Materials Horizons最新文献

Radiative-cooling-driven passive thermoelectric devices (RC-TEDs) offer a potentially sustainable energy solution. However, most RC-TED strategies utilize unsustainable polymers. Herein, a green and sustainable CO₂-crosslinked cellulose (Pulp-CO₂) was developed for simultaneous use as a passive radiative cooling membrane and an ionogel thermoelectric scaffold. The incorporation of CO₂ in the form of carbonate group linkages in the cellulose backbone resulted in a superior passive radiative cooling effect of the membrane and improved the thermoelectric efficiency of the ionogel compared to the pure pulp. The integrated RC-TED, comprising the Pulp-CO₂ membranes and ionogels, exhibited an impressive thermal voltage output of 1200 mV with a subambient temperature reduction of 5.0 °C under simulated solar radiation (280 W m^-2), highlighting its potential in low-grade energy harvesting. Thus, this all-cellulose inspired RC-TED device showcases a promising and sustainable strategy for converting solar energy into electricity cost-effectively.

Radiotherapy has become one indispensable treatment strategy for treating malignant tumors. However, the therapeutic effect of radiotherapy is limited due to the low sensitivity and large side effects of existing radiosensitizers. The rapid development of nanotechnology has created opportunities for various novel kinds of radiosensitizers with excellent radiosensitivity to sprout recently. In particular, due to the ease of modification and potential utilization capacity for a multifunctional radiotherapy platform, semiconductor radiosensitizers have attracted more and more attention. Recently, many novel semiconductor based radiosensitizers have been reported, which provides new ideas for the improvement of radiotherapy efficacy. To make further breakthroughs in semiconductor radiosensitizers, a systematic review is urgently needed and is herein provided. This review first elaborates on the principle of semiconductor induced radiosensitization, and then focuses on strategies such as doping and constructing heterojunctions to enhance the radiosensitivity of semiconductors. Next, it introduces in detail the principle and progress of different types of semiconductor radiosensitizers. Finally, challenges and perspectives of semiconductor radiosensitizers are proposed and discussed, offering guidance for future commercial applications of semiconductor radiosensitizers.

In biochemical sensing, substantial progress has been achieved in the design, development, and application of metallic nanoclusters (NCs) and metal-organic frameworks (MOFs) as distinct entities. Integration of these two nanostructured materials is a promising strategy to form innovative composites with improved properties. Some improvements include (i) supporting platform to minimize the aggregation of NCs and enhance the emission efficiency; (ii) dual-emitting NCs@MOFs from the fluorescent/non-fluorescent MOFs and/or fluorescent NCs; and (iii) stability enhancement. These improvements increase the sensitivity, signal-to-noise ratio, and color tonality, lower the limit of detection, and improve other analytical figures of merits. In this review, we outline the preparation methods of NCs@MOF composites with the improvements offered by them in the field of biochemical analysis. Analytical applications in different fields, such as bioanalysis, environmental monitoring and food safety, are presented. Finally, we address the challenges that remain in the development and application of these composites, such as ensuring stability, enhancing the fluorescence intensity, and improving selectivity and scalability. Furthermore, perspectives on future research directions in this rapidly evolving field are offered.

Dimeric acceptors (DMAs) exhibit significant potential for optimizing both the efficiency and stability of organic solar cells (OSCs). However, medium band-gap DMAs with a high open-circuit voltage (V_oc) for efficient OSCs remain underexplored. In this study, we designed and synthesized a medium bandgap dimeric acceptor, designated DYO-1, through the strategy of alkoxy side-chain substitutions. The resultant DYO-1 exhibited an upshifted lowest unoccupied molecular orbital (LUMO) level and blue-shifted absorption. Notably, an o-xylene (o-XY) processed OSC with a PM6:DYO-1 binary blend achieved an ultra-high V_oc of 1.022 V and a fill factor (FF) of 73.9%, resulting in a power conversion efficiency (PCE) of 15.1%. To our knowledge, this is the highest PCE reported thus far for dimer-based OSCs with a V_oc exceeding 1.0 V. Furthermore, DYO-1 was incorporated into a PM6:L8-BO-X blend film, effectively reducing excessive aggregation of the host blend film, thus improving the carrier transport efficiency and enhancing both the short-circuit current (J_sc) and FF. Alongside the improvement in V_oc, the PM6:L8-BO-X:DYO-1 based ternary OSC, which is prepared using an o-XY solvent, achieved a prominent PCE of 19.6%. Additionally, a module device with an effective area of 13.5 cm² exhibited a PCE of 15.8%, highlighting the potential for large-area fabrications. Our study unveils the importance of medium bandgap dimeric acceptors in achieving efficient and stable OSCs, providing valuable insights into the design of high-performance electron acceptors.

Metastasis is one of the main reasons for cancer treatment failure. Unfortunately, most treatment approaches inevitably damage the extracellular matrix (ECM) during tumor cell elimination, thereby augmenting the risk of metastasis. Herein, we proposed a "sieging tumor cells" strategy based on ferric coordination polymers (FeCPs), which involved anchoring tumor cells through ECM consolidation and selectively eliminating them in the tumor regions. Due to the weak coordination interactions and amorphous structure of FeCPs, the acidic tumor microenvironment facilitated their disintegration, releasing salicylic acid (SA), 2,5-dihydroxyterephthalic acid (DHTA) and Fe³⁺ ions. The released SA inhibited heparinase activity to consolidate the ECM, while Fe-mediated chemodynamic therapy (CDT) was enhanced by DHTA due to its fast electron transport behavior, ultimately inhibiting tumor growth and metastasis. The results from the orthotopic 4T1 breast tumor model indicated that lung metastasis was reduced by about 90%, and the survival rate improved by 70% after FeCP treatment. Overall, this "sieging tumor cells" strategy provides an emerging approach for the treatment of malignant tumors by consolidating the ECM in combination with self-enhanced CDT.

The design of smart photoelectrodes capable of stimulating the localized production of reactive oxygen species (ROS) on demand is of great interest for redox medicine therapies. In this work, poly(3-hexylthiophene) semiconducting polymer nanoparticles (P3HT SPNs) are used with a dual role to fabricate light-responsive hydrogels. First, P3HT SPNs act as visible-light photoinitiators to induce the photopolymerization of acrylic monomers such as acrylamide (AAm), 2-(hydroxyethyl) acrylate (HEA), and poly(ethylene glycol) diacrylate (PEGDA). This leads to the formation of acrylic hydrogels loaded with the P3HT SPNs, as demonstrated by photo-rheology and infrared spectroscopy. Furthermore, P3HT SPNs are also successfully used as photoinitiators for digital light processing (DLP) 3D printing purposes to fabricate shape-defined intelligent hydrogels. Interestingly, P3HT SPNs retain their photoelectrochemical properties when embedded within the polymer hydrogels, showing photocurrent densities that range from ∼0.2 to ∼1.1 μA cm⁻² depending on the intensity of the visible light-lamp (λ = 467 nm). Second, they can be used as photosensitizers (PS) to generate reactive oxygen species (ROS), 12–15 μM H₂O₂, on demand. The acrylic hydrogels containing P3HT SPNs do not exhibit cytotoxic effects under normal physiological conditions in the darkness against mouse glioma 261 (GL261) cells and S. aureus bacteria. However, they induce a ∼50% reduction GL261 cancer cell viability and a ∼99% S. aureus cell death in contact with them upon illumination (λ = 467 nm) due to the localized overproduction of ROS, which makes them attractive candidates for photodynamic therapies (PDT).

Achieving fully transparent electronic devices requires improving p-type transparent conducting materials (TCMs) to match their n-type counterparts. This study explores novel p-type TCMs using high-throughput screening via an automatic spray pyrolysis system. The performance of conducting wide bandgap chalcogenide based on CuS can be improved by incorporating various cations, with Mg emerging as the most promising candidate. The optimized CuS-Mg films exhibited superior transparency and conductivity, comparable to state-of-the-art p-type TCMs. Density functional theory (DFT) calculations linked the inverse correlation between transparency and conductivity to changes in Cu 3d and S 3p orbital coupling with varying Mg content. The best CuS-Mg composition demonstrated high hole concentration (5 × 10²¹ cm^-3), low sheet resistance (266 Ω □^-1), and high transparency (∼75%). The transmittance increased by ∼30% compared with pristine CuS. The successful application of a p-CuS-Mg/n-CdS heterojunction as a semi-transparent photodiode highlights its potential for smart displays and window-integrated electronics. This study demonstrates the value of combining experimental and theoretical methods for accelerated material discovery.

Electrical manipulation of spin-polarized current is highly desirable yet tremendously challenging in developing ultracompact spintronic device technology. Here we propose a scheme to realize the all-electrical manipulation of spin-polarized current in an altermagnetic bilayer. Such a bilayer system can host layer-spin locking, in which one layer hosts a spin-polarized current while the other layer hosts a current with opposite spin polarization. An out-of-plane electric field breaks the layer degeneracy, leading to a gate-tunable spin-polarized current whose polarization can be fully reversed upon flipping the polarity of the electric field. Using first-principles calculations, we show that a CrS bilayer with C-type antiferromagnetic exchange interaction exhibits a hidden layer-spin locking mechanism that enables the spin polarization of the transport current to be electrically manipulated via the layer degree of freedom. We demonstrate that sign-reversible spin polarization as high as 87% can be achieved at room temperature. This work presents the pioneering concept of layer-spintronics which synergizes altermagnetism and bilayer stacking to achieve efficient electrical control of spin.

Achieving precise control over the composition and architecture of nanomaterial-based aerogels remains a significant challenge. Here, we introduce a droplet-templating approach to engineer ultra-lightweight aerogels via the interfacial co-assembly of nanoparticles-surfactants (NPSs) at polar/apolar liquid interfaces. This approach enables the creation of aerogels with tailored compartmentalized or welded bead architectures, exhibiting multilayer, gradient, and hybrid morphologies from a range of 1D and 2D nanomaterials. By precisely controlling evaporation and freeze-drying processes, we fabricate aerogels with customizable micro-domains, without requiring chemical binders. Our approach provides a platform for developing soft materials with tunable properties, paving a new path for applications in soft matter and aerogel engineering.

Anisotropy is a fundamental prerequisite for achieving significant birefringence (Δn) in optical materials, yet optimizing it to surpass the ideal range (Δn > 0.3) remains a substantial hurdle. In the unabated quest for novel birefringent genes, we have figured out that π-conjugated aminopyrazine, [APZ], is capable of producing low-dimensional linear structures for achieving enhanced birefringence due to their structural diversity and inherent anisotropy. Herein, the systematic substitutions of non-π-conjugated [(H₂PO₄)^- and (BF₄)^-] with heteroatom-substituted tetrahedral anions [(CF₃SO₃)^-, (NH₂SO₃)^-, (CH₃SO₃)^-] and subsequently with the aliphatic [C₄H₆O₄] anion, while keeping the cationic end constant, yield a series of seven compounds with a significant boost in Δn_calc = (0.145-0.658@546 nm) which is optimal in their respective families. The substantial increase in birefringence is ascribed to dimensional transition and the propensity of [APZ] to form low-dimensional frameworks, modulated by hydrogen bonds. The intralayer [N-H⋯O], [O-H⋯N], and [N-H⋯F] interactions regulate the perfect coplanar arrangement (ϑ = 0°) of birefringent active units resulting in more pronounced in-plane anisotropy. Moreover, theoretical calculations corroborate that the sequential anion exchange brings variations in optical polarizability, leading to superior linear optical performance of birefringent materials. This work presents a novel birefringent gene, offering promising prospects for synthesizing compounds with exceptional birefringence within low-dimensional systems.