Pub Date : 2025-01-17DOI: 10.1021/acs.nanolett.4c06067
Wei Li, Jing Li, Lebing Wang, Yan Wang, Zhirui Zhang, Shilong Liu, Bo Gong, Yunjiao Wang, Liang Wang
Watson–Crick and Hoogsteen hydrogen bonds aid the formation of highly ordered structures in genomic DNA that dynamically govern genetic modes such as gene regulation and replication. Hence, measuring and distinguishing these two types of hydrogen bonds in different DNA contexts are essential for understanding DNA architectures. However, due to their transient nature and minimal structure differences at the sub-nanometer scale, differentiating Watson–Crick hydrogen bonds from Hoogsteen hydrogen bonds is difficult. Relying on nanopore technology, we successfully discriminated the two types of hydrogen bonds in multiple DNA contexts in the presence of epigenetic modification, changes in DNA structures, and proton strength in the environment. Our results indicate that Watson–Crick and Hoogsteen hydrogen bonds show different susceptibilities to changes in physicochemical characteristics that matter in stabilizing DNA hydrogen bonds. This work provides insight into the features of hydrogen bonds at the nanoscale and may benefit profiling complex DNA architectures by measuring subtle structural changes.
{"title":"Nanopore Discriminates Watson–Crick and Hoogsteen Hydrogen Bonds in Multiple DNA Contexts","authors":"Wei Li, Jing Li, Lebing Wang, Yan Wang, Zhirui Zhang, Shilong Liu, Bo Gong, Yunjiao Wang, Liang Wang","doi":"10.1021/acs.nanolett.4c06067","DOIUrl":"https://doi.org/10.1021/acs.nanolett.4c06067","url":null,"abstract":"Watson–Crick and Hoogsteen hydrogen bonds aid the formation of highly ordered structures in genomic DNA that dynamically govern genetic modes such as gene regulation and replication. Hence, measuring and distinguishing these two types of hydrogen bonds in different DNA contexts are essential for understanding DNA architectures. However, due to their transient nature and minimal structure differences at the sub-nanometer scale, differentiating Watson–Crick hydrogen bonds from Hoogsteen hydrogen bonds is difficult. Relying on nanopore technology, we successfully discriminated the two types of hydrogen bonds in multiple DNA contexts in the presence of epigenetic modification, changes in DNA structures, and proton strength in the environment. Our results indicate that Watson–Crick and Hoogsteen hydrogen bonds show different susceptibilities to changes in physicochemical characteristics that matter in stabilizing DNA hydrogen bonds. This work provides insight into the features of hydrogen bonds at the nanoscale and may benefit profiling complex DNA architectures by measuring subtle structural changes.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"131 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987575","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 manufacturing of biomimetic bone characterized by an organic–inorganic combination and fibrous structure has garnered significant attention. Inspired by the formation of multi-layered fibrous structures in bone tissue, this study is based on the fibril assembled from poly(γ-benzyl-L-glutamate) (PBLG) in helicogenic solvent, proposing a non-solvent-assisted 3D printing method for realizing the PBLG 3D printing while generating biomimetic fiber structures in One-Step to mimic the formation of collagen fiber bundles. The unprintable mixture of PBLG and hydroxyapatite nanoparticles (nHA) in 1,4-dioxane exhibits extrudability, self-supporting properties, and plasticity in ethanol. Meanwhile, ethanol-assisted printing leads to the spontaneous growth of PBLG-fibrils into submicron-fibers. Moreover, the integration of nHA with PBLG-fibers through hydrogen bonding contributes to the improvement of printability and mechanical properties. This method of ethanol-assisted fiber generation is successful with concentrated PBLG solutions, overcoming the limitation of previous research that focused only on dilute solutions. To expand the printable window, an ethanol-gel is developed as a support to achieve omnidirectional printing, resolving the issue of interlayer collapse caused by gravity and the conflict between printability and biomimetic fibers generation, optimizing the biomimetic bone manufacturing, leading to the precise biomimetic design of bone structures.
{"title":"Biomimetic Fibrous Bone Substitute Manufacture Through Non-Solvent-Assisted 3D Printing","authors":"Kunxi Zhang, Haowei Fang, Xiangyang Cheng, Jinyan Li, Jiujiang Zeng, Tao Zhang, Haiyan Cui, Huijie Gu, Jingbo Yin","doi":"10.1002/adfm.202419464","DOIUrl":"https://doi.org/10.1002/adfm.202419464","url":null,"abstract":"The manufacturing of biomimetic bone characterized by an organic–inorganic combination and fibrous structure has garnered significant attention. Inspired by the formation of multi-layered fibrous structures in bone tissue, this study is based on the fibril assembled from poly(γ-benzyl-L-glutamate) (PBLG) in helicogenic solvent, proposing a non-solvent-assisted 3D printing method for realizing the PBLG 3D printing while generating biomimetic fiber structures in One-Step to mimic the formation of collagen fiber bundles. The unprintable mixture of PBLG and hydroxyapatite nanoparticles (nHA) in 1,4-dioxane exhibits extrudability, self-supporting properties, and plasticity in ethanol. Meanwhile, ethanol-assisted printing leads to the spontaneous growth of PBLG-fibrils into submicron-fibers. Moreover, the integration of nHA with PBLG-fibers through hydrogen bonding contributes to the improvement of printability and mechanical properties. This method of ethanol-assisted fiber generation is successful with concentrated PBLG solutions, overcoming the limitation of previous research that focused only on dilute solutions. To expand the printable window, an ethanol-gel is developed as a support to achieve omnidirectional printing, resolving the issue of interlayer collapse caused by gravity and the conflict between printability and biomimetic fibers generation, optimizing the biomimetic bone manufacturing, leading to the precise biomimetic design of bone structures.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"95 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987698","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}
Ni An, Guzailinuer Yasen, Ximu Li, Xianbao Shi, Yongjun Wang, Hongzhuo Liu
Alopecia areata (AA) is a prevalent autoimmune condition that causes sudden hair loss and poses significant psychological challenges to affected individuals. Current treatments, including corticosteroids and Janus kinase inhibitors, fail to provide long-term efficacy due to adverse effects and relapse after cessation. This study introduces a nanoparticle (NP) system that codeliver diphenylcyclopropenone (DPCP) and rapamycin (RAPA) prodrugs to induce immune tolerance and promote hair regeneration. The results demonstrated that the coassembled NPs exhibited uniformity and stability, were efficiently taken up by antigen-presenting cells (APCs), and successfully induced dendritic cells (DCs) to differentiate into tolerogenic phenotypes in vitro. In vivo studies on a mouse model of alopecia showed that these NPs significantly accelerated the transition of hair follicles from the telogen phase to the anagen phase, promoting hair regrowth. This research presents a promising therapeutic strategy for AA and offers insights into treating autoimmune diseases where autoantigens are unclear.
{"title":"Nanoparticle Adjuvants Incorporating Haptens Drive Potent Immune Tolerance to Accelerate Hair Regrowth","authors":"Ni An, Guzailinuer Yasen, Ximu Li, Xianbao Shi, Yongjun Wang, Hongzhuo Liu","doi":"10.1021/acsami.4c17068","DOIUrl":"https://doi.org/10.1021/acsami.4c17068","url":null,"abstract":"Alopecia areata (AA) is a prevalent autoimmune condition that causes sudden hair loss and poses significant psychological challenges to affected individuals. Current treatments, including corticosteroids and Janus kinase inhibitors, fail to provide long-term efficacy due to adverse effects and relapse after cessation. This study introduces a nanoparticle (NP) system that codeliver diphenylcyclopropenone (DPCP) and rapamycin (RAPA) prodrugs to induce immune tolerance and promote hair regeneration. The results demonstrated that the coassembled NPs exhibited uniformity and stability, were efficiently taken up by antigen-presenting cells (APCs), and successfully induced dendritic cells (DCs) to differentiate into tolerogenic phenotypes <i>in vitro</i>. <i>In vivo</i> studies on a mouse model of alopecia showed that these NPs significantly accelerated the transition of hair follicles from the telogen phase to the anagen phase, promoting hair regrowth. This research presents a promising therapeutic strategy for AA and offers insights into treating autoimmune diseases where autoantigens are unclear.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"55 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987870","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}
Pub Date : 2025-01-17DOI: 10.1016/j.jallcom.2025.178658
Shiyu Xiao, Zhaorun Dong, Mingliang Zhang, Wei Yan, Ye Li, Xue Chen, Xiaodong Wang
Low-dimensionalization has emerged as a novel approach for thermoelectric material modification. Cu2-xTe has been proposed as promising thermoelectric material, yet its structure and properties upon low-dimensionalization remain largely unknown. Nanofilms with varying thicknesses from 20 nm to 340 nm were synthesized by RF magnetron sputtering, and their structures were characterized using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray diffraction (XRD). By modulating thickness of the nanofilms, we observed a novel layered structure of Cu2-xTe and formation of three room-temperature stable phases and their size-induced evolution. Furthermore, we demonstrate that the electrical properties of nanofilms are significantly modulated by size control. Since, we have achieved direct size-induced control over the structure and electrical properties of Cu2-xTe nanofilms.
{"title":"Size-dependent phase evolution and electrical properties of Cu2-xTe thermoelectric nanofilms","authors":"Shiyu Xiao, Zhaorun Dong, Mingliang Zhang, Wei Yan, Ye Li, Xue Chen, Xiaodong Wang","doi":"10.1016/j.jallcom.2025.178658","DOIUrl":"https://doi.org/10.1016/j.jallcom.2025.178658","url":null,"abstract":"Low-dimensionalization has emerged as a novel approach for thermoelectric material modification. Cu<sub>2-x</sub>Te has been proposed as promising thermoelectric material, yet its structure and properties upon low-dimensionalization remain largely unknown. Nanofilms with varying thicknesses from 20 nm to 340 nm were synthesized by RF magnetron sputtering, and their structures were characterized using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray diffraction (XRD). By modulating thickness of the nanofilms, we observed a novel layered structure of Cu<sub>2-x</sub>Te and formation of three room-temperature stable phases and their size-induced evolution. Furthermore, we demonstrate that the electrical properties of nanofilms are significantly modulated by size control. Since, we have achieved direct size-induced control over the structure and electrical properties of Cu<sub>2-x</sub>Te nanofilms.","PeriodicalId":344,"journal":{"name":"Journal of Alloys and Compounds","volume":"30 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988026","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}
Pub Date : 2025-01-17DOI: 10.1016/j.ijplas.2025.104247
Xuejian Yang, Mingyang Jiao, Zhijia Liu, Hui Zhao, Yan Peng, Lu Wu, Yu Wu, Rongjian Pan, Baodong Shi
During practical forming processing, strong anisotropic mechanical behavior of dual phase (DP) steels is usually detected due to texture, which further determines subsequent processing optimization with loading paths changing. In order to clarify the underlying deformation mechanisms of DP steels under multi-axial loading, the mechanical response of DP780 under different biaxial loading paths was examined in detail. More precisely, anisotropic behavior of DP780 in complete “σxx-σyy” space was investigated through mechanical testing, microstructure characterization, and crystal plasticity computation based on dislocation density. In particular, biaxial compression test of thin plate is realized by using specifically designed fixture, and consequently yield loci in complete “σxx-σyy” space is detected experimentally. It is found that stronger anisotropy is observed under biaxial loading compared with that under uniaxial loading at macro scale, and biaxial Bauschinger effect is detected with biaxial preloading. At the micro scale, the texture evolution is affected directly by loading paths, and the compression load contributes more to the texture evolution. The distribution of the Taylor Factor under different biaxial loading paths reveals the impact of tension and compression on the main activated slip systems (MASS). Under biaxial tension and biaxial compression loading, the MASS of DP780 is the {112} slip system. Under combined biaxial tension and compression loading, the MASS is the {110} slip system. Using crystal plasticity, the evolution of dislocation density under different biaxial loading is captured. The relationship between the biaxial Bauschinger effect and MASS is clarified. It is found that the dislocation multiplication of the {112} slip system is more affected by changes in loading path than the {110} slip system. And during the subsequent loading process, the {110} slip system transform to {112} by preloading. Additionally, the relationship between the alteration of the MASS and the evolution of texture, as well as the resulting macroscopic anisotropic behavior has been elucidated.
{"title":"Mechanical responses and microstructure evolution of DP780 in complete σxx-σyy space: experiments and crystal plasticity characterization","authors":"Xuejian Yang, Mingyang Jiao, Zhijia Liu, Hui Zhao, Yan Peng, Lu Wu, Yu Wu, Rongjian Pan, Baodong Shi","doi":"10.1016/j.ijplas.2025.104247","DOIUrl":"https://doi.org/10.1016/j.ijplas.2025.104247","url":null,"abstract":"During practical forming processing, strong anisotropic mechanical behavior of dual phase (DP) steels is usually detected due to texture, which further determines subsequent processing optimization with loading paths changing. In order to clarify the underlying deformation mechanisms of DP steels under multi-axial loading, the mechanical response of DP780 under different biaxial loading paths was examined in detail. More precisely, anisotropic behavior of DP780 in complete “σ<sub>xx</sub>-σ<sub>yy</sub>” space was investigated through mechanical testing, microstructure characterization, and crystal plasticity computation based on dislocation density. In particular, biaxial compression test of thin plate is realized by using specifically designed fixture, and consequently yield loci in complete “σ<sub>xx</sub>-σ<sub>yy</sub>” space is detected experimentally. It is found that stronger anisotropy is observed under biaxial loading compared with that under uniaxial loading at macro scale, and biaxial Bauschinger effect is detected with biaxial preloading. At the micro scale, the texture evolution is affected directly by loading paths, and the compression load contributes more to the texture evolution. The distribution of the Taylor Factor under different biaxial loading paths reveals the impact of tension and compression on the main activated slip systems (MASS). Under biaxial tension and biaxial compression loading, the MASS of DP780 is the {112} slip system. Under combined biaxial tension and compression loading, the MASS is the {110} slip system. Using crystal plasticity, the evolution of dislocation density under different biaxial loading is captured. The relationship between the biaxial Bauschinger effect and MASS is clarified. It is found that the dislocation multiplication of the {112} slip system is more affected by changes in loading path than the {110} slip system. And during the subsequent loading process, the {110} slip system transform to {112} by preloading. Additionally, the relationship between the alteration of the MASS and the evolution of texture, as well as the resulting macroscopic anisotropic behavior has been elucidated.","PeriodicalId":340,"journal":{"name":"International Journal of Plasticity","volume":"12 1","pages":""},"PeriodicalIF":9.8,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988058","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}
Structure defects of advanced two-dimensional (2D) transition metal dichalcogenides (TMDCs) have provided enormous opportunities for modified band structures and fascinating properties to facilitate the development of fundamental studies, among which intrinsic defects can be spontaneously introduced to 2D materials to expand the functional diversity. Except for unary intrinsic defects, structure–activity relationships of multiplex intrinsic defects and modulated properties still remain to be released for practical applications. Herein, binary intrinsic defects in exfoliated molybdenum disulfide (MoS2), including sulfur monovacancies and oxygen substitution, were studied for revealing the sensing mechanism of 2,4,4′-trichlorobiphenyl (PCB28). They theoretically tended to form homosteric associated pairs and promote molecular anchoring synergistically. Appropriate molecular adsorption and efficient electron transfer enabled the excellent sensing performances for PCB28 including considerable linear region of 100 ng mL−1 ∼ 1 mg mL−1 and low detection limit of 7.96 ng mL−1, which was also inspirable for the design of other small-molecule sensors.
{"title":"Binary intrinsic defects in Two-Dimensional molybdenum disulfide toward detection mechanism of 2,4,4′-trichlorobiphenyl","authors":"Hailin Zheng, Demin Zhu, Chengyi Xiong, Xiquan Hu, Miao-Miao Chen, Shengfu Wang, Yao Xiao, Xiuhua Zhang","doi":"10.1016/j.apsusc.2025.162414","DOIUrl":"https://doi.org/10.1016/j.apsusc.2025.162414","url":null,"abstract":"Structure defects of advanced two-dimensional (2D) transition metal dichalcogenides (TMDCs) have provided enormous opportunities for modified band structures and fascinating properties to facilitate the development of fundamental studies, among which intrinsic defects can be spontaneously introduced to 2D materials to expand the functional diversity. Except for unary intrinsic defects, structure–activity relationships of multiplex intrinsic defects and modulated properties still remain to be released for practical applications. Herein, binary intrinsic defects in exfoliated molybdenum disulfide (MoS<sub>2</sub>), including sulfur monovacancies and oxygen substitution, were studied for revealing the sensing mechanism of 2,4,4′-trichlorobiphenyl (PCB28). They theoretically tended to form homosteric associated pairs and promote molecular anchoring synergistically. Appropriate molecular adsorption and efficient electron transfer enabled the excellent sensing performances for PCB28 including considerable linear region of 100 ng mL<sup>−1</sup> ∼ 1 mg mL<sup>−1</sup> and low detection limit of 7.96 ng mL<sup>−1</sup>, which was also inspirable for the design of other small-molecule sensors.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"93 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988061","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}
Wanli Zhang, Xinpeng Mou, Yunpeng Ma, Yi Zheng, Sixu Wang, Liang Shu, Ziwan Du, Chenguang Deng, Qiong Yang, Rong Yu, Jing-Feng Li, Qian Li
PbZrO3 (PZO) thin films, as a classic antiferroelectric material, have attracted tremendous attention for their excellent dielectric, electromechanical, and thermal switching performances. However, several fundamental questions remain unresolved, particularly the existence of an intermediate phase during the transition from the antiferroelectric (AFE) to ferroelectric (FE) state. Here, a phase coexistence configuration of an orthorhombic AFE phase and a tetragonal-like (T-like) phase is reported in epitaxial antiferroelectric PZO thin films, with thickness ranging from 16 to 110 nm. This configuration is evidenced both macroscopically by distinct shoulder-cape-shaped dielectric behavior and microscopically through scanning transmission electron microscopy (STEM) analysis. Remarkably, a 49 nm PZO film achieves an ultrahigh dielectric tunability of 90.1%, while a 59 nm film exhibits significant electromechanical strain of 0.66%. Microscopically, HAADF-STEM reveals the presence of the intermediate phase with a dipole arrangement of vertically diagonal up-up-down-down pattern, and first-principles calculations further confirm the role of this intermediate phase during AFE-to-FE phase transition, which is responsible for the unusual dielectric peaks of ɛr-E curves. These findings not only enhance the understanding of phase transition in antiferroelectric materials but also exhibit great potential for high-performance tunable and nano-electromechanical device applications.
{"title":"Phase Coexistence Induced Giant Dielectric Tunability and Electromechanical Response in PbZrO3 Epitaxial Thin Films","authors":"Wanli Zhang, Xinpeng Mou, Yunpeng Ma, Yi Zheng, Sixu Wang, Liang Shu, Ziwan Du, Chenguang Deng, Qiong Yang, Rong Yu, Jing-Feng Li, Qian Li","doi":"10.1002/smll.202410260","DOIUrl":"https://doi.org/10.1002/smll.202410260","url":null,"abstract":"PbZrO<sub>3</sub> (PZO) thin films, as a classic antiferroelectric material, have attracted tremendous attention for their excellent dielectric, electromechanical, and thermal switching performances. However, several fundamental questions remain unresolved, particularly the existence of an intermediate phase during the transition from the antiferroelectric (AFE) to ferroelectric (FE) state. Here, a phase coexistence configuration of an orthorhombic AFE phase and a tetragonal-like (T-like) phase is reported in epitaxial antiferroelectric PZO thin films, with thickness ranging from 16 to 110 nm. This configuration is evidenced both macroscopically by distinct shoulder-cape-shaped dielectric behavior and microscopically through scanning transmission electron microscopy (STEM) analysis. Remarkably, a 49 nm PZO film achieves an ultrahigh dielectric tunability of 90.1%, while a 59 nm film exhibits significant electromechanical strain of 0.66%. Microscopically, HAADF-STEM reveals the presence of the intermediate phase with a dipole arrangement of vertically diagonal up-up-down-down pattern, and first-principles calculations further confirm the role of this intermediate phase during AFE-to-FE phase transition, which is responsible for the unusual dielectric peaks of <i>ɛ</i><sub>r</sub>-<i>E</i> curves. These findings not only enhance the understanding of phase transition in antiferroelectric materials but also exhibit great potential for high-performance tunable and nano-electromechanical device applications.","PeriodicalId":228,"journal":{"name":"Small","volume":"69 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988106","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}
To reduce the environmental impact of plastics, an increasing number of high-performance sustainable materials have emerged. Among them, wood-based high-performance structural materials have gained growing attention due to their outstanding mechanical and thermal properties. Here, we introduce phosphate groups onto the wood veneers for surface nanofibrillation, effectively altering both the molecular structure and surface morphology of wood, which enhances the interactions between wood veneers and endows the wood with excellent fire resistance properties. With these phosphorylated wood-based building blocks, “chemical welding” structural materials (CWSMs) obtained through chemical cross-linking exhibit excellent mechanical properties. The flexural strength of CWSM reaches 225 MPa, and the modulus reaches 16 GPa, surpassing those of various types of natural wood. At the same time, phosphorylation has endowed CWSM with excellent fire resistance, with a limiting oxygen index reaching 49%, making it completely noncombustible. More importantly, as a biomass-based structural material, CWSM exhibits mechanical, thermal, and fire resistance properties and degradability far superior to those of traditional petroleum-based plastics, making it an ideal candidate for plastic replacement.
{"title":"Strong and Fireproof Regenerated Wood via a Combined Phosphorylation-Surface Nanofibrillation and Ionic Cross-Linking Strategy","authors":"Wen-Bin Sun, Zi-Meng Han, Xiao-Han Luo, Huai-Bin Yang, Zhao-Xiang Liu, De-Han Li, Kun-Peng Yang, Qing-Fang Guan, Shu-Hong Yu","doi":"10.1021/acsnano.4c13857","DOIUrl":"https://doi.org/10.1021/acsnano.4c13857","url":null,"abstract":"To reduce the environmental impact of plastics, an increasing number of high-performance sustainable materials have emerged. Among them, wood-based high-performance structural materials have gained growing attention due to their outstanding mechanical and thermal properties. Here, we introduce phosphate groups onto the wood veneers for surface nanofibrillation, effectively altering both the molecular structure and surface morphology of wood, which enhances the interactions between wood veneers and endows the wood with excellent fire resistance properties. With these phosphorylated wood-based building blocks, “chemical welding” structural materials (CWSMs) obtained through chemical cross-linking exhibit excellent mechanical properties. The flexural strength of CWSM reaches 225 MPa, and the modulus reaches 16 GPa, surpassing those of various types of natural wood. At the same time, phosphorylation has endowed CWSM with excellent fire resistance, with a limiting oxygen index reaching 49%, making it completely noncombustible. More importantly, as a biomass-based structural material, CWSM exhibits mechanical, thermal, and fire resistance properties and degradability far superior to those of traditional petroleum-based plastics, making it an ideal candidate for plastic replacement.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"23 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988170","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}
Xiangyu Jiang, Bo Jiang, Manrui Mu, Tongyi Wang, Shi Sun, Jiaxin Xu, Shutao Wang, Yan Zhou, Jun Zhang, Wenle Li
Core–shell structures demonstrate superior capability in customizing properties across multiple scales, offering valuable potential in catalysis, medicine, and performance materials. Integrating functional nanoparticles in a spatially controlled manner is particularly appealing for developing sophisticated architectures that support heterogeneous characteristics and tandem reactions. However, creating such complex structures with site-specific features remains challenging due to the dynamic microenvironment during the shell-forming process, which considerably impacts colloidal particle assembly. Here, we describe a method to spatially deploy nanoscale assemblies within microscale structures comprising a dense shell and a liquid core through colloidal surface decoration coupled with emulsion-based synthesis. Exploiting a spectrum of nanoparticles grafted with incrementally varying densities of organic ligands, we reveal that nanofeatures can be selectively sculpted onto the shell exterior, within the shell wall, and on the interior surface. The versatility of this mechanism is validated by systematically arranging nanoparticles with various compositions, shapes, and dimensions. Spatially integrated nanotitania endows the core–shell structures with localized photocatalytic abilities. Additionally, distinctive surface modifications enable the simultaneous yet independent implantation of diverse nanoparticles, yielding intricate architectures with programmable functions. This generalizable approach showcases a synthetic strategy to attain structural complexity and functional sophistication reminiscent of those of biological systems in nature.
{"title":"Complex Core–Shell Architectures through Spatially Organized Nano-Assemblies","authors":"Xiangyu Jiang, Bo Jiang, Manrui Mu, Tongyi Wang, Shi Sun, Jiaxin Xu, Shutao Wang, Yan Zhou, Jun Zhang, Wenle Li","doi":"10.1021/acsnano.4c17322","DOIUrl":"https://doi.org/10.1021/acsnano.4c17322","url":null,"abstract":"Core–shell structures demonstrate superior capability in customizing properties across multiple scales, offering valuable potential in catalysis, medicine, and performance materials. Integrating functional nanoparticles in a spatially controlled manner is particularly appealing for developing sophisticated architectures that support heterogeneous characteristics and tandem reactions. However, creating such complex structures with site-specific features remains challenging due to the dynamic microenvironment during the shell-forming process, which considerably impacts colloidal particle assembly. Here, we describe a method to spatially deploy nanoscale assemblies within microscale structures comprising a dense shell and a liquid core through colloidal surface decoration coupled with emulsion-based synthesis. Exploiting a spectrum of nanoparticles grafted with incrementally varying densities of organic ligands, we reveal that nanofeatures can be selectively sculpted onto the shell exterior, within the shell wall, and on the interior surface. The versatility of this mechanism is validated by systematically arranging nanoparticles with various compositions, shapes, and dimensions. Spatially integrated nanotitania endows the core–shell structures with localized photocatalytic abilities. Additionally, distinctive surface modifications enable the simultaneous yet independent implantation of diverse nanoparticles, yielding intricate architectures with programmable functions. This generalizable approach showcases a synthetic strategy to attain structural complexity and functional sophistication reminiscent of those of biological systems in nature.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"98 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988171","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}
Wei Cao, Marc Figueras-Valls, Francesc Viñes, Francesc Illas
The interaction between molybdenum carbide (MoCy) nanoparticles and both flat and curved graphene surfaces, serving as models for carbon nanotubes, was investigated by means of density functional theory. A variety of MoCy nanoparticles with different sizes and stoichiometries have been used to explore different adsorption sites and modes across models with different curvature degrees. On flat graphene, off-stoichiometric MoCy featuring more low-coordinated Mo atoms exhibits stronger interaction and increased electron transfers from the carbide to the carbon substrate. This preferentially occurs through support C and Mo atoms leading to the formation of additional Mo–C bonds. Notably, the MoCy adsorption strength increases on concave surfaces and decreases on convex surfaces, showing a strong linear correlation with the surface curvature. This curvature-dependent behavior alters the charge state of the nanoparticles, making them more/less positively charged in concave/convex regions. The present results demonstrate that the interaction strength can be effectively tuned by manipulating the carbide stoichiometry, the substrate curvature, and the local concave/convex environments, providing valuable guidelines for the rational design of MoCy/C-based catalysts.
{"title":"Understanding the Curvature Effect on the Structure and Bonding of MoCy Nanoparticles on Carbon Supports","authors":"Wei Cao, Marc Figueras-Valls, Francesc Viñes, Francesc Illas","doi":"10.1021/acsami.4c17904","DOIUrl":"https://doi.org/10.1021/acsami.4c17904","url":null,"abstract":"The interaction between molybdenum carbide (MoC<sub><i>y</i></sub>) nanoparticles and both flat and curved graphene surfaces, serving as models for carbon nanotubes, was investigated by means of density functional theory. A variety of MoC<sub><i>y</i></sub> nanoparticles with different sizes and stoichiometries have been used to explore different adsorption sites and modes across models with different curvature degrees. On flat graphene, off-stoichiometric MoC<sub><i>y</i></sub> featuring more low-coordinated Mo atoms exhibits stronger interaction and increased electron transfers from the carbide to the carbon substrate. This preferentially occurs through support C and Mo atoms leading to the formation of additional Mo–C bonds. Notably, the MoC<sub><i>y</i></sub> adsorption strength increases on concave surfaces and decreases on convex surfaces, showing a strong linear correlation with the surface curvature. This curvature-dependent behavior alters the charge state of the nanoparticles, making them more/less positively charged in concave/convex regions. The present results demonstrate that the interaction strength can be effectively tuned by manipulating the carbide stoichiometry, the substrate curvature, and the local concave/convex environments, providing valuable guidelines for the rational design of MoC<sub><i>y</i></sub>/C-based catalysts.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"8 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988325","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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