Migon Choi, Nelson Rivera, Steven P. Harvey, Chuanzhen Zhou, Sameera Pathiranage, Yadong Zhang, Stephen Barlow, Seth R. Marder, David B. Mitzi
Mixed tin–lead halide perovskites are emerging as promising candidates to address the toxicity issues of lead-based perovskites and to provide additional bandgap tunability for optoelectronic applications. Electron-transfer doping offers a prospective pathway to modulate electronic properties of metal-halide perovskites, while not disturbing the underlying crystal structure. However, limited research exists comparing molecular dopants for these systems. Our study investigates the p-type electron-transfer doping of the mixed tin–lead halide perovskite MAPb0.5Sn0.5I3 (MA = methylammonium) using a sequential deposition approach (perovskite film followed by dopant incorporation) and the molecular dopants F4TCNQ and Mo(tfd-COCF3)3. Up to 3 orders of magnitude higher carrier density and up to 2 orders of magnitude greater conductivity are achieved relative to the undoped samples, with F4TCNQ and Mo(tfd-COCF3)3 demonstrating similar doping efficiencies (associated with the ratio of mobile charges added to the number of dopant molecules incorporated) of 0.031(3) % and 0.024(3) %, respectively. Differences in the doping effectiveness for a given molarity doping solution likely follow from variations in dopant incorporation within the film during the spin coating deposition step.
{"title":"P-Type Doping of Mixed Tin–Lead Halide Perovskites Using Electron Transfer to Mo(tfd-COCF3)3 and F4TCNQ","authors":"Migon Choi, Nelson Rivera, Steven P. Harvey, Chuanzhen Zhou, Sameera Pathiranage, Yadong Zhang, Stephen Barlow, Seth R. Marder, David B. Mitzi","doi":"10.1021/acsami.5c19800","DOIUrl":"https://doi.org/10.1021/acsami.5c19800","url":null,"abstract":"Mixed tin–lead halide perovskites are emerging as promising candidates to address the toxicity issues of lead-based perovskites and to provide additional bandgap tunability for optoelectronic applications. Electron-transfer doping offers a prospective pathway to modulate electronic properties of metal-halide perovskites, while not disturbing the underlying crystal structure. However, limited research exists comparing molecular dopants for these systems. Our study investigates the p-type electron-transfer doping of the mixed tin–lead halide perovskite MAPb<sub>0.5</sub>Sn<sub>0.5</sub>I<sub>3</sub> (MA = methylammonium) using a sequential deposition approach (perovskite film followed by dopant incorporation) and the molecular dopants F<sub>4</sub>TCNQ and Mo(tfd-COCF<sub>3</sub>)<sub>3</sub>. Up to 3 orders of magnitude higher carrier density and up to 2 orders of magnitude greater conductivity are achieved relative to the undoped samples, with F<sub>4</sub>TCNQ and Mo(tfd-COCF<sub>3</sub>)<sub>3</sub> demonstrating similar doping efficiencies (associated with the ratio of mobile charges added to the number of dopant molecules incorporated) of 0.031(3) % and 0.024(3) %, respectively. Differences in the doping effectiveness for a given molarity doping solution likely follow from variations in dopant incorporation within the film during the spin coating deposition step.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"14 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718223","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}
Light-curing adhesives (LCAs) play an indispensable role in the field of electronic packaging due to their rapid polymerization response under illumination. However, conventional LCAs typically lack detachability and self-healing capability and often encounter challenges related to closed-loop recyclability and bonding strength adjustability. Herein, a self-photosensitive atoxic prepolymer is developed by the simple esterification of natural lipoic acid (TA) with polycaprolactone diol (PCL), enabling complete light-curing within 2 min without additional photoinitiators. The disulfide bond in the prepolymer can endow the green adhesives with detachability (heating at 120 °C for 16 s), dual-stimuli-responsive self-repairing properties (UV radiation for 10 min or heating at 60 °C for 3 h), and efficient closed-loop recycling performance. Moreover, the crystallization behavior of PCL contributes to the versatile adhesives with controllable bonding strength after photocuring, along with a maximum adhesion strength of 5.1 MPa (cured adhesive for 20 min of crystallization). This novel strategy grants the LCA versatility, which opens up an original way for designing electronic packaging adhesives with higher practical value.
{"title":"Detachable, Self-Repairing, and Closed-Loop Recyclable Self-Initiated Light-Curing Adhesives with Controllable Bonding Strength","authors":"Zhao Liu, Xiaoming Ren, Hua Zheng, Junjian Xie, Qiuyu Zhang","doi":"10.1021/acsami.5c20306","DOIUrl":"https://doi.org/10.1021/acsami.5c20306","url":null,"abstract":"Light-curing adhesives (LCAs) play an indispensable role in the field of electronic packaging due to their rapid polymerization response under illumination. However, conventional LCAs typically lack detachability and self-healing capability and often encounter challenges related to closed-loop recyclability and bonding strength adjustability. Herein, a self-photosensitive atoxic prepolymer is developed by the simple esterification of natural lipoic acid (TA) with polycaprolactone diol (PCL), enabling complete light-curing within 2 min without additional photoinitiators. The disulfide bond in the prepolymer can endow the green adhesives with detachability (heating at 120 °C for 16 s), dual-stimuli-responsive self-repairing properties (UV radiation for 10 min or heating at 60 °C for 3 h), and efficient closed-loop recycling performance. Moreover, the crystallization behavior of PCL contributes to the versatile adhesives with controllable bonding strength after photocuring, along with a maximum adhesion strength of 5.1 MPa (cured adhesive for 20 min of crystallization). This novel strategy grants the LCA versatility, which opens up an original way for designing electronic packaging adhesives with higher practical value.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"9 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718225","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}
Covalently grafted liquid-like polymer brushes are central to liquid-repellent coatings but remain extremely difficult to regenerate once abraded. Here, we present a supramolecular strategy to overcome this limitation by constructing a highly dense hydrogen-bonded matrix capable of repeated brush grafting. The matrix was formed by 2-ureido-4[1H]-pyrimidinone (UPy) functionalized polyhedral oligomeric silsesquioxane (POSS), which established a rigid yet dynamic network. Poly(dimethylsiloxane) with polar terminal groups (BHPDMS) was subsequently inserted via hydrogen bonding and dipole interactions at elevated temperatures, creating a covalent-analogous polymer brush coating that resists fluid erosion while preserving dynamically reconfigurable. This coating exhibits hardness of 0.34 GPa, modulus of 5.91 GPa, and >90% optical transparency. Its liquid-repellent performance includes water sliding angle of 1.8°, together with antismudge and antigraffiti functionality. Moreover, the coating reduces ice adhesion to 20.4 kPa and extends freezing delay more than 10-fold relative to glass. Importantly, once abraded, BHPDMS can be repeatedly reinserted into the dense UPy-POSS framework at elevated temperatures, enabling full restoration of liquid-repellent functionality. This work establishes a supramolecular design principle that reconciles covalent-analogous stability with regraftable adaptability, opening new directions for durable and sustainable surface engineering.
{"title":"Dynamic Graftable Liquid-Like Polymer Brush Coatings with Restorable Liquid Repellency","authors":"Shidong Zhao, Bo Peng, Shuxue Zhou","doi":"10.1021/acsami.5c22242","DOIUrl":"https://doi.org/10.1021/acsami.5c22242","url":null,"abstract":"Covalently grafted liquid-like polymer brushes are central to liquid-repellent coatings but remain extremely difficult to regenerate once abraded. Here, we present a supramolecular strategy to overcome this limitation by constructing a highly dense hydrogen-bonded matrix capable of repeated brush grafting. The matrix was formed by 2-ureido-4[1H]-pyrimidinone (UPy) functionalized polyhedral oligomeric silsesquioxane (POSS), which established a rigid yet dynamic network. Poly(dimethylsiloxane) with polar terminal groups (BHPDMS) was subsequently inserted via hydrogen bonding and dipole interactions at elevated temperatures, creating a covalent-analogous polymer brush coating that resists fluid erosion while preserving dynamically reconfigurable. This coating exhibits hardness of 0.34 GPa, modulus of 5.91 GPa, and >90% optical transparency. Its liquid-repellent performance includes water sliding angle of 1.8°, together with antismudge and antigraffiti functionality. Moreover, the coating reduces ice adhesion to 20.4 kPa and extends freezing delay more than 10-fold relative to glass. Importantly, once abraded, BHPDMS can be repeatedly reinserted into the dense UPy-POSS framework at elevated temperatures, enabling full restoration of liquid-repellent functionality. This work establishes a supramolecular design principle that reconciles covalent-analogous stability with regraftable adaptability, opening new directions for durable and sustainable surface engineering.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"8 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718226","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}
Shuyan Zhao,Boyan Zhao,Yong Wang,Yanrong Li,Essy Kouadio Fodjo,Wei Deng,Dan Li
Gold nanostructures (GNSs) have tunable optical absorption and catalytic properties and thus are increasingly used in molecular sensing and nanomanufacturing. However, the rapid design of GNSs with specific optical properties is limited by various factors, making it difficult to achieve efficient design by conventional trial-and-error methods. Here, we report a SHapley Additive exPlanations (SHAP)-assisted extreme gradient boosting (XG-Boost) model for conducting the preparation of GNSs with preferential plasmonic features using silver nitrate (AgNO3) and ascorbic acid in different surfactants at room temperature. The XG-Boost model achieves exceptional predictive accuracy (R2 > 0.98, RMSE < 0.03). Importantly, SHAP elucidates the underlying mechanism linking synthetic conditions to plasmonic properties of GNSs, particularly revealing the contribution of surfactants to predictions, which was previously underestimated. Guided by the XG-Boost-SHAP strategy, GNSs with tunable localized surface plasmon resonance peaks and high stability are designed and precisely synthesized in various shapes. The GNSs were successfully applied to thiourea detection, Hg2+ recognition, glucose analysis, and fabrication of luminescent chips. The results demonstrate the remarkable potential of the machine-learning framework in tailoring GNSs with personalized features to realize various objectives.
{"title":"Utilizing a SHAP-Assisted Machine Learning Algorithm for Optimization of Plasmonic Properties of Gold Nanostructure.","authors":"Shuyan Zhao,Boyan Zhao,Yong Wang,Yanrong Li,Essy Kouadio Fodjo,Wei Deng,Dan Li","doi":"10.1021/acsami.5c18616","DOIUrl":"https://doi.org/10.1021/acsami.5c18616","url":null,"abstract":"Gold nanostructures (GNSs) have tunable optical absorption and catalytic properties and thus are increasingly used in molecular sensing and nanomanufacturing. However, the rapid design of GNSs with specific optical properties is limited by various factors, making it difficult to achieve efficient design by conventional trial-and-error methods. Here, we report a SHapley Additive exPlanations (SHAP)-assisted extreme gradient boosting (XG-Boost) model for conducting the preparation of GNSs with preferential plasmonic features using silver nitrate (AgNO3) and ascorbic acid in different surfactants at room temperature. The XG-Boost model achieves exceptional predictive accuracy (R2 > 0.98, RMSE < 0.03). Importantly, SHAP elucidates the underlying mechanism linking synthetic conditions to plasmonic properties of GNSs, particularly revealing the contribution of surfactants to predictions, which was previously underestimated. Guided by the XG-Boost-SHAP strategy, GNSs with tunable localized surface plasmon resonance peaks and high stability are designed and precisely synthesized in various shapes. The GNSs were successfully applied to thiourea detection, Hg2+ recognition, glucose analysis, and fabrication of luminescent chips. The results demonstrate the remarkable potential of the machine-learning framework in tailoring GNSs with personalized features to realize various objectives.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"1 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145711047","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}
Li6.4La3Zr1.4Ta0.6O12 (LLZTO)-based solid-state lithium metal batteries (SSLMBs) are regarded as promising candidates for next-generation energy storage, owing to their nonflammability and high energy density. Nevertheless, practical application is hindered by poor interfacial contact and structural degradation at the Li/LLZTO interface during stripping processes, which induces lithium dendrite growth and battery failure. In this study, a ternary Li-Ag-Zn alloy anode (LAZ10) is in-situ constructed by introducing 10% Ag and Zn into molten lithium, which markedly improves interfacial adhesion and facilitates Li+ transport. As a result, LAZ10/LLZTO/LAZ10 symmetric cells demonstrate ultralow interfacial resistance of 4 Ω·cm2, high critical current density (CCD) of 1.6 mA cm-2, and long cycle life of 2800 h at 0.3 mA cm-2. Furthermore, full cells LAZ10/LLZTO/LiFePO4 exhibit outstanding electrochemical performance. This work provides an effective interfacial design strategy for developing high-performance, dendrite-free SSLMBs.
基于Li6.4La3Zr1.4Ta0.6O12 （LLZTO）的固态锂金属电池（sslmb）由于其不可燃性和高能量密度而被认为是下一代储能的有希望的候选者。然而，在剥离过程中，由于Li/LLZTO界面接触不良和结构退化，导致锂枝晶生长和电池失效，阻碍了实际应用。本研究通过在熔融锂中引入10%的Ag和Zn，原位构建了Li-Ag-Zn三元合金阳极（LAZ10），显著提高了界面附着力，有利于Li+的输运。结果表明，LAZ10/LLZTO/LAZ10对称电池具有4 Ω·cm2的超低界面电阻、1.6 mA cm-2的高临界电流密度（CCD）和在0.3 mA cm-2下2800 h的长循环寿命。此外，充满电池LAZ10/LLZTO/LiFePO4表现出优异的电化学性能。这项工作为开发高性能、无枝晶的sslmb提供了一种有效的接口设计策略。
{"title":"Interfacial Engineering of a Lithiophilic Li-Ag-Zn Ternary Alloy Anode for Long-Life Garnet-Based Solid-State Batteries.","authors":"Pingmei Li,Yibo Liu,ShiYu Yu,Mingxin Zhang,Yaqing Wei,Daming Chen,De Li,Liang Yang,Yong Chen","doi":"10.1021/acsami.5c18349","DOIUrl":"https://doi.org/10.1021/acsami.5c18349","url":null,"abstract":"Li6.4La3Zr1.4Ta0.6O12 (LLZTO)-based solid-state lithium metal batteries (SSLMBs) are regarded as promising candidates for next-generation energy storage, owing to their nonflammability and high energy density. Nevertheless, practical application is hindered by poor interfacial contact and structural degradation at the Li/LLZTO interface during stripping processes, which induces lithium dendrite growth and battery failure. In this study, a ternary Li-Ag-Zn alloy anode (LAZ10) is in-situ constructed by introducing 10% Ag and Zn into molten lithium, which markedly improves interfacial adhesion and facilitates Li+ transport. As a result, LAZ10/LLZTO/LAZ10 symmetric cells demonstrate ultralow interfacial resistance of 4 Ω·cm2, high critical current density (CCD) of 1.6 mA cm-2, and long cycle life of 2800 h at 0.3 mA cm-2. Furthermore, full cells LAZ10/LLZTO/LiFePO4 exhibit outstanding electrochemical performance. This work provides an effective interfacial design strategy for developing high-performance, dendrite-free SSLMBs.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"26 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145711048","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}
Nickel oxide (NiOx) serves as the preferred hole transporting layer (HTL) for inverted perovskite solar cells (PSCs) due to its good chemical stability and facile solution processability. However, the uncompetitive device performance of PSCs using the pristine NiOx layer has been limited by its intrinsic defect stacking and poor interface contact. Herein, we propose a cooperative interfacial modification strategy to tailor the electronic properties of NiOx by introducing the self-assembled molecule (SAM) interlayer with PABr modification. The SAM molecule can effectively passivate the oxygen vacancies on the surface and regulate the energy level of NiOx by forming an interfacial dipole. In addition, the PABr molecule can further optimize the molecular arrangement of the SAMs and modify the surface wetting of HTLs. The high-quality perovskite film with improved grain sizes and reduced defect density was achieved on the modified NiOx layer, facilitating enhanced charge transport and significantly alleviated nonradiative recombination loss within devices. Consequently, the target device achieved an improved efficiency of 25.13%, outperforming 23.28% of the NiOx. In addition, the 107.0 cm2 flexible solar modules achieve an impressive efficiency of 16.24%, illustrating the feasibility of the proposed molecular modification for scalable fabrication. Our work underscores the importance of interfacial tailoring on the buried interface to boost the efficiency and stability of PSCs.
{"title":"Synergistic Molecular Modification of NiOx for High-Performance Inverted Perovskite Solar Cells","authors":"Hui Wang, Xiaochun Zhang, Tianqi Niu, Likun Wang, Xin Yue, Zhenghui Wan, Xiao Jiang, Weidong Zhu, Kai Wang, Shengzhong Liu, Chunfu Zhang","doi":"10.1021/acsami.5c17339","DOIUrl":"https://doi.org/10.1021/acsami.5c17339","url":null,"abstract":"Nickel oxide (NiO<sub><i>x</i></sub>) serves as the preferred hole transporting layer (HTL) for inverted perovskite solar cells (PSCs) due to its good chemical stability and facile solution processability. However, the uncompetitive device performance of PSCs using the pristine NiO<sub><i>x</i></sub> layer has been limited by its intrinsic defect stacking and poor interface contact. Herein, we propose a cooperative interfacial modification strategy to tailor the electronic properties of NiO<sub><i>x</i></sub> by introducing the self-assembled molecule (SAM) interlayer with PABr modification. The SAM molecule can effectively passivate the oxygen vacancies on the surface and regulate the energy level of NiO<sub><i>x</i></sub> by forming an interfacial dipole. In addition, the PABr molecule can further optimize the molecular arrangement of the SAMs and modify the surface wetting of HTLs. The high-quality perovskite film with improved grain sizes and reduced defect density was achieved on the modified NiO<sub><i>x</i></sub> layer, facilitating enhanced charge transport and significantly alleviated nonradiative recombination loss within devices. Consequently, the target device achieved an improved efficiency of 25.13%, outperforming 23.28% of the NiO<sub><i>x</i></sub>. In addition, the 107.0 cm<sup>2</sup> flexible solar modules achieve an impressive efficiency of 16.24%, illustrating the feasibility of the proposed molecular modification for scalable fabrication. Our work underscores the importance of interfacial tailoring on the buried interface to boost the efficiency and stability of PSCs.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"32 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718224","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}
Gel-type hemostatic agents possess irreplaceable advantages over other material forms in managing irregular wounds and deep tissue bleeding. However, their clinical application remains limited in treating lethal massive hemorrhage due to inadequate fluid absorption, swelling-induced detachment, and insufficient procoagulant activity. This study developed a coagulation-mediated self-gelling microparticle powder composed of Yam mucilage and halloysite nanoclay (HNTs) for robust wet tissue adhesion and rapid massive hemorrhage control. The microparticles in ∼20 μm spontaneously form through physical interactions (hydrogen bonding, van der Waals forces, and surface encapsulation effects) between the HNTs and Yam mucilage, which exhibit excellent rehydration capacity and achieve autonomous gelation via the procoagulant properties of the HNTs. Yam@HNT microparticle-treated blood induced immediate hydrogel layer formation at the blood-material interface within 1 min, followed by complete blood coagulation within 2 min, which represented a 7.5-fold acceleration compared to that of raw blood. In vitro hemostasis/adhesion tests and rat models of liver/arterial massive hemorrhage confirmed its excellent hemostatic performance, strong tissue adhesion, and biocompatibility. The Yam@HNT microparticles accelerate clotting through an intrinsic coagulation pathway activation, platelet aggregation, and hemorheological modulation. This natural plant-derived mucilage and biocompatible clay composite microparticles achieve in situ fluid absorption, coagulation-triggered self-gelling, and durable adhesion, which provides an effective treatment strategy for emergency hemostasis of complex wounds.
{"title":"Nanoclay-Triggered In Situ Self-Gelling Yam Microparticles via Coagulation Activation for Robust Wet Tissue Adhesion and Instant Hemostasis.","authors":"Bing Xu,Yijin Wu,Di Liu,Yaxin Geng,Xiaohui Li,Guochao Liao,Xiang Luo,Di Deng,Kun Liu,Xiaoxiao Qi,Ying Wang,Qingguo Li,Chuanxi Wang,Rong Zhang,Mingxian Liu,Yue Feng,Zhongqiu Liu","doi":"10.1021/acsami.5c18393","DOIUrl":"https://doi.org/10.1021/acsami.5c18393","url":null,"abstract":"Gel-type hemostatic agents possess irreplaceable advantages over other material forms in managing irregular wounds and deep tissue bleeding. However, their clinical application remains limited in treating lethal massive hemorrhage due to inadequate fluid absorption, swelling-induced detachment, and insufficient procoagulant activity. This study developed a coagulation-mediated self-gelling microparticle powder composed of Yam mucilage and halloysite nanoclay (HNTs) for robust wet tissue adhesion and rapid massive hemorrhage control. The microparticles in ∼20 μm spontaneously form through physical interactions (hydrogen bonding, van der Waals forces, and surface encapsulation effects) between the HNTs and Yam mucilage, which exhibit excellent rehydration capacity and achieve autonomous gelation via the procoagulant properties of the HNTs. Yam@HNT microparticle-treated blood induced immediate hydrogel layer formation at the blood-material interface within 1 min, followed by complete blood coagulation within 2 min, which represented a 7.5-fold acceleration compared to that of raw blood. In vitro hemostasis/adhesion tests and rat models of liver/arterial massive hemorrhage confirmed its excellent hemostatic performance, strong tissue adhesion, and biocompatibility. The Yam@HNT microparticles accelerate clotting through an intrinsic coagulation pathway activation, platelet aggregation, and hemorheological modulation. This natural plant-derived mucilage and biocompatible clay composite microparticles achieve in situ fluid absorption, coagulation-triggered self-gelling, and durable adhesion, which provides an effective treatment strategy for emergency hemostasis of complex wounds.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"395 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145711077","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}
Nicolas H. Voelcker*, , , Giuseppe Barillaro, , , Lluis F. Marsal, , and , Jan M. Macak,
{"title":"Advances in Porous Semiconductor Science and Technology","authors":"Nicolas H. Voelcker*, , , Giuseppe Barillaro, , , Lluis F. Marsal, , and , Jan M. Macak, ","doi":"10.1021/acsami.5c22792","DOIUrl":"https://doi.org/10.1021/acsami.5c22792","url":null,"abstract":"","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"17 49","pages":"66067–66068"},"PeriodicalIF":8.2,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145705188","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}
Chandan Kumar Panda,Shabbir Madad Naqvi,Hong Gu Lee,Tufail Hassan,Aamir Iqbal,Young Su Choi,Kwang-Yong Choi,Chong Min Koo,Jungseek Hwang
Micrometer-thick freestanding MXene films offer a rare opportunity to probe intrinsic bulk optical and electronic properties without the influence of a substrate. Yet, quantitative optical constants over a broadband spectral range remain elusive due to the mechanically flexible nature of such films. Here, we report the first comprehensive far-infrared-to-ultraviolet (150-36,000 cm-1) optical spectroscopic study of freestanding Ti3C2Tx MXene films with thicknesses of 1 and 4 μm. By a combination of attaching the freestanding films on flat and smooth brass plates and using an in situ metal-evaporation method, we obtained highly reliable reflectance spectra. Kramers-Kronig analysis, coupled with a two-Drude-Lorentz model, reveals multiple free-carrier populations at the Fermi level, yielding carrier densities of 7.31 × 1021 and 7.50 × 1021 cm-3 and mobilities of 8.15 and 4.98 cm2 V-1 s-1 for the 1- and 4-μm-thick freestanding films, respectively. The spectra further identify a 1.61 eV feature arising from interband-plasmon coupling and a 3.84 eV interband transition, with small thickness dependence, highlighting the bulk-dominated plasmonic response in micrometer-scale films. This work establishes a quantitative, noncontact framework for mapping intrinsic charge dynamics in MXenes, unlocking pathways for their integration into broadband plasmonic, optoelectronic, infrared, and THz devices.
{"title":"Quantitative Broadband Optical Spectroscopy of Freestanding Ti3C2Tx MXene Films: Unveiling Intrinsic Bulk Charge Carrier Dynamics.","authors":"Chandan Kumar Panda,Shabbir Madad Naqvi,Hong Gu Lee,Tufail Hassan,Aamir Iqbal,Young Su Choi,Kwang-Yong Choi,Chong Min Koo,Jungseek Hwang","doi":"10.1021/acsami.5c17297","DOIUrl":"https://doi.org/10.1021/acsami.5c17297","url":null,"abstract":"Micrometer-thick freestanding MXene films offer a rare opportunity to probe intrinsic bulk optical and electronic properties without the influence of a substrate. Yet, quantitative optical constants over a broadband spectral range remain elusive due to the mechanically flexible nature of such films. Here, we report the first comprehensive far-infrared-to-ultraviolet (150-36,000 cm-1) optical spectroscopic study of freestanding Ti3C2Tx MXene films with thicknesses of 1 and 4 μm. By a combination of attaching the freestanding films on flat and smooth brass plates and using an in situ metal-evaporation method, we obtained highly reliable reflectance spectra. Kramers-Kronig analysis, coupled with a two-Drude-Lorentz model, reveals multiple free-carrier populations at the Fermi level, yielding carrier densities of 7.31 × 1021 and 7.50 × 1021 cm-3 and mobilities of 8.15 and 4.98 cm2 V-1 s-1 for the 1- and 4-μm-thick freestanding films, respectively. The spectra further identify a 1.61 eV feature arising from interband-plasmon coupling and a 3.84 eV interband transition, with small thickness dependence, highlighting the bulk-dominated plasmonic response in micrometer-scale films. This work establishes a quantitative, noncontact framework for mapping intrinsic charge dynamics in MXenes, unlocking pathways for their integration into broadband plasmonic, optoelectronic, infrared, and THz devices.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"16 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145711043","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}
Yao Dai,Xuerong Shi,Peng Zhao,Xingzhe Chen,Chaofan Liu,Kaihang Yue,Jin Yang,Ruihu Lu,Xueyang Tu,Laiquan Li,Ya Yan
Electrochemical NOx- reduction offers an attractive approach for the sustainable production of ammonia (NH3). Copper (Cu)-based materials are commonly used catalysts but suffer from a complex reaction pathway and low NH3 selectivity. Herein, we report an electron delocalization strategy by inducing oxygen vacancy and chlorine (Cl) coordination sites as a dual modulator for the active Cu sites. Our model catalyst (Cu2O1-xCl2) could deliver high NH3 yields over a wide potential window, with a maximum NH3 yield rate of 10.05 mg h-1 cm-2 and a Faradaic efficiency (FE) of 95.1%, exceeding most reported metal catalysts. A combination of experimental and theoretical investigations reveals that the dual modulator induces a favorable electron delocalization around the active Cu sites, resulting in an alteration of the rate-determining step (RDS) from NO2* hydrogenation to the one proton-electron coupling of NO* to form NOH*. This thus enables rapid hydrogenation, avoids the occurrence of side reactions, and significantly improves the selectivity and yield of NH3. When assembled into a membrane electrode electrolyzer, the cell can achieve an industrial current density of 340 mA cm-2 with an NH3 production rate of about 21.36 mg h-1 cm-2 and stably operates for up to 200 h. This RDS regulation strategy provides an innovative solution for enhancing the selectivity and efficiency of target products in electrocatalysis.
电化学NOx还原为氨（NH3）的可持续生产提供了一种有吸引力的方法。铜基材料是常用的催化剂，但其反应途径复杂，NH3选择性低。在此，我们报道了一种电子离域策略，通过诱导氧空位和氯（Cl）配位作为活性Cu位的双调节剂。我们的模型催化剂（Cu2O1-xCl2）可以在宽的电位窗口内提供高的NH3产率，NH3的最大产率为10.05 mg h-1 cm-2，法拉第效率（FE）为95.1%，超过了大多数报道的金属催化剂。实验和理论研究表明，双调制器在活性Cu位点周围诱导了有利的电子离域，导致NO2*氢化的速率决定步骤（RDS）改变为NO*形成NOH*的单质子-电子耦合。这样可以实现快速加氢，避免副反应的发生，显著提高NH3的选择性和产率。当组装到膜电极电解槽中时，该电池可以达到340 mA cm-2的工业电流密度，NH3的产率约为21.36 mg h-1 cm-2，并且稳定运行长达200 h。这种RDS调节策略为提高电催化中目标产物的选择性和效率提供了一种创新的解决方案。
{"title":"Electron Delocalization-Induced Modulation of Rate-Determining Step of Copper Catalyst for Efficient Ammonia Electrosynthesis.","authors":"Yao Dai,Xuerong Shi,Peng Zhao,Xingzhe Chen,Chaofan Liu,Kaihang Yue,Jin Yang,Ruihu Lu,Xueyang Tu,Laiquan Li,Ya Yan","doi":"10.1021/acsami.5c18571","DOIUrl":"https://doi.org/10.1021/acsami.5c18571","url":null,"abstract":"Electrochemical NOx- reduction offers an attractive approach for the sustainable production of ammonia (NH3). Copper (Cu)-based materials are commonly used catalysts but suffer from a complex reaction pathway and low NH3 selectivity. Herein, we report an electron delocalization strategy by inducing oxygen vacancy and chlorine (Cl) coordination sites as a dual modulator for the active Cu sites. Our model catalyst (Cu2O1-xCl2) could deliver high NH3 yields over a wide potential window, with a maximum NH3 yield rate of 10.05 mg h-1 cm-2 and a Faradaic efficiency (FE) of 95.1%, exceeding most reported metal catalysts. A combination of experimental and theoretical investigations reveals that the dual modulator induces a favorable electron delocalization around the active Cu sites, resulting in an alteration of the rate-determining step (RDS) from NO2* hydrogenation to the one proton-electron coupling of NO* to form NOH*. This thus enables rapid hydrogenation, avoids the occurrence of side reactions, and significantly improves the selectivity and yield of NH3. When assembled into a membrane electrode electrolyzer, the cell can achieve an industrial current density of 340 mA cm-2 with an NH3 production rate of about 21.36 mg h-1 cm-2 and stably operates for up to 200 h. This RDS regulation strategy provides an innovative solution for enhancing the selectivity and efficiency of target products in electrocatalysis.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"7 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145711042","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}
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