首页期刊导航|Advanced Materials
期刊信息/Journal information
Advanced Materials
VCH Publishers
Advanced Materials

VCH Publishers

半月刊

0935-9648

Advanced Materials/Journal Advanced MaterialsSCIISTPEIAHCI
正式出版
收录年代

    Origin of B-Type Blinking at 2D/3D Heterojunction Interfaces

    Tao ZhouDongyang WanYuwei ZhangLei Gao...
    e10833.1-e10833.8页
    查看更多>>摘要：Photoluminescence blinking is a common phenomenon that occurs across various low-dimensional materials, like 0D quantum dots or 1D nanowires. Two blinking types in 0D and 1D systems have been observed and extensively studied, revealing the mechanisms of non-equilibrium photocarrier kinetics, thereby enhancing emission stability and optimizing emitter performance. However, the origin of blinking in 2D materials is still less understood compared to those in quantum dots and single molecules and only the A-type blinking has been reported. Here, a B-type photoluminescence blinking is identified at the WS_2/Si heterointerface through the statistics of fluorescence lifetime-intensity distribution. Temperature-dependent photoluminescence and transient absorption spectra show that the blinking arises from the dynamic competition between two hot carrier relaxation pathways: one leading to A exciton emission and the other to localized exciton recombination. Moreover, Foerster resonance energy transfer modulates the localized exciton density at the heterointerface and sustains the blinking phenomenon, which is distinct from other B-type blinking. This B-type blinking broadens the understanding of photocarrier dynamics in 2D/3D systems, which will benefit the development of optoelectronic devices based on 2D materials.
      原文链接:
    • NETL
    • NSTL
    • Wiley

    Flow-Regime-Controlled Fabrication of CNT-Bridged Vertically Aligned rGO/MXene Fibers for High-Performance Fiber Supercapacitors

    Tuxiang GuanWeiguo HuShuo ShenYue Han...
    e16561.1-e16561.11页
    查看更多>>摘要：The directional construction of electrode frameworks aligned with the transport pathways of ions/electron is critical for electrochemical processes. However, conventional fabrication strategies suffer from bottlenecks such as complex processes, and difficulty in scaling up production. In this work, a flow-driven wet-spinning strategy is developed to fabricate carbon nanotube (CNT)-bridged vertically aligned reduced graphene oxide (rGO)/MXene fibers (CNT-VA-GMFs). Enabled by precisely regulating of flow regimes, the vertical aligned rGO/MXene nanosheets and CNT-bridged structure collaboratively establish open porous channels for rapid ion transport, continuous conductive networks for efficient electron transfer, and abundant accessible active sites for enhanced charge storage. Consequently, the CNT-VA-GMF electrode exhibits improved ion transport, exceptional specific capacitance (740 F g~(-1),and outstanding long-term cycling stability (98% retention after 30 000 cycles) in H_2SO_4 electrolyte. The assembled flexible asymmetric supercapacitor achieves a remarkable energy density of 224 Wh kg~(-1) (at 1200 W kg~(-1)) while maintaining robust mechanical flexibility.
      原文链接:
    • NETL
    • NSTL
    • Wiley

    Facet-Engineered Rubidium Lead Halide Nanocrystals for Pyro-Phototronic Broadband Photodetection

    Diptam NasipuriSougata KarmakarAkram Hossain SarkarNaveen Goyal...
    e10226.1-e10226.12页
    查看更多>>摘要：Cesium lead halide has been extensively studied as efficient materials for optoelectronic device applications. Beyond Cs(Ⅰ), the exploration of other inorganic A-site monovalent cations remains limited, though Rb(Ⅰ) stands out as a potential alternative whose role in colloidal nanocrystals is largely unexplored. Here, Rb (Ⅰ) is employed as an effective A-site cation in forming monoclinic-phase RbPb_2Cl_5, where Pb (Ⅱ) heptahedrally coordinated. A template-mediated cation exchange strategy is employed where 0D Rb_4CdCl_6 used as host nanocrystals. Upon introduction of Pb (Ⅱ), fast Cd to Pb ion exchange triggers and 2D RbPb_2Cl_5 in rhombic prism, hexagonal prism or hexagonal platelet-shaped nanocrystals are formed depending on the reaction conditions. Further to explore the optoelectronic properties, photo response measurements are carried out which exhibit significant pyro-photocurrent response from these nanocrystals even under ultra-low-intensity light illumination (7 nW cm~(-2)) across ultraviolet (UV) to near-infrared (NIR) spectral range. Despite its centrosymmetric structure, RbPb_2Cl_5 generates pyro-photocurrent due to surface halide deficiencies, supported by DFT which shows surface polarization of |△P| = 0.173 C ~(-2). These findings highlight the pivotal role of Rb (Ⅰ) in stabilizing these nanostructures and open a new avenue for their application in advanced optoelectronic devices.
      原文链接:
    • NETL
    • NSTL
    • Wiley

    Integrated Hollow Microfibers of Covalent Organic Framework on Cu Foil as a Gradient Zn Metal Anode Host for Bottom-Up Deposition

    Huan YuShichao SunMingzai WuChangzhou Yuan...
    e17197.1-e17197.9页
    查看更多>>摘要：Rechargeable aqueous Zn metal batteries are promising choices for future grid-scale energy storage because of cost-effectiveness, high-rate performance and safety. Nonetheless, the sluggish desolvation of hydrated Zn~(2+) ions usually leads to uncontrolled Zn dendrite growth and detrimental side reactions on Zn metal anodes (ZMAs). Herein, we report the formation of integrated hollow microfibers of covalent organic frameworks on Cu foil (denoted as HMCOF-Cu) as a ZMA host with gradient design. Of note, interactions between carbonyl groups of HMCOF and H_2O in [Zn(H_2O)6]~(2+) promote rapid desolvation of hydrated Zn~(2+). Besides, 3D HMCOF network can accelerate Zn~(2+) diffusion and accommodate the volumetric deformation during the deposition/stripping cycles. Moreover, the gradient design can induce bottom-up deposition for dendrite-free ZMA. As a result, the HMCOF-Cu host enables stable Zn plating/stripping processes over 2500 h at 10 mA cm~(-2) . Moreover, the full cell based on HMCOF-Cu@Zn anode presents a long-term stability over 7000 cycles at 10 A g~(-1) .
      原文链接:
    • NETL
    • NSTL
    • Wiley

    Frontal Polymerization-Enabled 3D Printing of Recyclable High-Performance Carbon Fiber Reinforced Polymers

    Siqi HuangZhuangpeng ChenZhijie FengHongchao Zhao...
    e15033.1-e15033.13页
    查看更多>>摘要：Thermoset composites often face a challenging trade-off between recyclability and high performance. In this study, an innovative closed-loop manufacturing approach that integrates frontal ring-opening metathesis polymerization (FROMP) with 3D printing to produce fully recyclable carbon fiber-reinforced polymers (c-CFRPs) is presented. A self-propagating FROMP-enabled direct ink writing (DIW) printing technology is developed, enabling in situ curing within seconds. This breakthrough eliminates the need for post-processing and reduces energy consumption by two orders of magnitude compared to traditional autoclave methods. By copolymerizing dicyclopentadiene (DCPD) with a commercial spiroacetal monomer (≤3 wt.%), acid-degradable resins that retain the tensile strength of conventional thermosets are introduced while allowing for matrix depolymerization under mild conditions. The DCPD-based c-CFRPs demonstrate remarkable tensile strengths of up to 817 MPa and glass transition temperatures exceeding 160℃. In a significant advancement, the recovered carbon fibers retain their pristine morphology and over 95% of their original mechanical properties, enabling repeated recycling without performance loss. Additionally, recovered oligomers can be repolymerized into new resins, further enhancing sustainability. This work presents a groundbreaking solution for high-performance composite manufacturing, addressing critical energy and waste challenges in the thermoset industry.
      原文链接:
    • NETL
    • NSTL
    • Wiley

    Infrared and Thermo Co-Driven Catalysis for CO_2 Conversion to Valuable Chemicals

    Enqi ChenChao WangLunqiao XiongYaxuan Zheng...
    e12626.1-e12626.12页
    查看更多>>摘要：Conversion of CO_2 into high value chemicals presents a promising pathway for CO_2 mitigation and utilisation. The direct synthesis of dimethyl carbonate from CO_2 and methanol is one of such carbon-neutral pathways. However, thermal catalytic processes for direct dimethyl carbonate synthesis have reached a performance bottleneck at elevated temperatures. This work explores the synergy of photon and thermal energy to enhance the dimethyl carbonate production rate to 30 mmol/g/h, together with 100% selectivity, thanks to a defect-modified and noble-metal free cerium oxide catalyst. Fundamentally, it is found that the defects in cerium oxide can provide energy levels that enable IR light absorption and generate holes with a moderate oxidation potential, so avoiding the unfavorable overoxidation pathway and enhancing the production rate of dimethyl carbonate. The thermal energy has been proved to remarkably facilitate the relaxation of IR-induced charge carriers and to enhance the dimethyl carbonate formation process. This work introduces a strategy of IR photons and thermo co-driven catalysis and achieves a breakthrough in dimethyl carbonate formation.
      原文链接:
    • NETL
    • NSTL
    • Wiley

    A Sono-Responsive Nanoplatform Integrating STING Activation and CXCR4 Blockade for Synergistic Immunotherapy of Glioblastoma

    Xiaoying KangWenwen ChenYuan ZhangJingyi Ma...
    e12104.1-e12104.18页
    查看更多>>摘要：Glioblastoma (GBM), an aggressive brain tumor with a highly immunosuppressive microenvironment, remains a therapeutic challenge due to its resistance to conventional treatments. In this study, a novel multi-function therapeutic platform that integrates ultrasound-triggered sonodynamic therapy (SDT), STING pathway activation, and CXCR4 inhibition for synergistic immunotherapy of GBM is presented. Through systematic comparison of a series of organic molecules with subtle substituted atom alterations, a new selenium-containing compound is identified with outstanding sonodynamic properties. The high-performance sonosensitizer is co-assembled with a STING agonist prodrug, which is further cloaked with glioma cell membrane and CXCR4-targeting peptides for dual homing and immune modulation. Under ultrasound irradiation, the nanoplatform triggers robust reactive oxygen species production, in combination with the self-accelerating STING agonist release, significantly stimulating both innate and adaptive immune responses while disrupting the CXCL12/CXCR4 signaling axis to suppress immunosuppressive cell infiltration. This tripartite strategy, which integrates SDT-mediated tumor ablation, STING-induced systemic immunity, and CXCR4 blockade, synergistically suppresses primary tumor growth, prevents postoperative recurrence, and extends survival in GBM-bearing mice. This approach presents a promising sono-triggered multimodal paradigm for overcoming GBM’s immunosuppressive barriers and enhancing therapeutic outcomes.
      原文链接:
    • NETL
    • NSTL
    • Wiley

    Disorder Scattering Induced Large Room Temperature Nonlinear Anomalous Hall Effect in a Semiconductor CdGeAs_2

    Seng Huat LeeTakumi IwayaKosuke NakayamaTing Yong Lim...
    e14217.1-e14217.9页
    查看更多>>摘要：The nonlinear Hall effect (NLHE) with time-reversal symmetry has emerged as a transformative phenomenon within the Hall effect family, attracting significant interest due to its profound implications for both fundamental physics and technological applications. While prior studies have predominantly focused on NLHE in 2D materials, advancements in practical applications have been constrained by low operating temperatures and limited responsivity, typically below 10~(-4) m/V. Achieving significant responsivity at room temperature (RT) in 3D systems has proven challenging, particularly for scattering-induced NLHE. Here, the discovery of disorder scattering-induced NLHE in chalcopyrite-type CdGeAs_2 bulk single crystals is reported, demonstrating a remarkable responsivity of up to 10~(-3) m/V at RT. The studies reveal that NLHE not only facilitates ac-driven second harmonic and rectification Hall responses but also induces an exceptionally large anomalous Hall angle. Through band structure measurements by ARPES, DFT calculations, as well as symmetry and nonlinear Hall conductivity scaling analyses, disorder scattering is identified as the dominant mechanism for the NLHE in CdGeAs_2. Leveraging the observed strong responsivity of NLHE at RT, its broadband electronic frequency mixing capability in the MHz range is further demonstrated. This work sets the foundation for integrating scatteringinduced NLHE in 3D materials into very high-frequency mixing technologies.
      原文链接:
    • NETL
    • NSTL
    • Wiley

    Promoting Active Hydrogen Supply and Nitrate Adsorption by Disordering Tetrahedral-Octahedral Structure of CuAl_2O_(4-δ) for Efficient Nitrate Reduction

    Liyan NiuYasen WangHaitao YinTan Wang...
    e17303.1-e17303.11页
    查看更多>>摘要：Modulating the local coordination environment can optimize the electronic structure and reaction pathway of nitrate reduction to ammonia (NO_3RR), beneficial to enhance the catalytic activity and selectivity. Herein, a disordered tetrahedral-octahedral structure of CuAl_2O_(4-δ)(CAO) is proposed by Co doping as an efficient catalyst. Theoretical calculations reveal Co doping induces strong Co-Al orbital interactions at octahedral sites, which lowers the energy barrier for water dissociation, and meanwhile, Oxygen vacancies (Vos) induced by Co doping not only enhance NO_3~-adsorption, but also serve as reservoir sites for transient *H storage, thereby promoting hydrogenation steps. The synergistic Cu-Vo interaction facilitates the conversion of *NO_3~- to *NO_2~– and the interfacial electron transfer between Co and Cu suppresses the hydrogen evolution reaction (HER). The substitution of 30% Co in CAO (Co-3) nanofibers creates the most Vos, resulting in a high Faradaic efficiency (FE) of 92.00% and a substantial NH3 yield rate of 27.86 mg h~(-1) mg~(-1) cat. in neutral media. Additionally, it exhibits exceptional long-term electrochemical durability and chemical stability. Thermodynamic analysis unveils the potential-determining step of *NO_2 to *NO for Co-3 possesses a low free energy of only 0.05 eV, highly superior to 0.29 eV for the pristine CAO.
      原文链接:
    • NETL
    • NSTL
    • Wiley

    Nanopore-Based Label-Free and Single-Molecule Sequencing toward Precision Diagnosis

    Yufan CuiYueming ZhaiYongxi ZhaoXingyi Ma...
    e13613.1-e13613.37页
    查看更多>>摘要：Nanopore-based single-molecule sequencing (SMS) is a powerful tool for acquiring detailed heterogeneous information on critical building blocks of life, such as nucleic acids, proteins, and a wide array of biomolecules, at the single-molecule level. Real-time current-intensity fluctuations corresponding to the passage of target molecules through nanopores enable long-read length, high-throughput, and high-accuracy detection, thus meeting the stringent demands of precision diagnosis. Herein, a concise overview of various principles and fabrication methods is provided for nanopores, with particular emphasis on recent advancements in nanopore-based DNA and protein sequencing, revealing innovative approaches for effectively capturing and translocating target molecules, and rapid and accurate identification. Further typical cases of nanopore-based SMS applications in precision diagnosis are analyzed, focusing on genetic disorders, infectious diseases, cancers, and abnormal post-translational modifications to highlight the clinical potential of nanopores. Additionally, the inherent limitations and challenges of nanopores in terms of sensitivity, detection range, and selectivity are discussed and present the latest strategies for enhancing nanopore performance. Finally, perspectives are provided on the future of nanopore-based SMS, particularly at the intersection of microfluidic devices, surface functionalization, and machine learning, to facilitate more diverse and advanced developments in this field.
      原文链接:
    • NETL
    • NSTL
    • Wiley