ACS Applied Materials & Interfaces最新文献

In the past decades, conjugated polyelectrolytes (CPEs) have become prominent in sensing applications due to their unique properties, including strong and tunable light absorption, high sensitivity, water solubility, and biocompatibility. Inspired by mammalian olfactory and gustatory systems, CPE-based sensor arrays have made significant strides in discriminating structurally similar analytes and complex mixtures for various applications. This review consolidates recent advancements in CPE-based sensor arrays, highlighting rational design, controllable fabrication, and effective data processing methods. It covers the fundamentals of CPE fluorescence sensing, emphasizing design strategies for sensor array units and data processing techniques. The broad applicability of CPE-based sensor arrays is demonstrated across diverse domains, including environmental monitoring (e.g., detecting metal ions and explosives), medical diagnostics (e.g., sensing disease markers and analyzing biological samples), and food safety (e.g., assessing the freshness, quality, and source of food products). Further, challenges and future directions in the field are discussed to inspire further research and development in this area.

Rational design of high-performance catalysts for CO₂ electroreduction is crucial for achieving carbon neutrality, yet effective modification strategies remain scarce. In this study, we present the microwave heating approach to incorporate La³⁺ ions into Sn-based perovskite oxides, significantly enhancing their electrocatalytic performance for the reduction of CO₂ to formate. Through comprehensive characterization techniques, including X-ray photoelectron spectroscopy, synchrotron radiation X-ray absorption spectroscopy, electrochemical measurements (Tafel analysis and impedance spectroscopy), and density functional theory calculations, we demonstrate that La³⁺ substitution effectively modulates the Sn-O bond distance in BaSnO₃. This structural modification induces local charge density enrichment, facilitates CO₂ adsorption, and enhances electron transfer kinetics, resulting in a substantial improvement in the formate Faradaic efficiency. In situ Raman spectroscopic analysis and postreaction XPS characterization confirmed the structural integrity of the perovskite framework and the preservation of Sn valence states under negative potentials. This work provides fundamental insights into the CO₂ reduction reaction mechanism on perovskite electrocatalysts and establishes a framework for the design of advanced tin-based electrocatalysts.

Flexible photodetectors have garnered significant attention in recent years due to their vast potential. Among these, amorphous Ga₂O₃ (a-Ga₂O₃) stands out as a highly promising candidate for flexible solar-blind ultraviolet photodetectors, owing to its wide band gap, low-temperature fabrication advantages, and exceptional stability under extreme conditions. However, the fabrication of a-Ga₂O₃ inevitably introduces oxygen vacancy (V_O) defects, leading to declined photodetection performance and compromised corrosion resistance. In this study, we developed a zirconium (Zr) self-compensation doping strategy with concentration optimization to suppress V_O defects, thus enhancing the optoelectronic performance and durability of flexible a-Ga₂O₃ photodetectors. The introduction of Zr significantly eliminated intrinsic V_O defects in Ga₂O₃ films, lowering the dark current by over 3 orders of magnitude from ∼10^-8 to ∼10^-11 A and reducing the response time by a factor of 50, achieving a response time of 6 μs. The detectivity of the optimized devices reached a high level of 3 × 10¹⁴ Jones, indicating exceptional sensitivity to ultraviolet light. Durability tests further demonstrated that the optimized devices exhibited outstanding mechanical robustness, maintaining over 95% of their initial performance after 10,000 bending cycles, and stable photodetection performance even under harsh salt spray conditions for 72 h. This work provides an effective solution for developing high-performance flexible photodetectors tailored for wearable devices and applications in harsh environments.

Endowing flexible sensors with self-powering capabilities is of significant importance. However, the thermoelectric conversion gels reported so far suffer from the limitations of insufficient flexibility, signal distortion under repetitive deformation, and insufficient comprehensive performance, which seriously hinder their wide application. In this work, we designed and prepared eutectogels by an ionic liquid and a polymerizable deep eutectic solvent (PDES), which exhibit good mechanical properties, adhesion, and excellent thermoelectric conversion and thermoelectric response performance. The Seebeck coefficient (S_i) can reach 30.38 mV K^-1 at a temperature difference of 10 K. To amplify the self-powered performance of individual gel units, we assembled them into arrays and further prepared temperature sensors. The combination of the K-means clustering algorithm of machine learning can filter out the noise of traditional thermoelectric sensors and improve the consistency of signals, thereby enabling the prediction of absolute temperature under the conditions of 10 or 20 K temperature difference. This study also demonstrates potential application of these eutectogels in thermoelectric self-powered sensing.

Traditional optical communication systems are constrained by fixed photoresponse values and light intensity, significantly impairing the potential for data transmission and protection. Here, a single-band bipolar-response perovskite self-powered photodetector is demonstrated on the (PEA)₂PbI₄/BaTiO₃/Si heterojunction. By employing BaTiO₃ as the intrinsic layer, the device demonstrates a low dark current on the order of 10^-12 A at a 5 V bias. When BaTiO₃ functions as the ferroelectric layer, the variation in the depolarization field not only achieves multilevel modulation of the photoresponse magnitude but also reverses the sign. Leveraging the bipolar characteristics of the device, a secure optical communication system has been developed, featuring a dual-channel optical signal reception specifically designed for information transmission. One channel is designated for receiving encrypted information, while the other channel receives key information. The device only needs to identify the positive and negative values of the input signals with arbitrary light intensity without distinguishing the strength of the signal values. The accurate retrieval of transmitted information is contingent upon the application of an encryption algorithm, thereby enhancing the security of the communication system. This work provides novel perspectives for the realization of more secure and reliable encrypted optical communication systems.

Lithium (Li) metal is regarded as a desired anode candidate for high-energy-density rechargeable battery systems in the future because of its high specific capacity and low redox potential. However, Li dendritic growth and volume expansion during cycling severely hinder its practical application. Herein, an artificial organophosphorus-inorganic Li hybrid flexbile solid electrolyte interphase (SEI) layer was designed by a prereaction between phytic acid (PA) and lithium hydroxide (LiOH) to generate metal chelates for quick Li⁺ conductivity. The organic-polyphosphate (PALi) layer not only can provide numerous channels for Li⁺ to migrate quickly but also can improve its lithiophilicity due to the uniform distribution of phosphorus (P) in the PALi layer; meanwhile, flexibility due to the existence of hydrogen bonds in the PALi layer effectively alleviates the effect of Li volume expansion on the SEI layer. Therefore, the PALi@Cu∥Li cells exhibit a high Coulombic efficiency of 98.85% over 500 cycles at a current density of 0.5 mA cm^-2, and the PALi@Cu-Li∥Li symmetrical cells also can maintain good cycling stability with low voltage hysteresis of 20 mV for 2000 h at a current density of 1 mA cm^-2. This organic-inorganic hybrid strategy provides a feasible way to fabricate a stable and efficient artificial SEI layer for the practical applications of Li metal batteries.

Photodynamic therapy (PDT) has been utilized to treat various malignant cancers for more than a century. However, many photosensitizers (e.g., derivatives of porphyrins, chlorins, etc.) central to PDT are still suffering from limitations such as water insolubility, dark toxicity, photo/thermal-instability, difficult synthesis/preparation, and poor tumor selectivity. Numerous effective strategies include designing new synthetic photosensitizers by exploiting heavy atom effect, aggregation-induced emission effect (AIE), and electronic/energy effects (donor-acceptor, and Förster resonance energy transfer: FRET), and the linkage of activatable and targeting molecules has been developed to address one or more of these limitations. However, these structural modifications of photosensitizing organic molecules are synthetically challenging and unpredictable in terms of efficacy versus toxicity. Herein, we report a new and simple strategy for effective PDT by combining natural spinach-derived chlorophylls (photosensitizer) with natural water-soluble chlorophyll proteins (WSCPs) derived originally from plants and produced heterologously by bacteria (E. coli). The recombinant WSCPs (chlorophyll-WSCP) are tetrameric and stable under air/thermal conditions and importantly can produce highly reactive singlet oxygen under red/far-red light irradiation to induce cancer cell death. Our in vivo mouse model studies (melanoma xenografts) further validate the efficacy of the recombinant WSCPs as a new class of water-soluble, nontoxic, and highly efficient photosensitizers for PDT. This work represents the first example of the application of WSCPs in PDT and may advance the clinical applications of PDT for cancer treatment.

Two-dimensional (2D) semiconductors have been of great interest in phototransistors in recent years due to their unique optoelectronic and electronic properties. However, their discernible spectral range and the efficiency of light absorption are usually restricted. Here, we present phototransistors based on mixed-dimensional heterostructures formed by zero-dimensional (0D) boron nitride quantum dots (BNQDs) and molybdenum diselenide (MoSe₂), which have high responsivity (R), specific detectivity (D*), and external quantum efficiency (EQE), especially in the ultraviolet (UV) spectral range. The heterostructure phototransistors showed a 440% increase in R at 375 nm (from 5.6 to 24.7 A/W) and a 260% increase in D* (from 3.3 to 8.7 × 10¹¹ Jones) compared to bare MoSe₂ at the wavelength of 375 nm and a bias of 1 V. A series of characterization and comparison experiments show that charge transfer on BNQDs/MoSe₂ results in the photogating effect and optical gain. Meanwhile, the high-performance BNQDs/MoSe₂ heterostructure phototransistors exhibit broadband imaging capabilities and thus hold great promise for ultrasensitive light detection, neuromorphic visual sensing, and in-sensor computing applications.

Emerging as a promising functional material, metal nanoclusters that emit near-infrared (NIR) radiation have garnered significant attention due to their distinctive properties. Nonetheless, the rational design of NIR-emissive metal nanoclusters still faces substantial challenges. Herein, we demonstrate a self-assembly strategy for constructing NIR-emissive nanocomposites (abbreviated as Ag₉-NCs/PEI) using water-soluble Ag₉-NCs (Ag₉(mba)₉, where H₂mba = 2-mercaptobenzoic acid) and branched polyethylenimine (PEI) (M_w = 750,000). The Ag₉-NCs/PEI exhibits excellent phosphorescent properties, demonstrating a broad NIR phosphorescence band spanning from 750 to 1200 nm (NIR: >750 nm) and three-component microsecond lifetimes (τ₁ = 2.22 μs; τ₂ = 33.31 μs; τ₃ = 230.76 μs) at room temperature. This behavior is attributed to the incorporation of three triplet emitting states, as verified by temperature-dependent steady/transient emission spectra and time-resolved transient emission spectra (TRES). More importantly, the Ag₉-NCs/PEI nanocomposite also demonstrates exceptional photothermal conversion properties, with the temperature elevating promptly from 22 to 310 °C within just 10 s upon 660 nm laser irradiation (0.8 W/cm²). The notable phosphorescence, especially in the NIR region, is rarely observed in silver cluster nanocomposites.