Diabetic foot ulcers (DFU) are notoriously challenging to heal due to severe infection, excessive inflammation, and difficulty in angiogenesis. In response to these problems, first, a pH/glucose dual-responsive hydrogel dressing (HPC) is constructed using dual dynamic crosslinking through Schiff base and phenylboronate ester between m-aminophenylboronic acid and adipic dihydrazide bifunctionalized hyaluronic acid (AHP) and oxidized chondroitin sulfate (OCS). Then, polydopamine-reduced graphene oxide compounded glycine-modified fullerene (GPC) with photothermal/photodynamic synergistic antibacterial properties and the drug pirfenidone (PFD) with pro-angiogenesis and suppress inflammatory are loaded into the above HPC hydrogel. Based on the response of Schiff base/phenylboronate ester to pH/glucose, the HPC/GPC/PFD (HPCG/PFD) hydrogel can accelerate the release of PFD, thereby improving excessive inflammation and angiogenesis in DFU. In addition, dual dynamic crosslinking provided the hydrogel with good on-demand removal and self-healing performance, while GPC brought good tissue adhesion, antioxidation, and electrical conductivity to the hydrogel. The rheology, morphology, mechanical properties, swelling, degradation, and biocompatibility of the hydrogel have been well verified. Finally, in the DFU model of rats, this hydrogel can promote wound repair by reducing infection and inflammation, accelerating wound closure, and enhancing epidermal regeneration, collagen deposition, and angiogenesis, showing promoting effect on diabetic wound healing.
{"title":"Photothermal/Photodynamic Synergistic Antibacterial Hydrogel Dressing with pH/Glucose Dual Responsive Pirfenidone Release for Diabetic Foot Ulcers","authors":"Guoying Pan, Meng Li, Lei Mu, Ying Huang, Yongping Liang, Baolin Guo","doi":"10.1002/adfm.202416205","DOIUrl":"https://doi.org/10.1002/adfm.202416205","url":null,"abstract":"Diabetic foot ulcers (DFU) are notoriously challenging to heal due to severe infection, excessive inflammation, and difficulty in angiogenesis. In response to these problems, first, a pH/glucose dual-responsive hydrogel dressing (HPC) is constructed using dual dynamic crosslinking through Schiff base and phenylboronate ester between m-aminophenylboronic acid and adipic dihydrazide bifunctionalized hyaluronic acid (AHP) and oxidized chondroitin sulfate (OCS). Then, polydopamine-reduced graphene oxide compounded glycine-modified fullerene (GPC) with photothermal/photodynamic synergistic antibacterial properties and the drug pirfenidone (PFD) with pro-angiogenesis and suppress inflammatory are loaded into the above HPC hydrogel. Based on the response of Schiff base/phenylboronate ester to pH/glucose, the HPC/GPC/PFD (HPCG/PFD) hydrogel can accelerate the release of PFD, thereby improving excessive inflammation and angiogenesis in DFU. In addition, dual dynamic crosslinking provided the hydrogel with good on-demand removal and self-healing performance, while GPC brought good tissue adhesion, antioxidation, and electrical conductivity to the hydrogel. The rheology, morphology, mechanical properties, swelling, degradation, and biocompatibility of the hydrogel have been well verified. Finally, in the DFU model of rats, this hydrogel can promote wound repair by reducing infection and inflammation, accelerating wound closure, and enhancing epidermal regeneration, collagen deposition, and angiogenesis, showing promoting effect on diabetic wound healing.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"12 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642789","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}
Wangqi Mao, Liang Liu, Chenni Xu, Liu Yang, Ruotian Lin, Xiaoxia Wang, Mingming Jiang, Hongxing Dong, Long Zhang, Anlian Pan
Single‐mode lasers are highly desirable for applications in optical communication, quantum information, and photonic computing, but their realization is challenging due to the competition of multiple closely spaced resonant modes in microcavities. This paper proposes a novel approach, termed mode structure breaking, to achieve high‐performance single‐mode lasing in an individual laser cavity. By introducing selective spatial structure defects, the mode structure of competing modes can be broken, enabling single‐mode selection without huge losses. As proof of concept, femtosecond (fs)‐laser ablation is experimentally employed to introduce external angle defects on a microdisk cavity, effectively eliminating mismatched competing modes and thus achieving single‐mode lasing output. The lasing characteristics are further optimized by incorporating a punched hole to suppress remaining high‐order lasing modes. Notably, the fabricated perovskite laser sources, which are called mode‐structure‐breaking lasers, demonstrate excellent single‐mode lasing properties, including stability, an ultralow threshold (≈2.31 µJ cm−2), and a narrow linewidth (≈0.15 nm). Conclusively, this comprehensive study of manipulating lasing mode by breaking mode structure may provide a promising approach to realizing single‐mode lasing in a single structure, which is significant for producing on‐chip laser source arrays for use in photonic integrated circuits.
{"title":"Single‐Mode Lasing by Selective Mode Structure Breaking","authors":"Wangqi Mao, Liang Liu, Chenni Xu, Liu Yang, Ruotian Lin, Xiaoxia Wang, Mingming Jiang, Hongxing Dong, Long Zhang, Anlian Pan","doi":"10.1002/adfm.202418280","DOIUrl":"https://doi.org/10.1002/adfm.202418280","url":null,"abstract":"Single‐mode lasers are highly desirable for applications in optical communication, quantum information, and photonic computing, but their realization is challenging due to the competition of multiple closely spaced resonant modes in microcavities. This paper proposes a novel approach, termed mode structure breaking, to achieve high‐performance single‐mode lasing in an individual laser cavity. By introducing selective spatial structure defects, the mode structure of competing modes can be broken, enabling single‐mode selection without huge losses. As proof of concept, femtosecond (fs)‐laser ablation is experimentally employed to introduce external angle defects on a microdisk cavity, effectively eliminating mismatched competing modes and thus achieving single‐mode lasing output. The lasing characteristics are further optimized by incorporating a punched hole to suppress remaining high‐order lasing modes. Notably, the fabricated perovskite laser sources, which are called mode‐structure‐breaking lasers, demonstrate excellent single‐mode lasing properties, including stability, an ultralow threshold (≈2.31 µJ cm<jats:sup>−2</jats:sup>), and a narrow linewidth (≈0.15 nm). Conclusively, this comprehensive study of manipulating lasing mode by breaking mode structure may provide a promising approach to realizing single‐mode lasing in a single structure, which is significant for producing on‐chip laser source arrays for use in photonic integrated circuits.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"46 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642837","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}
Binru Han, Shota Fujii, André J. van der Vlies, Masoud Ghasemi, Joshua T. Del Mundo, Sarah N. Kiemle, Esther W. Gomez, Enrique D. Gomez, Ralph H. Colby, Urara Hasegawa
Thermogels that exhibit a sol‐gel transition at body temperature represent a promising class of injectable biomaterials for biomedical applications. Thermogels reported thus far are generally composed of amphiphilic block copolymer micelles with an isotropic thermosensitive surface that induces intermicellar aggregation upon heating. Despite the promise, these hydrogels exhibit low mechanical strengths due to their uncontrollable aggregation resulting in void formation. To gain better control over intermicellar assembly, herein a novel thermogel design concept is presented based on patchy polymeric micelles bearing multiple thermosensitive surface domains. These domains serve as “patches” to bridge the micelles to form a percolated network structure. Patchy micelles are prepared from a binary mixture of amphiphilic block copolymers: Poly(N‐acryloylmorpholine)‐b‐poly(N‐benzylacrylamide) (PAM‐PBzAM) and poly (N‐isopropyl acrylamide)‐b‐poly(N‐benzylacrylamide) (PNIPAM‐PBzAM), where PBzAM, PAM and PNIPAM are the hydrophobic, hydrophilic and thermosensitive blocks, respectively. At 25 °C, the polymers self‐assembled into mixed shell micelles having a phase‐separated shell with PAM‐ and PNIPAM‐rich domains. At 37 °C, the PNIPAM domains undergo a hydrophilic‐to‐hydrophobic transition to induce intermicellar assembly into entangled worm‐like structures resulting in hydrogel formation. Patchy micelles form a homogeneous network structure without voids. The micelle design significantly affects the inter‐micellar assembly, the thermogelling behavior, and the mechanical properties of the hydrogels.
{"title":"Thermally Induced Gelling Systems Based on Patchy Polymeric Micelles","authors":"Binru Han, Shota Fujii, André J. van der Vlies, Masoud Ghasemi, Joshua T. Del Mundo, Sarah N. Kiemle, Esther W. Gomez, Enrique D. Gomez, Ralph H. Colby, Urara Hasegawa","doi":"10.1002/adfm.202417544","DOIUrl":"https://doi.org/10.1002/adfm.202417544","url":null,"abstract":"Thermogels that exhibit a sol‐gel transition at body temperature represent a promising class of injectable biomaterials for biomedical applications. Thermogels reported thus far are generally composed of amphiphilic block copolymer micelles with an isotropic thermosensitive surface that induces intermicellar aggregation upon heating. Despite the promise, these hydrogels exhibit low mechanical strengths due to their uncontrollable aggregation resulting in void formation. To gain better control over intermicellar assembly, herein a novel thermogel design concept is presented based on patchy polymeric micelles bearing multiple thermosensitive surface domains. These domains serve as “patches” to bridge the micelles to form a percolated network structure. Patchy micelles are prepared from a binary mixture of amphiphilic block copolymers: Poly(<jats:italic>N</jats:italic>‐acryloylmorpholine)‐<jats:italic>b</jats:italic>‐poly(<jats:italic>N</jats:italic>‐benzylacrylamide) (PAM‐PBzAM) and poly (<jats:italic>N</jats:italic>‐isopropyl acrylamide)‐<jats:italic>b</jats:italic>‐poly(<jats:italic>N</jats:italic>‐benzylacrylamide) (PNIPAM‐PBzAM), where PBzAM, PAM and PNIPAM are the hydrophobic, hydrophilic and thermosensitive blocks, respectively. At 25 °C, the polymers self‐assembled into mixed shell micelles having a phase‐separated shell with PAM‐ and PNIPAM‐rich domains. At 37 °C, the PNIPAM domains undergo a hydrophilic‐to‐hydrophobic transition to induce intermicellar assembly into entangled worm‐like structures resulting in hydrogel formation. Patchy micelles form a homogeneous network structure without voids. The micelle design significantly affects the inter‐micellar assembly, the thermogelling behavior, and the mechanical properties of the hydrogels.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"6 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642838","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}
Antian Wang, Jialin Huang, Minxiu Ji, YuKun Huang, Lin Chen, Yidong Peng, Chunyi Wang, Kexin shi, Chenyun Zhang, Renhe Yu, Gan Jiang, Xiaodong Sun, Hongzhuan Chen, Qingxiang Song, Xiaoling Gao
Neurotropic factors, crucial for neural cell maturation and proliferation, hold great therapeutic potential for treating neurodegenerative diseases but face challenges in brain delivery. This study introduces a novel membrane budding‐inspired lipoprotein biomimetic nanocarrier for efficient packaging and precise brain delivery of brain‐derived neurotrophic factor (BDNF). The nanocarrier is created by mixing protein‐loaded biomimetic gel with liposomes composed of lipids prone to forming liquid‐disordered and liquid‐ordered phases. This interaction triggers phase separation and lipid membrane rearrangement, enabling effective protein encapsulation. To enhance blood‐brain barrier permeability and target damaged cerebral vasculature in Alzheimer's Disease, the nanocarrier (RAP‐BHP‐rHDL) is functionalized with Apolipoprotein E3 and αRAP peptides. The obtained RAP‐BHP‐rHDL alleviates neuronal damage, promotes neurogenesis, normalizes the cerebral microvasculature, improves the function of neurovascular units, and restores memory function in 5 × FAD mice. This innovative packaging approach and biomimetic nanocarrier design offer a promising strategy for delivering neurotropic factors to the central nervous system, potentially advancing the management of neurodegenerative diseases.
{"title":"Membrane Budding Inspired Biomimetic Nanocarrier Delivers Brain‐derived Neurotrophic Factor to Improve AD Cognition","authors":"Antian Wang, Jialin Huang, Minxiu Ji, YuKun Huang, Lin Chen, Yidong Peng, Chunyi Wang, Kexin shi, Chenyun Zhang, Renhe Yu, Gan Jiang, Xiaodong Sun, Hongzhuan Chen, Qingxiang Song, Xiaoling Gao","doi":"10.1002/adfm.202416572","DOIUrl":"https://doi.org/10.1002/adfm.202416572","url":null,"abstract":"Neurotropic factors, crucial for neural cell maturation and proliferation, hold great therapeutic potential for treating neurodegenerative diseases but face challenges in brain delivery. This study introduces a novel membrane budding‐inspired lipoprotein biomimetic nanocarrier for efficient packaging and precise brain delivery of brain‐derived neurotrophic factor (BDNF). The nanocarrier is created by mixing protein‐loaded biomimetic gel with liposomes composed of lipids prone to forming liquid‐disordered and liquid‐ordered phases. This interaction triggers phase separation and lipid membrane rearrangement, enabling effective protein encapsulation. To enhance blood‐brain barrier permeability and target damaged cerebral vasculature in Alzheimer's Disease, the nanocarrier (RAP‐BHP‐rHDL) is functionalized with Apolipoprotein E3 and αRAP peptides. The obtained RAP‐BHP‐rHDL alleviates neuronal damage, promotes neurogenesis, normalizes the cerebral microvasculature, improves the function of neurovascular units, and restores memory function in 5 × FAD mice. This innovative packaging approach and biomimetic nanocarrier design offer a promising strategy for delivering neurotropic factors to the central nervous system, potentially advancing the management of neurodegenerative diseases.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"75 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642888","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}
Tao Zhong, Tian Xu, Liuting Zhang, Li Wang, Fuying Wu, Xuebin Yu
Exploring high‐performance catalysts for hydrogen storage in magnesium hydride (MgH2) is crucial but still a challenge. Herein, Nb2CTx with controllable surface termination groups is developed as an efficient catalyst and the bifunctional modulation (adsorption energy and work function) of different surface termination groups (F, O, OH, or defects) is explored. First, compared to F and O, the introduction of OH on the surface or the direct removal of functional groups both leads to a significant increase in the adsorption of H by Nb2CTx. Second, compared to the surface bare, OH‐rich Nb2CTx has a lower work function, making it easier for hydrogen to enter Mg/MgH2 from the Nb2CTx surface or escape from the Mg/MgH2 surface into the Nb2CTx, thus facilitating the hydrogen ad/desorption properties of MgH2, i.e., the rate‐determining step (RDS) shifts from penetration to diffusion. The Nb2CTx‐KOH‐catalyzed MgH2 with optimal surface termination groups, therefore exhibits a release of 6.56 wt.% H2 in 5 min at 250 °C, and 6.46 wt.% H2 uptake within 5 min at 150 °C. The dehydrogenation and hydrogen uptake activation energies show 49.5% and 60.1% enhancements over pristine MgH2. In addition, a storage capacity of 5.51 wt.% is maintained after 50 dehydrogenation/hydrogenation cycles.
{"title":"Modulation on Surface Termination Groups to Optimize the Adsorption Energy and Work Function of Nb2CTx for Enhanced Hydrogen Storage in Magnesium Hydride","authors":"Tao Zhong, Tian Xu, Liuting Zhang, Li Wang, Fuying Wu, Xuebin Yu","doi":"10.1002/adfm.202418230","DOIUrl":"https://doi.org/10.1002/adfm.202418230","url":null,"abstract":"Exploring high‐performance catalysts for hydrogen storage in magnesium hydride (MgH<jats:sub>2</jats:sub>) is crucial but still a challenge. Herein, Nb<jats:sub>2</jats:sub>CT<jats:sub>x</jats:sub> with controllable surface termination groups is developed as an efficient catalyst and the bifunctional modulation (adsorption energy and work function) of different surface termination groups (F, O, OH, or defects) is explored. First, compared to F and O, the introduction of OH on the surface or the direct removal of functional groups both leads to a significant increase in the adsorption of H by Nb<jats:sub>2</jats:sub>CT<jats:sub>x</jats:sub>. Second, compared to the surface bare, OH‐rich Nb<jats:sub>2</jats:sub>CT<jats:sub>x</jats:sub> has a lower work function, making it easier for hydrogen to enter Mg/MgH<jats:sub>2</jats:sub> from the Nb<jats:sub>2</jats:sub>CT<jats:sub>x</jats:sub> surface or escape from the Mg/MgH<jats:sub>2</jats:sub> surface into the Nb<jats:sub>2</jats:sub>CT<jats:sub>x</jats:sub>, thus facilitating the hydrogen ad/desorption properties of MgH<jats:sub>2</jats:sub>, i.e., the rate‐determining step (RDS) shifts from penetration to diffusion. The Nb<jats:sub>2</jats:sub>CT<jats:sub>x</jats:sub>‐KOH‐catalyzed MgH<jats:sub>2</jats:sub> with optimal surface termination groups, therefore exhibits a release of 6.56 wt.% H<jats:sub>2</jats:sub> in 5 min at 250 °C, and 6.46 wt.% H<jats:sub>2</jats:sub> uptake within 5 min at 150 °C. The dehydrogenation and hydrogen uptake activation energies show 49.5% and 60.1% enhancements over pristine MgH<jats:sub>2</jats:sub>. In addition, a storage capacity of 5.51 wt.% is maintained after 50 dehydrogenation/hydrogenation cycles.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"39 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642968","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}
The rapid development of new energy industry is leading to the scarcity of lithium (Li) metal. Rational design of adsorbents for efficient separation of Li+ ion from aqueous media is pivotal to solve the recovery of this valuable resource. Current adsorbents generally suffer from the drawbacks in adsorption capacity, kinetics, and selectivity. Herein, a novel and ultra-stable metal–organic framework is designed for Li+ separation. The dense oxygen atoms on the cambered wall of its 1D channel encircle to form angstrom-level tetrahedral ion pockets array, acting as the dominant adsorption sites. This rational distribution of the array avoids the pore blockage caused by the pre-adsorbed ions, thereby accelerating the diffusion of subsequent ions into the interior pore. Meanwhile, this tetrahedral pocket shows distinct electronegativity and strong chelation effect for Li+. Benefiting from these specifics, this adsorbent exhibits a record-breaking adsorption capacity for Li+ (76.1 mg g−1) and short equilibrium time (30 min). Moreover, the selective adsorption of Li+ over Na+, K+, Ca2+, and Mg2+ is achieved due to the matched Li+ ion diameter with the pocket/channel sizes and lower energy barrier for dehydration. Thus, this work proposes a feasible strategy for the construction of novel MOFs for ions adsorption.
{"title":"Constructing Angstrom-Level Ion Pocket Array in 1D Channel Wall for Efficient Lithium Ion Sieving","authors":"Xudong Zhao, Xueyan Zhang, Xinxin Xing, Fenglan Bian, Xinli Gao, Baosheng Liu, Sufang Song, Yuezhong Zhang, Hongliang Huang","doi":"10.1002/adfm.202416628","DOIUrl":"https://doi.org/10.1002/adfm.202416628","url":null,"abstract":"The rapid development of new energy industry is leading to the scarcity of lithium (Li) metal. Rational design of adsorbents for efficient separation of Li<sup>+</sup> ion from aqueous media is pivotal to solve the recovery of this valuable resource. Current adsorbents generally suffer from the drawbacks in adsorption capacity, kinetics, and selectivity. Herein, a novel and ultra-stable metal–organic framework is designed for Li<sup>+</sup> separation. The dense oxygen atoms on the cambered wall of its 1D channel encircle to form angstrom-level tetrahedral ion pockets array, acting as the dominant adsorption sites. This rational distribution of the array avoids the pore blockage caused by the pre-adsorbed ions, thereby accelerating the diffusion of subsequent ions into the interior pore. Meanwhile, this tetrahedral pocket shows distinct electronegativity and strong chelation effect for Li<sup>+</sup>. Benefiting from these specifics, this adsorbent exhibits a record-breaking adsorption capacity for Li<sup>+</sup> (76.1 mg g<sup>−1</sup>) and short equilibrium time (30 min). Moreover, the selective adsorption of Li<sup>+</sup> over Na<sup>+</sup>, K<sup>+</sup>, Ca<sup>2+</sup>, and Mg<sup>2+</sup> is achieved due to the matched Li<sup>+</sup> ion diameter with the pocket/channel sizes and lower energy barrier for dehydration. Thus, this work proposes a feasible strategy for the construction of novel MOFs for ions adsorption.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"21 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642791","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}
Kun Cheng, Shaobin Li, Qingyu Cheng, Li Zhang, Yufeng Jiang, Fengbo Li, Huiyuan Ma, Deqing Zhang
The underutilization of active sites limits the performance enhancement of 2D transition metal boride (MBene) in electrocatalytic nitrogen reduction reaction (NRR). Herein, a highly efficient NRR electrocatalyst with S atoms bridging Fe and Mo atoms on the surface of MBene is successfully constructed by using an active site electron optimization strategy, which increases the charge density around the Mo active site and enhances the activation ability of the catalyst to N2 molecules. It is noteworthy that FeS2-MBene demonstrates a low intrinsic potential for NRR (−0.2 V vs RHE). It is more favorable for the adsorption of nitrogen atoms in comparison to hydrogen atoms, thereby it can effectively inhibit the hydrogen evolution reaction (HER). Under a potential of −0.2 V versus RHE, the ammonia yield rate is 37.13 ± 1.31 µg h−1 mg−1, and the FE is 55.97 ± 2.63%. Density functional theory (DFT) calculations demonstrate that Mo on the surface of MBene serves as a site for the adsorption of N2. The formation of the heterostructure enhances electron transfer, resulting in the Mo active site becoming an electron-rich state in favor of subsequent hydrogenation steps. This work offers significant insights into the design and utilization of 2D MBene-based catalysts in NRR.
活性位点利用不足限制了二维过渡金属硼化物（MBene）在电催化氮还原反应（NRR）中的性能提升。本文通过活性位点电子优化策略，成功构建了一种高效的氮还原电催化剂，其S原子桥接了MBene表面的Fe和Mo原子，增加了Mo活性位点周围的电荷密度，增强了催化剂对N2分子的活化能力。值得注意的是，FeS2-MBene 显示出较低的 NRR 本征电位（-0.2 V vs RHE）。与氢原子相比，它更有利于吸附氮原子，因此能有效抑制氢进化反应（HER）。在相对于 RHE 的 -0.2 V 电位下，氨的产率为 37.13 ± 1.31 µg h-1 mg-1，FE 为 55.97 ± 2.63%。密度泛函理论（DFT）计算表明，MBene 表面的 Mo 是 N2 的吸附位点。异质结构的形成增强了电子传递，导致钼活性位点成为富电子状态，有利于后续的氢化步骤。这项研究为在非还原反应中设计和利用二维 MBene 催化剂提供了重要启示。
{"title":"The Electron-Rich Interface Regulated MBene by S-Bridge Guided to Enhance Nitrogen Fixation under Environmental Conditions","authors":"Kun Cheng, Shaobin Li, Qingyu Cheng, Li Zhang, Yufeng Jiang, Fengbo Li, Huiyuan Ma, Deqing Zhang","doi":"10.1002/adfm.202417914","DOIUrl":"https://doi.org/10.1002/adfm.202417914","url":null,"abstract":"The underutilization of active sites limits the performance enhancement of 2D transition metal boride (MBene) in electrocatalytic nitrogen reduction reaction (NRR). Herein, a highly efficient NRR electrocatalyst with S atoms bridging Fe and Mo atoms on the surface of MBene is successfully constructed by using an active site electron optimization strategy, which increases the charge density around the Mo active site and enhances the activation ability of the catalyst to N<sub>2</sub> molecules. It is noteworthy that FeS<sub>2</sub>-MBene demonstrates a low intrinsic potential for NRR (−0.2 V vs RHE). It is more favorable for the adsorption of nitrogen atoms in comparison to hydrogen atoms, thereby it can effectively inhibit the hydrogen evolution reaction (HER). Under a potential of −0.2 V versus RHE, the ammonia yield rate is 37.13 ± 1.31 µg h<sup>−1</sup> mg<sup>−1</sup>, and the FE is 55.97 ± 2.63%. Density functional theory (DFT) calculations demonstrate that Mo on the surface of MBene serves as a site for the adsorption of N<sub>2</sub>. The formation of the heterostructure enhances electron transfer, resulting in the Mo active site becoming an electron-rich state in favor of subsequent hydrogenation steps. This work offers significant insights into the design and utilization of 2D MBene-based catalysts in NRR.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"36 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637076","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}
Flexible visual sensors hold great potential for application in wearable electronics and health monitoring. However, the separate acquisition of various visual signals without mutual interference and their functional integration in internal biomedical devices remains a significant challenge. Here, a functional material that integrates mechanoluminescent units with biosensing units through supramolecular interactions, enabling bimodal non-interfering visual detection of orthodontic force and bacterial infection is presented. The orthodontic force induces fluorescence by facilitating the release of electrons from trapped energy levels, caused by the disruption or rearrangement of defect structures within strontium aluminate crystals. Meanwhile, the seamlessly integrated biosensing component can effectively detect lactic acid in a dose-dependent manner, underscoring its multifunctional capabilities in biosensing applications. Moreover, the development of a cloud-based deep learning server can achieve a 97.7% accuracy in the precise decoupling of visual signals, facilitating remote monitoring and enabling early intervention during orthodontic treatment. The proposed artificial intelligence-enhanced bimodal visual sensors represent a new paradigm for orthodontic monitoring, suitable for a wide range of biomedical applications.
{"title":"Bimodal Visual Sensors Based on Mechanoluminescence and Biosensing for Artificial Intelligence-Assisted Orthodontics","authors":"Hao Feng, Yuesong Lv, Xin Yang, Jian Wang, Xinxing Zhang, Xibo Pei","doi":"10.1002/adfm.202416437","DOIUrl":"https://doi.org/10.1002/adfm.202416437","url":null,"abstract":"Flexible visual sensors hold great potential for application in wearable electronics and health monitoring. However, the separate acquisition of various visual signals without mutual interference and their functional integration in internal biomedical devices remains a significant challenge. Here, a functional material that integrates mechanoluminescent units with biosensing units through supramolecular interactions, enabling bimodal non-interfering visual detection of orthodontic force and bacterial infection is presented. The orthodontic force induces fluorescence by facilitating the release of electrons from trapped energy levels, caused by the disruption or rearrangement of defect structures within strontium aluminate crystals. Meanwhile, the seamlessly integrated biosensing component can effectively detect lactic acid in a dose-dependent manner, underscoring its multifunctional capabilities in biosensing applications. Moreover, the development of a cloud-based deep learning server can achieve a 97.7% accuracy in the precise decoupling of visual signals, facilitating remote monitoring and enabling early intervention during orthodontic treatment. The proposed artificial intelligence-enhanced bimodal visual sensors represent a new paradigm for orthodontic monitoring, suitable for a wide range of biomedical applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"575 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637077","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}
Qing An, Dawei Li, Wenhe Liao, Tingting Liu, Zhi Qu, Gang Wang, Xiangjia Li
3D metastructure absorbers have gained attention for their lightweight, load-bearing capabilities, and superior electromagnetic wave absorption. However, the complex interplay between unit cell geometry, material properties, and electromagnetic response is not well understood, hindering the design of high-performance devices. A multi-scale model, validated is presented by simulations and experiments, that clarify the relationship between materials, structures, and electromagnetic behavior in 3D metastructures. By systematically investigating strut-based and sheet-based structures, volume fraction, unit size, crystal lattice orientation, and density gradient within TPMS-based unit cells, it is revealed that unit geometry significantly influences electromagnetic field propagation and reflection loss. Specifically, under the same unit size, sheet-based TPMS metastructures exhibit stronger reflectivity than strut-based ones, while multilayer structures show the opposite trend. The direct correlation is also further confirmed between geometric symmetry and polarization insensitivity, with orthogonal isotropic superstructures displaying excellent polarization-insensitive properties. This finding provides a new design principle for achieving robust, angle-independent absorption in these materials. This work enhances understanding of the structure-electromagnetic behavior interplay, guiding the design of next-generation broadband, wide-angle, and polarization-insensitive devices.
{"title":"Electromagnetic Absorption Mechanism of TPMS-Based Metastructures: Synergy Between Materials and Structures","authors":"Qing An, Dawei Li, Wenhe Liao, Tingting Liu, Zhi Qu, Gang Wang, Xiangjia Li","doi":"10.1002/adfm.202414629","DOIUrl":"https://doi.org/10.1002/adfm.202414629","url":null,"abstract":"3D metastructure absorbers have gained attention for their lightweight, load-bearing capabilities, and superior electromagnetic wave absorption. However, the complex interplay between unit cell geometry, material properties, and electromagnetic response is not well understood, hindering the design of high-performance devices. A multi-scale model, validated is presented by simulations and experiments, that clarify the relationship between materials, structures, and electromagnetic behavior in 3D metastructures. By systematically investigating strut-based and sheet-based structures, volume fraction, unit size, crystal lattice orientation, and density gradient within TPMS-based unit cells, it is revealed that unit geometry significantly influences electromagnetic field propagation and reflection loss. Specifically, under the same unit size, sheet-based TPMS metastructures exhibit stronger reflectivity than strut-based ones, while multilayer structures show the opposite trend. The direct correlation is also further confirmed between geometric symmetry and polarization insensitivity, with orthogonal isotropic superstructures displaying excellent polarization-insensitive properties. This finding provides a new design principle for achieving robust, angle-independent absorption in these materials. This work enhances understanding of the structure-electromagnetic behavior interplay, guiding the design of next-generation broadband, wide-angle, and polarization-insensitive devices.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"62 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637075","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}
Steven C. Gauci, Paul Somers, Mohammed Aljuaid, Martin Wegener, Christopher Barner-Kowollik, Hannes A. Houck
Classical photoresists utilized in direct laser writing (DLW) rely on photoinitiators and radical polymerization mechanisms to induce the cross-linking process. Herein, a simple initiator-free photoresist is introduced that enables the rapid fabrication of intrinsically thermally degradable 3D microstructures via DLW. The reported photoresist exploits the [2 + 2] photo-dimerization reaction of a multifunctional monosubstituted thiomaleimide compound while harvesting on-demand microstructure degradation through the intrinsic thermally reversible nature of the photocrosslinks. The photoresist exceeds attainable DLW printing speeds for non-chain growth resins, readily attaining 1500 µm s−1 and up to 5000 µm s−1, making it a promising system to compete with traditional photo-initiator containing resists while introducing on-demand post-printing degradability.
{"title":"Intrinsically Thermally Degradable Microstructures Fabricated by Photodimerization in Rapid 3D Laser Printing","authors":"Steven C. Gauci, Paul Somers, Mohammed Aljuaid, Martin Wegener, Christopher Barner-Kowollik, Hannes A. Houck","doi":"10.1002/adfm.202414713","DOIUrl":"https://doi.org/10.1002/adfm.202414713","url":null,"abstract":"Classical photoresists utilized in direct laser writing (DLW) rely on photoinitiators and radical polymerization mechanisms to induce the cross-linking process. Herein, a simple initiator-free photoresist is introduced that enables the rapid fabrication of intrinsically thermally degradable 3D microstructures via DLW. The reported photoresist exploits the [2 + 2] photo-dimerization reaction of a multifunctional monosubstituted thiomaleimide compound while harvesting on-demand microstructure degradation through the intrinsic thermally reversible nature of the photocrosslinks. The photoresist exceeds attainable DLW printing speeds for non-chain growth resins, readily attaining 1500 µm s<sup>−1</sup> and up to 5000 µm s<sup>−1</sup>, making it a promising system to compete with traditional photo-initiator containing resists while introducing on-demand post-printing degradability.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"13 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637080","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}
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