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Metal catalysts for CO2 reduction reaction (CO2RR) face challenges such as high cost, limited durability and environmental impact. Although various diverse and functional metal-free catalysts have been developed, they often suffer from slow kinetics, low selectivity, and non-recyclability, significantly limiting their practical applications. In this study, we introduce a recyclable non-metallic polymer material (vitrimer) for a new platform in contact-electro-catalysis. This approach harnesses the contact charges generated between water droplets and vitrimer to drive CO2RR, achieving methanol selectivity exceeding 90%. The imine groups within the vitrimer play a dual role, facilitating CO2 adsorption and enriching friction-generated electrons, thereby mediating efficient electron transfer between the imine groups and CO2 to promote CO2RR. After 84 h, the system achieved a methanol production rate of 13 nmol·h-1, demonstrating the excellent stability of the method. Moreover, the vitrimer retains its high-performance electrocatalytic activity even after recycling. Mechanistic studies reveal that, compared to traditional metal catalysts, the N-O bond in the imine, which adsorbs the key intermediate *OCH3, breaks more readily to produce methanol, resulting in enhanced product selectivity and yield. This efficient and environmentally friendly contact-electroreduction strategy for CO2 offers a promising pathway toward a circular carbon economy by leveraging natural water droplet-based contact-electrochemistry., (© 2025 Wiley‐VCH GmbH.)

Perovskite-based tandem solar cells (PTSCs) are promising for achieving higher efficiency limits, making them promising candidates for energy supply. However, the commercialization in complex scenarios necessitate extreme stability and reliability of tandem devices, particularly in ambient conditions. Herein, the use of a high-efficiency and air-stable quaternary all-polymer bulk heterojunction (BHJ) is pioneered to optimize spectral absorption, facilitate charge transport, and suppress exciton recombination, resulting in 18.0% of power conversion efficiency (PCE) in the organic subcell. The resultant monolithic perovskite/organic tandem solar cell (POTSC) delivers an impressive PCE of 24.8%, with minimal efficiency distribution and negligible hysteresis. Ambient stability tests on tandem devices reveal  outstanding ambient stability, which is attributed to the reduced increase in exciton recombination. Remarkably, the unencapsulated tandem device maintained 88% of its initial efficiency after exposure to air for 500 h. The superior stability is owing to the enhanced resistance of the hydrophobic all-polymer BHJ to water and oxygen, thereby protecting the perovskite active layer. This work provides a novel approach from an organic perspective for achieving superior efficiency and stability in POTSC devices and holds promise for future real-world applications in the field of tandem solar cells., (© 2025 Wiley‐VCH GmbH.)

Understanding gas-involved physicochemical reactions is undoubtedly one of the most significant challenges in the modern chemical industry. To clarify how those reactions precede requires deep insights into the real-time visualization of reaction dynamics within a gas environment. The emergence and rapid development of in situ environmental electron microscopy (EEM) including scanning electron microscopy (ESEM) and transmission electron microscopy (ETEM) have enabled multiscale observation of dynamic gas-involved physicochemical reactions. This review examines the state-of-art EEM technologies, categorizing those gas reactions into various physical and chemical processes and detailing the corresponding dynamic behaviors. It begins by reviewing the state-of-the-art EEM techniques and is followed by detailing their application in typical physical processes. It clarifies physical vapor condensation, deposition, and geometric reshaping with gaseous involving. More importantly, all the gas-involved chemical reactions into electrochemical reactions, thermochemical reactions, chemical crystal growth, and catalytic reactions are thoroughly explored and categorized. Finally, the review highlights the technical challenges and valuable perspectives provided by in situ EEM for addressing critical gas-involved issues. Overall, this article offers a multiscale and comprehensive understanding of the physicochemical origins associated with gas-involved reactions, envisioning fundamental strategies for designing high-performance gas-involved functional materials., (© 2025 Wiley‐VCH GmbH.)

The contradiction between high transmittance and favorable conductivity poses a great challenge in developing effective cathode interlayer (CIL) materials with sufficient thickness tolerance, which hinders the further advancement of organic solar cells (OSCs). Herein, a completely new class of alcohol processable polyimide-ionene hybrids (PIIHs) is proposed by melding pyromellitic diimide (PMD) subunits into imidazolium-based ionenes backbone covalently. These PIIHs, named PMD-DI and PMD-PD, boast high transparency, suitable energy levels, and decent conductivity. A higher PMD content endows PMD-PD with improved work function tunability, electrical properties, and crystallinity, enabling PMD-PD as CIL material with excellent thickness-insensitive characteristics, while simultaneously improving device stability significantly. Furthermore, PMD-PD also exhibits good compatibility with various electrodes and active layers, offering solar cell efficiencies of up to 19.91% and 19.29% with Ag and Cu cathodes, respectively. More importantly, the application of PMD-PD can improve the performance of semi-transparent OSCs without losing transmittance, thereby drastically enhancing the light utilization efficiency to 4.04% with an ultrathin, low-cost Cu cathode, that competes with leading optical modulation-free semitransparent OSCs with expensive Ag cathodes. This work opens a pathway to realize transparent and conductive interlayers by strategic molecular design, leading to highly efficient, stable, and cost-effective OSCs suitable for diverse applications., (© 2025 Wiley‐VCH GmbH.)

Blue light activation of N,N-dichlorocarbamates facilitates a direct 1,2-aminochlorination of unactivated olefins to yield 1,2-chloro-N-Cl compounds under ambient conditions. Mechanistic studies suggest that N,N-dichlorocarbamates undergo a photochemical excitation to yield a neutral nitrogen-centered radical, which rapidly reacts with olefins in an anti-Markovnikov fashion. Using this method, a range of functionally diverse substrates are successfully aminochlorinated to yield the corresponding 1,2-chloro-N-Cl compounds., (© 2025 Wiley‐VCH GmbH.)

Properties of hybridized local and charge-transfer (HLCT) materials can be tuned by adjusting locally excited (LE) and charge-transfer (CT) components, resulting in either quasi-equivalent hybridization or non-equivalent hybridization. These HLCT materials are easily designed on the molecular level to be applied in organic light-emitting diodes (OLEDs), which have advantages in the aspects of external quantum efficiency (EQE), efficiency roll-off, and color purity. In previous work, an HLCT silole derivative with an electron donor (D) - acceptor (A) structure modified at 1-position achieved a breakthrough in the external quantum efficiency (EQE) of 9.1%. Whereas such molecular design generally leads to low PLQYs, limiting the further improvement of EQE. Thinking a more rigid structure design strategy, in this work, silole is replaced with a more rigid benzosilole structure that is selectively modified by a carbazole (Cz) or 9,9-dimethyl-9,10-dihydroacridine (Ac) unit as donor and triazine (TRZ) unit as the acceptor, leading to higher PLQYs of the CT-like HLCT molecule DCz-BS-TRZ, and quasi-equivalent HLCT molecule DAc-BS-TRZ. Among these two molecules, the DCz-BS-TRZ-based OLED device has shown a remarkable 13% EQE max , which is the highest EQE for silole-based OLEDs., (© 2025 Wiley‐VCH GmbH.)

Silver-telluride-based nanowires (STNWs) are promising thermoelectric (TE) materials for room temperature (RT) applications, can be utilized to fabricate flexible TE composites or inks to facilitate TE conversion in various situations. However, current research on doping design and morphology optimization of STNWs is still limited. Such strategies are expected to enhance the TE performance and flexibility, thereby improving the compatibility of STNWs for TE applications. Herein, we report a simple yet efficient iodide ion-assisted strategy for doping design and morphology optimization, significantly enhancing both the TE performance and flexibility of the STNW films. Iodide ions serve dual roles of regulating the chemical transformation process and acting as a effective dopant, ultimately achieving a 1.97-fold increment in the power factor of the STNW films at RT, as well as promoting the formation of a structure of bundles composed of morphology-optimized STNWs, which significantly improves the flexibility of STNW films. On this basis, flexible TE composite films and TE devices are fabricated and systematically evaluated, demonstrating the excellent potential of STNWs for practical applications. This study paves the way for the development of STNW-based TE materials and provides insights for synthesis of other nanostructured TE materials., (© 2025 Wiley‐VCH GmbH.)

Developing a thoroughgoing recovery technology that allows simultaneously separating and recovering all functional layers of the end-of-life perovskite solar cells (PSCs), in keeping with maintaining potent device efficiency and eco-environment friendliness, is crucial toward the sustainability of PSCs. Herein, we propose a facile closed-loop recycling strategy to realize the acquisition and reutilization of hole transport material and other retrievable components from obsolete PSCs, employing chlorobenzene and dimethylformamide to sequentially dissolve the spiro-OMeTAD and perovskite layers. Surprisingly, the recycled spiro-OMeTAD, i.e., oxidized spiro-OMeTAD (spiro-OMeTAD •+ ) endows reinforced conductivity and hole mobility, favorable energy band alignment, and mitigated perovskite defects, thus resulting in expedited hole extraction and lessened nonradiative recombination loss. Along with the dissolution of the spiro-OMeTAD and perovskite layers, other functional materials involving Ag, PbI 2 , and ITO/SnO 2 are concurrently recovered. Note that the solubilizers are also recycled to eliminate the alien reagents to environmental hazards. The refabricated PSC based on the recovered materials delivers an upgrading power conversion efficiency of up to 23.41% together with an open circuit voltage of 1.17 V, outperforming the control device based on fresh materials (20.77%, 1.11 V). Overall, this strategy holds promise for realizing closed-loop recycling of end-of-life PSCs, and thus pushes future PSCs sustainability., (© 2025 Wiley‐VCH GmbH.)

The upcycling of polyethylene terephthalate (PET)-derived ethylene glycol (EG) to glycolic acid (GA, a biodegradable polymer monomer) via electrocatalysis not only produces valuable chemicals but also mitigates plastic pollution. However, the current reports for electrooxidation of EG-to-GA usually operate at reaction potentials of >1.0 V vs reversible hydrogen electrode (RHE), much higher than the theoretical potential (0.065 V vs RHE), resulting in substantial energy wastage. Herein, body-centered cubic RhIn intermetallic compounds (IMCs) anchored on carbon support (denoted as RhIn/C) are synthesized, which shows excellent performance for the EG-to-GA with an onset potential of only 0.35 V vs RHE, lower than the values reported in current literature. The catalyst also possesses satisfactory GA selectivity (85% at 0.65 V vs RHE). Experimental results combined with density functional theory calculations demonstrate that RhIn IMCs enhance the adsorption of EG and OH - , facilitating the generation of reactive oxygen species and thereby improving catalytic performance. RhIn/C also exhibits excellent electrocatalytic performance for hydrogen evolution reaction, ensuring that it can be used as a bifunctional catalyst in the two-electrode system for EG electrooxidation coupled with hydrogen production. This work opens new avenues for reducing the energy consumption of electrocatalytic upcycling of PET-derived EG and clean energy production., (© 2025 Wiley‐VCH GmbH.)

Numerous modification strategies have been proposed to enhance the performance of the Zn anode and carbon cathode in aqueous zinc-ion hybrid capacitors (ZIHCs). However, one efficient strategy to modify both the anode and cathode is still lacking. Herein, taurine (Tau), the key ingredient of energy drinks, is used as the electrolyte additive and carbon precursor for ZIHCs simultaneously. As the electrolyte additive, Tau achieves the preferential growth of Zn (002) plane by preferentially adsorbing on other crystal planes. Moreover, Tau accelerates Zn 2+ transference kinetics by regulating the Zn 2+ solvation structure and constructs a functional solid electrolyte interphase layer, enabling suppressed hydrogen evolution, inhibited corrosion reaction, and dendrite-free deposition. The Zn//Zn cells using the Tau-modified·ZnSO 4 electrolyte (Tau-ZSO) can stably work for 1000 h at 76.95% depth of discharge at room temperature and 5200 h at -10 °C. Meanwhile, the taurine-derived carbon (Tau-C) exhibits N, S heteroatom doping, hierarchical porous structure, and high specific surface area, which contributes to a high cathode capacity. By using the Tau-C cathode, limited Zn anode (10 µm), and the Tau-ZSO electrolyte, the assembled ZIHCs demonstrate reduced polarization and high discharge capacities (119.4 mA h g -1 under 3 A g -1 at room temperature and 80.0 mA h g -1 under 1 A g -1 at -10 °C) with high energy density of 101.1 Wh kg -1 and long lifetime (operating stably over 2000 cycles)., (© 2025 Wiley‐VCH GmbH.)

Achieving the "on-off" control of hydrogen release remains a huge challenge in efficiently harnessing hydrogen energy on demand. In this work, a controlled hydrogen production strategy is proposed. Hydrogen carrier ammonia borane (AB) and Co catalyst are loaded into kaolinite aerogel (KA) to obtain a composite AB@Co/KA monolith. The results show that Co particles with surface-oxidized species are uniformly decorated on the surface of aerogel, and AB can fill the pores of aerogel to form a composite hydrogen storage material. Hydrogen generation is modulated on AB@Co/KA by tuning the amount of water added, which achieves an "on-off" hydrogen release on demand. The Co-modified KA (Co/KA) can be repackaged multiple times for recycling use after the AB is completely hydrolyzed. This work provides a promising approach for controlling the release of hydrogen neither the input of additional energy nor foreign reagents added to the reaction system., (© 2024 Wiley-VCH GmbH.)

Global concerns regarding the depletion and strategic importance of phosphorus resources have increased demand for the recovery and recycling. However, waste-derived phosphorus compounds, primarily as chemically inert phosphoric acid or its salts, present a challenge to their direct conversion into high-value chemicals. We aimed to develop an innovative technology that utilizes the large quantities of sewage waste, bypasses the use of white phosphorus, and enables esterification of phosphoric acid to produce widely applicable phosphate triesters. Tetraalkyl orthosilicates emerged as highly effective reagents for the direct triple esterification of 85 % phosphoric acid, as well as the esterification of organophosphinic and phosphonic acids. Furthermore, we achieved esterification of recovered phosphoric acid with tetraalkyl orthosilicate, thus pioneering a recycling pathway from sewage waste to valuable phosphorus chemicals. Experimental and theoretical investigations revealed a novel mechanism, wherein tetraalkyl orthosilicates facilitate multimolecular aggregation to achieve alkyl transfer from tetraalkylorthosilicate to phosphoric acid via multiple proton shuttling., (© 2024 Wiley-VCH GmbH.)

Pentose oxidation and reduction, processes yielding value-added sugar-derived acids and alcohols, typically involve separate procedures necessitating distinct reaction conditions. In this study, a novel one-pot reaction for the concurrent production of xylonic acid and xylitol from xylose is proposed. This reaction was executed at ambient temperature in the presence of a base, eliminating the need for external gases, by leveraging Pt-supported catalysts. Initial experiments using commercially available metal-supported carbon catalysts validated the superior activity of Pt. However, a notable decline in recycling performance was observed in Pt/C, which is attributed to the sintering of Pt nanoparticles. In contrast, the synthesized Pt-supported ZrO 2 catalysts exhibited enhanced recycling performance because of the strong metal-support interaction between Pt and the ZrO 2 support. Furthermore, mechanistic insights and density functional theory calculations show that product desorption involves a significantly higher energy barrier compared to substrate adsorption and hydrogenation, highlighting an efficient transfer hydrogenation mechanism leading to equivalent yields of both xylonic acid and xylitol. This study introduces a promising approach for the simultaneous production of sugar-derived acids and alcohols, with implications for sustainable catalysis and process optimization., (© 2024 The Authors. ChemSusChem published by Wiley-VCH GmbH.)

Quinolines have emerged as essential components in various medicinal agents, playing a key role in treating various ailments. Numerous drugs with a quinoline core have been recognized for their antimalarial, antibacterial, and anticancer activities and have been successfully commercialized, including chloroquine, ciprofloxacin, topotecan, etc. Over the past two decades, a tremendous expansion in the C-H bond functionalization of quinoline scaffolds to widen this chemical space for drug discovery have been witnessed. This review article summarizes the efforts toward C(sp 3 )-H functionalization of 8-methylquinolines for C(sp 3 )-C/X bond formation under metal and metal-free strategies. Each section briefly overviews the C(sp 3 )-H functionalization of 8-methylquinoline, highlighting the metal and metal-free approaches., (© 2024 Wiley-VCH GmbH.)

Mechanochromic materials, known for their ability to change color in response to mechanical stimuli such as pressure, stretching, grinding, or rubbing, hold significant importance due to their diverse applications. In this study, we synthesized and characterized two novel pyridine-tethered imidazo[1,2-a]pyridine mechanoresponsive luminogens with appended tetraphenylethene, named GBY-10 and GBY-11. GBY-10 exhibited reversible mechanofluorochromism, while GBY-11 did not revert to its original color after solvent fuming. The photophysical properties of these luminogens were significantly influenced by the position of the terminal pyridine. Additionally, we created color-tunable mechanoresponsive molecular salts by co-grinding GBY-11 with various aryl acid derivatives. Co-grinding GBY-11 with pentafluorobenzoic acid resulted in a significant bathochromic shift of the emission maxima by 66 nm, compared to 37 nm and 12 nm shift for benzoic acid and para-nitrobenzoic acid, respectively. This counter-ion-dependent luminescence suggests strong electronic interactions between the counter ions. These luminogens also demonstrated reversible pH-responsive behaviour, making them suitable for anti-counterfeiting applications. Furthermore, the pyridine-functionalized luminogen, GBY-10, showed metal ion detection (Mn 2+ , Ag + , Fe 3+ ) ability in water, with detection limits as low as 0.0043, 0.015, and 0.0029 mM, respectively. This report opens new avenues for designing promising AIE-active materials for potential applications in anti-counterfeiting, sensing, optoelectronics, and biomedicine. A de-novo approach of engineering imidazo[1,2-a]pyridine scaffold to mechanoresponsive AIE-active molecules for anti-counterfeiting and metal sensing applications. By co-grinding the designed luminogens with various aryl acid derivatives, color tuneable mechanoresponsive molecular salts can be further developed., (© 2025 Wiley-VCH GmbH.)

Covalent organic frameworks (COFs) are a new type of porous organic crystalline material, which have become an emerging platform for promoting the development of green energy technology due to their high surface area, adjustable pores, low skeleton density, and easy functionalization. In recent years, with the continuous advancement of synthesis technology, the synthesis efficiency and sustainability of COFs have been significantly improved, from traditional solvothermal methods to the emergence of various green synthesis strategies such as ion thermal, mechanochemical, and ultrasound assisted methods. This article reviews the main synthesis methods of COFs and explores their applications in the field of green energy, such as photocatalysis, gas adsorption and separation, electrocatalysis, battery, supercapacitor and Proton exchange membrane fuel cell. By analyzing the performance and mechanism of COFs in these applications in detail, this article further looks forward to the challenges and future development trends faced by COFs in green energy technology, aiming to provide valuable reference and inspiration for researchers in related fields., (© 2025 Wiley-VCH GmbH.)

The urea oxidation reaction (UOR) is characterized by a lower overpotential compared to the oxygen evolution reaction (OER) during electrolysis, which facilitates the hydrogen evolution reaction (HER) at the cathode. Charge distribution, which can be modulated by the introduction of a heterostructure, plays a key role in enhancing the adsorption and cleavage of chemical groups within urea molecules. Herein, a facile all-room temperature synthesis of functional heterojunction NiCo 2 S 4 /CoMo 2 S 4 grown on carbon cloth (CC) is presented, and the as-prepared electrode served as a catalyst for simultaneous hydrogen evolution and urea oxidation reaction. The Density Functional Theory (DFT) study reveals spontaneous transfer of charge at the heterointerface of NiCo 2 S 4 /CoMo 2 S 4 , which triggers the formation of localized electrophilic/nucleophilic regions and facilitates the adsorption of electron donating/electron withdrawing group in urea molecules during the UOR. The NiCo 2 S 4 /CoMo 2 S 4 // NiCo 2 S 4 /CoMo 2 S 4 electrode pair required only a cell voltage of 1.17 and 1.18 V to deliver a current density of 10 and 100 mA cm -2 respectively in urea electrolysis cell and display very good stability. Tests performed in real urine samples show similar catalytic performance to urea electrolytes, making the work one of the best transition metal-based catalysts for UOR applications, promising both efficient hydrogen production and urea decomposition., (© 2025 Wiley‐VCH GmbH.)

Biodegradable polyesters provide an attractive alternative to non-degradable plastics but often encounter a tradeoff between biodegradability and mechanical properties because esters are rotational and lack hydrogen bonds. Conversely, natural polyamides, i.e., silk exhibit excellent mechanical strength because amides are non-rotational and form hydrogen bonds. Unlike esters, the nitrogen in amides can enhance microbial biodegradation. However, protein engineering exhibits limited productivity, and artificial polyamides, i.e., nylon remain non-degradable due to their hydrophobic nature. Herein, a method is proposed for developing poly(ester amide)s (PEA)s, a polyester and polyamide hybrid, to address prevailing production challenges. These materials are synthesized from upcycled monomers in a 10 L reactor and converted into films and yarns. They achieve a tensile strength of 109 MPa and tenacity of 5.0 g de -1 , while withstanding ironing temperatures. They achieve a remarkable 92% marine biodegradability in 12 months, which is rarely attained by current bioplastics, and exhibit low environmental impact in terms of greenhouse gas emissions. While biodegradable polyesters have remained within the performance range of commodity plastics, PEAs fall into the high-performance category, potentially reaching markets that existing biodegradable plastics have not, such as fishing lines and clothing., (© 2024 Wiley‐VCH GmbH.)

Thermoplastic polyurethane (TPU) exhibits re-processable properties, but the properties of TPU is deteriorated during the reprocessing for the oxidation and degradation of polymer chains. Meanwhile, although thermoset polyurethane exhibits excellent mechanical properties, it cannot be recycled for permanent crosslinking. Hence, it's still a challenge to obtain PU which exhibits the balance between the recyclability and mechanical properties. In this work, a new dynamic bond obtained from the reaction between enaminone and isocyanate is used to prepare re-processable millable polyurethane, and the morphology of network can be tuned via the dissociation of the cross-linked sites of PU. Interestingly, the cross-linked network can transform into a linear polymer by adding the amine which can be used when reacted with isocyanate to generate new re-crosslinked PU. This process can be carried out in a Haake mixer without any solvents. The mechanical properties of the re-crosslinked polyurethane can be tuned via the controlling of the amine and isocyanate addition, and the maximum tensile strength increase by 178.4% after processing for four times, realizing mechanical reinforcement after recycling. This kind of recycling achieves through one-step melting method in solvent-free conditions provides a feasible way to prepare recyclable PU with good mechanical performance and customizable properties., (© 2025 Wiley‐VCH GmbH.)

The confining effect is essential to regulate the activity and stability of single-atom catalysts (SACs), but the universal fabrication of confined SACs is still a great challenge. Here, various lattice-confined Pt SACs supported by different carriers are constructed by a universal co-reduction approach. Notably, Pt single atoms confined in the lattice of Ni(OH) 2 (Pt 1 /Ni(OH) 2 ) with a high electron-deficient state exhibit excellent activity for basic hydrogen evolution reaction (HER). Specifically, Pt 1 /Ni(OH) 2 just requires 15 mV to get 10 mA cm -2 and the mass activity of Pt 1 /Ni(OH) 2 is 15 times of commercial Pt/C. Moreover, Pt 1 /Ni(OH) 2 assembled in an alkaline water electrolyzer shows 1030 h durability under the industrial current density of 800 mA cm -2 . In situ spectroscopy techniques reveal Pt─H and "free" OH radical can be directly observed for Pt 1 /Ni(OH) 2 , confirming the lattice-confined Pt single atoms play a key role during HER. Further density functional theory uncovers the Pt 3d orbital strongly hybridizes with O 2p and Ni 3d orbitals in Ni(OH) 2 , which quickly optimizes the electronic state of the Pt site, thus largely reducing the energy barrier of the rate-determining step to 0.16 eV for HER. Finally, this synthesis method is extended to construct other 9 lattice-confined SACs., (© 2025 Wiley‐VCH GmbH.)

This study focuses on applying microbial self-healing cement in repairing cracks in cement-based materials and enhancing its resistance to water penetration performance. Traditional cement is susceptible to environmental influences, leading to the formation of microcracks and a reduction in durability. This research used Bacillus pseudofirmus to prepare microcapsules through sodium alginate gelation technology. We mixed microcapsules into the cement. The results indicate that the microbial self-healing cement, with a 1% self-healing agent added, increased its resistance to water penetration ability by 29.2% after 28 days. This improvement rose to 39.3% after 84 days. Additionally, we used the embedded needle method to make mortar blocks through microcracks, mimicking the cracks found in real cement. The self-healing effect of the microcapsules was especially noticeable for cracks under 0.3 mm in diameter, compared to the commonly used commercial crystallization penetration technology. This is attributed to the crystalline bodies formed by the self-healing agent in the microcapsules blocking the cracks and preventing water penetration. This study provides an environmentally friendly solution for the repair of cracks in cement-based materials using microbial self-healing technology and lays the foundation for improving the repair efficiency and durability and exploring stability and reliability in the future. Practical Application: This study investigated the application of microbial self-healing cement in repairing cracks in cement-based materials and enhancing its resistance to water penetration properties. Cement, a material widely used in infrastructure, has low tensile strength and often forms microcracks. These microcracks reducing the durability of cement and posing risks to the economy and safety. Adding 1% self-healing agent to microbial self-healing cement significantly increases the resistance to water penetration pressure of the mortar blocks. Compared to the standard specimens, the resistance to water penetration ability increased by 29.2% at 28 days and further increased to 39.3% at 84 days. Microbial self-healing cement could effectively restore the resistance to water penetration performance of the mortar blocks after repairing cracks. The repairing results are significantly better than the methods of mixing or applying cement crystalline materials., Competing Interests: The authors have declared no conflicts of interest., (© 2025 The Author(s). Engineering in Life Sciences published by Wiley‐VCH GmbH.)

Chiral supramolecular polymers with stimuli-responsive circularly polarized luminescence (CPL) are highly desirable for smart flexible optoelectronic devices, but remain rarely reported. Here, a simple solvent-free supramolecular polymerization for preparing chiral polyurethanes is presented by in situ induced self-assembly strategy, using cellulose nanocrystals (CNCs)-based isocyanate prepolymers and macromolecular polyols as precursors, achieving precise control over polymer chain assembly with spot-like arrangement. More importantly, by further incorporating a π-conjugated luminescent dihydroxynaphthalene molecule, CPL-active flexible polyurethane films with feather-like nanostructures are constructed, which promote the ordered arrangement of CNCs-based isocyanate segments due to the increased spatial resistance. The π─H bond network between CNCs and urethane-linked benzene rings drives the self-assembly, enabling higher-level chiral amplification and enhanced fluorescence. Interestingly, the prepared chiral fluorescent polyurethanes display multimodal chiroptical stimuli responsiveness under various stimuli, such as temperature, solvent polarity, pH, and polarized light, due to the sensitivity of the π─H bond network. This work offers new insights into designing solvent-free chiral supramolecular polymers with significant chiroptical potentials., (© 2025 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

The electrochemical CO 2 reduction reaction (CO 2 RR) exhibits significant potential to efficiently convert CO 2 into ethylene (C 2 H 4 ). However, achieving high C 2 H 4 selectivity remains a considerable challenge due to the difficulty in effective C─C coupling and stringent requirements on CO 2 purity. Herein, a novel contact-electro-catalysis method for CO 2 RR is presented by constructing dual-active-site catalysts on the electronegative tribolayer of a triboelectric nanogenerator (TENG), including single copper atom anchored polymeric carbon nitride (Cu─PCN) and CuO nanoparticle, achieving an outstanding C 2 H 4 Faradaic efficiency of 63.5% in dilute CO 2 . Experimental and theoretical studies indicate that Cu─PCN active sites exhibit the ability to heighten * H adsorption and facilitate its migration into CuO nanoparticles. This process effectively modulates the coverage of * H on CuO and promotes the transformation of * CO into * CHO. Subsequently, * CHO undergoes dimerization on the CuO surface, ultimately yielding C 2 H 4 . Furthermore, the electric field generated by the TENG enhances the coverage of * H and * CO on both the Cu─PCN and CuO surfaces, which subsequently reduces the energy barrier for C─C coupling. This work provides a new route to enhance the selective reduction of CO 2 to C 2 H 4 by integrating contact electrocatalysis with dual active site technologies., (© 2025 Wiley‐VCH GmbH.)

Here we report the synthesis of a geometrically distinct three-dimensional (3D) chiral nanocarbon, which is composed of three π-extended [6]helicene subunits fused on a [3,3,3]propellane with P,P,M/M,M,P configurations in the helicene subunits. This nanocarbon can isomerize into the thermodynamically more stable isomer with PPP/MMM configurations in the helicene subunits. Both 3D nanocarbons display a very stable configuration, which can be separated by chiral HPLC. Notably, the nanocarbons display significantly enhanced chiroptical properties compared to the refer-ence π-extended [6]helicene, due to the improved alignment of magnetic and electric transition dipole moments. The twisted [6]helicene subunits in the nanocarbon provide concave surfaces that are suitable-albeit relatively weak-host for C60, forming a 1:2 host-guest complex in the solid state., (© 2025 Wiley‐VCH GmbH.)

Positive temperature coefficient (PTC) materials exhibit significant potential in thermal management due to their adaptive temperature regulation. However, current PTC materials are often constrained in the thermal regulation within the low-temperature range due to the high Curie temperatures. Achieving low Curie temperatures often requires small-molecule polymer matrices, which can compromise mechanical properties and lead to phase change material leakage. To overcome this challenge, this study innovatively proposes a generalized design strategy for bi-continuous phase thermally controlled PTC composite materials (PTCCM) based on polyimide aerogel (PIA) encapsulation. PIA forms a continuous backbone structure, while 1-Tetradecanol serves as a fibrous phase change matrix. Additionally, multi-doped conductive fillers construct an efficient fiber bundle-like network. In the temperature range of 10-50 °C, the PTC strength achieves 3.55, with a low resistivity of 1.5 Ω m. Thanks to its stable PIA skeleton and perfect conductive network, PTCCM can accurately stabilize the device temperature at 29.5 ± 1.5 °C under different low-temperature environments and voltages. The temperature control accuracy is as high as 0.03 °C, presenting excellent cycling stability. These characteristics make it promising in meeting stringent thermal management demands., (© 2025 Wiley‐VCH GmbH.)

Relay catalysis represents significant efficacy in alleviating competition among different reactants during coupling reactions. However, a comprehensive understanding of the reaction mechanism underlying relay catalysis for the urea electrosynthesis remains challenging. Herein, we have developed a catalyst (CuAC-CuSA@NC) comprising Cu atomic clusters (CuAC) with satellite Cu-N4 single atoms (CuSA) sites on the nitrogen-doped porous interconnected carbon skeleton (NC), enabling elucidation of a relay catalysis process for co-reduction of CO2 and NO3-. The designed CuAC-CuSA@NC catalyst exhibits an approximately threefold higher urea yield rate compared to that of CuSA@NC at -1.3 V vs. RHE. Ex-situ experimental results and in-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy analysis reveal a formation sequence between the *NH2 and *NH2CO species on CuAC-CuSA@NC with increasing reduction potential. The combination of theoretical calculations further elucidates that the relay catalysis pathway involves "CuAC" sites facilitating the conversion of *NO3 to *NOx, followed by a hydrogenation process to form *NH2 with *H from water dissociation promoted by "CuSA" sites, which subsequently couples with *CO2 to produce urea. This work provides novel insights into the investigation of coupling reactions, but not limit to, urea synthesis., (© 2025 Wiley‐VCH GmbH.)

Developing efficiently mixed electronic-ionic (MEI) conductive pathways within a single functional material at the microscale is essential yet challenging for various electronic devices. Covalent organic frameworks (COFs) feature pre-designed functionalities and uniform pores, making them highly desirable platforms for the transport of electrons and ions. However, for MEI conductive COFs, achieving high crystallinity when incorporating high-density ionic groups within the extensively π-electron delocalized skeletons remains a challenge due to intermolecular interactions. Herein, we reported a "pre-polymerization followed by self-ionization" approach to synthesize new thiazolium-linked COFs (MEICOFs, M = Cu, Co, Fe), where the ionic groups synthesized following the connection of building blocks. These MEICOFs demonstrated broad ultraviolet-visible-near-infrared absorption bands and narrow band gaps. As a proof of concept, the mixed electronic and hydroxide ionic conductivity of CuEICOF were determined to be 55.2 and 0.01 S m-1, respectively. Moreover, MEICOFs film could directly catalyze the oxygen reduction reaction without additional conductive agent and the rotation of electrode., (© 2025 Wiley‐VCH GmbH.)

Photoswitchable molecules can transit between two distinct isomers, enabling them to perform highly controllable imaging and therapeutic functions under certain laser irradiation. Dithienylethenes (DTEs), a class of photoswitchable molecules, exhibit strong thermal stability and high fluorescence quantum yield. However, the short excitation wavelength poses a significant challenge for the application of DTEs in photocontrolled imaging and therapy. Therefore, the development of DTE-based derivatives or hybrid materials with near-infrared (NIR) excitation is of great importance. In this study, two novel DTE derivatives are synthesized, whose closed-ring isomers exhibit strong absorption in the NIR region. Compared with a DTE derivative previously reported and commercially available ones, these two DTE derivatives show higher photoswitching efficiency and extended absorption wavelength. Notably, the supramolecular assembly between DTE derivatives and albumin confers NIR-activated photothermal switching ability on DTE molecules in aqueous solution. In addition, DTE-albumin nanoparticles are further developed to enable photoswitchable photoacoustic imaging (PAI) and photothermal therapy (PTT) for in vivo antitumor applications. Finally, by integrating a thermo-responsive free radical initiator into DTE-albumin nanoparticles, photoswitchable PTT and chemodynamic therapy (CDT) are achieved, effectively inhibiting tumor growth and preventing tumor metastasis., (© 2025 Wiley‐VCH GmbH.)

Herein, bis-sulfonimide (BSI), characterized by multiple d-pπ bonds rather than typical p-pπ bonds, is unprecedently utilized as a general and extendable building block to develop a series of multifunctional cathode interlayer materials (CIMs) for organic solar cells (OSCs). An illustrative CIM, BSIz-TT-PDI, demonstrates favorable alcohol processability, superior work function tunability, appropriate energy levels, strong self-doping effect, and decent crystallinity. These attributes contribute to its high conductivity exceeding 5×10-3 S/cm, as well as precise optimization of the interfacial connection between the active layer and metal cathode. Therefore, BSIz-TT-PDI-based OSCs delivers an outstanding efficiency of 18.08% using PM6:Y6 active layer while retaining 84% of its initial performance after tracking at the maximum power point under continuous illumination for 1100 hours. Additionally, the devices maintain over 94% of the optimal performance across a film thickness range of BSIz-TT-PDI from 5 to 90 nm. Moreover, BSIz-TT-PDI exhibits high compatibility with various active layers, enabling a record efficiency of 19.80% with the PM6:BTP-eC9:L8-BO active layer. This work not only introduces a new library of water/alcohol-soluble n-type semiconductors containing BSI, while also pioneers the creation of thickness-insensitive CIMs for stable and efficient OSCs by integrating electron-withdrawing components with d-pπ bonds., (© 2025 Wiley‐VCH GmbH.)

Upcycling carbon dioxide (CO2) into long-chain compounds has attracted considerable attention with respect to mitigating environmental problems and obtaining value-added feedstocks, but remains a great challenge. Herein, we report a tandem photocatalysis-biosynthesis strategy for efficient CO2 reduction to energy-rich sucrose or α-farnesene. Firstly, photocatalytic reduction of CO2 to CH4 was optimized over the transitional metal doped ZnO (M-ZnO). The as-prepared Ni-ZnO preferentially reduces CO2 to CH4 with a production rate of 1539.1 µmol g-1 h-1 and a selectivity of 90%, owing to the unique interface structure (Znδ+-O-Niβ+). Subsequently, Methylomicrobium buryatense 5GB1C was genetically engineered to produce sucrose or α-farnesene using photocatalytically-obtained CH4 as the sole carbon source, with a titer of 96.3 and 43.9 mg L-1, respectively. This study provides a green, low-energy pathway for the synthesis of long-chain compounds from CO2 as the carbon source, which sheds new light on tackling long-term energy demands and sustainable CO2 upcycling., (© 2025 Wiley‐VCH GmbH.)

Supramolecular polymers driven by the metal-ligand coordination possess reversible bonds, making them promising candidates for integrating the therapeutic functions of metal ions and small-molecule drugs, and subsequently releasing these components within cells after endocytosis. In this study, a kind of supramolecular polymer, SHICU, is developed, composed of Shikonin ligand and Cu(II) ion. Upon reduction by intracellular glutathione (GSH), SHICU dissociates to release Shikonin, Cu(II), and SHICU fragments. The released Shikonin and Cu(II) exhibit a synergistic antitumor effect through the reactive oxygen species (ROS)-dependent necrosis. Meanwhile, the released SHICU that remains structural integrity induces a distinct antitumor mechanism by triggering cuproptosis in tumor cells. This dual functionality, combining ROS-dependent necrosis and cuproptosis, highlights the potential of SHICU in advancing antitumor therapies, while the integration of supramolecular polymers with the emerging cell death mechanism of cuproptosis facilitates the development of innovative cancer drugs., (© 2025 Wiley‐VCH GmbH.)

Electrocatalytic organic oxidation coupled with hydrogen (H 2 ) production emerges as a profitable solution to simultaneously reduce overall energy consumption of H 2 production and synthetic high-value chemicals. Noble metal catalysts are highly efficient electrocatalysts in oxidation reactions, but they deactivate easily weakening the benefit in actual production. Herein, we report a universal asymmetric pulse potential strategy to achieve long-term stable operation of noble metals for various alcohol oxidation reactions and noble metal catalysts. For example, by pulsed potentials between 0.8 V and 0 V vs. RHE, palladium (Pd)-catalyzed glycerol (GLY) electrooxidation can continuously proceed for more than 2800 h with glyceric acid (GLA) selectivity of >70 %. Whereas, Pd electrocatalyst becomes nearly deactivated within 6 h of reaction under conventional potentiostatic strategy. Experimental and theoretical calculation results reveal that the generated electrophilic OH* from H 2 O/OH - oxidation on Pd (denoted as Pd-OH*) acts as main active species for GLY oxidation. However, Pd-OH* is prone to be oxidized to PdO x resulting in performance decay. When a short reduction potential (e.g., 0 V vs. RHE for 5 s) is powered, PdO x can be reversibly reduced to restore the current. Moreover, we tested the feasibility of this strategy in a flow electrolyzer, verifying the practical application potential., (© 2024 Wiley-VCH GmbH.)

Electrocatalytic reduction of NO 3 - is a green and sustainable method that not only helps to treat industrial pollutants in wastewater, but also produces valuable chemicals. However, the slow dynamics of the proton-coupled electron transfer process results in a high barrier and low conversion efficiency. In this work, the Se-deficient FeSe 2 /Fe 3 O 4 heterojunction was synthesized, which showed excellent electrochemical performance in 0.1 M nitrate reduction reaction, superior to most currently reported catalysts. The high activity of Se-deficient FeSe 2 /Fe 3 O 4 is due to the synergistic effect between FeSe 2 and Fe 3 O 4 to achieve relay catalytic NO 3 - reduction. Among them, the Se-deficient FeSe 2 contributes to NO 3 - deoxygenation and subsequent hydrogenation, and Fe 3 O 4 promotes H 2 O decomposition to provide H proton, jointly promote NO 3 RR. Finally, the online differential electrochemical mass spectra (DEMS), in situ Raman and DFT calculation confirmed the optimal pathway for NO 3 RR to NH 3 on Se-deficient FeSe 2 /Fe 3 O 4 (100). This strategy of relay catalysis provides a potential way to treat wastewater with high concentration nitrate., (© 2024 Wiley-VCH GmbH.)

The development of high-performance, low-cost non-precious-metal electrocatalysts as alternatives to Pt-based catalysts for the oxygen reduction reaction (ORR) is crucial for promoting the commercial application of fuel cells and metal-air batteries. In this work, we report a novel type of ORR electrocatalyst with Fe and Co sites anchored on N,P-codoped hierarchically ordered macro-/mesoporous carbon (FeCo/NP-HOMMC) through a facile one-pot controllable synthesis method with the aid of dual-templating technology. The FeCo/NP-HOMMC catalyst shows robust ORR performance under alkaline conditions with a half-wave potential (E1/2) of 0.90 V vs. reversible hydrogen electrode (RHE), significantly surpassing the commercial 20 wt% Pt/C catalysts, while also exhibiting remarkable long-term stability and great methanol tolerance. Control experiments reveal that the superior performance of the FeCo/NP-HOMMC catalyst for ORR benefits from the synergistic catalysis of highly dispersed Fe and Co dual active sites, and the advantages of the unique hierarchically ordered macro-/mesoporous structure, which can provide improved accessibility active site, excellent conductivity, and maximized mass/charge transport., (© 2025 Wiley‐VCH GmbH.)

Blade coating is a promising tool for upscaling organic solar cells (OSCs). However, the performances of blade-coated OSCs still lag behind their spin-coated counterparts, limiting their competitive edge towards commercialization. One of the main reasons is that controlling the film aggregation kinetics and morphology becomes challenging during the transition from spin coating to blade coating, especially when using high boiling point solvents, which can result in excessive aggregation. Therefore, a deeper understanding and appraisal of film formation kinetics influenced by coating methods is crucial. In this work, it is demonstrated that ink solubility tuning by incorporating a twisted third component (BTP-4Cl) can induce rapid crystallization behavior and promote fine phase separation between the donor polymer (PM6) and the acceptor (BTP-eC9) in blade coating. As a result, a high power conversion efficiency (PCE) of 19.67% is obtained in OSCs (0.04 cm 2 ), one of the state-of-the-art efficiencies among the reported blade-coated OSCs (19.76% for the spin-coated devices). In addition, it is found that the inhibited phase aggregation contributes to enhancing the light stability of the device. This strategy offered novel insights into the effectiveness of solubility-tuning approaches for achieving highly efficient and stable OSCs under open-air coating conditions., (© 2025 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

Understanding and steering the stability of earth-abundant electrocatalysts in acidic medium is essential for proton exchange membrane (PEM) water electrolyzer. Manganese oxide (MnO 2 ) is one of the promising candidates for acidic oxygen evolution reaction (OER), but it still suffers from the overoxidation and the underlying mechanism remains elusive. Here, we observed that lattice oxygen was involved in the OER process on γ-MnO 2 via Mars-van-Krevelen mechanism. Combined with theoretical calculation, we revealed that the release of lattice oxygen lowers the energy barrier of Mn dissolution and compromises the electrode durability. Based on this finding, we propose a strategy to efficiently stabilize lattice oxygen and suppress Mn overoxidation by replacing OER with glucose oxidation to formic acid, which follows a Langmuir-Hinshelwood mechanism. As a result, the durability of γ-MnO 2 was enhanced by 1100 times, enabling long stability up to 960 hours. Moreover, we demonstrated a production rate of 487.1 mmol h -1 for formic acid and 16.7 L h -1 for H 2 at 40 A in a PEM electrolyzer, providing a sustainable and scalable route for converting water and biomass into valuable chemicals and fuels., (© 2025 Wiley-VCH GmbH.)

Lithium-sulfur (Li-S) batteries featuring high energy density are expected to be next-generation energy storage devices, but are severely impeded by the suppressive Li + -solvents desolvation process at the electrode/electrolyte interface. Herein, a novel electrochemical in situ doping coupled with a self-assembly strategy is proposed to fabricate the graphene membrane anchored by Ni single atoms (Ni-SA-G), aimed at promoting the dissociation kinetics of Li + -solvents complex by combining electrocatalysis and nanochannel sieving effect. Theoretical simulation and in situ Raman spectroscopy characterizations revealed that the Ni-O 5 configuration within the Ni-SA-G membrane is capable of lowering the Li + -solvent dissociation energy barrier and promoting free Li + migration, thereby delivering the fast sulfur redox kinetics. In addition, taking advantage of the Ni-SA-G membrane with a special transport channel, the large-sized solvent molecules and polysulfides were sieved and confined to a great degree. As a result, the Li-S batteries with the Ni-SA-G on separator as cathode front-faces exhibit a high capacity of 1169 mAh g -1 with a good rate performance and outstanding long-term cycling stability, where a capacity decay of only 0.024 % per cycle after 700 cycles can be achieved. Furthermore, the cell with a sulfur loading of 4.78 mg cm -2 delivers a high areal capacity of 4.0 mAh cm -2 at 0.2 C., (© 2025 Wiley-VCH GmbH.)

Nano-catalysts demonstrate exceptional performance in heterogeneous reactions, yet their potential is often underutilized due to a lack of attention to engineering design. In this study, an innovative encapsulated structure is presented for nano-catalysts and a corresponding catalytic system. Using an oil-in-water droplet strategy, millimeter-sized hollow spherical alumina (Al 2 O 3 -HS) is fabricated with an average diameter of ≈3 mm and a hollow void size of ≈1 mm. This approach enables the one-step encapsulation of nanoscale Pd/Al 2 O 3 within the Al 2 O 3 -HS. The resulting assembly is immobilized within a tubular reactor for the hydrogenation of 2-ethylanthraquinone, with hydrogen introduced from the bottom of the reactor. Remarkably, the encapsulated catalyst achieved twice the H 2 O 2 productivity of conventional supported catalysts. This enhancement is attributed to the cavity-constrained fluidization behavior of Pd/Al 2 O 3 within the hollow alumina spheres. The design introduces a novel catalytic system that combines shell-immobilization with the fluidization of encapsulated nano-catalysts. As the gas velocity exceeds the minimum fluidization velocity, the Pd/Al 2 O 3 particles remain highly accessible while allowing efficient gas and product flow. This hybrid approach integrates the advantages of fixed-bed and fluidized-bed systems, offering a promising solution to the technical challenges limiting the industrial application of nano-catalysts., (© 2025 Wiley‐VCH GmbH.)

Dynamic wound care presents significant challenges for conventional dressings due to the complex environment and high-frequency motion associated with such injuries. In this study, a multifunctional photo-crosslinked piezoelectric hydrogel (OAPS) is developed, incorporating heterojunction Se-doped KH570 modified BaTiO 3 nanoparticles (Se-BT570 NPs) as a core component, and designed to address antimicrobial and monitoring needs in wound care, particularly at sites with high-frequency movement. The OAPS hydrogel effectively utilizes the inherent high-frequency motion in dynamic wounds, enhancing antimicrobial efficacy and enabling real-time monitoring of wound and human health statuses. This is achieved through the synergistic effects of piezoelectric properties and nano-heterostructures that enable self-driven charge transfer. Such integration allows for dual applications in both diagnosis and treatment. Experimental results demonstrated that the OAPS hydrogel exhibits excellent mechanical strength and adhesive properties, effectively adapting to high-frequency motion. Additionally, the hydrogel can be activated by dynamic wound environments to perform antimicrobial and wound monitoring functions, significantly accelerating the healing of dynamic wounds, with an efficacy rate of 99.75%. This study highlights the potential of piezoelectric nanomaterials in dynamic wound healing, offering a promising strategy for managing complex, dynamic wound care., (© 2025 Wiley‐VCH GmbH.)

In order to make available new derivatives, diethyl α-amino-α-aryl-methylphosphonates were subjected to phosphorylation, phosphinoylation and even thiophosphinoylation by reaction with phosphoryl chlorides, diphenylphosphinoyl chloride, and with the mixture of diphenylchlorophosphine and elemental sulfur, respectively. The X-ray crystal structures of the diphenylphosphinoyl and the diphenylthiophosphinoyl derivatives revealed molecular and supramolecular similarities, as well as a few differences too. An essential conformation change, along with packing differences are attributable to a change of one heteroatom: an oxygen for a sulfur in one of the P=X function. The diethyl diethylphosphoryl-aminobenzylphosphonates showed the highest antiproliferative effects on multiple myeloma cells, while the thiophosphinoylated diethyl aminobenzylphosphonate was the most effective on pancreatic ductal adenocarcinoma cells., (© 2025 The Author(s). Chemistry - A European Journal published by Wiley-VCH GmbH.)

The treatment of pnictinidenes [2-(RNHCH2)-6-(RN=CH)C6H3]E (1As/Sb) (where E = As or Sb) with benzoyl peroxide provided compounds [2-(DippNCH2)-6-(DippN=CH)C6H3]E(O2CPh) (2As/Sb) as a result of two step procedure, i.e. oxidation of the pnictogen centre followed by the elimination of benzoic acid. The reaction between 1As and diphenyl disulfide proceeded in the same vein yielding thiophenol and [2-(DippNCH2)-6-(DippN=CH)C6H3]As(SPh) (3As). Analogous reaction of 1Sb furnished a mixture of [2-(DippNHCH2)-6-(DippN=CH)C6H3]Sb(SPh)2 (3´Sb), [2-(DippNCH2)-6-(DippN=CH)C6H3]Sb(SPh) (3Sb) and PhSH, while NMR studies proved the existence of a dynamic equilibrium between all three compounds in solution and removal of incipient PhSH was necessary for the isolation of 3Sb. Both 1As/Sb smoothly reacted with 2-nitrosotoluene leading to [2-(DippNCH2)-6-(DippN=CH)C6H3]E(O-NH-2-Me-Ph) 4As/Sb and with 4-phenyl-1,2,4-triazoline-3,5-dione giving [2-(DippNCH2)-6-(DippN=CH)C6H3]E[(N(CO)-NH(CO))N-Ph] 5As/Sb. All compounds were characterized by IR, Raman, NMR spectroscopy, and the molecular structures, except for 3As and 5Sb, were determined by single-crystal X-ray diffraction. Furthermore, we scrutinized the thermally induced reductive elimination of benzoic acid and thiophenol from 2-3As/Sb, respectively, and that of 4-phenylurazole from 5As. These eliminations involve C-H activation at the CH2N group, and the recovery of the pnictinidene center in [2,6-(RN=CH)2C6H3]E (6As/Sb). Using DFT calculations a plausible mechanism was suggested for all investigated reactions, which are in good agreement with the experimental observations., (© 2025 Wiley‐VCH GmbH.)

Tandem catalysis stands as a beacon of chemical sustainability. Although bifunctional catalysts have achieved wide success in two-step tandem reactions, achieving multi-step catalysis with three or more distinct and potentially incompatible catalytic sites and components remains an ambitious challenge. Here, we present a "tandem switch" strategy that transforms these incompatibilities into functional advantages, enabling on-demand production of primary, secondary, and tertiary aromatic amines, all with yields exceeding 96 %. A kinetic switch, enabled by phosphotungstic acid functionalization of the Ni-Ni(Al)O heterojunction catalyst, modulates the Ni-Ni and Ni-O boundary microenvironment to simultaneously accelerate the rate-determining steps in nitrobenzene hydrogenation, N-alkylation, and aza-Michael addition. Meanwhile, a thermodynamic switch, controlled by the competitive adsorption of ethanol, hydrogen, and acrylonitrile, stepwise minimizes Gibbs free energy to ensure a seamless reaction cascade. Hence, by toggling these tandem switches on or off, we achieve selective regulation of nitrobenzene conversion pathways into the production of targeted aromatic amine. Techno-economic analysis shows the developed process significantly reduces material and energy consumption for sustainable amine production., (© 2025 Wiley-VCH GmbH.)

Eutectogels with inherent ionic conductivity, mechanical flexibility, environment resistance, and cost-effectiveness have garnered considerable attention for the development of wearable devices. However, existing eutectogels rarely achieve a balance between strength, strain, and resilience, which are critical indicators of reliability in flexible electronics. Herein, poly(sodium styrenesulfonate) (PSS)-modified gold nanoparticles (AuNPs) in eutectic solvents are synthesized, and PSS-AuNP reinforced polyacrylic acid/polyvinylpyrrolidone (SAu-PAA/PVP) eutectogel is successfully prepared. Through the coordination between AuNPs and the PAA/PVP polymer chains, the SAu-PAA/PVP eutectogel exhibits significantly enhanced tensile strain (946%), mechanical strength (3.50 MPa), and resilience (85.3%). The high-performance eutectogel was demonstrated as a flexible sensor sensitive to strain and temperature, and the AuNPs provided near-infrared sensing capabilities. Furthermore, SAu-PAA/PVP eutectogel inherits the benefits of ES, including anti-drying and anti-freezing properties (-77 °C). Moreover, the eutectogel is microstructured using a simple molding method, and the resulting hierarchical pyramid microstructured eutectogel functions as ionic dielectric layer in a pressure sensor. This sensor exhibits high sensitivity (37.11 kPa -1 ), low detection limit (1 Pa), a fast response rate (36/54 ms), and excellent reproducibility over 5000 cycles, making them reliable and durable for detecting small vibrations, with potential applications in precision machinery, aerospace, and buildings., (© 2025 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

The electrocatalytic valorization of lignin provides a sustainable route to valuable chemicals under mild conditions, yet achieving high efficiency and selectivity remains challenging. Here, we develop gas diffusion electrodes (GDEs) modified with few-layer graphene (GR) and multi-walled carbon nanotubes (MWCNT) to enhance the oxygen reduction reaction (ORR) for efficient hydrogen peroxide (H 2 O 2 ) generation. The MWCNT-modified GDE exhibits the highest surface area and conductivity, achieving over 80 % selectivity for H 2 O 2 via the two-electron ORR pathway. Electrochemical lignin depolymerization using this optimized GDE yields 72.3 % low-molecular-weight aromatic compounds within 1 h. The MWCNT-GDE demonstrates exceptional durability, maintaining stable performance across ten consecutive cycles. This work highlights the potential of MWCNT-modified electrodes to advance scalable electrochemical lignin valorization through in-situ H 2 O 2 generation., (© 2025 Wiley-VCH GmbH.)

The novel chemically stable hybrid co-networks (PTA-Fe) of poly(thioctic acid) coordinated with molar content (C Fe ) of 1%∼12% Fe 3+ generated from [FeCl 4 ·POH] - can be in situ synthesized via controlled/living cationic ring-opening polymerization of α-thioctic acid (TA) with tert-butyl chloride(BCl)/FeCl 3 /isopropanol(POH) initiating system at 0 °C. The polymerizations are all in first order with respect to monomer, initiator and co-initiator. The resulting PTAs with desired molecular weights and relatively narrow unimodal molecular weight distribution can be obtained via quantitative initiation by changing [BCl] 0 . The livingness of polymerization without chain transfer and termination is confirmed from the linear relationship between molecular weights of the resulting PTAs and polymer yields and the unchanged average polymer chains during polymerization process by Incremental Monomer Addition and All Monomer In techniques. The possible mechanism of the above polymerization is proposed. Interestingly, it is found that the PTA-Fe hybrids can behave chemically stable during storage at room temperature for 24 months when C Fe ≥ 6.9%. To the best of the knowledge, it is the first example of in situ green synthesis of PTA-Fe hybrid co-networks with excellent chemical stability. The PTA-Fe hybrids would have potential application in the field of elastomer, adhesive and self-healing materials., (© 2025 Wiley‐VCH GmbH.)

Photoresponsive ion nanochannels have gained significant attention for their ability to regulate ionic transport in response to external stimuli. The potential of molecular and polymeric architectures in the nanochannels to further enhance and modulate these behaviors, however, remains underexplored. In this work, we explore the integration of spiropyran-based polymers into anodic aluminum oxide (AAO) nanochannels, resulting in tailored photoresponsive behaviors. Spiropyran undergoes reversible ring-opening isomerization upon UV irradiation, which leads to changes in the packing and polarity of polymer chains within the nanochannels. The polySp-coated and polySp-grafted AAO systems, fabricated via solution wetting and surface-initiated atom transfer radical polymerization (SI-ATRP), exhibit unique macroscopic and microscopic responses, including reversible color changes, wettability adjustments, and modulation of ion transport under UV and visible light. These findings demonstrate the potential of spiropyran-functionalized nanochannels for applications in optical information storage, photogated materials, and sensors. By manipulating molecular architecture and nanoconfinement, this work paves the way for the design of next-generation photoswitchable systems with enhanced multifunctionality., (© 2025 Wiley‐VCH GmbH.)

Peptide multifunctionalization is a crucial technique to develop peptide-based agents for various purposes. Porphyrin-peptide conjugates are a class of popular multifunctional peptides renowned for their multifunctional and multimodal properties. However, the tedious synthetic works for porphyrin building blocks are involved in most previous studies. In this work, a modular solid-phase synthetic approach is reported to construct trans-AB 2 C porphyrin on peptide chains without presynthesized porphyrin building blocks. The products from this approach, which inherit both functionalities from the porphyrins and the modules employed for constructing porphyrins, show potential in biomedical and biomaterial applications. Furthermore, by extending this synthetic approach, the first example of "resin-to-resin" reaction is reported to link two peptides together along the construction of porphyrin motifs to give porphyrin-peptide conjugates with two different peptide chains., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

Epstein-Barr virus (EBV) is a well-recognized oncogenic virus that promotes several lymphoid and epithelial cancers. The Epstein-Barr nuclear antigen 1 (EBNA1), which is known to be expressed in all EBV-positive cancers, plays a vital role in viral genome replication and maintenance and is therefore emerged as an attractive target for clinical intervention. Several EBNA1 inhibitors have shown potency in the growth inhibition of EBV-positive cancers, yet low bioavailability and in vivo unmonitored nature hamper their further implementation. Here a novel EBNA1 nano-inhibitor based on EBNA1-specific peptide inhibitor (P4) functionalized ZnGa 2 O 4 :Cr 3+ ultra-small near-infrared persistent luminescent (NIR-PL) nanoparticles (ZGOC-P4) is developed. Owing to the specific binding to EBNA1, ZGOC-P4 nano-inhibitor can quickly achieve nuclear internalization in EBV-positive nasopharyngeal carcinoma (NPC) cells (C666-1) and selectively inhibit their growth. In sharp contrast, ZGOC-P4 nano-inhibitor shows no inhibition effect on EBV-negative NPC cells (HK-1). Moreover, the results indicate that the well-designed nano-inhibitor enables efficient tumor-targeting accumulation in NPC xenograft model under the monitoring of autofluorescence interference-free NIR-PL imaging in vivo and suppresses EBV-associated tumor growth with an inhibition rate of 61.6%. This work highlights the potency of ZGOC-P4 on NPC treatment and may provide new sight into future research on EBV-associated diseases., (© 2025 Wiley‐VCH GmbH.)

Seawater electrolysis holds great promise for sustainable, green hydrogen production but faces challenges of high overpotentials and competing chlorine evolution reaction (CER). Replacing the oxygen evolution reaction with the methanol oxidation reaction (MOR) presents a compelling alternative due to its lower anodic potential which mitigates the risk of CER. While NiOOH is known for its MOR activity, its performance is limited by sluggish non-electrochemical kinetics and Cl-induced degradation. Herein, a MoO 4 2- -modified NiOOH electrocatalyst is reported that significantly enhances MOR-assisted seawater splitting efficiency. In situ leached MoO 4 2- from the heterojunction optimizes methanol adsorption and facilitates proton migration, thereby accelerating the non-electrochemical steps in MOR. Additionally, the adsorbed MoO 4 2- effectively repels Cl - , protecting the electrodes from Cl - -induced corrosion. The MOR-assisted electrolyzer using NiMo||Ni(OH) 2 /NiMoO₄ requires only 1.312 V to achieve 10 mA cm -2 , substantially lower than conventional alkaline seawater electrolysis (1.576 V). Furthermore, it demonstrates remarkable stability, sustaining high current densities (up to 1.0 A cm -2 ) for over 130 h. This work presents a promising strategy for designing high-performance electrocatalysts for efficient and sustainable green hydrogen production from seawater., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

While the outstanding stability of per- and polyfluoroalkyl substances (PFAS) paved the way for their widespread application in a huge variety of applications, it also resulted in their nickname "forever chemicals". The rising awareness for PFAS-related environmental and health concerns drives a discussion on the most effective ways to abate PFAS emissions into the environment, i.e. water, soil, and air, and remediation of contaminated matter. In order to address the knowledge gap regarding air pollution by PFAS, this minireview summarizes the current corpus of work in the field and outlines how catalysis can contribute to PFAS abatement in the gas phase. Beyond a mere collection of state-of-the-art knowledge, overarching challenges in catalytic PFAS removal are identified, spanning from fundamental organic and inorganic chemistry, i.e. C-F-bond activation, to heterogeneous catalysis, i.e. surface reactions at the gas-solid interface, to reaction engineering, i.e. scaling relations and technical hurdles. In addition, the article introduces concepts and workflows that aim at providing guidance during the design of technological solutions for the efficient control of gaseous PFAS emissions., (© 2025 Wiley‐VCH GmbH.)