Zhiqian Lin, Huaiqing An, Liyuan Qian, Yun Wang, Haibin Lin, Xiaofei Wang, Guojun Zou, Jinlong Zhu, Songbai Han
Propane dehydrogenation (PDH) is a key process for propylene production, but conventional catalysts are often constrained by high cost, environmental impact, and limited stability under harsh reaction conditions. Fe-based catalysts offer a cost-effective and sustainable alternative due to their intrinsic ability to activate C–H bonds in alkanes. However, precise control over the oxidation state and coordination environment of Fe species to balance PDH activity and stability remains challenging. Herein, we develop a molten-salt-assisted synthesis strategy integrated with CeO2–x-mediated interfacial engineering to finely tune the structural and electronic properties of Fe species supported on Al2O3. The molten salt medium enables uniform dispersion and controlled crystallization of Fe3O4, effectively mitigating its over-reduction during high-temperature H2 treatment. The subsequent incorporation of CeO2–x modulates the local electronic structure of Fe3O4, inducing a controlled partial reduction to metallic Fe0 and forming a well-defined Fe0–Fe3O4 dual-interface architecture. This interfacial electronic reconstruction enriches the electron density of low-valent Fe sites, facilitating efficient charge transfer during propane activation and promoting rapid propylene desorption. As a result, the optimized catalyst demonstrates accelerated PDH kinetics, high propylene selectivity, and enhanced resistance to coking. This work establishes a scalable route for constructing dual-interface active sites, providing a general design principle for low-cost, high-performance PDH catalysts.
{"title":"CeO2–x-Induced Interfacial Reconstruction of Fe3O4/Al2O3 for the Formation of Cooperative Fe0–Fe3O4 Dual Sites in Propane Dehydrogenation","authors":"Zhiqian Lin, Huaiqing An, Liyuan Qian, Yun Wang, Haibin Lin, Xiaofei Wang, Guojun Zou, Jinlong Zhu, Songbai Han","doi":"10.1021/acsami.5c22693","DOIUrl":"https://doi.org/10.1021/acsami.5c22693","url":null,"abstract":"Propane dehydrogenation (PDH) is a key process for propylene production, but conventional catalysts are often constrained by high cost, environmental impact, and limited stability under harsh reaction conditions. Fe-based catalysts offer a cost-effective and sustainable alternative due to their intrinsic ability to activate C–H bonds in alkanes. However, precise control over the oxidation state and coordination environment of Fe species to balance PDH activity and stability remains challenging. Herein, we develop a molten-salt-assisted synthesis strategy integrated with CeO<sub>2–<i>x</i></sub>-mediated interfacial engineering to finely tune the structural and electronic properties of Fe species supported on Al<sub>2</sub>O<sub>3</sub>. The molten salt medium enables uniform dispersion and controlled crystallization of Fe<sub>3</sub>O<sub>4</sub>, effectively mitigating its over-reduction during high-temperature H<sub>2</sub> treatment. The subsequent incorporation of CeO<sub>2–<i>x</i></sub> modulates the local electronic structure of Fe<sub>3</sub>O<sub>4</sub>, inducing a controlled partial reduction to metallic Fe<sup>0</sup> and forming a well-defined Fe<sup>0</sup>–Fe<sub>3</sub>O<sub>4</sub> dual-interface architecture. This interfacial electronic reconstruction enriches the electron density of low-valent Fe sites, facilitating efficient charge transfer during propane activation and promoting rapid propylene desorption. As a result, the optimized catalyst demonstrates accelerated PDH kinetics, high propylene selectivity, and enhanced resistance to coking. This work establishes a scalable route for constructing dual-interface active sites, providing a general design principle for low-cost, high-performance PDH catalysts.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"301 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146115969","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}
Ryan Limbocker, , , Corey M. James, , , F. John Burpo*, , and , Simuck F. Yuk,
{"title":"Editorial for Special Issue: Applied Materials and Interfaces Research at the United States Military Academy in Celebration of the 250th Birthday of US Army","authors":"Ryan Limbocker, , , Corey M. James, , , F. John Burpo*, , and , Simuck F. Yuk, ","doi":"10.1021/acsami.5c24498","DOIUrl":"https://doi.org/10.1021/acsami.5c24498","url":null,"abstract":"","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"18 4","pages":"6271–6272"},"PeriodicalIF":8.2,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146102304","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}
Constructing electrocatalysts with heterostructures has emerged as an efficient approach to cooperatively catalyze the conversion of lithium polysulfides (LiPSs) in lithium–sulfur (Li–S) batteries. However, it remains a formidable challenge to fundamentally understand the structure–activity relationship between the interfacial configuration and electrocatalytic performance, which is crucial for the rational design of electrocatalysts with heterojunctions. Herein, by leveraging molybdenum carbides (MoxC) with tunable crystal structures as model electrocatalysts, we systematically investigated the geometric-configuration-dependent catalytic activity for LiPS conversion. Experimental analyses confirmed that the cubic MoC with octahedrally coordinated Mo atoms (Mooct) is easily passivated because of its robust LiPS affinity, while the hexagonal Mo2C with triangularly coordinated Mo atoms (Motri) functions better in improving the interfacial charge transfer. Accordingly, the constructed heterointerfaces integrated with dual-geometric coordination endow MoC/Mo2C with moderate LiPS adsorption and favorable charge transfer kinetics to cooperatively catalyze LiPS conversion. Benefiting from these advantages, the Li–S batteries assembled with MoC/Mo2C demonstrate superior reversible specific capacities and cycling durability. This work highlights the critical role of interfacial geometric coordination in heterojunctions for LiPS retention and catalysis, offering a guiding approach for elevating the activity of heterojunction electrocatalysts.
{"title":"Efficient Heterojunction Electrocatalysts for Polysulfide Conversion in Li–S Batteries via Dual-Geometric Coordination at Heterointerfaces","authors":"Lei Wang, Jian-Rong Chen, Tong Chen, Chen Cheng, Cheng Yuan, Tianran Yan, Ziyang Huang, Pan Zeng, Ting-Shan Chan, Cheng-Wei Kao, Liang Zhang","doi":"10.1021/acsami.5c21599","DOIUrl":"https://doi.org/10.1021/acsami.5c21599","url":null,"abstract":"Constructing electrocatalysts with heterostructures has emerged as an efficient approach to cooperatively catalyze the conversion of lithium polysulfides (LiPSs) in lithium–sulfur (Li–S) batteries. However, it remains a formidable challenge to fundamentally understand the structure–activity relationship between the interfacial configuration and electrocatalytic performance, which is crucial for the rational design of electrocatalysts with heterojunctions. Herein, by leveraging molybdenum carbides (Mo<sub><i>x</i></sub>C) with tunable crystal structures as model electrocatalysts, we systematically investigated the geometric-configuration-dependent catalytic activity for LiPS conversion. Experimental analyses confirmed that the cubic MoC with octahedrally coordinated Mo atoms (Mo<sub>oct</sub>) is easily passivated because of its robust LiPS affinity, while the hexagonal Mo<sub>2</sub>C with triangularly coordinated Mo atoms (Mo<sub>tri</sub>) functions better in improving the interfacial charge transfer. Accordingly, the constructed heterointerfaces integrated with dual-geometric coordination endow MoC/Mo<sub>2</sub>C with moderate LiPS adsorption and favorable charge transfer kinetics to cooperatively catalyze LiPS conversion. Benefiting from these advantages, the Li–S batteries assembled with MoC/Mo<sub>2</sub>C demonstrate superior reversible specific capacities and cycling durability. This work highlights the critical role of interfacial geometric coordination in heterojunctions for LiPS retention and catalysis, offering a guiding approach for elevating the activity of heterojunction electrocatalysts.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"66 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111022","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}
Amyloidogenic peptides and proteins, including amyloid-β, tau, and α-synuclein, are key pathological factors in neurodegenerative diseases. Their misfolding and self-assembly into toxic oligomers and fibrils disrupt cellular homeostasis and lead to neuronal dysfunction. To address these pathogenic processes, diverse chemical strategies have been developed employing nanomaterials, small organic molecules, and metal complexes. These reagents chemically modify amyloidogenic peptides and proteins, thereby altering their aggregation pathways, attenuating associated toxicity, and demonstrating in vivo efficacy. In this review, we outline and discuss the design principles and mechanistic bases of these chemical interventions, with some examples that demonstrate anti-amyloidogenic effects. Collectively, these advances underscore the power of chemistry to modulate amyloid aggregation and provide mechanistic insights that can guide the development of innovative therapeutic strategies for amyloid-driven neurodegeneration.
{"title":"Chemical Strategies to Modulate Amyloidogenesis Associated with Neurodegenerative Diseases","authors":"Chanju Na,Youngeun Jang,Mikyung Son,Mi Hee Lim","doi":"10.1021/acsami.5c20362","DOIUrl":"https://doi.org/10.1021/acsami.5c20362","url":null,"abstract":"Amyloidogenic peptides and proteins, including amyloid-β, tau, and α-synuclein, are key pathological factors in neurodegenerative diseases. Their misfolding and self-assembly into toxic oligomers and fibrils disrupt cellular homeostasis and lead to neuronal dysfunction. To address these pathogenic processes, diverse chemical strategies have been developed employing nanomaterials, small organic molecules, and metal complexes. These reagents chemically modify amyloidogenic peptides and proteins, thereby altering their aggregation pathways, attenuating associated toxicity, and demonstrating in vivo efficacy. In this review, we outline and discuss the design principles and mechanistic bases of these chemical interventions, with some examples that demonstrate anti-amyloidogenic effects. Collectively, these advances underscore the power of chemistry to modulate amyloid aggregation and provide mechanistic insights that can guide the development of innovative therapeutic strategies for amyloid-driven neurodegeneration.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"1 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111282","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}
The design and synthesis of biomimetic molecules, guided by the principles of molecular architectonics, represent significant advancements in the development of functional materials. This approach facilitates the systematic investigation of how amino acid sequences influence the structural and functional properties of oligopeptides. In this study, we present the design and synthesis of decapeptides with opposite polarity, consisting of specific periodic amino acid sequences such as W5K5 (W: tryptophan, K: lysine) and W5E5 (W: tryptophan, E: glutamic acid), which spontaneously assemble into peptide nanoparticles in aqueous media. A 1:1 mixture of these peptides undergoes coassembly in a phosphate buffer, transitioning from nanoparticles to hierarchical architecture, specifically two-dimensional (2D) sheets with lateral dimension of several micrometers. The assembly process is driven by electrostatic interactions between oppositely charged decapeptides and the uniform distribution of hydrophobic and hydrophilic moieties. The formation and stability of these 2D sheets were studied by using various microscopy and spectroscopy techniques. The 2D peptide assemblies, with their large surface area and structural flexibility, demonstrate significant potential for biological applications, such as DNA interaction. Understanding and optimizing DNA–peptide interactions are essential for advancing applications in gene delivery, biosensing, and nanobiotechnology. This study investigates how coassembled 2D peptide nanostructures can enhance DNA-binding interactions. The coassembled 2D sheets exhibited markedly higher DNA interaction efficiency compared to individual peptide nanoparticles. This study offers a straightforward yet innovative strategy for fabricating peptide-based 2D materials via molecular assembly, providing a promising platform for advancements in DNA nanotechnology and related fields.
{"title":"Engineering the Peptide Coassembly into 2D Architectures for Enhanced DNA Interactions","authors":"Soumik Dinda, Debasis Ghosh, Milind Kumar Anand, Thimmaiah Govindaraju","doi":"10.1021/acsami.5c21522","DOIUrl":"https://doi.org/10.1021/acsami.5c21522","url":null,"abstract":"The design and synthesis of biomimetic molecules, guided by the principles of molecular architectonics, represent significant advancements in the development of functional materials. This approach facilitates the systematic investigation of how amino acid sequences influence the structural and functional properties of oligopeptides. In this study, we present the design and synthesis of decapeptides with opposite polarity, consisting of specific periodic amino acid sequences such as W<sub>5</sub>K<sub>5</sub> (W: tryptophan, K: lysine) and W<sub>5</sub>E<sub>5</sub> (W: tryptophan, E: glutamic acid), which spontaneously assemble into peptide nanoparticles in aqueous media. A 1:1 mixture of these peptides undergoes coassembly in a phosphate buffer, transitioning from nanoparticles to hierarchical architecture, specifically two-dimensional (2D) sheets with lateral dimension of several micrometers. The assembly process is driven by electrostatic interactions between oppositely charged decapeptides and the uniform distribution of hydrophobic and hydrophilic moieties. The formation and stability of these 2D sheets were studied by using various microscopy and spectroscopy techniques. The 2D peptide assemblies, with their large surface area and structural flexibility, demonstrate significant potential for biological applications, such as DNA interaction. Understanding and optimizing DNA–peptide interactions are essential for advancing applications in gene delivery, biosensing, and nanobiotechnology. This study investigates how coassembled 2D peptide nanostructures can enhance DNA-binding interactions. The coassembled 2D sheets exhibited markedly higher DNA interaction efficiency compared to individual peptide nanoparticles. This study offers a straightforward yet innovative strategy for fabricating peptide-based 2D materials via molecular assembly, providing a promising platform for advancements in DNA nanotechnology and related fields.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"215 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111000","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}
Md Sariful Sheikh, Lijie Guo, Qiyuan Chen, Bu Wang
Despite growing interest in biobased materials, rapid, low-temperature CO2 capture using amine-rich natural sorbents has received limited attention. Various porous solid sorbents have drawn significant research interest as promising carbon capture materials. However, high synthesis cost, limited CO2 adsorption capacity, sluggish adsorption–desorption kinetics, high sorbent regeneration temperature, and poor operational stability remain major challenges for their practical implementation. Here, we present silk-nanofibroin aerogels derived from natural mulberry silk as a sustainable, amine-rich, and porous solid-support-free sorbent platform for energy-efficient CO2 capture. The aerogels exhibit a CO2 adsorption capacity competitive with state-of-the-art amino acid and amino acid ionic liquid-based solid sorbents. Thermogravimetric analysis confirms high thermal stability up to ∼250 °C─substantially higher than that of conventional amine sorbents─while complete sorbent regeneration occurs at only 60 °C. Furthermore, the silk-nanofibroin aerogels demonstrate rapid adsorption–desorption kinetics, excellent multicycle stability, and full retention of CO2 adsorption capacity under humid conditions. Spectroscopic analyses (XPS, FTIR, Raman, and solid-state 13C NMR) confirm reversible CO2 chemisorption through intrinsic amine sites at the silk-fibroin surface. Overall, this work establishes silk-nanofibroin aerogels as a sustainable and low-cost route toward energy-efficient CO2 capture.
{"title":"Silk-Nano-Fibroin Aerogels: A Bio-Derived, Amine-Rich Platform for Rapid and Reversible CO2 Capture","authors":"Md Sariful Sheikh, Lijie Guo, Qiyuan Chen, Bu Wang","doi":"10.1021/acsami.5c21809","DOIUrl":"https://doi.org/10.1021/acsami.5c21809","url":null,"abstract":"Despite growing interest in biobased materials, rapid, low-temperature CO<sub>2</sub> capture using amine-rich natural sorbents has received limited attention. Various porous solid sorbents have drawn significant research interest as promising carbon capture materials. However, high synthesis cost, limited CO<sub>2</sub> adsorption capacity, sluggish adsorption–desorption kinetics, high sorbent regeneration temperature, and poor operational stability remain major challenges for their practical implementation. Here, we present silk-nanofibroin aerogels derived from natural mulberry silk as a sustainable, amine-rich, and porous solid-support-free sorbent platform for energy-efficient CO<sub>2</sub> capture. The aerogels exhibit a CO<sub>2</sub> adsorption capacity competitive with state-of-the-art amino acid and amino acid ionic liquid-based solid sorbents. Thermogravimetric analysis confirms high thermal stability up to ∼250 °C─substantially higher than that of conventional amine sorbents─while complete sorbent regeneration occurs at only 60 °C. Furthermore, the silk-nanofibroin aerogels demonstrate rapid adsorption–desorption kinetics, excellent multicycle stability, and full retention of CO<sub>2</sub> adsorption capacity under humid conditions. Spectroscopic analyses (XPS, FTIR, Raman, and solid-state <sup>13</sup>C NMR) confirm reversible CO<sub>2</sub> chemisorption through intrinsic amine sites at the silk-fibroin surface. Overall, this work establishes silk-nanofibroin aerogels as a sustainable and low-cost route toward energy-efficient CO<sub>2</sub> capture.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"223 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111023","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}
Wenqi Ma, Qianhe Wang, Alexey Zhizhchenko, He Li, Aleksandr Kuchmizhak, Junjie Zhang
While femtosecond laser-induced periodic surface structures (LIPSS) offer substantial potential in surface engineering, realizing a full spectrum of their demand-oriented functionalities depends critically on the precise and controllable tailoring of their key parameters, period, and orientation. This study proposes a strategy for precisely and simultaneously controlling both LIPSS characteristics by coupling the polarization and incidence angles of the laser beam, which is realized by a multiaxis femtosecond laser micromachining process integrated with neural network guidance. A multiaxis femtosecond laser micromachining system for LIPSS-based patterning is constructed, and its kinematic model is established to compensate for the polarization deviations induced upon the variation of the beam incidence angle. Back-propagation (BP) neural network and particle swarm optimization method is employed to optimize laser processing parameters (pulse energy, effective pulse number, and scanning line spacing) to ensure the LIPSS regularity and uniformity. Another BP neural network is established to elucidate the mapping relationship between laser processing parameters (incidence/polarization angles) and LIPSS geometry, which is experimentally validated by demonstrating the designed multilevel LIPSS-based structural coloring of SUS 304 stainless steel, where the period and orientation are simultaneously tailored. This work provides both a theoretical basis and technical guidance for the design and fabrication of LIPSS with on-demand characteristics.
{"title":"Regulating LIPSS Period and Orientation via Multiaxis Laser Processing and Neural Network Guidance","authors":"Wenqi Ma, Qianhe Wang, Alexey Zhizhchenko, He Li, Aleksandr Kuchmizhak, Junjie Zhang","doi":"10.1021/acsami.5c22382","DOIUrl":"https://doi.org/10.1021/acsami.5c22382","url":null,"abstract":"While femtosecond laser-induced periodic surface structures (LIPSS) offer substantial potential in surface engineering, realizing a full spectrum of their demand-oriented functionalities depends critically on the precise and controllable tailoring of their key parameters, period, and orientation. This study proposes a strategy for precisely and simultaneously controlling both LIPSS characteristics by coupling the polarization and incidence angles of the laser beam, which is realized by a multiaxis femtosecond laser micromachining process integrated with neural network guidance. A multiaxis femtosecond laser micromachining system for LIPSS-based patterning is constructed, and its kinematic model is established to compensate for the polarization deviations induced upon the variation of the beam incidence angle. Back-propagation (BP) neural network and particle swarm optimization method is employed to optimize laser processing parameters (pulse energy, effective pulse number, and scanning line spacing) to ensure the LIPSS regularity and uniformity. Another BP neural network is established to elucidate the mapping relationship between laser processing parameters (incidence/polarization angles) and LIPSS geometry, which is experimentally validated by demonstrating the designed multilevel LIPSS-based structural coloring of SUS 304 stainless steel, where the period and orientation are simultaneously tailored. This work provides both a theoretical basis and technical guidance for the design and fabrication of LIPSS with on-demand characteristics.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"3 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146115968","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}
Construction of aerogel-based composite photocatalytic materials is an effective way to completely eliminate pollutants in water. However, uniform dispersion of photocatalyst nanoparticles in porous aerogels and how to achieve efficient adsorption/photocatalysis synergy still face challenge. In this study, we have successfully addressed the challenge of achieving uniform loading of TiO2 photocatalyst nanoparticles in aramid nanofiber (ANF) aerogels using silica aerogel powder (SAP)-assisted dispersion, which significantly broadens the spectral response range of TiO2. The as-prepared ANF composite aerogel fibers exhibited excellent properties, such as low shrinkage (13.7%), high porosity (94.8%), and a high specific surface area (238.033 m2/g). Moreover, the as-prepared ANF/SAP/TiO2@TiOSO4 (M-TAST) composite aerogel film by using TiOSO4 aqueous solution as coagulation bath achieved a synergistic effect of internal/external photocatalysis, with further improved carrier separation and migration ability, and effectively inhibited the recombination of photogenerated electron–hole pairs. Thus, the as-prepared ANF-based composite aerogel film demonstrated excellent adsorption/photocatalytic degradation of tetracycline and organic dyes. In particular, the degradation efficiency of crystal violet (CV) reached 98% in 10 min, significantly outperforming P25. Additionally, the film also exhibited good photocatalytic performance within the pH range of 2–10 and excellent recycling stability. This unique photocatalyst loading strategy is crucial for achieving adsorption and internal/external photocatalysis synergy, and the constructed M-TAST composite aerogel film shows a promising prospect for application in environmental purification.
{"title":"Optimizing Strategies of in Situ Loading Photocatalysts in Aramid Nanofiber Aerogels: Harnessing Internal/External Synergistic Photocatalysis for Improving Degradation Efficiency of Pollutants","authors":"Pengfei Qiu, Jingxiao Liu, Keya Zhu, Fei Shi","doi":"10.1021/acsami.5c20126","DOIUrl":"https://doi.org/10.1021/acsami.5c20126","url":null,"abstract":"Construction of aerogel-based composite photocatalytic materials is an effective way to completely eliminate pollutants in water. However, uniform dispersion of photocatalyst nanoparticles in porous aerogels and how to achieve efficient adsorption/photocatalysis synergy still face challenge. In this study, we have successfully addressed the challenge of achieving uniform loading of TiO<sub>2</sub> photocatalyst nanoparticles in aramid nanofiber (ANF) aerogels using silica aerogel powder (SAP)-assisted dispersion, which significantly broadens the spectral response range of TiO<sub>2</sub>. The as-prepared ANF composite aerogel fibers exhibited excellent properties, such as low shrinkage (13.7%), high porosity (94.8%), and a high specific surface area (238.033 m<sup>2</sup>/g). Moreover, the as-prepared ANF/SAP/TiO<sub>2</sub>@TiOSO<sub>4</sub> (M-TAST) composite aerogel film by using TiOSO<sub>4</sub> aqueous solution as coagulation bath achieved a synergistic effect of internal/external photocatalysis, with further improved carrier separation and migration ability, and effectively inhibited the recombination of photogenerated electron–hole pairs. Thus, the as-prepared ANF-based composite aerogel film demonstrated excellent adsorption/photocatalytic degradation of tetracycline and organic dyes. In particular, the degradation efficiency of crystal violet (CV) reached 98% in 10 min, significantly outperforming P25. Additionally, the film also exhibited good photocatalytic performance within the pH range of 2–10 and excellent recycling stability. This unique photocatalyst loading strategy is crucial for achieving adsorption and internal/external photocatalysis synergy, and the constructed M-TAST composite aerogel film shows a promising prospect for application in environmental purification.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"106 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111019","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}
The development of efficient and durable nonprecious electrocatalysts for the oxygen evolution reaction (OER) is critical for sustainable hydrogen production. In this study, a defective CoFe-layered double hydroxide (LDH) support is engineered to stabilize isolated cerium atoms via a facile one-step coprecipitation approach. The resulting single-atom catalyst, denoted Ce0.2CoFe-LDH, is thoroughly characterized by atomic-resolution electron microscopy and synchrotron-based X-ray spectroscopy, which confirm the atomic dispersion of Ce3+ species anchored at cation vacancy sites within the LDH matrix. A strong electronic interaction between Ce and Co/Fe sites is observed, leading to charge redistribution that increases the valence states of transition metals and activates dynamic Ce3+/Ce4+ redox cycling. The optimized catalyst exhibits outstanding OER performance in alkaline media, achieving an overpotential as low as 227 mV at 10 mA·cm–2, a Tafel slope of 48.3 mV·dec–1, and excellent stability over 50 h of continuous operation. Electrochemical measurements indicate facilitated charge transfer and an increased electrochemically active surface area. First-principles calculations further reveal that Ce atoms occupying Co vacancies significantly optimize the adsorption of reaction intermediates, reduce the energy barrier of the rate-determining step to 1.81 eV, and induce metallic character through an upshift of the d-band center. This work establishes defect-driven single-atom anchoring as an effective strategy for electronic structure modulation and reaction pathway optimization in LDH-based electrocatalysts, offering valuable insights for the design of high-performance energy conversion materials.
{"title":"Atomic Cerium Boosts Oxygen Evolution via Electronic Coupling in Defective CoFe-Layered Double Hydroxides","authors":"Yangchun Guo, Tingting Wei, Xiaodong Hao, Xuan Zhao, Zhen-Hong He, Qiheng Ma, Zhuangzhuang Hu, Shufang Ma, Xiaoxu Liu, Bingshe Xu","doi":"10.1021/acsami.5c23886","DOIUrl":"https://doi.org/10.1021/acsami.5c23886","url":null,"abstract":"The development of efficient and durable nonprecious electrocatalysts for the oxygen evolution reaction (OER) is critical for sustainable hydrogen production. In this study, a defective CoFe-layered double hydroxide (LDH) support is engineered to stabilize isolated cerium atoms via a facile one-step coprecipitation approach. The resulting single-atom catalyst, denoted Ce<sub>0.2</sub>CoFe-LDH, is thoroughly characterized by atomic-resolution electron microscopy and synchrotron-based X-ray spectroscopy, which confirm the atomic dispersion of Ce<sup>3+</sup> species anchored at cation vacancy sites within the LDH matrix. A strong electronic interaction between Ce and Co/Fe sites is observed, leading to charge redistribution that increases the valence states of transition metals and activates dynamic Ce<sup>3+</sup>/Ce<sup>4+</sup> redox cycling. The optimized catalyst exhibits outstanding OER performance in alkaline media, achieving an overpotential as low as 227 mV at 10 mA·cm<sup>–2</sup>, a Tafel slope of 48.3 mV·dec<sup>–1</sup>, and excellent stability over 50 h of continuous operation. Electrochemical measurements indicate facilitated charge transfer and an increased electrochemically active surface area. First-principles calculations further reveal that Ce atoms occupying Co vacancies significantly optimize the adsorption of reaction intermediates, reduce the energy barrier of the rate-determining step to 1.81 eV, and induce metallic character through an upshift of the d-band center. This work establishes defect-driven single-atom anchoring as an effective strategy for electronic structure modulation and reaction pathway optimization in LDH-based electrocatalysts, offering valuable insights for the design of high-performance energy conversion materials.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"1 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111050","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}
F. John Burpo*, , , Ryan Limbocker, , , Corey M. James, , , Kevin Kit Parker, , and , Enoch A. Nagelli,
{"title":"A 250-Year Perspective on U.S. Army-Driven Materials Science and Engineering Innovation and Leadership Development","authors":"F. John Burpo*, , , Ryan Limbocker, , , Corey M. James, , , Kevin Kit Parker, , and , Enoch A. Nagelli, ","doi":"10.1021/acsami.5c24495","DOIUrl":"https://doi.org/10.1021/acsami.5c24495","url":null,"abstract":"","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"18 4","pages":"6265–6270"},"PeriodicalIF":8.2,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146102305","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}
京公网安备 11010802042870号
京ICP备2023020795号-1
扫码关注我们
求助内容：
应助结果提醒方式：