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Zinc oxide nanoparticles (ZnO NPs) have been actively pursued as the most effective electron transport layer for quantum-dot light-emitting diodes (QLEDs) in light of their unique optical and electronic properties and low-temperature processing. However, the high electron mobility and smooth energy level alignment at QDs/ZnO/cathode interfaces cause electron over-injection, which aggravates non-radiative Auger recombination. Meanwhile, the abundant defects hydroxyl group (-OH) and oxygen vacancies (O V ) in ZnO NPs act as trap states inducing exciton quenching, which synergistically reduces the effective radiation recombination for degrading the device performance. Here, we develop a bifunctional surface engineering strategy to synthesize ZnO NPs with low defect density and high environmental stability by using ethylenediaminetetraacetic acid dipotassium salt (EDTAK) as an additive. The additive effectively passivates surface defects in ZnO NPs and induces chemical doping simultaneously. Bifunctional engineering alleviates electron excess injection by elevating the conduction band level of ZnO to promote charge balance. As a result, state-of-the-art blue QLEDs with an EQE of 16.31% and a T 50 @100 cd m -2 of 1685 h are achieved, providing a novel and effective strategy to fabricate blue QLEDs with high efficiency and a long operating lifetime.

Due to the fast phase separation kinetics and small feature size, the self-assembly of giant molecules has attracted lots of attention. However, there is not much study on multicomponent giant surfactants. In this work, through a modular synthetic strategy, different polyhedral oligomeric silsesquioxane (POSS)-based molecular nanoparticles are installed with diverse functionalities (hydrophobic octavinyl POSS (VPOSS), hydrophilic dihydroxyl-functionalized POSS (DPOSS), and omniphobic perfluoroalkyl-chain-functionalized POSS (FPOSS)) on the ends of one polystyrene (PS) chain to build up a series of triblock bola-form giant surfactants denoted as XPOSS-PS n -FPOSS (X represents V or D). The target molecules are prepared by a combination of atom transfer radical polymerization (ATRP), esterification, as well as Cu(I)-catalyzed azide-alkyne cycloaddition (CuAAC) and thiol-ene "click" reactions. These macromolecules are thoroughly characterized by combined technologies including nuclear magnetic resonance (NMR), size exclusion chromatography (SEC), and matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS) analyses. It is revealed by small angle X-ray scattering (SAXS) and transmission electron microscopy (TEM) that VPOSS-PS n -FPOSS adopts a two-phase separation scenario where VPOSS and POSS are segregated in one phase. DPOSS-PS n -FPOSS with a third hydrophilic DPOSS shows a three-phase separation scenario, where highly ordered phase structures are difficult to develop owing to the competition of mutual phase separation processes and may be trapped in kinetically metastable states., (© 2022 Wiley-VCH GmbH.)

PROteolysis TArgeting Chimeras (PROTACs) has been exploited to degrade putative protein targets. However, the antitumor performance of PROTACs is impaired by their insufficient tumour distribution. Herein, we present de novo designed polymeric PROTAC (POLY-PROTAC) nanotherapeutics for tumour-specific protein degradation. The POLY-PROTACs are engineered by covalently grafting small molecular PROTACs onto the backbone of an amphiphilic diblock copolymer via the disulfide bonds. The POLY-PROTACs self-assemble into micellar nanoparticles and sequentially respond to extracellular matrix metalloproteinase-2, intracellular acidic and reductive tumour microenvironment. The POLY-PROTAC NPs are further functionalized with azide groups for bioorthogonal click reaction-amplified PROTAC delivery to the tumour tissue. For proof-of-concept, we demonstrate that tumour-specific BRD4 degradation with the bioorthogonal POLY-PROTAC nanoplatform combine with photodynamic therapy efficiently regress tumour xenografts in a mouse model of MDA-MB-231 breast cancer. This study suggests the potential of the POLY-PROTACs for precise protein degradation and PROTAC-based cancer therapy., (© 2022. The Author(s).)

Having benefited from the combination of different therapeutic modalities, functionalized nanoplatforms with synergistic strategies have aroused great interest in anticancer treatment. Herein, an engineered, a biodegradable hollow mesoporous organosilica nanoparticle (HMON)-based nanoplatform was fabricated for photothermal-enhanced chemotherapy of tumor. For the first time, we demonstrated that HMONs could serve as nanocarriers for co-delivering of both the paclitaxel and photothermal agent new indocyanine green (IR820), denoted as Paclitaxel/IR820@ HMONs-PEG. The as-prepared nanosystem exhibited a high paclitaxel-loading capacity of 28.4%, much higher than most paclitaxel-loaded nanoformulations. Furthermore, incorporating thioether bonds (S-S) into the HMONs' framework endowed them with GSH-responsive biodegradation behavior, leading to the controllable release of drugs under a tumor reducing microenvironment, and hindered the premature release of paclitaxel. Upon being irradiated with an NIR laser, the obtained co-delivery nanosystem exhibited great photothermal properties generated from IR820. The fabricated nanocomposites could significantly suppress tumor growth under NIR laser irradiation, as validated by in vitro and in vivo assessments. Combined with outstanding biocompatibility, the constructed nanosystem holds great potential in combinational antitumor therapy.

Immunotherapy shows promising therapeutic potential for long-term tumor regression. However, current cancer immunotherapy displays a low response rate due to insufficient immunogenicity of the tumor cells. To address these challenges, herein, intracellular-acidity-activatable dynamic nanoparticles for eliciting immunogenicity by inducing ferroptosis of the tumor cells are engineered. The nanoparticles are engineered by integrating an ionizable block copolymer and acid-liable phenylboronate ester (PBE) dynamic covalent bonds for tumor-specific delivery of the ferroptosis inducer, a glutathione peroxidase 4 inhibitor RSL-3. The nanoparticles can stably encapsulate RSL-3 inside the hydrophobic core via π-π stacking interaction with the PBE groups at neutral pH (pH = 7.4), while releasing the payload in the endocytic vesicles (pH = 5.8-6.2) by acidity-triggered cleavage of the PBE dynamic covalent bonds. Furthermore, the nanoparticles can perform acid-activatable photodynamic therapy by protonation of the ionizable core, and significantly recruit tumor-infiltrating T lymphocytes for interferon gamma secretion, and thus sensitize the tumor cells to RSL-3-inducible ferroptosis. The combination of nanoparticle-induced ferroptosis and blockade of programmed death ligand 1 efficiently inhibits growth of B16-F10 melanoma tumor and lung metastasis of 4T1 breast tumors, suggesting the promising potential of ferroptosis induction for promoting cancer immunotherapy., (© 2021 Wiley-VCH GmbH.)

Prodrug nanoparticles that codeliver the immune modulators to the tumor site are highly recommendable for cancer immunotherapy yet remain challenging. However, effective stimuli-responsive strategies that exploit the endogenous hallmarks of the tumor have paved the way for cancer immunotherapy. For the first time, the development of the Boolean logic prodrug nanoparticles (BLPNs) for tumor-targeted codelivery of immune modulators (e.g., immune activator and immune inhibitor) and combination immunotherapy is reported herein. A library of stimuli-activatable BLPNs is fabricated yielding YES/AND logic outputs by adjusting the input combinations, including extracellular matrix metalloproteins 2/9 (MMP-2/9), intracellular acidity (pH = 5.0-6.0), and reduction (glutathione) in the tumor microenvironment. Tunable and selective control over BLPNs dissociation and prodrug activation is achieved by specifying the connectivity of orthogonal stimuli-labile spacers while exploiting the endogenous signals at the tumor sites. The tumor-specific distribution of the BLPNs and stimuli-activation of the immune modulators for highly efficient cancer immunotherapy are further demonstrated. The results reported in this study may open a new avenue for tumor-specific delivery of immune therapeutics and precise cancer immunotherapy., (© 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Immunological tolerance of tumors is characterized by insufficient infiltration of cytotoxic T lymphocytes (CTLs) and immunosuppressive microenvironment of tumor. Tumor resistance to immune checkpoint inhibitors due to immunological tolerance is an ongoing challenge for current immune checkpoint blockade (ICB) therapy. Here, we report the development of tumor microenvironment-activatable anti-PDL1 antibody (αPDL1) nanoparticles for combination immunotherapy designed to overcome immunological tolerance of tumors. Combination of αPDL1 nanoparticle treatment with near-infrared (NIR) laser irradiation-triggered activation of photosensitizer indocyanine green induces the generation of reactive oxygen species, which promotes the intratumoral infiltration of CTLs and sensitizes the tumors to PDL1 blockade therapy. We showed that the combination of antibody nanoparticles and NIR laser irradiation effectively suppressed tumor growth and metastasis to the lung and lymph nodes in mouse models. The nanoplatform that uses the antibody nanoparticle alone both for immune stimulation and PDL1 inhibition could be readily adapted to other immune checkpoint inhibitors for improved ICB therapy., (Copyright © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works.)

Checkpoint blockade immunotherapy is promising for clinical treatment of various malignant tumors. However, checkpoint blockade immunotherapy suffers from a low response rate due to insufficient tumor immunogenicity and the immunosuppressive tumor microenvironment (ITM). In this study, a tumor-microenvironment-activatable binary cooperative prodrug nanoparticle (BCPN) is rationally designed to improve immunotherapy by synergistically modulating the immune tumor microenvironment. BCPN is purely constructed from a tumor acidity and reduction dual-responsive oxaliplatin (OXA) prodrug for triggering immunogenic cell death (ICD) and eliciting antitumor immunity, and a reduction-activatable homodimer of NLG919 for inactivating indoleamine 2,3-dioxygenase 1, which is a key regulator for ITM. Upon tumor-acidity-triggered cleavage of the poly(ethylene glycol) shell, PN shows negative to positive charge switch for enhanced tumor accumulation and deep penetration. OXA and NLG919 are then activated in the tumor cells via glutathione-mediated reduction. It is demonstrate that activated OXA promotes intratumoral accumulation of cytotoxic T lymphocytes by triggering ICD of cancer cells. Meanwhile, NLG919 downregulates IDO-1-mediated immunosuppression and suppresses regulatory T cells. Most importantly, PN shows much higher efficiency than free OXA or the combination of free OXA and NLG919 to regress tumor growth and prevent metastasis of mouse models of both breast and colorectal cancer., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Cancer immunotherapy is impaired by the intrinsic and adaptive immune resistance. Herein, a bispecific prodrug nanoparticle was engineered for circumventing immune evasion of the tumor cells by targeting multiple immune resistance mechanisms. A disulfide bond-linked bispecific prodrug of NLG919 and JQ1 (namely NJ) was synthesized and self-assembled into a prodrug nanoparticle, which was subsequently coated with a photosensitizer-modified and tumor acidity-activatable diblock copolymer PHP for tumor-specific delivery of NJ. Upon tumor accumulation via passive tumor targeting, the polymeric shell was detached for facilitating intracellular uptake of the bispecific prodrug. NJ was then activated inside the tumor cells for releasing JQ1 and NLG919 via glutathione-mediated cleavage of the disulfide bond. JQ1 is a bromodomain-containing protein 4 inhibitor for abolishing interferon gamma-triggered expression of programmed death ligand 1. In contrast, NLG919 suppresses indoleamine-2,3-dioxygenase 1-mediated tryptophan consumption in the tumor microenvironment, which thus restores robust antitumor immune responses. Photodynamic therapy (PDT) was performed to elicit antitumor immunogenicity by triggering immunogenic cell death of the tumor cells. The combination of PDT and the bispecific prodrug nanoparticle might represent a novel strategy for blockading multiple immune evasion pathways and improving cancer immunotherapy. Tumor microenvironment-activatable bispecific prodrug nanoparticles are reported for combinatory immunotherapy, which are composed of photosensitizer and bispecific prodrug for eliciting antitumor immunogenicity via photodynamic therapy, and circumventing inducible immune resistance. [Display omitted] [ABSTRACT FROM AUTHOR]

To improve quantum dot solar cell performance, it is crucial to make efficient use of the available incident sunlight to ensure that the absorption is maximized. The ability of metal nanoparticles to concentrate incident sunlight via plasmon resonance can enhance the overall absorption of photovoltaic cells due to the strong confinement that results from near-field coupling or far-field scattering plasmonic effects. Therefore, to simultaneously and synergistically utilize both plasmonic effects, the placement of different plasmonic nanostructures at the appropriate locations in the device structure is also critical. Here, we introduce two different plasmonic nanoparticles, Au and Ag, to a colloidal PbS quantum dot heterojunction at the top and bottom interface of the electrodes for further improvement of the absorption in the visible and near-infrared spectral regions. The Ag nanoparticles exhibit strong scattering whereas the Au nanoparticles exhibit an intense optical effect in the wavelength region where the absorption of light of the PbS quantum dot is strongest. It is found that these dual-plasmon layers provide significantly improved short-circuit current and power conversion efficiency without any form of trade-off in terms of the fill factor and open-circuit voltage, which may result from the indirect contact between the plasmonic nanoparticles and colloidal quantum dot films. [ABSTRACT FROM AUTHOR]

The modification of the equilibrium morphology to expose active facets of cobalt nanoparticles is essential for tailoring and controlling its catalytic performance. Periodic density functional theory (DFT) was applied to systematically investigate the structure and stability of exposed facets of hcp Co nanoparticles induced by Ru promoter in order to clarify the facet‐dependent equilibrium morphology of hcp Co nanoparticles stabilized by Ru promoter. The adsorption and migration of Ru atom can give rise to the change of the surface energy of exposed facets, thus affecting the equilibrium morphology of the hcp Co nanoparticles. Selectively exposed the high Miller index facets, such as Co(10‐12), Co(11‐20) and Co(11‐21) surfaces, can be tuned by adding Ru promoter. Our theoretical calculation results show that Co(11‐21) becomes the predominantly exposed facet accompanied with the decrease of exposed Co(10‐10) and Co(10‐11) with the increase of Ru loading. Further experimental studies suggest that the area of selectively exposed the Co(10‐11) surface for uniform Co nanoplates loaded with 3.0 wt % Ru will be reduced, which is in agreement with the theoretical predicted result. This work is helpful to design the desired Co‐based FTS catalysts rationally with well‐controlled surface structure. [ABSTRACT FROM AUTHOR]

Correction to: I Nature Communications i https://doi.org/10.1038/s41467-022-32050-4, published online 26 July 2022 The original version of this Article contained an error in Figures 6k (PED + N3@PGDA7 + Laser) and 6l (PED + N3@PGDA7), in which the images were duplicates of adjacent images and the correct images were missing. The original article can be found online at https://doi.org/10.1038/s41467-022-32050-4. [Extracted from the article]

A series of glycan-coated quantum dots were prepared to probe the effect of glycan presentation in intracellular localization in HeLa and SV40 epithelial cells. We show that glycan density mostly impacts on cell toxicity, whereas glycan type affects the cell uptake and intracellular localization. Moreover, we show that lactose can act as a 'Trojan horse' on bi-functionalized QDs to help intracellular delivery of other non-internalizable glycan moieties and largely avoid the endosomal/lysosomal degradative pathway. [ABSTRACT FROM AUTHOR]

Nitrogen-doped ordered mesoporous carbons (OMCs) were prepared by using a post-synthetic method with cyanamide as a nitrogen source; they were used as supports for the fabrication of the cobalt-based Fischer-Tropsch synthesis (FTS) catalysts. The obtained composites were well characterised by using nitrogen physisorption, Raman spectroscopy, high-angle annular dark-field scanning transmission electron microscopy, hydrogen chemisorption, X-photoelectron spectroscopy, thermogravimetry-MS, and in situ XRD to investigate the effects of nitrogen on the dispersion of cobalt species and successive autoreduction behaviour of cobalt oxide as well as the catalytic performance in the FTS. The results indicate that the doped nitrogen atoms, especially the pyridine-like nitrogen, actually serve as the anchoring sites for cobalt species. Consequently, the more uniform cobalt particle size is observed for the catalysts with nitrogen-doped OMCs as supports in comparison with their counterparts based on the pristine OMCs. In contrast, the autoreduction temperature of cobalt oxide in the as-synthesised catalysts lowers considerably after nitrogen doping, although slightly increased autoreduction temperature is observed for the catalysts with relatively high nitrogen content owing to the metal-support interaction. Dictated by the balance between decreasing particle size of cobalt and increasing strength of the metal-support interaction, the cobalt specific activity of the nitrogen-doped catalysts reaches a maximum and then decreases in the FTS with increasing nitrogen content. Notably, under optimum conditions, the cobalt specific activity on the nitrogen-doped sample with medium nitrogen content is 1.5 times higher than its analogue on the pristine OMC without compromising the selectivity to C5+ hydrocarbons. [ABSTRACT FROM AUTHOR]

A series of core-shell-structured catalysts that consist of different-sized Co3O4 nano-particles and silica shells were prepared by an in situ coating method. The reduced catalysts displayed uniform core sizes that ranged from 5.5-12.7 nm as ascertained by TEM, which concurred well with XRD analysis. The BET results revealed the highly mesoporous nature of the silica shell, which contributes to the facile access of the reactant gas to the active sites on the core particles. The degree of reduction of the calcined catalysts studied by H2 temperature-programmed reduction was enhanced with increased Co particle size. In the Fischer-Tropsch synthesis, a volcano-like curve was plotted as the CO conversion and Co-time-yield revealed a rapid growth if the particle size increased from 5.5 to 8.7 nm and then decreased with further increased particle size to 12.7 nm, which is an effect of the combination of Co dispersion and reducibility. However, the turnover frequency remained invariant for catalysts with particle sizes larger than 8.7 nm. If we consider the product selectivity, generally, larger particles led to a longer chain length of hydrocarbons with a larger chain-growth probability. The selectivity towards methane decreased and the corresponding heavy hydrocarbons (C19+) increased continuously with the increase of particle size. The catalyst with a particle size of 8.7 nm exhibited the highest selectivity and the maximum space-time-yield towards middle distillates (C5-C18) because of the modest chain-growth probability. [ABSTRACT FROM AUTHOR]

In the beginning: Intermediate species generated in the synthesis of Cu2ZnSn(S,Se)4 nanoparticles (see figure) in oleylamine have been identified. The solvent plays a central role in the reaction mechanism, determining the composition of the nanostructures. [ABSTRACT FROM AUTHOR]

Abstract: Silica-modified titanium dioxides were prepared by a hydrothermal method and then characterized by XRD, FT-IR, XPS, TEM, and UV–visible spectroscopy. The silica-modified titanium dioxides were in anatase phase and had large surface areas. There was strong interaction between SiO2 and TiO2, and Tih name="sbnd" />Si bonds formed during the hydrothermal process. The addition of silica in TiO2 particles could effectively suppress the formation of the rutile phase and the growth of titanium dioxide crystals. DRS spectra proved an increase in the band-gap transition with the increase of silica. The silica-modified TiO2 nanoparticles exhibited better photocatalytic activity, which increased with the silica amount, in comparison with pure TiO2 nanoparticles. Due to better thermal stability, the photocatalytic activity of the silica-modified TiO2 sample held good photocatalytic activity even after calcined at 1273 K. [Copyright &y& Elsevier]

Abstract: Titania–silica composite nanoparticles were prepared by sol–gel-hydrothermal and sol–gel routes, respectively, and their physico-chemical and photocatalytic properties were compared. The results of XRD, TEM and BET surface areas showed that sol–gel-hydrothermal route led to anatase titania–silica composite nanoparticles with large specific surface area, but the sol–gel route tended to form mixture of anatase and rutile. The composite nanoparticles prepared by sol–gel-hydrothermal route had better thermal stability against phase transformation from anatase to rutile, agglomeration and particle growth than those prepared by sol–gel route. On the basis of XRD, FT-IR, XPS and 29Si MAS-NMR, a strong interaction was found between SiO2 and TiO2, and Ti–O–Si bonds formed during both the two routes. But more Ti–O–Si bonds formed in the composite nanoparticles prepared by sol–gel-hydrothermal route than those prepared by sol–gel route. As a result, the titania–silica composite nanoparticles prepared by sol–gel-hydrothermal route exhibited higher photocatalytic activity in decomposition of methylene blue than that prepared by sol–gel route, and it had excellent photocatalytic activity even after calcined at 1000°C. [Copyright &y& Elsevier]

Abstract: This paper describes a novel self-assembly behavior of Ag2O nanoparticles to Ag2O nanowires. In the alkaline water–alcohol solution, Ag+ ions reacted with OH− ions on silica nanoparticles functionalized by N-(2-aminoethyl)-3-aminopropyl-trimethoxy-silane (AEAPTS) to form Ag2O nanoparticles. The Ag2O nanoparticles further self-assembled into Ag2O nanowires. The morphology of Ag2O nanowires could be controlled by adjusting Ag/Si molar ratios in the systems. With low Ag/Si molar ratio, uniform Ag2O nanowires were obtained with diameter of about 50 nm and length of tens micrometers. With the increase of Ag/Si molar ratio, Ag2O nanowires became thicker, shorter and irregular. It was shown by high-resolution transmission electron microscopy (HRTEM) that all Ag2O nanowires consisted of tiny Ag2O nanoparticles with diameter of 10–20 nm. The self-assembly of Ag2O nanoparticles into Ag2O nanowires was observed by transmission electron microscopy (TEM) and the corresponding growth mechanism was proposed. [Copyright &y& Elsevier]

Abstract: A visible light-activated TiO2 photocatalyst was successfully synthesized by the surface organic modification to sol–gel–hydrothermal synthesized TiO2. The surface hydroxyls of TiO2 nanoparticles reacted with the active –NCO groups of tolylene diisocyanate (TDI) to form a surface complex that was confirmed by the FT–IR and XPS spectra. Due to the existence of surface complex, the absorption edge of as-prepared TDI-modified TiO2 nanomaterial extended well into visible region. Compared with unmodified TiO2 and Degussa P25, the TDI-modified TiO2 photocatalysts showed higher activity for the photocatalytic degradation of methylene blue under visible light irradiation. [Copyright &y& Elsevier]

The acidic H 2 O 2 solution employed in the treatment of LaCoO 3 resulted in an improved porosity and the formation of Co 3 O 4 nanoparticles highly dispersed on the surface of LaCoO 3. The resulting solid exhibited superior catalytic activity towards propane combustion with T 50 as low as 254 °C, high stability with time on stream (up to 48 h) and excellent water tolerance. This catalytic behavior was associated with the increase in the concentration of oxygen vacancies in the formed perovskite solid support. • Acidic H 2 O 2 was firstly employed to treat the LaCoO 3 catalyst. • Highly dispersed Co 3 O 4 nanoparticles formed on the LaCoO 3 surface. • Superior activity towards C 3 H 8 combustion over the modified catalyst. • Abundant oxygen vacancies for the high activity. [ABSTRACT FROM AUTHOR]