Wenke Gui, Shan Jiang, Luyuan Wang, Chuangwei Liu, Zichao Huang, Li Wang, Jianping Yang
{"title":"Construction of Asymmetric Anion Layer to Accelerate Carrier Reaction Kinetics and Thermodynamically Promote Photocatalytic CO2 Reduction","authors":"Wenke Gui, Shan Jiang, Luyuan Wang, Chuangwei Liu, Zichao Huang, Li Wang, Jianping Yang","doi":"10.1002/adfm.202505919","DOIUrl":"https://doi.org/10.1002/adfm.202505919","url":null,"abstract":"The efficient photocatalytic reduction of CO<sub>2</sub> into value-added chemicals is significantly challenged by the charge carrier separation and transfer kinetics of photocatalysts as well as the thermodynamics of the CO<sub>2</sub> reduction process. Herein, it proposes a heterojunction with asymmetric W-Cl anion layer in Bi<sub>2</sub>WO<sub>6</sub> (abbreviated as BWOC). The asymmetric W-Cl anion layer results in unbalanced electron density distribution and thus enables to establish atomic-level donor–acceptor structure as well as larger electrostatic potential in the heterojunction, which facilitate the charge carrier separation and transfer kinetics. Simulation on the intermediates of the CO<sub>2</sub> photoreduction process demonstrates that Bi<sub>2</sub>WO<sub>6</sub> with asymmetric W-Cl anion layer possesses smaller energy barrier for the rate-determining step of *COOH endothermic formation, and it is thermodynamically more favorable to generate CO as further confirmed by the detection of intermediates over in situ Fourier transform infrared spectroscopy. As a result, BWOC achieved rather high CO yield with the value of 32.11 µmol g<sup>−</sup>¹ h<sup>−</sup>¹ which is nearly four times higher than that of pure Bi<sub>2</sub>WO<sub>6</sub>. The construction of asymmetric anion layer in this work provides new insights for the design of efficient photocatalytic systems toward CO<sub>2</sub> reduction.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"73 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736858","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Preparation and Supercapacitive Performance of K⁺-Doped Nickel-Cobalt-Based Perovskite Fluoride/Double Hydroxide Heterojunction with Ultra-Long Cycling Stability and High Mass Loading","authors":"Zheng Tao, Zhenming Xu, Jiahao Fang, Chunyan Guan, Pingfan Zhou, Peng Huang, Yuxue Deng, Hongfang Ma, Laifa Shen, Xiaogang Zhang, Hao Tong","doi":"10.1002/adfm.202502658","DOIUrl":"https://doi.org/10.1002/adfm.202502658","url":null,"abstract":"NiCo-LDH's low conductivity and structural instability limit its stability and cycle life, especially under high-mass-loading conditions. In this paper, a KCoNiF<sub>3</sub>/NiCo-LDH supported on activated carbon cloth (KCNF-LDH/ACC) heterojunction structural composite material is in situ synthesized on carbon cloth by doping K<sup>+</sup> into nickel-cobalt double hydroxide, and the loading amount can reach 12 mg cm<sup>−2</sup>. The doping of K⁺ can enhance the stability and rate performance of NiCo-LDH. The electrode with the optimal K<sup>+</sup> doping amount (KCNF-LDH-3/ACC) exhibits a capacitance of 10.1 F cm<sup>−2</sup> / 841 F g<sup>−1</sup> at 1 mA cm<sup>−2</sup>. When the current increases to 50 mA cm<sup>−2</sup>, capacitance can still maintain 85% of the initial capacity. The capacity retention rate reaches 91% after 20 000 cycles. An asymmetric supercapacitor is assembled with KCNFo-LDHo-3/ACC as the positive electrode and AC as the negative electrode. It outperformed the previously published NiCo-LDH supercapacitors with an energy density of 1.14 mWh cm<sup>−2</sup> at a power density of 4 mW cm<sup>−2</sup>. This demonstrated the viability of doping alkali metal cations into NiCo-LDH and explored the application potential of perovskite fluoride (ABF<sub>3</sub>) in the field of supercapacitors.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"42 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736906","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"A Sequential Therapeutic Strategy Based on Aptamer/Polymer-Functionalized PDA/Ag for Precise Acinetobacter Baumannii Imaging and Pneumonia Treatment","authors":"Yun Li, Zhuorui Dong, Yingfei Ma, Jian Zhang, Yanan Wang, Dandan Cui, Kaifang Wang, Baojie Du, Runzhi Li, Zhifei Wang, Ruixue Wang, Bing Cao, Ruiping Zhang","doi":"10.1002/adfm.202425625","DOIUrl":"https://doi.org/10.1002/adfm.202425625","url":null,"abstract":"<i>Acinetobacter baumannii</i> (<i>A. baumannii</i>) is a leading cause of pneumonia. Conventional antibiotics can increase the risk of drug resistance and non-specifically harm microflora, disrupting their balance. In addition to pathogenic bacteria, lung inflammation also damages tissue. This study develops an aptamer/polymer-functionalized mesoporous polydopamine/silver nanocomposite (Apt/ODEA-PDA/Ag-ICG) to specifically target <i>A. baumannii</i> and sequentially exhibit antibacterial/antioxidative properties for pneumonia treatment. After synthesizing the polyzwitterion (ODEA), the polymer/aptamer is conjugated with the PDA/Ag core, and ICG is further labeled to fabricate the nanocomposite. Upon intratracheal instillation, nanocomposites penetrate the mucus barrier with the help of polyzwitterions. The nanocomposite precisely targets <i>A. baumannii</i> through specific recognition by the aptamer, without affecting other microflora. Moreover, ICG is conjugated and distributed disorderedly within the polymer. ICG near the PDA/Ag core contributes to high NIR-I absorbance and good photothermal ability. ICG further from the PDA/Ag acts as a fluorescent molecule for specific <i>A. baumannii</i> imaging. Furthermore, PDA/Ag efficiently exhibits synergistic antibacterial activity owing to the acidic environment/heat-accelerated Ag<sup>+</sup> release and photothermal effect. Importantly, alongside Ag<sup>+</sup> release, the antioxidant ability of PDA scavenges reactive oxygen species and alleviates inflammation, thereby accelerating pneumonia treatment. In summary, nanocomposites provide an alternative approach for designing advanced antibacterial systems.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"90 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736855","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Crystal Growth Promotion Enables High-Performance Te0.7Se0.3 Thin-Film Shortwave Infrared Photodetector for Multispectral Imaging Applications","authors":"Hongbo Li, Chuanhao Li, Meng Peng, Kanghua Li, Chao Chen, Yuexing Chen, Zhuanghao Zheng, Zhenghua Su, Guangxing Liang, Shuo Chen","doi":"10.1002/adfm.202425690","DOIUrl":"https://doi.org/10.1002/adfm.202425690","url":null,"abstract":"Tellurium-selenium (Te<sub>x</sub>Se<sub>1-x</sub>) alloy compound is considered as an excellent light absorber layer for thin-film photodetector applications, owing to its suitable bandgap and excellent optoelectronic performance. Recently, the research on Te<sub>x</sub>Se<sub>1-x</sub> photodetectors has achieved considerable progress, especially under electron and/or hole transport layer engineering to improve the device responsivity. However, the intrinsic growth mechanism of Te<sub>x</sub>Se<sub>1-x</sub> thin film still needs investigation. In this work, based on the analysis of crystal growth thermodynamics and kinetics, Te<sub>0.7</sub>Se<sub>0.3</sub> light absorber with optimal (100) growth orientation can be achieved through thermal evaporation of pre-alloyed Te<sub>0.7</sub>Se<sub>0.3</sub> powder and atmosphere-assisted slow thermal annealing of Te<sub>0.7</sub>Se<sub>0.3</sub> thin film. Thanks to the optimized Te<sub>0.7</sub>Se<sub>0.3</sub> light absorber and Te<sub>0.7</sub>Se<sub>0.3</sub>/ZnO heterojunction interface, the champion self-powered thin-film photodetector possesses a wide spectral response range of 300–1600 nm, minimized dark current density of 3.1 × 10<sup>−5</sup> mA cm<sup>−2</sup>, accompanied with satisfactory responsivity of 0.06 A W<sup>−1</sup> and detectivity of 5.9 × 10<sup>9</sup> Jones at 1300 nm, and linear dynamic range exceeding 101 dB. Interestingly, an imaging system based on this photodetector can achieve high-precision color imaging and multispectral imaging from visible light to short wave infrared light, highlighting the intriguing application potential of Te<sub>0.7</sub>Se<sub>0.3</sub> photodetectors.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"31 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736856","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Tongtong Kang, Taiming Zhang, Fei Zhang, Mingbo Pu, Lianwei Chen, Hanlin Bao, Siran Chen, Anbin Du, Li Long, Yinghui Guo, Mingfeng Xu, Xiangang Luo
{"title":"Broadband High-Efficiency Nonreciprocal Transmission Enabled by Silicon/Vanadium Dioxide Catenary Metasurfaces","authors":"Tongtong Kang, Taiming Zhang, Fei Zhang, Mingbo Pu, Lianwei Chen, Hanlin Bao, Siran Chen, Anbin Du, Li Long, Yinghui Guo, Mingfeng Xu, Xiangang Luo","doi":"10.1002/adfm.202504593","DOIUrl":"https://doi.org/10.1002/adfm.202504593","url":null,"abstract":"Nonreciprocal transmission based on nonlinear optical materials has attracted considerable attention for eliminating the need for complex and bulky external bias systems and shows great potential for high-intensity laser protection. Strongly resonant structures are commonly used to achieve lower laser operating power and higher efficiency. However, this approach typically compromises other critical performance metrics, such as protection power range, maximum operating power, bandwidth, and angular range. Here, a novel strategy is proposed using weakly resonant structures to realize nonreciprocity while preserving high performance across these metrics. This achievement stems from the large out-of-plane refractive index asymmetry in the Si/VO<sub>2</sub> catenary structure, enabling robust nonreciprocal transmission with high efficiency across a broad bandwidth (8–11.5 µm) and angular range (>75°) theoretically. This design also shows a higher operating power ceiling and extends the existing tunable nonreciprocal range by an order of magnitude. Experiments validate the tunable nonreciprocal range at 10.6 µm wavelength. Protection capabilities are significantly enhanced through wavefront modulation, offering rapid and effective protection from below the phase transition to above the damage threshold. This work presents a novel paradigm for robust nonreciprocal metasurfaces, with considerable potential for applications in remote sensing, environmental monitoring, biomedicine, and industrial manufacturing.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"34 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736910","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Ultrahigh Energy Storage in Relaxor Ferroelectric Ceramics with Core–Shell Grains","authors":"Qizhen Chai, Peng Tan, Leiyang Zhang, Zhaobo Liu, Santan Dang, Zhanhui Peng, Di Wu, Xiaodong Xu, Bohan Xing, Xiaolian Chao, Houbing Huang, Shujun Zhang, Zupei Yang","doi":"10.1002/adfm.202503798","DOIUrl":"https://doi.org/10.1002/adfm.202503798","url":null,"abstract":"The achievement of record-high energy storage performance in relaxor-ferroelectric bulk ceramics represents a major advancement in the field of dielectric capacitors. Nonetheless, a trade-off between breakdown strength and polarization has typically limited the optimization of overall performance. Here, guided by a rational composition design, K<sub>0.5</sub>Na<sub>0.5</sub>NbO<sub>3</sub>-based bulk ceramics are fabricated with grain core–shell structures and polymorphic nanodomains, leading to a synergistic enhancement of breakdown strength and polarization. This results in an unprecedented recoverable energy density of ≈20.4 J·cm<sup>−3</sup> and an energy efficiency of ≈90% at an electric field of ≈1020 kV·cm<sup>−1</sup>. Additionally, the ceramics exhibits excellent charge–discharge performance, including a high discharge energy density of ≈6.0 J·cm<sup>−3</sup> and an ultrashort discharge time of ≈42 ns at 500 kV·cm<sup>−1</sup>, along with superior reliability and stability. These advancements are expected to provide valuable insights for the exploration and utilization of advanced dielectric materials.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"29 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143737171","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Bo Pang, Liping Wen, Linlin Zheng, Jia Wei, Tengda Xu, Yongyang Song, Juan Li, Shutao Wang
{"title":"Neutrophil Extracellular Traps: Emerging Biomarker and Prototype of Functional Materials","authors":"Bo Pang, Liping Wen, Linlin Zheng, Jia Wei, Tengda Xu, Yongyang Song, Juan Li, Shutao Wang","doi":"10.1002/adfm.202425035","DOIUrl":"https://doi.org/10.1002/adfm.202425035","url":null,"abstract":"Functional biomaterials composed of multiple biomacromolecules have significant advantages over those made from a single type. However, harmoniously integrating various biomacromolecules remains challenging. Neutrophil extracellular traps (NETs), an emerging biological structure released from neutrophils, serve as a natural prototype worth investigating and learning from. NETs consist of intricate biomacromolecules and exhibit web-like microstructure, endowing them with multifaceted roles in both physiological and pathological processes. In this review, research progress is systematically examined on NETs from a materials science perspective. First, the origin and transformation of NETs are introduced, and their functional mechanisms of various NET components are thoroughly dissected rather than conventionally treating NETs as a single entity. Second, given their complex components and functions, NETs are revealed as a potential biomarker for disease prediction. Third, typical characterization technologies for the analysis of NETs are summarized. Fourth, artificial materials inspired by NETs are discussed. In addition, the natural regulatory processes of NETs provide bio-inspired prototypes for the design of advanced functional materials. Finally, perspectives on the opportunities and challenges in advancing NETs are presented as emerging biomarkers and models for the development of bio-inspired materials.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"183 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736905","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yibin Zhang, Xuegang Niu, Xiaoyu Wang, Yi Wu, Jiangnan Sun, Shen Lin, Fuxin Lin, Yuanxiang Lin, Dezhi Kang, Bin Gao
{"title":"Pathogenesis Activated “In Situ Disassembly-Reassembly” Pattern Dual-Scavenges Cell-Free DNA/ROS for Hemorrhagic Stroke Management","authors":"Yibin Zhang, Xuegang Niu, Xiaoyu Wang, Yi Wu, Jiangnan Sun, Shen Lin, Fuxin Lin, Yuanxiang Lin, Dezhi Kang, Bin Gao","doi":"10.1002/adfm.202424358","DOIUrl":"https://doi.org/10.1002/adfm.202424358","url":null,"abstract":"Intracerebral hemorrhage (ICH) causes uncontrolled neuroinflammation/oxidative stress to aggravate secondary brain injury (SBI) for high mortality and disability but lacks effective pharmacotherapy in clinical practices. This represents an imperative need to discover potential targets and develop advanced therapeutic strategies. Herein, it is discovered that cell-free DNA (cfDNA, a driving factor of inflammation) level in serum positively correlates with SBI severity and it is speculated as a potential targeting molecule. However, traditional cfDNA-scavenging materials are mainly limited within the polycationic type and exist severe side effects. Herein, this work designs a drug delivery nanosystem, which utilizes a pathogenesis-activated sequential disassembly-reassembly process to in situ dual-scavenge cfDNA and ROS for the regulation of neuroinflammation/oxidative stress, thereby reducing SBI and preventing further damage in experimental mice. The findings not only demonstrate the importance of cfDNA in SBI but also provide an advanced pharmacotherapy to enhance therapeutic potential toward the effective alleviation on SBI following ICH.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"5 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736907","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Qingchuan Shi, Run Yang, Jinghan Yang, Pan Liu, Juan Liu, Peiyi Wang
{"title":"β-Cyclodextrin/Amantadine Co-Assembled Hollow Nanocapsules Realize the Rapid Leaf Adhesion and Bacterial Biofilm Disassembly for Rice and Citrus Protections","authors":"Qingchuan Shi, Run Yang, Jinghan Yang, Pan Liu, Juan Liu, Peiyi Wang","doi":"10.1002/adfm.202422669","DOIUrl":"https://doi.org/10.1002/adfm.202422669","url":null,"abstract":"A superior bactericide to accomplish its efficient bactericidal function requires breaking through stubborn biofilm barriers and achieving efficient leaf adsorption. To overcome this challenge, supramolecular self-assembly strategies are employed to fabricate multifunctional aggregates. Herein, a versatile supramolecular inclusion—AdA8@<i>β</i>-CD is constructed by loading an amantadine-modified bactericidal structure (AdA8) into <i>β</i>-cyclodextrin (<i>β</i>-CD) via host–guest recognition driving force, which spontaneously self-assembles into biocompatible hollow nanocapsules. This smart optimization not only allows the bactericides to quickly stay on the hydrophobic leaves, preventing their droplets from splashing and bouncing but also improves the performance of removing biofilm barriers. At a lower concentration of 5 µg mL<sup>−1</sup>, the disruption rate of AdA8@<i>β</i>-CD to <i>Xanthomonas</i> biofilm reaches 78.3%. Moreover, AdA8@<i>β</i>-CD enhances the limitation of bacterial motility and extracellular enzyme secretion, thereby reducing bacterial colonization and pathogenicity. These reformative properties are undoubtedly transmitted to in vivo activity, providing corresponding preventive efficacies of 51.1% and 73.2% against rice bacterial blight and citrus canker at 200 µg mL<sup>−1</sup>, which are notably better than those of traditional agrochemicals—thiodiazole-copper-20%SC (33.9%/37.4%), kasugamycin (28.7%), and AdA8 itself (43.8%/45.3%). Furthermore, this oligosaccharide-coated bactericide—AdA8@<i>β</i>-CD exhibits good biosafety and is more eco-friendly. This study is instructive for the creation of multifunctional green agrochemicals.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"31 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736909","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lei Ge, Jiaqi Li, Gaojing Du, Kai Sheng, Jingwei Hou, Binyu Zhou, Yatao Zhang, Bart Van der Bruggen, Junyong Zhu
{"title":"Microporous Polyacylhydrazone Membranes with 3D Interconnected Nanochannels for Accurate Molecular Sieving","authors":"Lei Ge, Jiaqi Li, Gaojing Du, Kai Sheng, Jingwei Hou, Binyu Zhou, Yatao Zhang, Bart Van der Bruggen, Junyong Zhu","doi":"10.1002/adfm.202504997","DOIUrl":"https://doi.org/10.1002/adfm.202504997","url":null,"abstract":"Microporous membranes featuring 3D nanochannels present a compelling avenue for energy-efficient liquid separations, attributable to their tunable interconnected through-pore structures. However, the rational design of 3D-nanochannel membranes that simultaneously achieve high permeance and selectivity remains a challenge, arising from the scarcity of appropriate molecular building blocks and the reliance on empirical synthetic methods. Herein, an innovative 3D polyacylhydrazone (PAH) membrane with unique pore-interconnected structures is constructed on a porous hydrogel using contorted tetrahedral aldehydes (TFS) monomers via an in situ interface-confined strategy. Manipulation of side alkyl chain lengths within terephthalohydrazide (TPH) derivates enabled the enhancement of microporosity and tunable pore environment of PAH nanofilms. Molecular dynamics simulations revealed that TPH<sub>EO</sub> linkers with higher reactivity and moderate steric hindrance facilitate superior pore interconnectivity and sharpened pore size distributions. The resulting PAH membranes achieved exceptional methanol permeances of 10.1 L m<sup>−2</sup> h<sup>−1</sup> bar<sup>−1</sup> and small molecular weight cut-offs of 310 Da, outperforming the state-of-the-art polyamide membranes. This further translated into an outstanding capability in the fractionation of active pharmaceutical ingredients within organic solvent systems. This work demonstrates the efficacy of rational molecular design in developing high-microporosity membranes with tailored interconnected nanochannels, underscoring the potential of 3D microporous membranes for accurate molecular separations.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"32 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736849","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}