ACS Materials Letters最新文献

Proton transport via a dynamic chemistry method is an essential pathway in both biology and chemistry. In chemical catalysis, proton-shuttling catalysts were developed by mimicking the proton-transport processes in biological systems. However, YH (Y = O, N, S, etc.) units are typically essential for enabling proton transport in these catalysts. Herein, we present a novel strategy for constructing in situ reversible proton-shuttling covalent organic framework catalysts, avoiding the need for Y–H functional groups. Specifically, we demonstrate that the 2D bis(imino)pyridine Cu-bipy-COF material could transform to a water proton-shuttling catalyst by using the reversible interconversion between imine and hemiamine. This catalyst could effectively catalyze the hydration of benzonitrile in neat water without the use of a toxic organic solvent.

CuS nanomaterials have attracted much attention for tumor therapy because of their excellent photothermal and photodynamic properties. Notably, Cu₂O can be converted in situ to CuS through sulfurization by H₂S in tumor cells. However, this approach is currently limited to colon cancer because other tumors exhibit comparatively lower H₂S concentrations. Herein, we reported a nanoplatform consisting of two key components, diallyl trisulfide (DATS) and Cu₂O-coated nanogapped gold nanoparticle (AuNNP). DATS reacted with upregulated glutathione (GSH) in tumor cells to release H₂S for gas therapy as well as the sulfurization of Cu₂O. AuNNPs further enhanced the photothermal and photodynamic effect of the in situ-formed CuS via surface plasmon resonance effect. Both H₂S-induced gas therapy and CuS-mediated photothermal/photodynamic therapy exhibited much higher toxicity to tumor cells than to normal cells. Given that GSH is typically overexpressed in cancer cells, the developed strategy is thus generally applicable for almost any tumors.

Currently, long-wavelength carbon dots have garnered widespread attention from researchers due to their unique luminescent properties. However, the industrial-scale production of carbon dots presents an inevitable challenge. This study successfully synthesized long-wavelength, fluorescence-tunable carbon dots (T-CDs) in gram-scale yield using a one-pot solvothermal method, followed by simple water washing for purification. The synthesized T-CDs exhibited tunable fluorescence in different solvents due to the combined effects of solvent polarity and hydrogen bond donor. Furthermore, solid-state tunable fluorescence was achieved in various matrices, and light-emitting diodes with various emission colors were prepared. High-efficiency white light-emitting diodes were fabricated based on T-CDs, exhibiting CIE color coordinates of (0.35, 0.35), a color rendering index of 91, and excellent luminescence performance and photostability. This study provides a straightforward method for gram-scale preparation of long-wavelength carbon dots, holding significant value in achieving tunable fluorescence in solution, the solid state, and high-performance lighting applications.

Nanotechnology is a promising strategy in the fight against cancer by leveraging the unique properties of nanomaterials for targeted drug delivery. A significant challenge in this domain is overcoming biological barriers and ensuring precise delivery to tumor sites. Immune cells, inherently adept at navigating the body’s defense systems and homing to tumor sites, present an excellent solution as Trojan horses for cancer nanotherapy. This review explores the utilization of immune cells as carriers or mediators of nanoparticle-based therapeutics. The Trojan horse strategy is presented in the context of nanomedicine and cancer, followed by a discussion of its advantages. Next, the diversity of nanoparticle systems that have shown positive therapeutic outcomes in preclinical studies is explored. The challenges of using immune cells as Trojan horses, such as nanoparticle loading and manipulation, are analyzed. Finally, strategies for fine-tuning nanoparticles to design an effective Trojan horse approach are suggested. By synthesizing current research findings, this review underscores the potential of nanotechnology in combination with immune cells for innovative and effective cancer treatments.

Metal-oxide semiconductor sensing materials with excellent sensing performance are highly desired for the detection of toxic, volatile, and flammable gases. However, the lack of material structure–property relationships and gas-sensing mechanisms has severely limited the rational design of gas-sensing materials. Herein, we try to understand how the electronic structure, d-band center, and atomic orbital bonding influence the gas adsorption energy, which exhibits a strong correlation with both the selectivity and sensitivity of gas-sensing materials. As a result, the lattice distortion induced by introducing heteroatoms prompts La atoms to actively participate in the gas adsorption process, which leads to the formation of multiatomic orbital hybridization bonds, significantly increasing the adsorption energy of ethanol and acetone molecules. This work illustrates that creating greater lattice distortion is an effective strategy to modulate the strength of gas adsorption, which is important for guiding the design and synthesis of metal-oxide semiconductor gas-sensing materials.

Luminescent solar concentrators (LSCs) are promising large-scale sunlight collectors for photovoltaics due to their affordability and suitability for building-integrated photovoltaics (BIPVs). However, the low photoluminescent efficiency, narrow Stokes shift, and poor processability of most luminescent materials restrain the performance of the fabricated transparent LSCs. This work reports a copper-iodide (Cu–I) cluster-based luminescent hybrid for high-performance LSCs. This C₁₁₄H₁₀₃Cu₄I₄N₂O₂P₆ (abbreviated as CuI-1) hybrid with the ethoxy solubilizing groups shows a significant Stokes shift of 219 nm, high photoluminescence quantum yield (PLQY) of 97.9%, and excellent solubility in polar organic solvents. We fabricated the transparent CuI-1/PVP-based LSCs via facile doctor blade coating, which achieves a η_opt of 5.89% and a η_PCE of 3.04%. In addition, we developed a series of Cu–I cluster hybrids by ligand modification for LSCs, which all display excellent optical properties for LSCs. Our results show the potential of Cu–I cluster-based hybrids for high-performance LSCs in BIPV systems.

Photocurable self-healing elastomers are promising candidates for producing complex soft devices that can mend damage. However, the practicality of these materials is limited by reliance on external stimuli, custom synthesis, manual realignment, and multihour healing cycles. This paper introduces a tough 3D-printable hybrid acrylate/thiol-ene elastomer (prepared with commercially available precursors) that exhibits nearly instantaneous damage repair in the absence of external stimuli. This rapid, hydrogen bond-driven self-healing enables meaningful restoration of mechanical properties, including tensile strains up to 344% post-damage. Furthermore, structured herringbone grafts are showcased as a compelling strategy to enable cohesive failure away from healed interfaces, realizing up to 18× increases in toughness from only modest increases in interfacial surface area. Prototype soft robotic devices fabricated using vat photopolymerization demonstrate self-healing within seconds under ambient conditions and without external intervention. These results demonstrate a scalable strategy to provide real-time, autonomous functionality restoration in damaged soft devices.

Photocurable self-healing elastomers are promising candidates for producing complex soft devices that can mend damage. However, the practicality of these materials is limited by reliance on external stimuli, custom synthesis, manual realignment, and multihour healing cycles. This paper introduces a tough 3D-printable hybrid acrylate/thiol-ene elastomer (prepared with commercially available precursors) that exhibits nearly instantaneous damage repair in the absence of external stimuli. This rapid, hydrogen bond-driven self-healing enables meaningful restoration of mechanical properties, including tensile strains up to 344% post-damage. Furthermore, structured herringbone grafts are showcased as a compelling strategy to enable cohesive failure away from healed interfaces, realizing up to 18× increases in toughness from only modest increases in interfacial surface area. Prototype soft robotic devices fabricated using vat photopolymerization demonstrate self-healing within seconds under ambient conditions and without external intervention. These results demonstrate a scalable strategy to provide real-time, autonomous functionality restoration in damaged soft devices.

Organic room temperature phosphorescence (RTP) has attracted increasing attention owing to its unique luminous properties and wide applications. However, the trade-off between the phosphorescence quantum yield (Φ_Phos) and the phosphorescence lifetime (τ_Phos) highlights the necessity for developing new strategies to enhance RTP performance. While research often focuses on guest components in polymer-based host–guest RTP systems, the host materials, which provide rigid environments, are less explored. This work introduces a simple and efficient strategy to develop RTP materials with high efficiency and long lifetime by employing covalent cross-linking to modify the rigidity of the polymer matrix. By suppressing nonradiative decay and decreasing luminescence quenching under ambient conditions, not only the Φ_Phos of cross-linked films is improved from 3.2% to 13.5%, but also the τ_Phos is extended from 482.34 to 625.23 ms. Thanks to its solution processability and water sensitivity, this RTP system was successfully applied in inkjet printing and binary anticounterfeiting.

Metal halide perovskite quantum dots (PQDs) are promising for next-generation optical displays, yet challenges persist in achieving pure-red emission (620–640 nm) due to a lack of effective ligand exchange methods for enhancing charge carrier transfer and stabilizing the PQDs structure/size during post-treatment. Herein, we report spectrally stable and efficient pure-red light-emitting diodes (LEDs) realized through sequential ligand post-treatment of all-inorganic CsPbI₃ PQDs. The as-synthesized CsPbI₃ PQDs (∼4 nm) undergo sequential purification steps, employing trioctylphosphine oxide (TOPO) and guanidinium iodide (GUAI) as ligands. This approach preserves the size and structure of the CsPbI₃ PQDs after two purification washes, improving the optoelectronic properties of CsPbI₃ PQD films and enables a stable electroluminescent emission centered at 640 nm with an external quantum efficiency (EQE) peaking near 15%. Our sequential ligand post-treatment successfully prevents the aggregation and coarsening of PQDs, presenting a novel approach toward enhancing the stability and efficiency of PQD-based LED technologies.