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Abstract: Developing green and efficient way for producing biofuel and high-value chemical from lignocellulosic biomass is of great significance for promoting green chemistry and sustainable development. Present work intended to explore a novel recyclable MnFe2O4 catalytic pre-treatment means to strengthen the synthesis of bioethanol and biofuel. The MnFe2O4 catalytic pre-treatment raised saccharification of lignocellulosic biomass, which was beneficial for the formation of ethanol intermediate and the production of biofuel. After MnFe2O4 catalytic pre-treatment, ethanol yield reached 34.2%. High ethanol conversion (93.8%) and good jet fuel selectivity (63.3%) were achieved in synthesizing biofuel process. According to catalyst’s characterization, lignocellulose’s characterization as well as radical’s detection, probable function/mechanism of MnFe2O4 catalytic pre-treatment was proposed. The MnFe2O4 catalyst facilitated the formation of hydroxyl radicals, thereby enhancing the depolymerization of lignocellulose and subsequent fuel synthesis. Considering that MnFe2O4 catalytic pre-treatment can be conducted by utilizing recyclable MnFe2O4 catalyst under gentle condition, this technology may provide an environmental-friendly pre-treatment means for facilitating the transformation of lignocellulose into biofuel. PubDate: 2025-04-15
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Abstract: Bismuth titanate shows great potential in the treatment of pollutants due to its good photocatalytic activity and stability. However, the non-selective degradation ability limits its application in pollutant treatment. Here, flake inorganic imprinted bismuth titanate (FII-BTO) with nanosheet structure was prepared by combining the inorganic imprinting technique with hydrothermal method. The formation of specific imprinting cavities on the surface of FII-BTO catalyst could specifically recognize and adsorb ciprofloxacin (CIP), and effectively improved the photoresponse and charge separation efficiency. The photodegradation rate of CIP by FII-BTO is 55.76%, and the reaction kinetic rate was increased by twice. Furthermore, compared with non-imprinted materials, FII-BTO selectively adsorbed CIP with Kselectivity value of 1.81, showing good selective photocatalytic degradation performance. This work provides valuable insights into the development of inorganic imprinting technology for selective degradation of pollutants, and provides promising directions for future catalyst applications. PubDate: 2025-04-12
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Abstract: Photonic crystals (PCs) with brilliant structural color constructed by polymer microspheres have received great interest in recent years. However, the development of PCs with multi-functions is still a challenge. By integrating the advantages of the fluorinated groups with low surface energy and the positively charged quaternary ammonium salt groups with antibacterial properties, poly(2,2,3,4,4,4-hexafluorobutyl acrylate/styrene/[3-(methylacrylamido)propyl] trimethylammonium chloride) (PASM) was successfully synthesized to construct the PCs coating with structural color and multi-functions on the fabrics. By adjusting the molar ratios of reactive monomers, PASM microspheres with different particle diameters were obtained, and subsequently were assembled into long-range order PCs coating with various structural colors on the fabrics. The structural color coating had excellent hydrophobicity with the static water contact angle greater than 140°, thereby endowing the fabrics with anti-fouling property. More importantly, the structural color coating showed excellent antibacterial performance including gram-negative bacteria and gram-positive bacteria with both antibacterial rates greater than 94%. Therefore, the PCs coating with structural color fabricated by PASM microspheres simultaneously exhibit anti-fouling and antibacterial functions, which are promising for designing multi-functional materials with brilliant colors in medical textile applications. PubDate: 2025-04-04
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Abstract: Platinum is a crucial anode catalyst in methanol oxidation reactions (MOR) due to its exceptional electrochemical performance, which has led to its widespread application. However, to enhance its catalytic activity and stability, platinum is typically supported on carrier materials, such as carbon-based substrates. Current commercial platinum-carbon catalysts exhibit limited activity, low utilization efficiency of metallic platinum, and a tendency to bind with intermediate species, leading to a decline in catalytic performance. To address these challenges, this study proposes the utilization of copper-doped carbon for the development of a composite support (Cu2C7). Compared with the pure carbon supported platinum catalyst (Pt@Cu0C7), the electrochemical activity of Cu2C7 supported platinum catalyst (Pt@Cu2C7) was significantly enhanced, as evidenced by a current density of 412 mA/cm2 and an onset potential of −0.8 V. In chronoamperometry experiments, after 2 h of electrochemical testing, the activity of Pt@Cu2C7 decreased by only 4.24%, whereas Pt@Cu0C7 experienced a significant reduction of 55% in activity. The incorporation of copper is hypothesized to provide additional active sites for the deposition of metallic platinum on the carrier, thereby enhancing the platinum loading capacity. According to inductively coupled plasma (ICP) analysis, when the copper-to-carbon ratio is 2:7, the platinum loading amount increases by 25.78%. Furthermore, some platinum forms an alloy with the copper embedded in the carbon, a phenomenon corroborated by X-ray diffraction (XRD) and transmission electron microscopy (TEM) techniques. The literature suggests that the formation of such alloys can significantly improve the catalyst’s resistance to poisoning. The incorporation of copper not only enhances the platinum loading capacity but may also induce a synergistic effect among the active platinum components, thereby further improving catalytic performance. In summary, the findings of this study offer critical theoretical insights and practical guidelines for the design of high-performance MOR electrocatalysts, laying a robust foundation for future advancements in catalyst development. PubDate: 2025-04-04
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Abstract: A tungsten-doping strategy was developed to enhance the photocatalytic dye degradation and corrosion resistance of graphitic carbon nitride (CN). Using WCl6 as a tungsten source, tungsten-doped CN (W-CN) was synthesized through a straightforward copolymerization process. Comprehensive characterization confirmed that tungsten ion incorporation modified the electronic band structure and disrupted local electron distribution, leading to extended visible light adsorption and improved separation and migration of photoexcited charge carriers. The resulting W-CN photocatalyst achieved a 5.14-fold increase in atrazine (ATZ) degradation rate. Additionally, the corrosion resistance of W-CN within waterborne polyurethane (WPU) coatings on metal substrates was evaluated. Enhanced hydrophobicity and a stronger physical barrier effect enabled the W-CN@WPU composite coating to significantly improve the corrosion resistance of Q235 carbon steel. This study demonstrates that tungsten doping not only boosts the photocatalytic degradation efficiency of organic pollutants by CN but also enhances the corrosion resistance of WPU coatings. PubDate: 2025-03-22
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Abstract: Elasticity of biodegradable fibrous scaffolds is one of essential requirements for soft tissue regeneration, and sufficient compliance of small-diameter vascular grafts is necessary. In this work, electrospun fibrous membranes with high resilience are prepared through blend electrospinning of poly(ε-caprolactone) (PCL)/methacrylated poly(glycerol sebacate) (PGS) and in situ photo-crosslinking with poly(ethylene glycol) diacrylate. The obtained PCL/PGS electrospun membranes have minor hemolysis, low platelet adherence, and favorable cytocompatibility. In the wet state, the PCL/PGS electrospun membranes in 5/5 or 4/6 mass ratio exhibit lowered modulus and reversible deformation with improved compliance in comparison with PCL, which can be comparable to the human saphenous vein. This study provides a feasible way to prepare electrospun fibrous scaffolds with high elasticity, that can be suitable for applications in vascular regeneration and relative soft tissue repair. PubDate: 2025-03-22
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Abstract: Photocatalysis is a promising approach for solar energy conversion and environmental remediation, which has garnered increasing attention. Advanced in situ characterization techniques enable real-time observation of dynamic changes in catalyst structure, charge transfer, and surface species during photocatalytic reactions, which is crucial for understanding the relationship between photocatalyst structure and activity. This review summarizes the main applications of in situ characterization techniques in photocatalysis, discusses their contributions to optimizing photocatalyst performance for enhanced solar energy conversion and environmental applications, provides guidance for designing in situ experiments to understand catalytic mechanisms, and presents an outlook on the future development of in situ characterization techniques in photocatalysis. PubDate: 2025-03-21
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Abstract: Bioelectrodes in cells can record and monitor monocellular or multicellular signals, contributing to early diagnosis, drug development and public health. To promote the cell analysis platform into integration, miniaturization and intellectualization, development of advanced bioelectrodes has attracted intense attention from both research and industrial communities. Here we present the research progress of bioelectrodes for cell analysis along four lines: materials, fabrications, principles and state-of-the-art applications. Covering from traditional noble metals to frontier conducting polymers, various conductive yet biocompatible materials have been used to develop bioelectrodes. Suitable materials are processed into micro/nano electrodes through electrochemical deposition, sol-gel processes, and self-assembly etc. The prepared bioelectrodes play roles in cellular analysis based on a biochemical process of direct electron transfer, mediator-assisted transfer or biocatalysis, which has been widely used in electrophysiological characterization, chemical analysis, metabolite detection and intercellular communication. To conclude this review, we summarize current challenges remained for cell electrodes in terms of foreign body response, biocompatibility, long-term stability, miniaturization, multifunctional integration, and intelligence, further suggesting possible solutions on performance optimization and material innovation. This review could provide guidance for understanding the working principles of bioelectrodes, designing a feasible cellular analysis platform, and building advanced cell analysis systems. PubDate: 2025-03-20
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Abstract: Mass spectrometry (MS) is widely used in medical applications, such as pharmacokinetics, drug discovery, and clinical diagnostics, as it enables medical researchers and practitioners to gain insights into pathogenic mechanisms, identify biomarkers for diagnosis and monitoring, and develop new treatments. Mass spectrometry imaging (MSI) is a powerful analytical technique that combines the spatial information from imaging with the chemical information from MS. MSI assists medical researchers in various ways, including biomarker discovery, drug development and evaluation, personalized medicine, tissue imaging, and histochemical analysis. In addition, MSI not only provides high-resolution images of sample structures and enables researchers to identify specific cell types and their functions, but also enables the simultaneous visualization of multiple biomolecules within a single cell and allows researchers to study complex biological processes with greater precision. In this review, we summarize recent advances in MSI for single cells and cellular-level analysis and discuss how this technology can be used to improve our understanding of diseases and develop new treatments. The potential challenges and limitations of MSI in single-cell analysis, as well as prospects in this field, are also highlighted. PubDate: 2025-03-18
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Abstract: Electrocatalytic reduction reaction of carbon dioxide (CO2RR) to formic acid is widely considered an effective strategy for addressing the greenhouse effect and enhancing energy conversion efficiency. However, existing catalytic systems are severely hampered by insufficient activity and significant hydrogen evolution reaction (HER), which substantially compromises the selectivity and stability of CO2RR, necessitating the development of highly efficient and stable electrocatalysts. Herein, we present a heteroatomic modification strategy to synthesize B-doped Bi and N-doped Bi electrocatalysts, and systematically investigate the regulation mechanism of incorporated elements on the electronic environment using X-ray absorption fine structure (XAFS) spectroscopy and other characterization techniques. The optimized B-doped Bi catalyst demonstrates exceptional catalytic performance, achieving a remarkable Faradaic efficiency of 95% for formic acid production at a high current density of −190 mA/cm2 under alkaline conditions, while maintaining excellent stability for 20 h. Through comprehensive experimental characterization and theoretical calculations, we reveal that the B-doping-induced electron-rich structure significantly promotes CO2 molecule activation and facilitates the formation of the key intermediate *OCHO, thereby achieving high selectivity and stability in CO2RR. This work not only elucidates the crucial role of electronic environment in CO2 electrocatalytic conversion but also provides innovative insights into the rational design of high-performance electrocatalysts. PubDate: 2025-03-18
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Abstract: The study of the metabolic toxicity of perfluorooctanoic acid (PFOA) is of great importance in assessing its potential impact on aquatic organisms and the aquatic environment, and provides a fundamental scientific basis for environmental protection and sustainable development. In this study, an electrospray ionization (ESI) source capable of direct analysis of solution samples was combined with a high-resolution Orbitrap Fusion Tribrid mass spectrometer to investigate the metabolic perturbations induced by different concentrations of perfluorooctanoic acid (PFOA) and their correlations in skin mucus and liver tissue of tilapia. Seven common metabolites were found in mucus and liver, and nitrogen metabolism pathways were disturbed in all of them. The up-regulation of glutamate in mucus may reflect an increased demand for amino acids and energy, whereas the down-regulation of glutamate in the liver may lead to dysregulation of nitrogen metabolism, protein synthesis and amino acid metabolism. Enrichment analyses suggest a dysregulation of nitrogen metabolism pathways, which may lead to impaired maintenance of tissue function and dysregulated energy metabolism in tilapia. PubDate: 2025-03-18
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Abstract: Detection of small molecular metabolites in the body can reflect the overall health status of the human body, being essential for understanding metabolism and diagnosing diseases. For the detection and monitoring of small molecular metabolites in complicated biological systems, the sensitive detections of trace metabolites and their pathways have been pursued by different strategies. Mass spectrometry provides high sensitivity and specificity for metabolic studies, while commercial techniques normally require sample pretreatments to limit the multiple examining requirements. Fortunately, ambient mass spectrometry (AMS) can meet rapid clinical examinations due to its rapid and direct detection of biological molecules without or with fewer sample pretreatments. By virtue of AMS, the real-time and online monitoring of small molecular metabolites can be achieved for examining metabolism mechanisms and facilitating targeted interventions. This review summarizes the application of AMS in the monitoring of small molecular metabolites, including glucose, lipids, amino acids, nucleotides, and aldehydes, as well as examinations of reaction mechanisms in clinical applications. This would provide insights on constructing powerful diagnostic tools for clinical applications. PubDate: 2025-03-18
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Abstract: Nanomaterials have greatly received interest in various fields due to their excellent activity, typically attributed to their nanoscale physical and chemical properties. Transmission electron microscopy (TEM) as a powerful tool for characterizing nanomaterials can offer microscopic information with high spatial resolution. However, TEM faces challenges in obtaining information along the electron beam direction (Z direction), which limits its ability to explore the unique characteristics of nanomaterials on a three-dimensional (3D) scale. Electron tomography (ET) is an advanced imaging technique that allows for the visualization of 3D structures of nanomaterials. When combined with energy-dispersive X-ray spectroscopy (EDS) or electron energy loss spectroscopy (EELS), it enables researchers to reveal chemical changes in three dimensions, enhancing the understanding of the complex mechanisms underlying changes in chemical properties. This review summarizes and discusses the recent advancements in EDS/EELS (chemical-sensitive) ET imaging techniques, including the traditional reconstruction method, deep learning-based method, and multi-modal method, which provide detailed processes of reconstruction to facilitate the understanding of how they work for related researchers. Moreover, several successful applications are presented to show the capabilities of chemical-sensitive ET in diverse fields. Finally, the existing challenges and solutions are discussed to propel the development of ET imaging techniques. PubDate: 2025-03-17
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Abstract: Single-atom catalysts (SACs) have shown great potential in catalysis and energy-related applications. Among these, iron SACs stand out for their exceptional performance and environmental friendliness. In this study, we investigated the transformation of iron oxide nanoparticles into iron single atoms, exemplifying a top-down synthesis strategy. Using in-situ transmission electron microscopy (TEM), we directly observed the dynamic behaviors during the pyrolysis-induced atomization of Fe3O4 nanoparticles along the [110], [111], and [112] zone axes at atomic-scale resolution. Reducing gases were supposed to release during the thermal pyrolysis of an organic reducing agent and facilitate the generation of Fe single atoms. The rate-limiting step was the reaction of these gases with atoms at surface steps and vertices of Fe3O4 nanoparticles. Electron energy loss spectroscopy revealed a reduction in the Fe valence state and a transition in the Fe-O coordination environment after in-situ thermal treatment. The high-density dispersion of Fe single atoms was facilitated by the weak repulsive interactions between Fe atoms. This study enriches the understanding of the gas-assisted atomization mechanism and offers valuable insights for optimizing the production of high-density SACs. The methodology and findings can be extended to other material systems, broadening the scope of single-atom engineering and catalysis applications. PubDate: 2025-03-13
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Abstract: Promoting the photocatalytic proton-coupled electron transfer (PCET) kinetics in the two-electron oxygen reduction reaction (2e− ORR) is crucial for the photocatalytic hydrogen peroxide (H2O2) production. Herein, four kinds of covalent organic frameworks (COFs) were successfully prepared via a sub-stoichiometric strategy through a one-step solvothermal method. Among them, B1.5T1-COF with polar aldehyde groups displays a high photocatalytic H2O2 generation rate of 1081.8 µmol·g−1·h−1, which is 3 times higher than that of B1T1.5-COF and 2 times higher than that of B1T1-COF. Through the corresponding experiments and density functional theory (DFT) calculation, the photocatalytic mechanism is revealed that B1.5T1-COF with free aldehyde groups can raise the PCET kinetics for 2e− ORR with the aid of a stable transfer channel for e− and a favorable hydrogen donation for H+. This work might provide some insights for design and preparation of COFs with functional groups through a sub-stoichiometric strategy to modulate their photocatalytic activities. PubDate: 2025-03-13
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Abstract: An in-situ double-tilt holder has been made to integrate laser illumination and fluorescence-based spectroscopic analysis for conducting liquid-phase electron microscopy (LP-TEM) experiments using ordinary TEM. The setup differs from the existing geometry. Laser illumination and the collection of fluorescence signals were achieved using a single optical fiber, with efficiency optimized by adjusting the fiber position and grid tilt angle. Fluorescence emission of common organic dyes, propidium iodide (PI) and cyanine dyes, and Förster resonance energy transfer (FRET) signals of a FRET pair, Cy3/Cy5, were obtained from three types of liquid cells, including carbon film, graphene, and nanopipette liquid cells. The successful application of FRET-LPTEM enables LP-TEM experiments to be equipped with controlled light-triggering capability, detection of fluorogenic small molecules during chemical reactions, and the standard FRET experiments for macromolecules being conducted with LP-TEM. FRET-LPTEM presents opportunities for unraveling pathways underpinning the synthesis and assembly of optically active organic and biological materials. PubDate: 2025-03-11
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Abstract: Molecular motions in metal-organic frameworks (MOFs) play important roles in guest diffusion processes, which is crucial for gas capture and separations. Three-dimensional electron diffraction (3DED) has emerged as an advanced method to probe molecular motions, such as linker librations. For a study of molecular motions by 3DED, data quality is the key to the analysis and interpretation. Herein, we present a systematic work to investigate the effects of data completeness, resolution, and signal-to-noise ratio on the identification of molecular motion in MIL-140C. We determine the limits of completeness and resolution required for reliably analyzing molecular motions. In addition, data processing can affect the signal-to-noise ratio of data, and we demonstrate their influence on probing molecular motions. This work provides reference conditions on 3DED data quality to obtain reliable information on molecular motions. PubDate: 2025-03-08
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Abstract: Native proteins refer to proteins that exist in their natural state, have a correctly folded three-dimensional structure, and have biological functions. Characterization of protein higher-order structure and protein-protein interactions is crucial for a deeper understanding of protein structure and function, as well as drug development. Native mass spectrometry (nMS) can provide key information about the intact mass, subunit composition, stoichiometry, and post-translational modification sites of protein complexes or individual proteins. However, when directly analyzing complex mixtures, the resolution of nMS is reduced, and it becomes difficult to detect low-abundance proteins. Therefore, sample separation and purification play an important role in nMS studies of proteins. In this review, we describe the mainstream native separation methods coupled to mass spectrometry, including liquid chromatography and capillary electrophoresis, and discuss the challenges encountered when these technologies are combined with mass spectrometry and the latest advances in the characterization of native proteins. The article provides a comprehensive overview of non-denaturing separation methods, including practical application issues, such as buffer selection, flow rate control, and interface technology. At the same time, potential native separation technologies, such as gradient focusing and free-flow electrophoresis that have not been widely used in nMS are also introduced, providing new perspectives for high-resolution detection of complex samples and detection of low-abundance proteins. PubDate: 2025-03-08
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Abstract: Hyperpolarized 129Xe magnetic resonance imaging (MRI) is a powerful tool for detecting respiratory system diseases. However, 129Xe is an inert gas and lacks specific detection capability. Entrapping xenon within molecular cages to enable specific detection is a challenging task, and numerous molecular cages have been developed and evaluated to address this challenge. Herein, we report that the aluminum-based metal-organic framework, CAU-1, can effectively entrap xenon for hyperpolarized 129Xe MRI in aqueous solutions. This platform exhibits high water stability and good dispersibility, and shows excellent xenon entrapment capability, even at a concentration as low as 50 µg/mL. Importantly, it is responsive to pH changes across a range from 6.6 to 5.0, making it promising for monitoring the weakly acidic environment in tumors or metabolic abnormality. Furthermore, the scalable and cost-effective production of this molecular cage will facilitate future advancements in molecular imaging and chemical sensing applications. PubDate: 2025-03-08