Sodium-ion batteries (SIBs) are promising alternatives to lithium-ion batteries, yet carbon-based anodes suffer from capacity fading and severe performance degradation at low temperatures due to increased interfacial impedance and sluggish ion transport. Herein, a phosphorus‑nitrogen co-doping strategy is proposed to reconstruct the solid electrolyte interphase (SEI). While nitrogen and phosphorus synergistically enhance the bulk electronic conductivity and defect density, phosphorus uniquely converts intrinsic P-C/P-N bonds into a thermodynamically stable, amorphous NaxPOy-rich SEI layer. This inorganic SEI endows the electrode with excellent mechanical strength and isotropic low-energy-barrier pathways for rapid Na+ migration. Consequently, the optimized electrode maintains high cycling stability at temperatures as low as -15 °C. Furthermore, a Long Short-Term Memory (LSTM)-based model is explored as a supplementary tool for rapid capacity forecasting across temperatures. This work provides a rational design paradigm for high-performance, wide-temperature-range SIB anodes, with preliminary full-cell tests demonstrating practical applicability.

The development of multifunctional organic pi-conjugated molecules has been of great interest due to their potential use in sustainable energy applications. Some progress has been made in the development of n-type, electron-acceptor molecules with very low LUMO levels, but the diversity of suitable molecular scaffolds remains strictly limited. Along similar lines, phosphorus incorporation into ring-fused organic scaffolds has proven to create molecules with beneficial optical and electrochemical properties and electron-acceptor character, as well as exceptional tunability. Herein, we report a detailed structure-property study of the dithieno[2,3-b;3 ',2 '-e]-4-keto-1,4-dihydrophosphinine system, an intriguing scaffold that has remained largely unexplored to date. Through various targeted approaches, we comprehensively explore a series of dithienoketophosphinine-based electron-acceptor species functionalized at the phosphorus center, the carbonyl group, and the thieno-backbone to explore and more deeply understand the impact on the electrochemical, optical, and structural properties of the system. Our study convincingly establishes the superior electron-acceptor properties of the scaffold that outcompete state-of-the-art materials, as well as its high degree of tunability that also unlocks valuable emission features upon extension of the core.

Bowl-shaped conjugated materials have emerged as a compelling class of materials due to their unique structural topology and exceptional chiral optoelectronic characteristics. Among these, phosphorus-embedded curved polycyclic aromatic phosphangulenes represent a particularly intriguing yet underexplored family, as their development has been hindered by synthetic challenges. We present an efficient synthetic strategy for two novel π-extended phosphangulene derivatives (P-PTz and P-DOPTz), establishing their first application in circularly polarized luminescence (CPL) systems. The chalcogen-dependent electronic modulation through sulfur oxidation enables remarkable emission color tuning across blue, green, and red spectral regions, with additional solvent-polarity-responsive characteristics. Notably, these compounds exhibit strong phosphorescence emission in cryogenic solution and thin-film states. This study not only validates the potential of bowl chirality in phosphangulenes as a design principle for CPL-active materials but also provides a foundation for developing advanced functional materials with multifarious optoelectronic applications.

The development of organic electrodes featuring a high density of redox units and enhanced stability is of great theoretical and practical importance for advancing energy storage technologies. In this work, we present tris-amido naphthoquinone (TANQ) as a cathode material for high-performance aqueous zinc-organic batteries (ZOBs), achieved through molecular extension via amide linkages. The material benefits from synergistic hydrogen-bonding networks and pi-pi stacking, which strengthen intermolecular interactions and effectively suppress dissolution. Owing to its high density of redox centers, TANQ undergoes reversible multi-electron redox reactions, giving a high specific capacity of 213 mAh g-1 at 0.2 A g-1, primarily via a Zn2+ storage mechanism. This high capacity enables TANQ to achieve a notable specific discharge energy of 140 Wh kg-1 at 0.2 A g-1. TANQ also exhibits outstanding rate capability (153 mAh g-1 at 2 A g-1) and long-term cycling stability, retaining 94% of its capacity after 700 cycles.

We report a urea-integrated phenothiazine-based small molecule (MPT-U) as a high-potential, two-electron cathode for lithium organic batteries.

Bio-derived redox-active motifs are highly promising for next-generation energy storage applications owing to their inherent electrochemical functionality and sustainable sourcing from natural resources. To achieve superior electrochemical performance, a critical prerequisite is suppressing dissolution in electrolytes. Herein, we report a molecular design strategy that couples bio-derived carbonyl pyridinium derivatives with anthraquinone (AQ) to construct three novel organic electrode materials. This molecular expansion approach enables multiple reversible redox processes while effectively inhibiting material dissolution, resulting in significantly improved battery performance with anion and cation co-insertion mechanism. Systematic investigation of the carbonyl pyridinium components reveals that anthraquinone-azafluorenone (AQ-AF), with a more planar carbonyl pyridinium unit, exhibits the most favorable physicochemical properties among the series, including the lowest unoccupied molecular orbital (LUMO) energy level, narrowest optical bandgap, and minimal solubility. When paired with Li anode, AQ-AF delivers the highest specific capacity (259 mAh g-1 at 0.05 A g-1) and optimal cycling stability (73% retention after 400 cycles at 0.1 A g-1). This work presents an innovative molecular engineering approach for diversifying bio-derived carbonylpyridinium systems, facilitating controlled multi-electron transfer processes to advance high-performance energy storage technologies.

Solution‐processable electrochromic materials are promising to fabricate thin film with low manufacturing cost production and allow a variety of applications in smart windows and optical displays. In this work, a positively‐charged tetrachlorinated perylene diimide (PDI‐CHO) with two aldehyde functional groups has been designed as a new building block, to prepare redox‐active polymer PDI‐BTH. Benefiting from the charged backbone, the obtained polymer shows good solubility in polar DMSO solvent, allowing cost‐effective fabrication of high‐quality thin film with controllable thickness by simple drop‐casting method. The obtained film exhibited multi‐electrochromic behavior including red, gray, and blue colors as a result of the two‐step redox process. It Is further demonstrated that this polymer film exhibits fast switching times (1.2 s), remarkably high coloration efficiency (1093 cm 2 C −1 ), great optical contrast (60% at 650 nm), and good cycle stability (90% optical retention over 125 cycles). It is believed that the presented molecular design would also be adaptable to a wide range of aromatic dimides with tunable optoelectronic properties.

Transition metal chalcogenides (TMCs) have garnered significant attention as high-capacity anode materials, yet the unconventional role of the Cu collector meditating atomic-level substitution of metal-site cations by Cu4+ ions during electrochemical cycling remains mechanistically unclear. To address this, herein, Cu-doped MoSe2@C ultrathin nanosheets were synthesized via the solvothermal process and carbonization strategies. A systematic investigation was conducted to elucidate the underlying driving forces for Cu4+ substitution at Mo4+ sites and the crucial regulatory effects of solid electrolyte interphase (SEI) formation. The substitution mechanism was elucidated through the Hard and Soft Acid-Base principle, where Cu4+ (classified as a soft acid) demonstrates significantly stronger coordination affinity with Se2- anions (soft bases) compared to the native Mo4+ cations (hard acids). This electrochemical transition is mediated by ether-based electrolytes coupled with the Cu collector, where the in situ formation of a thin, inorganic-rich SEI layer establishes synergistic ion-transport highways for accelerated Na+/Cu4+ co-diffusion. Temperature-dependent studies reveal Arrhenius-type kinetics: charge transfer is kinetically hindered at ≤ 0 °C but thermally activated at 50-70 °C, confirming that interfacial charge transfer requires thermal energy to overcome activation barriers. This work provides a fundamental guideline for designing stable metal chalcogenide electrodes through interface engineering and electrolyte optimization.

Exploration of new π-conjugated building blocks for construction of supramolecular polymers is at the forefront of self-assembly. Herein, we incorporate a highly planar anthanthrene skeleton into the design of two supramolecular monomers 1 and 2. Their supramolecular polymerization have been comprehensively investigated by spectroscopic studies. Our results reveal that the number and/or position of the amide groups exert pronounced effect on the molecular aggregations and the mechanisms of the supramolecular polymerization. Monomer 1 self-assembles in a cooperative manner to form 1D nanofibers though face-to-face H-type aggregation. In contrast, 2 adopts J-aggregation to form supramolecular polymer via isodesmic mechanism.

Rational design of organic cathode materials with suppressed solubility is crucial yet challenging for achieving high‐capacity and long‐cycling rechargeable batteries. This study presents a facile synthesis strategy for three naphthoquinone derivatives (NQ1‐NQ3) featuring tunable amide functionalities and molecular dimensions, followed by a systematic evaluation of their electrochemical performance in lithium‐organic batteries (LOBs). The strategic incorporation of multiple amide motifs and molecular size expansion in NQ2 and NQ3 effectively enhances intermolecular interactions through hydrogen‐bonding networks and π–π stacking, resulting in remarkable solubility suppression and superior cycling stability. Notably, the NQ3‐based cathode demonstrates an intriguing structural evolution involving progressive particle pulverization during cycling, which facilitates intimate contact with conductive carbon additives and significantly improves electrode conductivity. These synergistic effects enable the best LOB performance of NQ3, such as a high specific capacity (224 mAh g −1 at 0.1 A g −1 ), good rate capability (162 mAh g −1 at 2 A g −1 ) and cycling stability, outperforming most reported organic cathode materials. This work provides molecular‐level insights into suppressing dissolution through non‐covalent interaction engineering for high performance LOBs.

Morphology optimization of organic electrodes with more exposed redox-active sites and large contact area between active materials and conductive carbon is crucial for higher actual capacity, and improved rate performance, however, is also challenging. In this work, we report a self-assembled perylene diimide disodium salts (PDI-ONa)-based cathode for sodium organic batteries (SOBs) and unveil an in situ electro-induced reorganization process that optimizes the nanostructured morphology and significantly improves the ionic and electronic transport. Experimental and theoretical data suggest that such reorganization is driven by the continuous dissociation/restacking of PDI-ONa during cycling. The resulting reorganized PDI-ONa electrode exhibits excellent rate (136 and 126 mA h g-1 at 0.2 and 100 A g-1) and cycling performance (141 mA h g-1 after 24,000 cycles at 3 A g-1). Even at -30 °C, it can also perform well (140 mA h g-1 after 500 cycles at 0.1 A g-1). Our findings provide a fresh perspective on optimizing organic nanostructured electrodes for high-performance SOBs.

Redox-active p-type phenothiazine based organic cathodes have captured increasing attention for lithium-organic batteries due to their high voltage output and rich chemical modification. However, their capacities are generally limited to one redox event per molecule; while the di-cation states are subject to rapid decomposition and cannot be effectively utilized. Herein, a scalable synthesis of phenothiazine-based polymer (MPT-CC) is reported, that can fully utilize the two-electron storage by raising its highest occupied molecular orbital (HOMO). Lithium-organic batteries using this polymer as cathode displayed a high specific capacity of 178 mAh g-1 at 0.2 A g-1. This polymer also displays excellent cycling stability. After 1000 cycles at 0.2 A g-1, a stable capacity of 194 mAh g-1 with approximate to 100% capacity retention can be obtained. Even at 2 A g-1 after 10,000 cycles, 98 mAh g-1 can be reversibly achieved. Its practical applicability has been successfully demonstrated in MPT-CC//graphite full cell, also displaying good performance. This work contributes to a major advancement of phenothiazine-based polymer design for high performance energy storage devices. A phenothiazine-based polymer is rationally designed for lithium organic batteries. As a result of raised HOMO energy level, two-electron storage of redox centers can be fully utilized, leading to much improved specific capacity and cycling lifespan. This work contributes to a major advancement of phenothiazine-based polymer design for high performance energy storage applications. image

Organic p-type cathodes have captured increasing attention for lithium-organic batteries due to their high voltage output. However, because of the low electronic and ionic conductivity, the p-type organic electrode materials often show sluggish reaction kinetics and hence low capacities and poor cyclability. In this work, three conjugated polymers (Pz-TPPO, Pz-TPPS, and Pz-TPP) based on p-type phenazine linked with triphenyl phosphine are reported with different chemical modifications of phosphorus atom. Through oxidation and sulfuration of phosphorus atoms, the electron-accepting property strength is increased, resulting in higher electronic conductivity of Pz-TPPO and Pz-TPPS. It is also found that the P & boxH;O unit in Pz-TPPO exhibits stronger Li+ coordination, which can bring anions into close proximity to the redox centers, further improving the anion shuttling during charge and discharge. All these lead to the best lithium-organic battery performance of Pz-TPPO, such as high voltage output (3.1-3.9 V), high reversible specific capacity (149 mAh g-1 at 0.2 A g-1) and excellent cycle stability. The potential application has also been demonstrated in Pz-TPPO//graphite full battery. This work provides a novel strategy for designing donor-acceptor (D-A) conjugated polymer by simple phosphorus modification toward high-performance organic batteries. Three conjugated polymers (Pz-TPPO, Pz-TPPS, and Pz-TPP) based on p-type phenazine linked with triphenyl phosphine with different chemical modifications of phosphorus atom are designed and synthesized for lithium organic battery. The study clearly demonstrates that manipulation of phosphorus chemistry (lone pair, oxidation, and sulfuration) is an effective strategy to tune the battery performance. image

Two cationic luminescent cyclometalated Pt(II) complexes with adamantane-based isocyanide ligands are reported. This work provides important insights for the manipulation of the 1D and 2D self-assembly of Pt(II) complexes by controlling the geometry.

A series of N -arylated viologens with terminal aldehyde groups has been synthesized. The new building blocks were successfully used to construct solution-processible, redox-active ionic porous polymers, for high-performance electrochromic films.

One-dimensional (1D) covalent organic networks (CONs) with uniform hierarchical structure exhibit great potential in the application of functional electronic devices. However, reports on the facile template-free construction of 1D nanostructure materials are very rare. Herein, we report two viologen-embedded CONs via Zincke reaction by simply altering the core planarity without any template. Ultralong fibrous morphology was observed for TPB-V by using a more twisted core, while TRZ-V with planar linker displays large spherical morphology. The time-dependent experiment unveils an interesting morphological evolution from stacked 2D platelets to fibers, that could be rationalized through a dissolution-reconstruction mechanism. When serving as organic cathodes, TPB-V fibers have much improved lithium storage performance than TRZ-V spheres. Notably, we have also successfully demonstrated the fabrication of 1D carbon nanotubes by direct calcination of TPB-V fibers. Benefiting from its high surface area and unique hollow tube morphology, the resulting soft carbon has been successfully utilized as a high-performance anode material for lithium-ion batteries. This work provides a new insight to optimize the 1D morphology of viologen-embedded CONs, and may bring up opportunities for developing functional materials with unprecedented properties and extensive applications.

Developing pure organic materials with ultralong lifetimes and balanced quantum efficiency is attractive but challenging. In this study, we propose a novel strategy to investigate external heavy atoms by linking molecular emitters with halogen through a flexible alkyl chain. X-ray crystal analysis clearly reveal the halogen C−X-π interactions, which can be tuned by halogen donors, as well as the distance and geometry between them. Impressively, DOPTZ-C3Cl featuring a chloride atom as donor, exhibits a balanced long phosphorescence lifetime of 1351 ms and a phosphorescence quantum yield of 10.1 %. We also first demonstrate that Cl can induce more positive effect than heavier halogens (Br and I) on prolonging the lifetime. We envisage that the present study will expedite new molecular design to manipulate the room temperature phosphorescence via external heavy atom effect, and highlight a special C−Cl⋅⋅⋅π interaction for the development of ultralong phosphorescent materials.

Design and integration of multiple redox-active organic scaffolds into tailored polymer structures to enhance the specific capacity and cycling life is a long-term research goal. Inspired by nature, we designed and incorporated a 4-electron accepting dicarbonylpyridinium redox motif into linear (DBMP) and cross-linked polymer (TBMP) structures. Benefiting from the suppressed solubility and higher electronic conductivity, the cross-linked TBMP based electrode exhibits improved cycling stability and higher specific capacity than the linear counterpart. After 4000 cycles at 1 A g-1, TBMP can maintain a high capacity of 252 mA h g-1, surpassing the performance of many reported organic cathodes. The structural evolution and reaction kinetics during charge and discharge have been investigated in detail. This study demonstrates that cross-linking is an effective strategy to push the bio-derived carbonylpyridinium materials for high performance LOBs.