and are highly susceptible to oxidation, which severely limits their durability under reverse osmosis operating conditions. In this work, we introduce a stable 1T phase titanium disulfide (TiS2) constructing nanolaminate membranes from Group IVB, enabling the formation of tunable capillary channels and achieving a permeance up to 46.8 L m−2 h−1 bar−1. Experiments confirm that water-initiated hydrolysis, rather than direct oxidation by molecular O2, dominates the degradation of TiS2, while alkyl-chain hydrophobic barriers effectively suppress this water-triggered degradation. The enhanced surface hydrophobic properties simultaneously improve antioxidation stability and ensure sustained performance over 30 filtration cycles and 15 days of continuous operation. Functionalized membranes further reached 96.9
Electric field modulation offers a non-contact route to tune electromagnetic wave absorption (EWA) by controlling carrier behavior. However, current in-situ electric field modulation strategies are often hindered by multi-physics factors during synthesis, limiting a deeper understanding of the decoupled mechanism of the electric field. Here, we report a postprocessing strategy that employs direct current electric field to induce d-orbital electron migration, triggering the 2H to 1T-phase transition in MoS2, accompanied by dislocation generation. On one hand, the increased 1T-phase content optimizes the conductive loss. Meanwhile, the Fermi level mismatch at 2H/1T interfaces creates electron accumulation regions that drive polarization loss. On the other hand, positive and negative charges accumulate on opposite sides of the dislocation lines, forming ordered equivalent dipole arrays, markedly boosting polarization. After treatment at 6 V for 10 min, MoS2 achieves an effective absorption bandwidth of 6.72 GHz at 2.20 mm, a 440
Self-assembled monolayers (SAMs) are widely used as hole-transport layers (HTLs) in organic solar cells (OSCs), yet conventional single-component SAMs often form quasi-monolayers with incomplete coverage and interfacial defects that become increasingly detrimental upon device scaling. Here, we develop a co-assembled multilayered SAM (coSAMu) strategy that combines two SAM molecules, 2PACz and 2Cl-4PACz, with distinct dipoles and steric configurations through blend casting and sequential casting. Photoelectron spectroscopy, X-ray analysis, and molecular simulations support a layered structure in which a chemisorbed, 2PACz-rich bottom layer primarily sets the indium tin oxide (ITO) work function, while a 2Cl-4PACz-rich upper layer fills interfacial voids, improves molecular packing, and passivates defects. Consistent with this picture, coSAMu promotes a more favorable vertical composition near the ITO surface and suppresses trap-assisted recombination, enabling more efficient charge extraction and collection. Consequently, a representative D18:L8-BO OSC incorporating the sequential-cast coSAMu HTL achieves a power conversion efficiency of 20.1
Flexible electronics represent a paradigm shift in modern electronics, with flexible sensors serving as pivotal components in these systems. Despite significant advances driven by innovations in materials, structures, hardware, and algorithms, conventional design approaches that focus on optimizing individual hierarchies have inherent performance trade-offs, limiting further development. This review contends that future performance enhancements can no longer rely solely on breakthroughs in separate components. Still, it must adopt a new co-design paradigm spanning the “materials–structure–hardware–algorithm” hierarchy. In this review, we systematically organized the research landscape and representative advances across these four key hierarchies, analyzed the importance and recent breakthroughs in hierarchical synergy, and established a forward-looking theoretical framework to foster innovation and development in the field of flexible sensing.
Free-standing polymer films that are ultra-thin, lightweight, and robust hold significant promise for applications in flexible electronics. However, their performance has been constrained by the challenge of simultaneously enhancing mechanical strength and reducing density. Herein, an ultra-thin and robust polyimide (PI)-based covalent organic framework-modified multi-walled carbon nanotube (MWCNT-COF) film is demonstrated for high-specific-power flexible GaAs solar cells. The film exhibits a high Young’s modulus of 1.53 GPa, a tensile strength exceeding 97.53 MPa, and a low density of 0.73 g cm−3, representing a 45.1
The aqueous zinc metal batteries (AZMBs) are famous for high-safety and high-energy-density, but limited by severe challenges around the Helmholtz plane layer such as the strong ion–dipole interactions between Zn2+ and H2O, resulting in slow desolvation processes and limited transport kinetics as well as corresponding higher barriers. To reconstruct the ion–dipole surroundings, the interface chemistry of employing a high permanent dipole moment of L-Carnosine (L-CN) has been proposed, weakening the interactions between Zn2+ and H2O to realize a crowded Zn2+-conductive structure, accelerating the desolvation kinetics. As revealed, the strong affinity between L-CN and Zn2+ enables the L-CN molecules to repulse H2O, reconfiguring the inner Helmholtz plane layer, thereby inhibiting the active water molecular to form hydrogen evolution reactions. Consequently, the Zn//Zn symmetric cells with Helmholtz plane modulation achieve a long lifespan up to 7000 h, a high Coulombic efficiency of 99.72
To settle inherent irreversible phase transition and motivate re-dissolution of deposited “dead” MnO2 without acid and redox mediator addition, we introduced atomic-dispersed Co atoms with high-spin state into layered MnO2, denoted as Co–MnO2, via an in situ topological phase transformation strategy, thereby unlocking reversible multi-electron transfer chemistry for superb Zn–Mn batteries. Specifically, atomic-distributed Co atoms within Co–MnO2 effectively modulate [MnO6] octahedral symmetry and reduce Co–O bond covalency along with enhanced lattice oxygen activity. Based on this, high-spin Co (t2g4eg2) greatly mitigates the Jahn–Teller distortion as well as promotes electrolytic MnO2 deposited onto the cathode surface completely converted from adsorbed Mn2+ for inhibited “Mn dendrites”, achieving reversible MnO2/Mn3+ and electrolytic MnO2/Mn2+ reactions with highly thermodynamical favorability. Benefiting from the “two-step, three-electron” mechanism triggered by high-spin Co, Zn//Co–MnO2 battery delivers an outstanding capacity of 658 mAh g–1 and ultra-long lifespan over 15,000 cycles. This work reveals the critical role of transition-metal spin state modulation for energy-dense and durable Zn-MnO2 batteries with reversible multi-electron storage mechanisms.
Self-assembled monolayers (SAMs) are widely used as hole-transport layers (HTLs) in organic solar cells (OSCs), yet conventional single-component SAMs often form quasi-monolayers with incomplete coverage and interfacial defects that become increasingly detrimental upon device scaling. Here, we develop a co-assembled multilayered SAM (coSAMu) strategy that combines two SAM molecules, 2PACz and 2Cl-4PACz, with distinct dipoles and steric configurations through blend casting and sequential casting. Photoelectron spectroscopy, X-ray analysis, and molecular simulations support a layered structure in which a chemisorbed, 2PACz-rich bottom layer primarily sets the indium tin oxide (ITO) work function, while a 2Cl-4PACz-rich upper layer fills interfacial voids, improves molecular packing, and passivates defects. Consistent with this picture, coSAMu promotes a more favorable vertical composition near the ITO surface and suppresses trap-assisted recombination, enabling more efficient charge extraction and collection. Consequently, a representative D18:L8-BO OSC incorporating the sequential-cast coSAMu HTL achieves a power conversion efficiency of 20.1% (0.042 cm2), outperforming pristine 2PACz. Importantly, when scaled to a 17.14 cm2 mini-module (six serially connected subcells), coSAMu delivers 17.0% efficiency versus 12.2% for the 2PACz control. This work demonstrates controlled multilayer co-assembly as an effective strategy for scalable OSC interface engineering that is broadly applicable to multiple donor-acceptor systems.
Self-assembled monolayers (SAMs) have emerged as highly versatile interfacial materials in perovskite solar cells (PSCs), offering tunable molecular structures, favorable energy-level alignment, high optical transparency, and minimized non-radiative recombination losses. With the rapid advancement of inverted (p-i-n) PSC architectures, SAM-based hole-selective contacts have demonstrated distinct advantages in achieving superior power conversion efficiency, cost-effective fabrication, and strong compatibility with scalable manufacturing processes. This review first summarizes the evolution of SAM applications, with a particular focus on SAM-based materials in p-i-n PSCs. Subsequently, the fundamental aspects of SAMs are systematically discussed. Further, common preparation methods of SAMs are reviewed, along with the key challenges encountered in achieving uniform SAM coating. Based on this, recent progress in SAM-based PSCs is comprehensively summarized, including their applications in high-efficiency single-junction devices, perovskite tandem solar cells, and large-area photovoltaic modules. The crucial roles of SAMs in energy-level modulation, interfacial modification, defect passivation, and charge transport are highlighted. Finally, the remaining challenges and future prospects of SAMs in inverted PSCs are discussed, with particular emphasis on interfacial stability and long-term operational reliability. This review aims at providing systematic insights and guidance for the further development of SAM-based inverted PSCs.
Aerogel fibers have been considered as a promising solution for thermal protection textiles due to their high porosity and low thermal conductivity. However, the scalable production of sustainable and mechanical strong aerogel fibers remains a critical challenge. Here, inspired by the porous core–shell structure of polar bear hair, we report a continuous strategy to fabricate all-biomass aerogel fibers featuring an encapsulated core–shell architecture using silk fibroin as the core and cellulose as the shell. This tunable structure, with radially aligned sheet-like pores and adjustable shell thickness, is achieved through hydrogen bond-driven cellulose contraction and alcohol-induced curing of sheet-like silk fibroin. Such a porous architecture effectively suppresses convective heat transfer and promotes a multi-reflective effect for infrared radiation. The resulting fibers exhibit good mechanical robustness with a tensile load of a single aerogel fiber is up to 200 g without reinforcement. Meanwhile, the aerogel fiber maintains high porosity (79.78
Photothermal superhydrophobic textiles represent an emerging paradigm integrating active light-driven functionality with passive liquid repellency. While previous reviews treated superhydrophobicity and photothermal effects in isolation, this work pioneers a systematic analysis of their synergistic interplay-a critical, underexplored mechanism where superhydrophobicity preserves photothermal efficiency by minimizing water-induced heat loss, while photothermal activity prevents surface fouling that compromises non-wetting performance. Through detailed case studies of advanced material systems, this review highlights how this synergy supports significant advancements in adaptive wearable technology, energy-efficient infrastructure, and eco-friendly water treatment. This review presents an original "lab-to-life" roadmap that structurally links material design to durability assessment, environmental impact evaluation, and scalable manufacturing strategies-a holistic framework absent in existing literature. The review emphasizes urgent sustainability priorities including green material substitutions, non-toxic solvent processing methodologies, and circular design principles aligned with global environmental regulations. By connecting fundamental mechanisms to real-world deployment scenarios while outlining transformative future directions such as AI-accelerated material discovery, stimulus-responsive systems, and intelligent manufacturing protocols, this work provides a timely and actionable reference for advancing next-generation textiles toward technological sophistication and practical viability in sustainable development.
Achieving precise and on-demand steering of the oxygen reduction reaction (ORR) pathway between the efficient 4e− route to H2O and the valuable 2e− route to H2O2 remains a pivotal challenge in electrocatalysis. Herein, we address this challenge by designing a bioinspired molecular magnetic field-responsive catalyst (MMFR-C) via magnetic single-atom-anchored Salen-based covalent organic frameworks (MSA-Salen COFs) onto magnetic nanoparticles (single/multi-domain Fe3O4). Mimicking cytochrome c oxidase, the MMFR-C employs MSA-Salen COFs as an ordered proton-transfer channel and well-defined N2-M-O2 moieties as enzymatic O2 activation sites, with Fe3O4 providing a built-in magnetic field for remote regulation of the active-site electronic structure. The bioinspired MMFR-C exhibits switchable ORR pathways. Relative to the pristine Co-Salen COF (26
