Atomically precise Cu clusters with stabilized low-coordinated Cu species demonstrate promising deep CO reduction capability, although product selectivity requires enhancement. To address this, two Cu clusters, [Cu(PPh)(PET)](BF) and [CuS(PPh)(PET)] (denoted as Cu and Cu, respectively) were constructed via ligand-mediated assembly of Cu triangular units. Both clusters effectively catalyze deep CO reduction, with CH as the dominant product (FE = 60.
View Article and Find Full Text PDFSalicylic acid (SA) is a ubiquitous plant hormone with a long history in human civilization. Because of the central role of SA in orchestrating plant pathogen defence, understanding SA biosynthesis is fundamental to plant immunity research and crop improvement. Isochorismate-derived SA biosynthesis has been well defined in Arabidopsis.
View Article and Find Full Text PDFAgricultural production is currently facing numerous abiotic and biotic stresses. To mitigate the impacts of these stresses on crop yields, conventional agrochemicals have been widely employed to support farming practices. However, these chemicals exhibit limited functionality and are prone to overuse and residue accumulation on agricultural products, leading to environmental concerns such as pollution and bioaccumulation, which may hinder the development of sustainable agriculture.
View Article and Find Full Text PDFThree-way catalysts are widely used to control criterion pollutant emissions from the increasing gasoline engines. With the stringent requirements of automotive pollutant emission standards in various countries, Rh has become an irreplaceable component of three-way catalysts due to its superior NO elimination, high N selectivity, and simultaneous elimination of CO and hydrocarbons. In this review, we systematically review the recent development of Rh-based three-way catalysts in terms of potential supports and effective active center construction strategies.
View Article and Find Full Text PDFSelective oxidation of double bonds in aldehyde-containing molecules is critical for synthesizing multifunctional organic compounds; however, conventional methods struggle to preserve aldehyde integrity due to competitive over-oxidation. Here, an electrochemical strategy is presented that achieves precise double bond oxidation without aldehyde degradation, using hydroperoxyl radicals (OOH) generated by a molybdenum-based catalyst (Mo─N─O). Under mild, energy-efficient conditions (-200 mA), this approach converts cinnamaldehyde to benzaldehyde with complete conversion (100%) and >99% selectivity, outperforming traditional harsh oxidants.
View Article and Find Full Text PDFChemical conversion of waste plastics into valuable products holds immense significance for pollution control and resource conservation. Dual-catalyst systems exhibit improved overall efficiency compared with conventional bifunctional catalysts in hydrocracking processes, but they continue to grapple with the issues of high noble metal loadings and the necessity for meticulously controlled synthesis steps. Herein, we propose a minimalist design for a dual-catalyst system that combines exceptional catalytic efficiency, minimal noble metal consumption, and a streamlined synthesis process.
View Article and Find Full Text PDFGlioblastoma (GBM) is the most lethal primary brain tumor with limited therapeutic efficiency because of resistance to Temozolomide (TMZ), which is the standard chemotherapy drug. Here, we developed the metabolic adaptive strategy based on the complex TMZ resistance mechanisms, and engineered metal-phenolic networks (TBFP-MT MPNs) by self-assembly of PEG-polyphenol encapsulating Fe, TMZ, and dihydroorotate dehydrogenase (DHODH) inhibitor, modifying T and cMBP for blood-brain barrier (BBB) penetration and targeting resistant cells. TBFP-MT suppressed drug efflux by inhibiting mesenchymal epithelial transition (MET) signaling and reduced DNA repair protein O6-methylguanine-DNA-methyltransferase (MGMT) by blocking pyrimidine synthesis via DHODH inhibition.
View Article and Find Full Text PDFPyroptosis can trigger strong immunogenic cell death (ICD) of tumor cells for antitumor immunotherapy. However, metabolic disorders of fumarate in the tumor microenvironment (TME) can significantly reduce the pyroptosis rate and render T lymphocytes dysfunctional. Here, the ultrasound (US)-driven piezoelectric charges assisted Fe-based SAzyme (BFTM) with co-loaded triphenylphosphonium (TPP) and methyl (Z)-4-(chloro(2-phenylhydrazono)methyl)benzoate (MMB, a bioorthogonal reagent of fumarate) for activating pyroptosis and regulating fumarate metabolism is developed.
View Article and Find Full Text PDFLanthanide (Ln)-based metal halides with excellent luminescence properties, large Stokes shifts, and low toxicity have aroused wide attention as scintillators for X-ray imaging. However, the lack of fast and mild synthesis methods of Ln-based metal halides, as one of the technical challenges, limits their applications. Here, benefiting from the innovative selection of methanol and ethanol as the solvent and anti-solvent, respectively, a series of CsLnCl (Ln = Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu) microcrystals (MCs) were prepared via the recrystallization method at room temperature for the first time.
View Article and Find Full Text PDFMethane combustion reactions hold significant promise for addressing environmental issues, particularly the greenhouse effect attributed to anthropogenic emissions. However, current catalysts face challenges in simultaneously achieving low-temperature activity and high-temperature stability. In this work, a CeMn solid solution decorated with palladium single atoms (Pd/CeMn-AR) was synthesized a one-pot auto-redox method.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
July 2025
Ru-based catalysts have exhibited significant promise in converting waste plastics into valuable long-carbon chain products. However, their efficiency is hindered by the uncontrollable cascade hydrogenation, which stems from their exceptional reactivity for C─C cleavage. Herein, we reported a multi-scale regulation strategy by selectively anchoring Fe single atoms (SAs) and FeO nanoclusters (NCs) by Ru NCs-decorated CeO substrates.
View Article and Find Full Text PDFγ-MoN catalysts exhibit excellent activity and stability in ammonia decomposition reactions. However, the influence of oxygen on its activity is still unknown. In this work, two γ-MoN catalysts with different oxygen content are synthesized using temperature-programmed nitridation of α-MoO.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
April 2025
Chemical conversion of CO is providing an opportunity to mitigate the global warming induced by the overconsumption of fossil fuel. Cu has been regarded as one of the most powerful contenders in catalyzing CO conversion, yet the precise manipulation of its surface state and the nearby chemical environment continues to pose a formidable challenge. In this work, we report a high-efficiency catalyst by utilizing CeO and pure silicon zeolite (S1) to co-activate Cu species.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
Fluorescence thermometry based on metal halide perovskites is increasingly becoming a hotspot due to its advantages of high detection sensitivity, noninvasiveness, and fast response time. However, it still presents certain technical challenges in practical applications, such as complex synthesis methods, the use of toxic solvents, and being currently mainly based on the visible/first near-infrared light with poor penetration and severe autofluorescence. In this study, we synthesize the second near-infrared (NIR-II) luminescent crystals based on Yb/Nd-doped zero-dimensional CsScCl·HO by a simple "dissolve-dry" method.
View Article and Find Full Text PDFSalicylic acid (SA) is a prominent defense hormone whose basal level, organ-specific accumulation, and physiological role vary widely among plant species. Of the 2 known pathways of plant SA biosynthesis, the phenylalanine ammonia lyase (PAL) pathway is more ancient and universal but its biosynthetic and physiological roles in diverse plant species remain unclear. Studies in which the PAL pathway is specifically or completely inhibited, as well as a direct comparison of diverse species and different organs within the same species, are needed.
View Article and Find Full Text PDFConverting CO to methanol is crucial for addressing fuel scarcity and mitigating the greenhouse effect. Cu-based catalysts, with their diverse surface states, offer the potential to control reaction pathways and generate reactive H* species. However, a major challenge lies in oxidizing active Cu species by water generated during the catalytic process.
View Article and Find Full Text PDFChemical conversion has emerged as an effective approach for disposing waste plastics; however, the product diversity in traditional methods leads to pressing challenges in product separation and purification. As a pioneering advancement, the comprehensive transformation of waste plastics into CH presents an attractive prospect: directly yielding high-purity products. Significantly, CH is an important hydrogen carrier and an industrial feedstock.
View Article and Find Full Text PDFCombining chemo/photodynamic therapy (CDT/PDT) to generate highly harmful reactive oxygen species and cause mitochondria dysfunction is considered a potential strategy to improve the efficiency of anticancer treatment. However, within tumor, the relatively deficient concentration of HO, hypoxic microenvironment, and overexpressed reduced glutathione (GSH) seriously suppress the efficacy of dynamic therapy. Herein, a multi-functional cascade nanoreactor, bovine serum albumin modified ZnO@CeO-ICG, is reported for remodeling tumor microenvironment (TME) to boost dynamic therapy and realize mitochondria dysfunction via reactive oxygen species (ROS) storm/Zn ions overload.
View Article and Find Full Text PDFAdv Sci (Weinh)
December 2024
Advancing and deploying Fenton-inactive Cd that combines excellent catalytic activity, selectivity, and stability remains a serious challenge, predominantly owing to the difficulty in regulating the intrinsic electronic states and local geometric structures of such fully occupied ds configuration. In this work, a combination of experiments and theoretical calculations reveals that the incorporation of boron (B) enables the tuning of the average oxidation state of Cd to Cd, facilitating electron localization and implementing a different electrocatalytic preference compared to conventional d-electron configurations. The resulting Cd(B) catalyst demonstrates high selectivity (>90% on average) in the O-to-HO conversion, negligible activity loss over 100 h, and a superior HO production rate (15.
View Article and Find Full Text PDFThe low immunogenicity of tumors, along with the abnormal structural and biochemical barriers of tumor-associated vasculature, impedes the infiltration and function of effector T cells at the tumor site, severely inhibiting the efficacy of antitumor immunotherapy. In this study, a cobaloxime catalyst and STING agonist (MSA-2)-coloaded Wurster-type covalent organic framework (Co-TB COF-M) with internal electron transfer-enhanced catalytic capacity was developed as a COF-based immune activator. The covalently anchored cobaloxime adjusts the energy band structure of TB COF and provides it with good substrate adsorption sites, enabling it to act as an electron transmission bridge between the COF and substrate in proton reduction catalytic reactions.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Exploring structural phase transitions and luminescence mechanisms in zero-dimensional (0D) metal halides poses significant challenges, that are crucial for unlocking the full potential of tunable optical properties and diversifying their functional capabilities. Herein, we have designed two inter-transformable 0D Cu(I)-based metal halides, namely (CHP)CuI and (CHP)CuI, through distinct synthesis conditions utilizing identical reactants. Their optical properties and luminescence mechanisms were systematically elucidated by experiments combined with density functional theory calculations.
View Article and Find Full Text PDFElaborated structural modulation of Pt-based artificial nanozymes can efficiently improve their catalytic activity and expand their applications in clinical diagnosis and biochemical sensing. Herein, a highly efficient dual-site peroxidase mimic composed of highly dispersed Pt and Mo atoms is reported. The obtained Mo-Pt/CeO exhibits exceptional peroxidase-like catalytic activity, with a V as high as 34.
View Article and Find Full Text PDFHuman society is facing increasingly serious problems of environmental pollution and energy shortage, and up to now, achieving high NH-SCR activity at ultra-low temperatures (<150 °C) remains challenging for the V-based catalysts with V content below 2%. In this study, the monoatomic V-based catalyst under the weak current-assisted strategy can completely convert NO into N at ultra-low temperature with V content of 1.36%, which shows the preeminent turnover frequencies (TOF = 1.
View Article and Find Full Text PDFBioact Mater
October 2024
Invasive tumors are difficult to be completely resected in clinical surgery due to the lack of clear resection margins, which greatly increases the risk of postoperative recurrence. However, chemotherapy and radiotherapy as the traditional means of postoperative adjuvant therapy, are limited in postoperative applications, such as multi-drug resistance and low sensitivity, etc. Therefore, an engineered magnesium alloy rod is designed as a postoperative implant to completely remove postoperative residual tumor tissue and inhibit tumor recurrence by gas and mild magnetic hyperthermia therapy (MMHT).
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