Latest ArticlesAtomically precise metal nanoclusters (NCs) have been deemed as a new generation of metal nanomaterials in the field of solar energy conversion due to their unique atomic stacking manner, quantum confinement effects, light-harvesting capability and multitude of active sites. Nonetheless, wide-spread application of monometallic NCs is blocked by the ultrashort carrier lifespan, uncontrollable charge transport pathway, and light-induced poor stability, impeding the construction of robust and stable metal NC-based photosystems. Herein, we report the fabrication of stable alloy (Au1-xPtx) NCs photosystem, for which tailor-made negatively charged l-glutathione (GSH)-capped Au1-xPtx NCs as the building blocks are controllably deposited on the BiVO4 (BVO) by a self-assembly approach for steering enhanced light absorption and interfacial charge transfer over alloy NCs-based photoanodes (Au1-xPtx/BVO). The self-assembled Au1-xPtx/BVO composite photoanode exhibits the significantly enhanced photoelectrochemical water oxidation performances compared with pristine BVO and Aux/BVO photoanodes, which is caused by the Pt atom doping into the Aux NCs for elevating photosensitivity and boosting the stability. The synergy of Au and Pt atoms in alloy NCs protects the gold core from rapid oxidation, improving the photostability and accelerating the surface charge transfer kinetics. Our work would significantly inspire ongoing interest in unlocking the charge transport characteristics of atomically precise alloy NCs for solar energy conversion.
In this work, we developed plasmonic photocatalyst composed of CuPd alloy nanoparticles supported on TiN, the optimized Cu3Pd2/TiN catalyst shows excellent conversion (> 96%) and selectivity (> 99%) for Heck reaction at 50 ℃ under visible light irradiation. By in-situ spectroscopic investigations, we find that visible light excitation could achieve stable metallic Cu species on the surface of CuPd alloy nanoparticles, thereby eliminating the inevitable surface oxides of Cu based catalyst. The in-situ formed metallic Cu species under irradiation take advantage of the strong interactions of Cu with visible light, and manifest in the localized surface plasmon resonances (LSPR) photoexcitation. Visible light excitation could further promote the charge transfer between catalytic Pd component and the support TiN, resulting in electron-rich Pd sites on CuPd/TiN. Moreover, light excitation on CuPd/TiN generates strong chemisorption of iodobenzene and styrene, favoring the activation of reactants for Heck reaction. DFT calculations suggest that electron-rich CuPd sites ideally lower the activation energy barrier for the coupling reaction. This work provides valuable insights for mechanistic understanding of plasmonic photocatalysis.
Gastric Carcinoma (GC) is a highly fatal malignant tumor with a poor prognosis. Its elevated mortality rates are primarily due to its proclivity for late-stage metastasis. Exploring the metabolic interactions between tumor microenvironment and the systemic bloodstream could help to clearly understand the mechanisms and identify precise biomarkers of tumor growth, proliferation, and metastasis. In this study, an integrative approach that combines plasma metabolomics with mass spectrometry imaging of tumor tissue was developed to investigate the global metabolic landscape of GC tumorigenesis and metastasis. The results showed that the oxidized glutathione to glutathione ratio (GSSH/GSH) became increased in non-distal metastatic GC (M0), which means an accumulation of oxidative stress in tumor tissues. Furthermore, it was found that the peroxidation of polyunsaturated fatty acids, such as 9,10-EpOMe, 9-HOTrE, etc., were accelerated in both plasma and tumor tissues of distal metastatic GC (M1). These changes were further confirmed the potential effect of CYP2E1 and GGT1 in metastatic potential of GC by mass spectrometry imaging (MSI) and immunohistochemistry (IHC). Collectively, our findings reveal the integrated multidimensional metabolomics approach is a clinical useful method to unravel the blood-tumor metabolic crosstalk, illuminate reprogrammed metabolic networks, and provide reliable circulating biomarkers.
Precise tumor targeting and therapy is a major trend in cancer treatment. Herein, we designed a tumor acidic microenvironment activatable drug loaded DNA nanostructure, in which, we made a clever use of the sequences of AS1411 and i-motif, which can partially hybridize, and designed a simple while robust DNA d-strand nanostructure, in which, i-motif sequence was designed to regulate the binding ability of the AS1411 aptamer to target tumor. In the normal physiological environment, i-motif inhibits the targeting ability of AS1411. In the acidic tumor microenvironment, i-motif forms a quadruplex conformation and dissociates from AS1411, restoring the targeting ability of AS1411. Only when acidic condition and tumor cell receptor are present, this nanostructure can be internalized by the tumor cells. Moreover, the structure change of this nanostructure can realize the release of loaded drug. This drug loaded A-I-Duplex DNA structure showed cancer cell and spheroid targeting and inhibition ability, which is promising in the clinical cancer therapy.
Highly toxic phosgene, diethyl chlorophosphate (DCP) and volatile acyl chlorides endanger our life and public security. To achieve facile sensing and discrimination of multiple target analytes, herein, we presented a single fluorescent probe (BDP-CHD) for high-throughput screening of phosgene, DCP and volatile acyl chlorides. The probe underwent a covalent cascade reaction with phosgene to form boron dipyrromethene (BODIPY) with bright green fluorescence. By contrast, DCP, diphosgene and acyl chlorides can covalently assembled with the probe, giving rise to strong blue fluorescence. The probe has demonstrated high-throughput detection capability, high sensitivity, fast response (within 3 s) and parts per trillion (ppt) level detection limit. Furthermore, a portable platform based on BDP-CHD was constructed, which has achieved high-throughput discrimination of 16 analytes through linear discriminant analysis (LDA). Moreover, a smartphone adaptable RGB recognition pattern was established for the quantitative detection of multi-analytes. Therefore, this portable fluorescence sensing platform can serve as a versatile tool for rapid and high-throughput detection of toxic phosgene, DCP and volatile acyl chlorides. The proposed "one for more" strategy simplifies multi-target discrimination procedures and holds great promise for various sensing applications.
Membrane electrode assembly (MEA) is widely considered to be the most promising type of electrolyzer for the practical application of electrochemical CO2 reduction reaction (CO2RR). In MEAs, a square-shaped cross-section in the flow channel is normally adopted, the configuration optimization of which could potentially enhance the performance of the electrolyzer. This paper describes the numerical simulation study on the impact of the flow-channel cross-section shapes in the MEA electrolyzer for CO2RR. The results show that wide flow channels with low heights are beneficial to the CO2RR by providing a uniform flow field of CO2, especially at high current densities. Moreover, the larger the electrolyzer, the more significant the effect is. This study provides a theoretical basis for the design of high-performance MEA electrolyzers for CO2RR.
Copper (Cu) is widely used in the electrochemical carbon dioxide reduction reaction (ECO2RR) for efficient methane (CH4) product. However, the morphology and valence of Cu-based catalysts are usually unstable under reaction conditions. In this work, we prepared Ce-doped MOF-199 precursor (Ce/HKUST-1) and further obtained nanoparticle electrocatalyst Ce/CuOx-NPs by cyclic voltammetry (CV) pretreatment. The Faradic efficiency of methane () maintains above 62% within a broad potential window of 350 mV and the maximum reaches 67.4% with a partial current density of 293 mA/cm2 at −1.6 V vs. a reversible hydrogen electrode. Catalyst characterization and theoretical calculations revealed that the unique electronic structure and large ionic radius of Cerium (Ce) not only promoted the generation of key intermediate *CO but also lowered energy barrier of the *CO to *CHO step. This study provides a novel and efficient catalyst for methane production in ECO2RR and offers profound insights into constructing high performance Cu-based catalysts.
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