Materials Chemistry Frontiers最新文献

{"title":"A food-additive-inspired bifunctional proton buffering-iron capture route to low-defect Prussian blue cathodes for sodium-ion batteries","authors":"Jiayi Zhang, Dongshu Liu, Shibo Meng, Wenxian Liu, Fangfang Wu, Wenhui Shi and Xiehong Cao","doi":"10.1039/D5QM00917K","DOIUrl":"https://doi.org/10.1039/D5QM00917K","url":null,"abstract":"<p >The quest for sustainable and cost-effective energy storage systems has propelled the development of sodium-ion batteries. Iron-based Prussian blue (PB) and its analogues are among the most promising cathode candidates due to their open framework, facile sodium intercalation, and elemental abundance. However, their practical deployment is severely hampered by intrinsic structural imperfections. These defects, primarily in the form of hexacyanoferrate ([Fe(CN)<small>₆</small>]) vacancies and interstitial water molecules, lead to insufficient active sites and poor cycling stability. To mitigate these issues, conventional synthetic strategies often require harsh conditions to slow nucleation. In this study, a novel strategy inspired by food processing additives is developed for effective synthesis of low-defect PB, which employs a bifunctional organophosphate reagent to buffer protons and sequester Fe ions during preparation. This obviates the need for harsh reaction conditions and guarantees a controlled release of H<small>⁺</small> to promote ligand dissociation, leading to retarded nucleation, as well as limited Fe(CN)<small>₆</small> vacancies and interstitial water. The prepared Prussian blue cathode delivers enhanced cycling stability in sodium-ion batteries, retaining 90% of its capacity after 1000 cycles at 5C. This work presents a simple, sustainable, and scalable route to high-performance PB under mild conditions.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 9","pages":" 1428-1436"},"PeriodicalIF":6.4,"publicationDate":"2026-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147808128","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Bi/Bi4O5Br2 Ohmic-like heterojunction drives enhanced photocatalytic antibacterial action via electron transfer and ROS","authors":"Yan Liu, Xiaomeng Liu, Ruixuan Yang, Zhiguo Song, Yongjin Li, Qiyan Li and Jie Pan","doi":"10.1039/D5QM00929D","DOIUrl":"https://doi.org/10.1039/D5QM00929D","url":null,"abstract":"<p >Electron transfer plays a pivotal role in catalytic reactions and physiological processes, with its modulation capable of altering catalytic efficiency and interfering with microbial metabolic pathways to enhance antibacterial outcomes. In this study, we designed a Bi/Bi<small>₄</small>O<small>₅</small>Br<small>₂</small> nanosheet Ohmic-like heterojunction as a photodynamic therapy (PDT)-compatible semiconductor nano-agent. Under visible light irradiation, this heterojunction engineer's electron transfer pathways at both abiotic (material) and abiotic–biotic (material–bacteria) interfaces. The tightly contacted atom-sharing Bi heterostructure within the heterointerface generates an intrinsic electric field, which promotes the transfer of photogenerated electrons from Bi<small>₄</small>O<small>₅</small>Br<small>₂</small> to Bi nanoparticles at the Bi–Bi<small>₄</small>O<small>₅</small>Br<small>₂</small> interface, significantly boosting reactive oxygen species (ROS) production. Notably, the high conductivity of metallic Bi further activates direct electron transfer from the Bi<small>₄</small>O<small>₅</small>Br<small>₂</small> interface to the bacterial surface. This dual electron-transfer mechanism—coupled with ROS generation—induces synergistic damage: ROS downregulate genes associated with ribosome, DNA, and ATP synthesis in <em>Escherichia coli</em>, while electron interference disrupts the bacterial electron transport chain, upregulating genes linked to membrane and ion transport. The resulting photoresponsive dual-interface system demonstrates excellent safety and potent antibacterial efficacy against both <em>Escherichia coli</em> and <em>Staphylococcus aureus</em>. Our findings highlight the critical role of targeted electron transfer (beyond ROS alone) in PDT for combating pathogenic bacterial infections and antibiotic resistance, offering a design strategy for next-generation multifunctional antimicrobial photocatalysts.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 8","pages":" 1265-1277"},"PeriodicalIF":6.4,"publicationDate":"2026-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147720916","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Diazadioxa[8]circulene – a platform for stable antiaromatic radicals with strong NIR absorption","authors":"Cecilia Bruschi, Ihor Sahalianov, Yuri Tanuma, Levani Skhirtladze, Rashid Valiev, Xinyi Cai, Feng Gao, Mikhail Vagin, Yann Lie, Michael Pittelkow, Renee Kroon and Glib Baryshnikov","doi":"10.1039/D6QM00054A","DOIUrl":"https://doi.org/10.1039/D6QM00054A","url":null,"abstract":"<p >Stable organic radicals exhibiting absorption capabilities in the visible and near-infrared regions (NIR) are appealing candidates for a wide range of applications, including photovoltaics, photothermal applications, anticounterfeiting and information encryption/decryption. Hetero[8]circulenes represent a promising π-extended platform for stable delocalized radicals with rich possibilities for chemical tuning. In this paper, we present the stable cation radical of diazadioxa[8]circulene with reduced symmetry showing a sharp and strong peak (<em>ε</em> ∼ 2 × 10<small>⁴</small> M<small>⁻¹</small> cm<small>⁻¹</small>) in the NIR at 939 nm. The diazadioxa[8]circulene cation radical can be obtained <em>via</em> chemical doping using Magic Blue, or <em>via</em> electrochemical doping. It remains stable for several days without any significant change in the absorption spectra. Furthermore, according to magnetic criteria of aromaticity, it exhibits antiaromatic behaviour. Advanced theoretical calculations predict NIR emission for the radical cation through an anti-Kasha D<small>₄</small> → D<small>₀</small> transition, which is experimentally not detectable due to non-radiative deactivation pathways. Our RI-CC2 theoretical calculations also corroborate the blue emission of neutral circulene from the bright lowest singlet excited state S<small>₁</small>, which was previously unexplained due to TD-DFT artefact predicting the dark S<small>₁</small> state. These results open the opportunities for the practical application of diazadioxa[8]circulene cation radicals in photovoltaics, sensors and photothermal imaging.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 9","pages":" 1418-1427"},"PeriodicalIF":6.4,"publicationDate":"2026-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/qm/d6qm00054a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147808175","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Selective ethanol vapour sensing enabled by amine-functionalized MOF–polyetherimide hybrid membranes","authors":"Sasikumar B., Hemanth Kumar K., Gnanasekaran Gnanaselvan, Arthanareeswaran G., Mangalaraja Ramalinga Viswanathan and Karthikumar Sankar","doi":"10.1039/D5QM00828J","DOIUrl":"https://doi.org/10.1039/D5QM00828J","url":null,"abstract":"<p >A hybrid polymeric membrane for ethanol gas sensing was fabricated <em>via</em> a facile solution-casting approach by incorporating MOF-71 and amine-functionalized MOF-71 (NH<small>₂</small>-MOF-71) nanoparticles into a polyetherimide (PEI) matrix. The resulting PEI/MOF-71 and PEI/NH<small>₂</small>-MOF-71 composite membranes were systematically characterised using Fourier transform infrared spectroscopy, thermogravimetric analysis, scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy, and N<small>₂</small> adsorption–desorption isotherms to evaluate chemical interactions, thermal stability, morphology, elemental distribution, and porosity. The incorporation of MOF-71 and NH<small>₂</small>-MOF-71 enhanced membrane porosity, surface area, and gas diffusivity, leading to improved sensing performance. Notably, the PEI/NH<small>₂</small>-MOF-71 membrane exhibited superior sensitivity and selectivity toward ethanol vapour, with detectable responses at concentrations as low as 25 ppm under ambient conditions and a calculated limit of detection of approximately 8–12 ppm. Rapid and reproducible response and recovery times of approximately 300 s and 360 s were achieved at ethanol concentrations of 100–125 ppm. The enhanced sensing performance is attributed to the presence of amine functional groups, which promote stronger ethanol adsorption through hydrogen bonding and dipole–dipole interactions. These results demonstrate that NH<small>₂</small>-MOF-71/PEI composite membranes provide a simple and effective platform for room-temperature, ppm-level ethanol detection with potential applications in industrial safety and environmental monitoring.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 7","pages":" 1096-1106"},"PeriodicalIF":6.4,"publicationDate":"2026-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147558472","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"First-principles modelling of circularly polarized luminescence in one-handed helical ladder polymers","authors":"Giovanni Bella, Marco Milone, Giuseppe Bruno and Antonio Santoro","doi":"10.1039/D5QM00921A","DOIUrl":"https://doi.org/10.1039/D5QM00921A","url":null,"abstract":"<p >The idea of helical chirality bridges the gap between stereogenic asymmetry at the local scale and intrinsic non-superimposability in larger secondary structures (DNA, RNA, α-helix protein, <em>etc.</em>). Novel synthetic breakthroughs allowed the ascent of a brand-new subclass of chiral materials based on defect-free single-handed helical ladder polymers, reducing the conceptual barrier between small artificial helical foldamers and helical biomacromolecules. Beyond their extraordinary physicochemical properties, the interference of circularly polarized radiation with optically pure one-handed helical ladder polymers paved the way for pronounced circularly polarized luminescence events. This work, through a systematic theoretical investigation, tackled the CPL spectral profiles of a multitude of enantiomeric ladder-type polymers with diversified helical arrangements and topological cavities. The computational protocol integrated a preliminary ground state treatment of chiral monomeric units with excited-state molecular dynamics of oligomeric and polymeric systems to understand how key geometrical parameters of ladderization precursors vary upon photoexcitation for chemical architectures of increasing size. The consolidation of APFD and O3LYP functionals performances, through the rigorous assessment of chiroptical descriptors (emission energies, rotational strengths, electric/magnetic transition dipole moments and their angle), allowed us to evaluate how the chiral dimensionality orients the CPL spectra of one-handed helical ladder polymers in terms of peak position, band shape, chiral sign and signal magnitude.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 8","pages":" 1312-1326"},"PeriodicalIF":6.4,"publicationDate":"2026-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/qm/d5qm00921a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147720920","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Indolo[3,2-b]carbazole-based hyper-cross-linked polymers for blue-light-driven selective organic sulfide oxidation in water","authors":"Si-Jia Wang, Zhou-Rui Yan, Zi-Yi Zhao, Jin-Peng Liu, Fan Li, Guoliang Liu and Lin-Bing Sun","doi":"10.1039/D5QM00814J","DOIUrl":"https://doi.org/10.1039/D5QM00814J","url":null,"abstract":"<p >The development of metal-free and water-stable photocatalysts for visible light-induced environmentally friendly organic transformations in water is of great significance in the context of green and sustainable development. In this work, two hyper-cross-linked polymers (HCPs), NUT-19 and NUT-19-Me, were successfully synthesized through the covalent linkage of two cross-linkers containing different groups with indolo[3,2-<em>b</em>]carbazole (ICZ) derivatives. Their pore structures and photochemical properties were characterized. Driven by 420 nm blue light, both exhibited good catalytic activity (NUT-19: 99% conversion in 8 h; NUT-19-Me: 98% conversion in 11 h) and high selectivity (greater than 95% for sulfoxide) for organic sulfide oxidation in water. NUT-19 outperformed NUT-19-Me due to its superior photochemical properties. Extended to other sulfide derivatives, both maintained efficient catalytic activity and selectivity. The photocatalytic performance can be well-maintained over eight cycles in water, indicating good stability. Mechanistic studies revealed that under blue light irradiation, the materials could generate singlet oxygen (<small>¹</small>O<small>₂</small>), which achieved the selective oxidation of sulfides to sulfoxides. This work provides new insights into the development of ICZ-based stable and environmentally friendly photocatalysts and opens up new avenues for their application in green chemical synthesis.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 8","pages":" 1286-1294"},"PeriodicalIF":6.4,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147720918","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"One arrow two eagles: design and synthesis of “all-in-one” nanoscale Cu-IR825 nanoparticles for photothermally augmented chemodynamic therapy","authors":"Wei Wang, Dan Luo, Yuzi Huang, Yuting Zhang, Peng Geng, Qiancheng Jin, Wenquan Huang and Shuzhang Xiao","doi":"10.1039/D5QM00881F","DOIUrl":"https://doi.org/10.1039/D5QM00881F","url":null,"abstract":"<p >The combination of photothermal therapy (PTT) and chemodynamic therapy (CDT) has shown great promise in tumor treatment. However, developing a nanoplatform that integrates efficient photothermal conversion, photothermally enhanced Fenton-like reaction activity, and ideal biodegradability remains a significant challenge. In this study, we successfully synthesized Cu-IR825 nanoparticles using a simple one-step coordination-driven self-assembly strategy, which exhibit effective photothermal-enhanced chemodynamic combined therapy. These nanoparticles are formed by coordinating the near-infrared dye IR825 with Cu<small>²⁺</small><em>via</em> carboxyl groups, with an average size of approximately 100 nm. The nanoparticles exhibit strong light absorption in the near-infrared region, with a photothermal conversion efficiency of 33.4%, and excellent photothermal stability. Additionally, the Cu<small>²⁺</small> component provides significant Fenton-like catalytic activity, and the localized thermal effects generated by PTT further enhance the Fenton-like reaction rate by 1.68 fold, enabling “photothermal-enhanced CDT”. In a tumor-bearing mouse model, intravenous injection of Cu-IR825/PEG nanoparticle dispersion resulted in a tumor inhibition rate of 87.5% in the combined PTT–CDT group. Notably, the coordination-driven self-assembly structure, based on non-covalent coordination bonds, enables Cu-IR825 nanoparticles to degrade efficiently and be rapidly cleared <em>in vivo</em>. Hematological, histological, and biodistribution studies confirmed their excellent biocompatibility and biosafety. This research not only presents an efficient and safe “all-in-one” nano-platform for theranostics, but also provides a novel approach for developing biodegradable coordination-driven self-assembled nano-drugs for synergistic cancer therapy.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 7","pages":" 1133-1146"},"PeriodicalIF":6.4,"publicationDate":"2026-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147558475","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Post-polymerization modification and release of functional groups based on an NIR light-emitting organoboron π-conjugated polymer","authors":"Masashi Nakamura, Masayuki Gon and Kazuo Tanaka","doi":"10.1039/D5QM00730E","DOIUrl":"https://doi.org/10.1039/D5QM00730E","url":null,"abstract":"<p >We developed a near-infrared (NIR) light-emitting organoboron π-conjugated polymer that can be functionalized through post-polymerization modification with click chemistry. The perpendicularly protruding substituents at the boron center are reactive and almost electronically independent from the polymer main chain. These properties allow the quantitative chemical modification of functional groups as side-chains even after polymerization, without any influence on the main-chain properties. In particular, to the best of our knowledge, we first demonstrate that the boron-fused azobenzene complex can release the introduced functional units at the boron center upon treatment with reactive agents, such as nucleophilic bases and photo-radical initiators. We observed that the release of pyrene side-chains can be monitored by the disappearance and appearance of the NIR and blue emissions, respectively, even for water-dispersible polymer nanoparticles. This study provides a novel design strategy for stimuli-responsive theranostic systems based on NIR-fluorescent π-conjugated polymers.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 8","pages":" 1278-1285"},"PeriodicalIF":6.4,"publicationDate":"2026-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/qm/d5qm00730e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147720917","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Vacuum-responsive and water-soluble lanthanide(iii)/2-oxonicotinate coordination polymers with high photoluminescence efficiency","authors":"Maialen Terceño-Carrillo, Laura Razquin-Bobillo, Sergio Carrasco, Patricia Horcajada, Garikoitz Beobide, Jose Angel García, Pablo Salcedo-Abraira, Andoni Zabala-Lekuona, Antonio Rodríguez-Diéguez and Javier Cepeda","doi":"10.1039/D6QM00036C","DOIUrl":"https://doi.org/10.1039/D6QM00036C","url":null,"abstract":"<p >In this work, we report on the structural and physicochemical characterization and an in-depth photophysical study of a family of isostructural coordination polymers (CPs) with the general formula {[M<small>₂</small>(μ<small>₃</small>-2onic)<small>₄</small>(H<small>₂</small>O)<small>₄</small>](ClO<small>₄</small>)<small>₂</small>·2H<small>₂</small>O}<small>_<em>n</em></small> (where M(<small>III</small>) = Y (<strong>1<small>_Y</small></strong>), Nd (<strong>2<small>_Nd</small></strong>), Eu (<strong>3<small>_Eu</small></strong>), Gd (<strong>4<small>_Gd</small></strong>), Tb (<strong>5<small>_Tb</small></strong>), Dy (<strong>6<small>_Dy</small></strong>), Er (<strong>7<small>_Er</small></strong>) and Yb (<strong>8<small>_Yb</small></strong>) and 2onic = 2-oxonicotinate). They consist of a cationic 2D layered structure in which two eight-coordinated rare-earth centres are interconnected by means of 2onic ligands, which demonstrates great flexibility with respect to changes in temperature and pressure (vacuum) derived from partial dehydration implying both lattice and coordination water molecules, which in turn promotes the rearrangement of the hydrogen-bonded network. Similar structural breathing effects are observed under variable gas-pressurization conditions, leading to some metastable phases while vacuum conditions are maintained. Periodic density functional theory (PDFT) calculations performed on <strong>1<small>_Y</small></strong> with variable amounts of water successfully reproduced the structural evolution during dehydration. The fact that the vacuum-/pressure-induced effect is fully reversible in addition to the significantly improved photoluminescence (PL) shown by the vacuum-/pressure-activated compounds shifts the attention towards these compounds as potential pressure and humidity sensors. <strong>2<small>_Nd</small></strong> and <strong>8<small>_Yb</small></strong>, in addition to acting as emitters in the visible range, behave as near-infrared (NIR) emitters, with the former displaying characteristic emission even at room temperature. A thorough analysis of the excitations and energy-transfers by means of semi-empirical methods and multi-configurational calculations on suitable fragment models, and further confirmation by density of states (DOS) theory on the PDFT-optimized structure, allows elucidating the PL mechanism operating in the variable emission in the solid state. The water solubility of the compounds allows the study of the PL properties of the complexes, which surprisingly present quantum efficiencies exceeding those of the solid state especially in the solution of <strong>5<small>_Tb</small></strong> (with the quantum yield (QY) increased from 1.6 to 21.5%).</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 8","pages":" 1295-1311"},"PeriodicalIF":6.4,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/qm/d6qm00036c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147720919","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Fully recyclable and regeneratable plant-based adhesives","authors":"Qiuyu Wang, Mengnan Lai, Yao Zhou, Shiyang Shi, Pengyu Chen, Shuning Li, Qiqi Huang, Dingling Zhong, Yaokang Zhang and Xuechang Zhou","doi":"10.1039/D5QM00937E","DOIUrl":"https://doi.org/10.1039/D5QM00937E","url":null,"abstract":"<p >Recyclable adhesives promise lower cost and environmental impact, but combining full reversibility, high strength, and facile regeneration using only benign, natural components is still difficult. Building on highly tunable and dynamic supramolecular interactions, we present a fully recyclable and regenerable plant-based supramolecular adhesive (RRPA) composed of tannic acid (TA), β-cyclodextrin (β-CD), and water. Extensive hydrogen bonding among TA and β-CD, with water acting as a dynamic bridging component, forms a reversible network that enables strong cohesion and interfacial adhesion while preserving the water-triggered debonding feature. Spectroscopic and spectrometric analyses, including FT-IR, variable-temperature <small>¹</small>H-NMR, and 2D-NOESY, evidence temperature-sensitive, reversible hydrogen bonds. Guided by molecular simulation and DFT-level thermodynamic analysis, we identify an optimal β-CD : TA molar ratio of 1 : 3 and a residual water content of 15 wt%, which together balance cohesive strength and interfacial hydrogen bonding. The optimized RRPA achieves lap-shear strengths exceeding 3.1 MPa on alumina and &gt;2.7 MPa on stainless steel, with strong adhesion to hydrophilic substrates (<em>e.g.</em>, wood, glass) and lower strength on hydrophobic polymers (PET, PI, PTFE). The adhesive is fully water-dissolvable, enabling closed-loop recycling by simple dissolution and redrying; after 100 cycles, it retains ∼70–80% of its initial adhesion strength (∼1.7 MPa), with thermal stability up to ∼250 °C prior to TA decomposition. The water-triggered debonding of the RRPA enables temporary bonding under dry conditions and complete recycling in water, making it attractive for reversible assembly, recyclable composites, and conservation of sensitive artifacts.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 8","pages":" 1256-1264"},"PeriodicalIF":6.4,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147720915","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}