Journal of Materials Chemistry A最新文献

{"title":"Electrooxidation of Ammonia to Nitrate on Magnetite via Slow Dehydrogenation and Nitric Oxide Formation","authors":"Hirak Kumar Basak,Pandiyan Sivasakthi,Deepak Kumar Sahu,Asit Dutta,Pralok K. Samanta,Biswarup Chakraborty","doi":"10.1039/d6ta06280f","DOIUrl":"https://doi.org/10.1039/d6ta06280f","url":null,"abstract":"Electrocatalytic ammonia oxidation reaction (AOR) to nitrogen oxyanion products, [NO2]-, and/or [NO3]- is, although a sustainable alternative to the Ostwald process, scrambling of NOx products is often observed due to sluggish reaction kinetics of the multistep proton-coupled-electron-transfer pathway. Herein, oxygen vacancy-rich cubic-phase ~37 (±10) nm Fe3O4 particles are prepared, and their surface and bulk characteristics are analyzed through various microscopic and spectroscopic techniques. The anode made of Fe3O4 on carbon paper (CP) delivers a limiting current near 1.1 V (vs Hg/HgO) at low NH3 concentration in 0.5 M Na2SO4 while showing a catalytic current at high NH3 concentration, exhibiting AOR and a linear dependence of ja on NH3. AOR in different chronoamperometric (CA) conditions reveals 1.0 V (vs Hg/HgO) as an optimum potential to obtain [NO3]- selectively, while at higher potentials various parallel AOR products, including O2 from the oxygen evolution reaction (OER), are formed. Rotating ring-disk electrode (RRDE) reveals 2.0 (± 0.5) electron transfer with an apparent rate constant (kapp) of 2.1 (±1.3) × 10−3 cm s−1, indicating the first two-electron oxidation of ammonia as a kinetically controlled step, while the variable-temperature AOR studies provide an activation energy of 46- 65 kJ mol-1. The D-labelling study depicts almost 10-fold suppression of the AOR rate, giving a kinetic isotope effect (KIE) value of 7.4, inferring the cumulative contribution of multiple oxidative dehydrogenation steps as the rate-limiting. In situ infrared (IR) and 1H nuclear magnetic resonance (NMR) trapping of AOR intermediates confirm [NO] as one of the key intermediates. In silico study of AOR on the (001) surface of oxygen vacancy-rich Fe3O4 surface further validates that the dehydrogenation of *NH to *N and “N-O” bond formation have the highest energy barrier at anodic potentials, leading to a *[NO] intermediate formation as an energetically favourable process. A relatively less energy This study thereby demonstrates Fe3O4 as a robust catalyst for selective oxidation of NH3 to [NO3]- and provides a comprehensive mechanistic understanding of the AOR pathway.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"33 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218254","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":"Processing-enabled functional differentiation in spray-pyrolysed bilayer air electrodes for durable solid oxide cells","authors":"Víctor Zapata-Ramírez,Glenn C. Mather,Domingo Pérez-Coll","doi":"10.1039/d6ta06384e","DOIUrl":"https://doi.org/10.1039/d6ta06384e","url":null,"abstract":"Bilayer air electrodes offer a route to overcome the activity–stability trade-off that limits intermediate-temperature solid oxide cells, but their performance depends critically on how the individual layers are processed and integrated. Here, spray pyrolysis was used to fabricate compositionally differentiated air electrodes comprising an interfacial SrFe0.9Mo0.1O3−δ layer and an outer SrCo0.95Mo0.05O3−δ layer on Ce0.9Gd0.1O2−δ electrolyte. The resulting porous, well-adhered bilayer exhibited an area-specific polarisation resistance of 0.06 Ω cm2 at 700 °C, lower than either single-layer electrode. Impedance analysis supports complementary functional roles, with the SrCo0.95Mo0.05O3−δ-rich outer layer governing the more active oxygen-reduction response and the SrFe0.9Mo0.1O3−δ interlayer stabilising the electrode–electrolyte interface. The bilayer retained its performance during 100 h of ageing and ten thermal cycles more effectively than single-layer SCM. Importantly, spray pyrolysis reduced the polarisation resistance by more than 50% relative to an analogous slurry-coated bilayer, demonstrating that electrode architecture and fabrication route act cooperatively rather than independently. A Ni–Ce0.9Gd0.1O2−δ-supported cell delivered maximum power densities of 0.48, 0.66 and 0.94 W cm−2 at 650, 700 and 750 °C, respectively, including an approximately 78% improvement over a comparable SrFe0.9Mo0.1O3−δ cell at 650 °C. These results establish processing-enabled functional differentiation as an effective strategy for combining fast oxygen reduction with enhanced interfacial stability in cobalt-lean, rare-earth-free perovskite air electrodes.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"73 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218211","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":"Rethinking cathode porous transport layer degradation in PEM water electrolysis: a mechanism and a carbon-coating solution","authors":"Chen Ju,Congcong Yao,Huimin Sun,Runhao Zhang,Yixuan Ma,Chang Liu,Yang Liu,Ke Zhang,Tianrang Yang,Aidong Tan,Jianguo Liu","doi":"10.1039/d6ta07215a","DOIUrl":"https://doi.org/10.1039/d6ta07215a","url":null,"abstract":"Proton exchange membrane water electrolysis (PEMWE) is a cornerstone technology for green H2, where the Ti porous transport layer (Ti-PTL) is indispensable for sustaining mechanical integrity in high-pressure stacks. Yet, cathode Ti-PTL degradation remains contentiously attributed to hydrogen embrittlement, a hypothesis inherited from bulk-metal corrosion literature but rarely substantiated at realistic cathodic potentials. By decoupling anode and cathode contributions through an asymmetric Pt-coated-anode/uncoated-cathode configuration, we demonstrate that cathode degradation in PEMWE is governed not by hydride formation but by a previously overlooked “oxidative cathode” paradox, in which the Ti surface undergoes net anodic oxidation even under H2-evolving polarization. Quasi-in situ XPS and in situ Raman spectroscopy resolve the surface evolution at operating cathodic potentials (−0.1 V vs. RHE), identifying sub-stoichiometric, hydroxylated TiOx species that are thermodynamically unstable in the acidic cathodic environment, while ruling out Ti0 and TiHx. The latter species emerge only at potentials (≤−1.0 V) far beyond practical PEMWE cathodes, indicating that hydrogen embrittlement is not the operative mechanism. This unstable oxide thickens, increasing interfacial contact resistance, and dissolves, releasing Ti ions that poison Pt active sites in the cathode catalyst layer. Guided by this mechanism, a magnetron-sputtered carbon coating suppresses both degradation pathways, reducing the electrolyzer degradation rate from 31.9 to 1.9 µV h−1 over 1040 h at 2.0 A cm−2 and enabling operation of a differential-pressure stack at 3.0 MPa. This work redefines the dominant degradation pathway of cathode Ti-PTLs and establishes a mechanistically guided, PGM-free, and cost-effective PTL coating strategy for high-pressure PEMWE stacks.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"409 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218212","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":"Defect-Free Low-Fluorine MXenes (Nb2CTx/V2CTx) via Time-Optimized HF Etching: Achieving Superior Conductivity and Ultrahigh Capacitance for Supercapacitors","authors":"Bin Deng,Mingyue Gao,Donglong Bai,Ao Huang,Yun Zhao,Chuyi Xie,Jianguang Xu,Chi Chen,W Yao","doi":"10.1039/d6ta05373d","DOIUrl":"https://doi.org/10.1039/d6ta05373d","url":null,"abstract":"MXenes hold exceptional promise for supercapacitors owing to their high conductivity and 2D layered structure. However, the unavoidable fluorine terminations and structural defects in MXenes synthesized via conventional hydrofluoric acid (HF) etching critically undermine their theoretical energy storage potential. Here, we propose a time-optimized HF etching strategy to synthesize defect-free, low-fluorine MXenes (Nb2CTx and V2CTx) by precisely regulating the interaction dynamics between HF and large-particle MAX precursors. Mechanistic studies reveal that prolonged etching time significantly increases the content of -F functional groups while simultaneously exacerbating the cleavage of Nb-C bonds, whereas controlled termination of the etching process suppresses these effects while ensuring complete Al removal. This approach not only achieves a 60% yield of few-layer MXenes but also eliminates structural damage, resulting in record-breaking electrical conductivity of 5530 S m-1 for Nb2CTx and ultrahigh volumetric capacitance of 1989.57 F cm-3 at 2 mV s-1. The synergy between minimized -F content and intact 2D morphology enables efficient ion diffusion and charge transfer, as evidenced by stable cycling performance, showing 79.55% capacitance retention after 15,000 cycles. Our work establishes a universal paradigm for tailoring MXene surface chemistry and microstructure, paving the way for high-performance energy storage devices.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"16 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218252","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":"Understanding the selective synthesis of siliceous zeolite encaged metal particles","authors":"Zixuan Han,Samuel J. Page,Simon Kenneth Beaumont","doi":"10.1039/d6ta06266k","DOIUrl":"https://doi.org/10.1039/d6ta06266k","url":null,"abstract":"Encapsulating metals within silica \"nanoboxes\" offers unique opportunities for controlling catalytic reactions through nanoscale diffusion effects. Here, we systematically investigated the synthesis parameters governing the formation of metalencaged hollow silicalite-1, examining the influence of hydrothermal treatment time, synthesis conditions, additives, metal precursor identity, and turbulence. Statistical analysis of hollow structure-types from large-scale TEM datasets enabled robust quantification of structural distributions, revealing selectivities (often overlooked in the literature but critical for catalytic application). Optimisation of synthesis conditions enabled the preparation of both multihollow (MH) \"sponge-like\" structures and single-hollow (SH) nanoboxes with selectivities of up to 84% and 72%, respectively. Nitrogen physisorption and solid-state NMR provided complementary signatures of these different hollow architectures: SH-rich samples exhibited a characteristic low-pressure hysteresis loop and lower Q³/Q⁴ ratios, the latter consistent with reduced framework defect concentrations, whereas \"sponge-like\" MH-rich samples displayed pronounced mesoporosity centred at 5-6 nm. Finally, vapour-phase furfural hydrogenation was used as a test reaction to demonstrate that hollow-structure morphology influences catalytic selectivity, highlighting the role of architecture-dependent diffusion effects and providing a foundation for the rational use of encaged metal particles in catalysis.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"159 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218207","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":"Sacrificial Cr doping enables rapid reconstruction of NiFe-LDH for high-current oxygen evolution","authors":"Jingchun Zhang,Yue Wang,Yumiao Zhang,Shuai Zeng,Xin Lu,Haijin Li,Lingxia Zheng,Qi Wu","doi":"10.1039/d6ta07893a","DOIUrl":"https://doi.org/10.1039/d6ta07893a","url":null,"abstract":"NiFe-layered double hydroxides (LDHs) are promising OER catalysts, yet their activity is limited by sluggish reconstruction to the active oxyhydroxide phase. Here, we report a rapid, one-step strategy that combines Cr doping with in situ anodic leaching under high-current polarization to activate NiFe-LDH for oxygen evolution. The Cr incorporation not only lowers the energy barrier for reconstruction, promoting rapid conversion to NiFeOOH, but also releases soluble CrO42− species that remain trapped near the electrode interface. These interfacial anions, together with oxygen vacancies, modulate the electronic structure of the reconstructed NiFeOOH and upshift the Fe 3d band center, optimizing oxygen intermediate binding energetics. The reconstituted catalyst achieves overpotentials of only 223 mV at 100 mA cm−2 and 284 mV at 300 mA cm−2, with exceptional stability exceeding 300 h at 500 mA cm−2. This work reveals a synergistic mechanism where sacrificial Cr doping simultaneously facilitates phase reconstruction and generates self-retained anionic modifiers, offering a new design that couples compositional engineering with dynamic surface chemistry for robust OER electrocatalysis.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"40 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218210","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":"Decoding molecular weight effects in polyimide membranes for CO/CH separation: bridging experiments and simulations","authors":"Nesrin Özenir,Mütesir Temel,Tuba Erdoğan-Bedri,Sadiye Velioğlu","doi":"10.1039/d6ta06845f","DOIUrl":"https://doi.org/10.1039/d6ta06845f","url":null,"abstract":"Polymeric membranes offer an energy-efficient, operationally simple, and scalable platform for natural gas upgrading (CO2/CH4 separation). Among high-performance polymers, 6FDA-based polyimides stand out due to their superior thermal stability, mechanical strength, and tailored gas separation capability. However, the fundamental role of polymer molecular weight (Mw) in dictating the physicochemical architecture and gas transport mechanisms of polyimide membranes remains under-explored. In this study, homopolyimides (6FDA-DABA and 6FDA-pBAPS) and copolyimides (6FDA-pBAPS/DABA (3/1)) with varying Mw were systematically synthesized to elucidate Mw–structure–property–performance relationships. Experimental characterization revealed that increasing Mw diminishes excess free volume associated with chain ends, leading to a reduced fractional free volume (FFV) and a concomitant increase in glass transition temperature (Tg). Consequently, gas permeation measurements across all membrane series exhibited a distinct permselectivity trade-off: higher Mw resulted in reduced gas permeability but a marked enhancement in CO2/CH4 selectivity, reaching an optimal balance of 10.85 Barrer for CO2 permeability with a high selectivity of 54.25 for the highest-Mw copolyimide membrane (CoP140). Additionally, molecular simulations provided detailed atomic-level rationale for CO2 adsorption behaviors. The simulation results demonstrated that higher Mw chains enhance cohesive energy density and induce tighter polymer chain packing. Crucially, while this structural compaction restricts penetrant diffusion, it simultaneously stabilizes the matrix thermodynamically, leading to an increase in Henry's solubility coefficient (kD) with increasing Mw. Overall, this combined experimental and computational study underscores polymer Mw as a vital design parameter to tune chain packing, sorption thermodynamics, and separation efficiency in polyimide separation membranes.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"81 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218256","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":"MOF-derived confinement of defect-rich CeO/VN heterointerfaces for durable high-current alkaline water electrolysis","authors":"Seohyun Yoon,Junho Kim,Hyesu Yang,Daeun Yoo,Pei-chen Su,Jooheon Kim","doi":"10.1039/d6ta05147b","DOIUrl":"https://doi.org/10.1039/d6ta05147b","url":null,"abstract":"Engineering defect-rich oxide/nitride heterointerfaces is an effective strategy for accelerating alkaline hydrogen evolution, but maintaining highly dispersed interfacial structures under high-current electrolysis remains challenging. Herein, we present a MOF-derived confinement strategy to construct a CeO2−x@N-doped carbon–vanadium nitride (CeO2−x@NC–VN) hybrid catalyst from a CeO2@ZIF-8 core@shell precursor. During pyrolysis and nitridation, the ZIF-8 shell is converted into a porous NC framework that confines vanadium species and promotes the formation of finely dispersed VN coupled with oxygen-deficient CeO2−x. Structural and spectroscopic analyses confirmed a porous CeO2−x/VN/NC architecture with crystalline CeO2 and VN domains, abundant oxygen vacancies, homogeneous elemental distribution, and interfacial electronic interaction. Density functional theory calculations further revealed favorable interfacial electronic coupling and reaction energetics for H2O activation and H* adsorption, supporting the cooperative roles of CeO2−x and VN in alkaline HER. Benefiting from the synergistic roles of CeO2−x in water activation, VN in hydrogen-intermediate adsorption, and NC in charge transport and structural confinement, CeO2−x@NC–VN exhibits excellent HER activity in 1.0 M KOH, requiring overpotentials of 35 and 110 mV at 10 and 100 mA cm−2, respectively, with a Tafel slope of 28.21 mV dec−1. It also delivers a mass activity of 203 mA mg−1 at 100 mV, a charge-transfer resistance of 44 Ω, a double-layer capacitance of 37.5 mF cm−2, and a faradaic efficiency of 98.5%. Moreover, the catalyst maintains stable HER operation for 120 h. In a diaphragm-separated alkaline electrolyzer paired with RuO2, the CeO2−x@NC–VN‖RuO2 cell outperforms Pt/C‖RuO2 in iR-corrected cell voltage and operates stably at 500 mA cm−2 for 200 h with only 2.0% voltage decay. Post-OWS analyses confirmed the retention of the porous carbon-confined architecture, homogeneous elemental distribution, Ce3+/Ce4+ redox states, and V–N-related species. This work demonstrates MOF-derived confinement as a promising strategy for constructing durable defect-rich oxide/nitride cathodes for high-current alkaline hydrogen production.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"55 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218213","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":"Polarity-induced H surface coupling in nano-membrane N-polar InGaN/GaN quantum pyramids for efficient seawater splitting","authors":"Chandran Bagavath,Jeong-Kyun Oh,Jae-Hong Ju,Sung-Un Kim,Min-Seok Lee,Se-Bee Shin,Dong Ick Son,Cheul-Ro Lee,Yong-Ho Ra","doi":"10.1039/d6ta05459e","DOIUrl":"https://doi.org/10.1039/d6ta05459e","url":null,"abstract":"Direct photoelectrochemical splitting of natural seawater offers a scalable route to green hydrogen but is constrained by an interfacial paradox: alkaline conditions that accelerate hydrogen evolution also induce Mg/Ca hydroxide scaling, rapidly blocking semiconductor surfaces. Here, we report a membrane-defined III – nitride photocathode that stabilizes the seawater interface and enables catalyst-free hydrogen evolution directly in Yellow Sea seawater. N-polar InGaN quantum pyramids (QPs) integrated on vertical GaN nanowires (NWs) provide broadband (UV-NIR) absorption and a composition-graded “quantum-sliding” band profile, funneling photogenerated electrons toward the pyramid apex and the catalytically active N-polar surface. A conformal graphene-oxide/polylactic-acid (GO/PLA/SiO2) nano-membrane laminated on the nanowire forest serves as an ion-sieving transport layer, preserving water access while suppressing multivalent-ion-driven precipitation and electrode blockage. X-ray photoelectron spectroscopy quantifies heterointerfacial band offsets, while Raman spectroscopy and electron microscopy confirm conformal encapsulation and mitigated deposits after operation. A few-layer graphene coating on the PLA nanofiber-covered InGaN/GaN NWs nanostructure (M-QWs-NWs) photocathode sustains ∼0.5 mA cm−2 for over 200 h in untreated Yellow Sea seawater (pH 8.69) and achieves ∼16.51 mA cm−2 in Yellow Sea water containing 0.5 M NaOH. This membrane-band co-engineering strategy separates semiconductor photo physics from electrolyte complexity, paving the way for practical solar hydrogen production using unprocessed seawater.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"1 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218214","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":"Ultrathin layered alginate ionic network promoted by dynamic hydrogen bond for efficient cobalt recovery from spent lithium-ion batteries","authors":"Qian Huang,Shuang-Long Wang,Lei Zhang,Guo-Hong Tao,Ling He","doi":"10.1039/d6ta05298c","DOIUrl":"https://doi.org/10.1039/d6ta05298c","url":null,"abstract":"With resource constraints and environmental pollution becoming increasingly prominent, the recovery of cobalt from spent lithium-ion batteries has grown ever more urgent. Eco-friendly materials have attracted widespread attention owing to their sustainability, non toxicity, and biodegradability. This study developed a novel bio-based ionic polymer (DADDAlg) with layer-by-layer self-assembly behavior through dynamic hydrogen-bond cross-linking technology derived from alginate. The resulting ionic network is lightweight and exhibits excellent adsorption performance for Co(II), with a maximum adsorption capacity of 78.65 mg·g⁻¹. The material maintains high removal efficiency over a wide range of temperatures (10–45 °C), Co(II) concentrations (50–1200 mg·L⁻¹), and pH values (6–8), while showing good selectivity and anti interference ability. Functional groups such as dynamic hydrogen bonds (N–H···O), free amino groups, and hydroxyl groups can form a tetrahedral spatial coordination configuration with cobalt ions, thereby achieving high-selectivity recognition of cobalt ions. Furthermore, the material exhibits excellent reusability, maintaining a removal efficiency of over 95% even after five consecutive adsorption–desorption cycles. The successful recovery of cobalt from a lithium cobalt oxide (LCO) battery leachate confirms the practical feasibility of DADDAlg. These results demonstrate that DADDAlg is a promising, environmentally benign, and cost effective adsorbent, capable of facilitating the sustainable recycling of cobalt.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"15 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173188","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}