Redi Kristian Pingak, Oliver Conquest, Catherine Stampfl
{"title":"A DFT Investigation of Photocatalytic Water Splitting Properties of the InS/GaTe Heterostructure: Direct Z-Scheme vs Traditional Type-II","authors":"Redi Kristian Pingak, Oliver Conquest, Catherine Stampfl","doi":"10.1039/d5ta04464b","DOIUrl":"https://doi.org/10.1039/d5ta04464b","url":null,"abstract":"Density Functional Theory is used to predict the structural, electronic, and optical properties, as well as the reaction energetics, of the InS/GaTe heterostructure. The system is stable and found to have an ideal band gap of 1.34 eV, significantly lower than its monolayer counterparts. This makes it more effective in absorbing light in the visible region, as confirmed by our analysis of its optical properties. The oxygen evolution reaction (OER) was investigated for both the direct Z-scheme and the type-II mechanisms. The photogenerated hole potential for the Z-scheme ranges from 2.37 eV for pH=0 to 4.02 eV for pH=14, while that for the type-II mechanism is from 1.44 eV (pH=0) to 3.09 eV (pH=14). Based on the analysis of the electronic properties of the InS/GaTe heterostructure, and its Gibbs free energy reaction pathway for OER when the light is turned on, the transfer mechanism of the photogenerated electrons and holes in InS/GaTe is predicted to follow the direct Z-scheme mechanism. Notably, the OER reaction is predicted to be spontaneous for a wide pH range: 2 ≤ pH ≤ 14 (Z-scheme) and 3 ≤ pH ≤ 14 (type-II). This makes the InS/GaTe heterostructure more promising for OER compared to many other catalysts. While the type-II mechanism cannot facilitate HER, the Z-scheme mode of InS/GaTe is predicted to have good performance for HER, with an ideal Gibbs free energy of -0.02 eV at pH = 7. The solar-to-hydrogen efficiency is predicted to be 44.8%, which is higher than that of many other photocatalysts, and is far higher than the 10% threshold for commercial applications. These results strongly indicate that the InS/GaTe heterostructure, in its Z-scheme mode, holds high potential as a photocatalyst to facilitate both OER and HER for water splitting applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"54 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203540","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":"Ge Nanograin‐Enhanced Si/C Composite Anodes: Anchored Interfaces for Rapid Electron and Ion Conduction","authors":"Xintong Xu, Xiao Mu, Tao Huang, Aishui Yu","doi":"10.1039/d5ta05658f","DOIUrl":"https://doi.org/10.1039/d5ta05658f","url":null,"abstract":"Silicon (Si) anodes offer exceptionally high theoretical capacities for lithium-ion batteries. However, severe volume changes, low intrinsic conductivity, and fragile Si/C interfaces still hamper their practical application. To address these challenges, we developed a germanium-decorated silicon/carbon composites (ACGS@C) via chemical vapor deposition of Si into a porous carbon scaffold, concurrently introducing just 2 wt% Ge nanograins at the Si/C interface. These Ge nanograins not only build continuous electron/ion pathways but also chemically anchor Si, thus buffering expansion and mitigating interfacial degradation. Benefiting from the dual-function design, the ACGS@C-2 electrode exhibits a high initial reversible capacity of 1986.2 mAh g<small><sup>-1</sup></small> with an initial coulombic efficiency of 87.4%. Moreover, it delivers a specific capacity of 626 mAh g<small><sup>-1</sup></small> at 3.4 A g<small><sup>-1</sup></small> and retains 80% of its capacity after 270 cycles. This trace-Ge interfacial engineering strategy offers a scalable route to unlock the full potential of Si anodes without compromising energy density, rate capability, or cycling stability.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"37 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209770","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}
Jung Wang, Yu Wei, Bo-Hao Zhang, Weiya Huang, Kai yang, Kang-Qiang Lu
{"title":"Recent progress on ZnIn2S4 -based composite photocatalyst for photocatalytic hydrogen production coupling organic synthesis","authors":"Jung Wang, Yu Wei, Bo-Hao Zhang, Weiya Huang, Kai yang, Kang-Qiang Lu","doi":"10.1039/d5ta06861d","DOIUrl":"https://doi.org/10.1039/d5ta06861d","url":null,"abstract":"Compared with sacrificial-agent-dependent half-reactions in photocatalytic water-splitting hydrogen production, coupling photocatalytic organic synthesis with hydrogen production markedly boosts electron-hole utilization efficiency and cuts reaction costs. In recent years, hexagonal ZnIn2S4 has been widely applied in the field of photocatalytic hydrogen production coupled with organic synthesis due to its advantages such as narrow band gap, high hydrogen evolution efficiency, good chemical stability, non-toxicity, and low cost. Herein, we present a comprehensive review of the latest progress in ZnIn2S4-based photocatalysts. We first summarize the preparation methods of ZnIn2S4 and the strategies to improve its performance, including metal doping, morphological engineering, heterostructure construction and defect engineering. Subsequently, we focus on the research progress of ZnIn2S4-based photocatalysts in hydrogen production coupling organic synthesis, including the selective conversion of alcohols, oxidative coupling of amines, thiol dehydrogenation, and biomass oxidation. Finally, the challenges and opportunities that ZnIn2S4 face in the practical application are discussed. It is expected that this review will offer insightful guidance for the rational design of semiconductor-based dual-functional photoredox reaction systems, thereby injecting impetus into the research on harvesting environmentally solar fuel production as well as the high-value-added fine chemicals.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"99 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203597","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}
Madan Bahadur Saud, M. Bilal Faheem, Hansheng Li, Haining Zhang, Bilawal Khan, Samprash Risal, Abiral Baniya, Xinlu Wang, Yuchen Zhang, Ruosi Qiao, Poojan Kaswekar, Ian Dean Hosein, Yeqing Wang, Jr-Hau He, Zheng Fan, Quinn Qiao
{"title":"Synergy of metal halide doping and a polymeric interface enables improved electrochemical performance of all solid-state Li batteries","authors":"Madan Bahadur Saud, M. Bilal Faheem, Hansheng Li, Haining Zhang, Bilawal Khan, Samprash Risal, Abiral Baniya, Xinlu Wang, Yuchen Zhang, Ruosi Qiao, Poojan Kaswekar, Ian Dean Hosein, Yeqing Wang, Jr-Hau He, Zheng Fan, Quinn Qiao","doi":"10.1039/d5ta06438d","DOIUrl":"https://doi.org/10.1039/d5ta06438d","url":null,"abstract":"Sulfide solid-state electrolytes are promising candidates for all-solid-state lithium metal batteries (ASSLBs) having higher energy density and practical safety due to their high ionic conductivity and favorable mechanical properties. However, their practical integration is hindered by low critical current density (CCD), a narrow electrochemical stability window, and high impedance with electrodes. Herein, we demonstrate that doping lithium phosphorus sulfide (Li<small><sub>7</sub></small>P<small><sub>3</sub></small>S<small><sub>11</sub></small>) solid electrolyte with zirconium chloride (ZrCl<small><sub>4</sub></small>) significantly enhances its electrochemical performance. Unlike previously reported doping strategies, ZrCl<small><sub>4</sub></small> doping uniquely introduces dual dopants (Zr<small><sup>4+</sup></small> and Cl<small><sup>−</sup></small>) into the Li<small><sub>7</sub></small>P<small><sub>3</sub></small>S<small><sub>11</sub></small> matrix. Density functional theory (DFT) and <em>ab initio</em> molecular dynamics (AIMD) simulations reveal that the Zr<small><sup>4+</sup></small> ions increase dynamic structural flexibility, while Cl<small><sup>−</sup></small> ions create additional Li<small><sup>+</sup></small> vacancies, collectively enhancing structural stability and ionic conductivity beyond the capacity of single-element doping strategies. Optimized doping content of ZrCl<small><sub>4</sub></small> improved the CCD of Li<small><sub>7</sub></small>P<small><sub>3</sub></small>S<small><sub>11</sub></small> from 0.55 mA cm<small><sup>−2</sup></small> to 1.7 mA cm<small><sup>−2</sup></small>, while the ionic conductivity improved from 1.8 × 10<small><sup>−3</sup></small> S cm<small><sup>−1</sup></small> to 3.0 × 10<small><sup>−3</sup></small> S cm<small><sup>−1</sup></small>. Li/Li symmetrical cells with doped electrolyte exhibited improved cycling stability at 0.1 mA cm<small><sup>−2</sup></small> compared to the control counterparts. Furthermore, a thin solid polymer electrolyte (SPE) was used at the interface between the cathode and solid electrolyte to enable the stack pressure free operation of full cells. Li/LiFePO<small><sub>4</sub></small> (LFP) full cells using doped solid electrolyte (SE) in combination with SPE catholyte demonstrated stable performance compared to undoped SE based cells. The enhanced Li-dendrite suppression and improved electrochemical properties due to doped Li<small><sub>7</sub></small>P<small><sub>3</sub></small>S<small><sub>11</sub></small> and the stack free operation due to the addition of SPE as catholyte will add significant potential for advancing ASSLB technology.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"101 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203538","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":"Design and prompt synthesis of a hydrazone-linked covalent organic framework with binding pockets for lanthanides: Luminescent pH and ratiometric temperature sensing","authors":"Himanshi Bhambri, Sanjay Mandal","doi":"10.1039/d5ta06543g","DOIUrl":"https://doi.org/10.1039/d5ta06543g","url":null,"abstract":"Focusing on the exceptional traits of a highly functionalized, flexible, and yet infrequent hydrazone linkages, a new covalent organic framework, namely BTD, is synthesized by the fast crystallization technique within 1.5 h. Extensive characterization by various spectroscopic and microscopic techniques, powder X-ray diffraction, and computational simulation confirms its purity, structural features, and porous nature. The framework is locked due to the presence of secondary interactions such as intralayer (N···H-O and C-H···O=C), interlayer (N-H···O) H-bonding as well as π-π stacking, which provides in-plane rigidness in the staggered AB type stacking of layers. These strong interactions can be the possible reason for the prompt crystallization of BTD. The dual proton donor and acceptor sites offered by functionalized hydrazone linkage in BTD lead to the wide-range, colorimetric, luminescent detection of hydrogen ion concentration. Its luminescence is highest at pH 4 but quenched in strong basic medium (pH 13). Furthermore, to embark upon the characteristics of hydrazone connectivity and anchored functional groups (carbonyl and hydroxy), the trivalent lanthanides are incorporated onto the decorated pockets yielding Tb@BTD and Eu@BTD. Utilizing the remarkable thermal detection features of lanthanide-decorated COFs, the ratiometric temperature detection studies are performed in the aqueous and methanolic slurries. The computed relative sensitivity values for Tb@BTD and Eu@BTD are: 1.404 % K-1 and 1.118 % K-1 at 333 K in water and 2.73 % K-1 and 2.29 % K-1 at 313 K in methanol, respectively. For noting the utility of both COFs in real environmental conditions, the change in luminescence is studied in the temperature range of 308-320 K. With a quenching of 22%, Eu@BTD proves to be a better candidate to work for effective luminescent thermometric applications under physiological conditions.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"34 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209771","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}
Zhengwu Liu, Hongwei Liu, Xiaoliang Ren, Pusen Lu, Jianjun Ye, Kang Wang, Feng Jiang
{"title":"Effect of Ni-W-S electrocatalysts on the stability and electrochemical properties of photocathode","authors":"Zhengwu Liu, Hongwei Liu, Xiaoliang Ren, Pusen Lu, Jianjun Ye, Kang Wang, Feng Jiang","doi":"10.1039/d5ta06369h","DOIUrl":"https://doi.org/10.1039/d5ta06369h","url":null,"abstract":"Silicon-based photocathodes are attractive for photoelectrochemical (PEC) water splitting, yet their deployment is constrained by reliance on precious metal catalysts like platinum (Pt). Here, we introduce a cost-efficient, tungsten-doped nickel sulfide (NiWS) catalyst, photoelectrodeposited onto a TiO 2 -passivated silicon substrate. X-ray photoelectron spectroscopy reveals that W incorporation tailors the local electronic environment of Ni and S, facilitating charge redistribution and accelerating interfacial charge transfer kinetics. The engineered NiWS/TiO 2 /Si photocathode delivers a high photocurrent density of -30.8 mA cm -2 at 0 V RHE , with an onset potential of 0.58 V RHE , an applied bias photon-to-current efficiency (ABPE) of 4.47%, and a Faradaic efficiency of ~90% for hydrogen evolution in neutral phosphate buffer (pH 6.5). It also demonstrates exceptional durability, retaining stable operation over 1014 hours under continuous illumination. When integrated with a silicon photovoltaic cell in a tandem architecture, the system enables unbiased solar-driven water splitting, delivering a solar-to-hydrogen (STH) efficiency of 4.01% and sustaining performance for 115 hours under AM 1.5G conditions. This work positions NiWS as a scalable, earth-abundant alternative to noble metals for long-term PEC hydrogen production.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"6 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203549","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}
Yi Li, Junbo Zeng, Jiahao Mo, Fuping Zhou, Tao Duan, Youkui Zhang
{"title":"Graphene accelerates electron transfer over copper-cobalt nanoparticles for efficient electroreduction of nitrate to ammonia","authors":"Yi Li, Junbo Zeng, Jiahao Mo, Fuping Zhou, Tao Duan, Youkui Zhang","doi":"10.1039/d5ta06585b","DOIUrl":"https://doi.org/10.1039/d5ta06585b","url":null,"abstract":"Nitrate sewage will give rise to the hazarding of aquatic ecosystems and human life. Electrochemical reduction of nitrate to ammonia (NO 3 -RR) was reckoned as the prospective pathway for ecological remediation and nitrogen cycle but faced with challenges. In this work, through decorating graphene on copper-cobalt (CuCo) nanoparticles, the electron transferring between Co and Cu is intensified, which is conducive to NO 3 -RR. The optimized catalyst (CuCo-Gr0.1) performs eminent ammonia yield of 0.29 mmol h -1 cm -2 with Faradic efficiency (FE) of 97.2 % at -0.16 V versus reversible hydrogen electrode (vs RHE) and increasing to 0.91 mmol h -1 cm -2 at -0.56 V vs RHE in acid electrolyte. Besides, CuCo-Gr0.1 also exhibits high performance for the reduction of nitrate to ammonia in neutral condition, which can combine with uranyl ions to produce ammonium uranium oxide hydrate. The density functional theory calculations reveal that the decorated graphene on CuCo can promote electron transfer and NO 3 -adsorption, thus accelerating the catalytic kinetics of NO 3 - RR. This work provides new insights into the design of efficient NO 3 -RR electrocatalyst for nitrogen and uranium cycling in nuclear industry wastewater treatment.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"10 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203537","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":"Phase diagrams and chemical expansion upon hydration of proton conductors BaZrxCe0.8-xY0.1Yb0.1O2.9(H2O)n (0 ≤ x ≤ 0.8; 0 ≤ n ≤ 0.1)","authors":"Lozane Hamze, Olivier Joubert, Eric Quarez","doi":"10.1039/d5ta07218b","DOIUrl":"https://doi.org/10.1039/d5ta07218b","url":null,"abstract":"Proton-conducting ceramics are promising candidates for applications in sustainable energy technologies, with BaZrxCe0.8-xY0.1Yb0.1O2.9 (BZCYYb) perovskites standing out as excellent proton conductors. However, comprehensive structural studies of these materials, particularly concerning their hydrated and dehydrated states, as well as the effects of composition (x) and temperature, are still limited. This study explores the crystal structures of BaZrxCe0.8-xY0.1Yb0.1O2.9(H2O)n and BaZrxCe0.8-xY0.1Yb0.1O2.9 (0 ≤ x ≤ 0.8) using neutron and X-ray diffraction techniques. The chemical expansion due to water incorporation is quantified by measuring unit cell volumes via X-ray diffraction, showing strong agreement with mass loss data from thermogravimetric analysis (TGA). Phase diagrams for both hydrated and dehydrated phases are developed, revealing a decrease in symmetry and a reduction in phase transition temperatures as x increases. Hydration notably affects octahedral tilting, as evidenced by comparisons of hydrated and dehydrated structures at room temperature (RT). Furthermore, a bond valence sum (BVS)-based approach is proposed, offering improved predictions of octahedral tilting and structural stability compared to the traditional Goldschmidt tolerance factor. These structural insights, particularly the influence of hydration, are essential for advancing our understanding of these materials and providing a solid foundation for linking their structure to their properties.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"23 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203539","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}
Keerti Rathi, Viktoriya Pakharenko, Otavio Augusto Titton Dias, Colin van der Kuur, Ning Yan, Mohini Sain
{"title":"One-step dual process strategy for holey graphite towards scalable and stable lithium-ion battery anodes","authors":"Keerti Rathi, Viktoriya Pakharenko, Otavio Augusto Titton Dias, Colin van der Kuur, Ning Yan, Mohini Sain","doi":"10.1039/d5ta05487g","DOIUrl":"https://doi.org/10.1039/d5ta05487g","url":null,"abstract":"Our research demonstrates a one-step dual-process acid treatment approach for modifying graphite, which increases its interlayer distance and generates nanoscale holes, thereby effectively shortening the lithium-ion diffusion pathway without the need for heteroatom doping. Compared with pristine graphite (PG), the expanded holey graphite (EG) produced by this process achieves significantly enhanced electrochemical performance while maintaining structural integrity. The EG shows excellent electrochemical performance, reaching a specific capacity of 179.45 mAh g<small><sup>−1</sup></small> and retaining 89.3% of its capacity after 300 cycles in a full pouch cell combined with a commercial NMC523 cathode. High coulombic efficiency (approximately 93.8%) and improved cycling stability confirm the durability of the etched graphite. Beyond mere performance considerations, the study elucidates the degradation mechanisms inherent in commercial lithium-ion batteries (LIBs), thereby offering dependable guidance for electrode surface engineering and the optimization of cycling protocols. With this scalable and impurity-free approach to modification, purified etched graphite emerges as a promising candidate for next-generation LIB anodes, satisfying the high energy requirements and durability necessary for electric vehicles and advanced energy storage systems.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"3 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209772","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":"Stress and Airflow-Sensitive 3D-Printed Hydrogel Sensor Based on Cu2+-Alanine Coordination and Graphene Sheet Networks","authors":"Jiamin Wu, Xiangke Wang, Bo Liu, Jingzhi Tang, Xinyuan Wan, Gengsheng Weng","doi":"10.1039/d5ta06290j","DOIUrl":"https://doi.org/10.1039/d5ta06290j","url":null,"abstract":"Flexible sensors with applications in real-time monitoring of human health conditions, e.g., breath, are of vital importance. Herein, we report a 3D-printed hybrid network (HN) hydrogel sensor showing stress and airflow monitoring performance based on the sensitive Cu2+-alanine (Ala) coordination cross-linked poly(N,N-dimethylacrylamide-co-3-alanine-2-hydroxypropylmethacrylate) (PDA) network and the graphene (GR) filler network. The highly stress and airflow-sensitive HN hydrogel sensor is prepared by sequential 3D printing of the polyacrylic acid hydrogel layer and the patterned PDA/Cu/GR hydrogel layer cross-linked by the Cu2+-Ala coordination. The graphene sheets in the PDA/Cu/GR hydrogel form lamellar structures, which generate a rough and porous network structure. The stress sensitivity of the HN hydrogel sensor stems from the dynamic Cu2+-Ala coordination within the PDA network and the rough, porous network structure of the graphene filler, while its airflow sensitivity is attributed to the reversible and rapid water loss and reabsorption behavior. The sensor’s stress sensitivity enables the detection of the motion speed of the object, hand gestures, and facial expressions. The fist punching out/pulling back test and human breath detection demonstrate the application for airflow detection. Our work provides a new opportunity for fabricating multimodal hydrogel sensors with potential applications for human healthcare and activity monitoring.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"22 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203536","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}