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Atomically Dispersed Pt and NiO Clusters Synergistically Enhanced C–O Bond Hydrogenolysis

CCS Chemistry 2024年第3期6卷 709-718页

作者： Junjuan Yang Sen Luan Minghua Dong Yuxuan Wu Xueqing Xing Xingwu Liu Junfeng Xiang Zhijuan Zhao Shaopeng Li Bin Zhang Huizhen Liu Buxing Han Beijing National laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and ThermodynamicsInstitute of ChemistryChinese Academy of SciencesBeijing 100190 School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049 Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsBeijing 100049 National Energy Center for Coal to Liquids Synfuels China Co.Ltd.Huairou DistrictBeijing 101400 Center for physicochemical Analysis and Measurement Institute of ChemistryChinese Academy of SciencesBeijing 100190 Physical Science laboratory Huairou National Comprehensive Science CenterUniversity of Chinese Academy of SciencesBeijing 100049

C–Obond activation is a highly efficient,fundamental strategy in the depolymerization and hydrodeoxygenation of chemicals with oxygen-containing functional groups such as oil,coal,and *** efficient catalysts for C–Oactivation with ultralow-loading noble and non-noble metals is highly desirable for the improvement of metal atomic ***,bimetallic catalysts with atomically dispersed Pt and NiO clusters on different supports were fabricated,and the prepared Pt^(δ+)-NiO/Nb_(2)O_(5)and Pt^(δ+)-NiO/TiO_(2)showed outstanding activity for the hydrogenolysis of benzyl phenyl ether with>99%yield of phenol and toluene due to the excellent cooperation of atomically dispersed Pt and NiO *** synergy mechanism between Pt and Ni and their respective roles in the bimetallic catalyst for C–O hydrogenolysis were clearly *** findings deepen our understanding of the synergy of the two active components and are expected to provide new design concepts for the development of multicomponents catalysts.

关键词： bimetallic catalysis synergistic effect C-O bond activation hydrogenolysis hydrogen spillover

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Changes in the Non-targeted Metabolomic Profile of Three-year-old Toddlers with Elevated Exposure to Polycyclic Aromatic Hydrocarbons

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Biomedical and Environmental Sciences 2024年第5期37卷 479-493页

作者： LI Yang LIN Dan ZHANG Xiu Qin JU Guang Xiu SU Ya ZHANG Qian DUAN Hai Ping YU Wei Sen WANG Bing Ling PANG Shu Tao Department of Epidemiology and Health Statistics School of Public HealthQingdao UniversityQingdao 266021ShandongChina Department of Environmental Health Qingdao Municipal Center for Disease Control and PreventionQingdao Institute of Preventive MedicineQingdao 266033ShandongChina physicochemical laboratory Qingdao Municipal Center for Disease Control and PreventionQingdao Institute of Preventive MedicineQingdao 266033ShandongChina Section of Child Health Care Huangdao Maternity and Child Health Care Hospital of QingdaoQingdao 266499ShandongChina Qingdao Blood Center Qingdao 266071ShandongChina

Objective To investigate changes in the urinary metabolite profiles of children exposed to polycyclic aromatic hydrocarbons(PAHs)during critical brain development and explore their potential link with the intestinal *** Liquid chromatography-tandem mass spectrometry was used to determine ten hydroxyl metabolites of PAHs(OH-PAHs)in 36-month-old ***,37 children were categorized into low-and high-exposure groups based on the sum of the ten ***-high-performance liquid chromatography coupled with quadrupole time-of-flight mass spectrometry was used to identify non-targeted metabolites in the urine ***,fecal flora abundance was assessed by 16S rRNA gene sequencing using Illumina *** The concentrations of 21 metabolites were significantly higher in the high exposure group than in the low exposure group(variable importance for projection>1,P<0.05).Most of these metabolites were positively correlated with the hydroxyl metabolites of naphthalene,fluorine,and phenanthrene(r=0.336–0.531).The identified differential metabolites primarily belonged to pathways associated with inflammation or proinflammatory states,including amino acid,lipid,and nucleotide ***,these distinct metabolites were significantly associated with specific intestinal flora abundances(r=0.34–0.55),which were mainly involved in *** Higher PAH exposure in young children affected metabolic homeostasis,particularly that of certain gut microbiota-derived *** investigation is needed to explore the potential influence of PAHs on the gut microbiota and their possible association with neurodevelopmental outcomes.

关键词： Child Gut microbiota Non-targeted metabolomics Polycyclic aromatic hydrocarbons Urinary metabolite profile

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Recent advances in morphology control of platinum catalysts toward oxygen reduction reaction

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Frontiers in Energy 2024年第3期18卷 330-355页

作者： Shun CHEN Yanru LIU Xiaogang FU Wanglei WANG State Key laboratory of Solidification Processing Atomic Control and Catalysis Engineering LaboratorySchool of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072China State Key laboratory of Oral and Maxillofacial Reconstruction and Regeneration National Clinical Research Center for Oral DiseasesShaanxi Key Laboratory of StomatologyDepartment of Dental MaterialsSchool of StomatologyThe Fourth Military Medical UniversityXi’an 710032China

Exploring advanced platinum (Pt)-based electrocatalysts is vital for the widespread implementation of proton exchange membrane fuel cells (PEMFCs). Morphology control represents an effective strategy to optimize the behavior of Pt catalysts. In this work, an attempt is made to comprehensively review the effect of morphology control on the catalytic behavior of catalysts in the oxygen reduction reaction (ORR). First, the fundamental physicochemical changes behind morphology control, including exposing more active sites, generating appropriate lattice strains, and forming different crystalline surfaces, are highlighted. Then, recently developed strategies for tuning the morphologies of electrocatalysts, including core-shell structures, hollow structures, nanocages, nanowires, and nanosheets, are comprehensively summarized. Finally, an outlook on the future development of morphology control of Pt catalysts is presented, including rational design strategies, advanced in situ characterization techniques, novel artificial intelligence, and mechanical learning. This work is intended to provide valuable insights into designing the morphology and technological innovation of efficient redox electrocatalysts in fuel cells.

关键词： morphology platinum catalysts electrocatalysis ORR PEMFC

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Review and prospects on the low-voltage Na_(2)Ti_(3)O_(7) anode materials for sodium-ion batteries

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Journal of Energy Chemistry 2024年第1期88卷 446-460,I0011页

作者： Jun Dong Yalong Jiang Ruxing Wang Qiulong Wei Qinyou An Xiaoxing Zhang Hubei Key laboratory for High-efficiency Utilization of Solar Energy and Operation Control of Energy Storage System Hubei University of TechnologyWuhan 430068HubeiChina State Key laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile UniversityWuhan 430200HubeiChina Xiamen Key laboratory of High-Performance Metals and Materials College of MaterialsXiamen UniversityXiamen 361005FujianChina State Key laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina

Due to its low cost and natural abundance of sodium,Na-ion batteries(NIBs)are promising candidates for large-scale energy storage *** development of ultralow voltage anode materials is of great significance in improving the energy density of ***-voltage anode materials,however,are severely lacking in *** all the reported insertion oxides anodes,the Na_(2)Ti_(3)O_(7) has the lowest operating voltage(an average potential of 0.3 V ***^(+)/Na)and is less likely to deposit sodium,which has excellent potential for achieving NIBs with high energy densities and high *** significant progress has been made,achieving Na_(2)Ti_(3)O_(7) electrodes with excellent performance remains a severe *** paper systematically summarizes and discusses the physicochemical properties and synthesis methods of Na_(2)Ti_(3)O_(7).Then,the sodium storage mechanisms,key issues and challenges,and the optimization strategies for the electrochemical performance of Na_(2)Ti_(3)O_(7) are classified and further ***,remaining challenges and future research directions on the Na_(2)Ti_(3)O_(7) anode are *** review offers insights into the design of high-energy and high-safety NIBs.

关键词： Sodium-ion batteries Low-voltage anode materials Na_(2)Ti_(3)O_(7) Electrochemical performances Electrochemical mechanism

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Predesigned covalent organic framework with sulfur coordination: Anchoring Au nanoparticles for sensitive colorimetric detection of Hg(Ⅱ)

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Chinese Chemical Letters 2024年第5期35卷 392-396页

作者： Guorong Li Yijing Wu Chao Zhong Yixin Yang Zian Lin Ministry of Education Key laboratory of Analytical Science for Food Safety and Biology Fujian Provincial Key Laboratory of Analysis and Detection Technology for Food SafetyCollege of ChemistryFuzhou UniversityFuzhou 350108China

Targeted construction of new covalent organic frameworks(COFs)with specific purposes and rationalities to build colorimetric assay platform for environmental pollutant monitoring have attracted increasing ***,it is still challenging due to lack of available coordination sites inside COFs pores and only a slight bonding ability for anchoring *** this work,a two-dimensional(2D)COFs(termed as Tz-COF)with high crystallinity,excellent chemical stability,and abundant sulfur coordination in its skeletons was synthesized and used for the confined growth of Au *** was found that the Au NPs showed significant dispersibility for the support of *** proposed Tz-COF@Au NPs possessed outstanding Hg^(2+)-activated peroxidase-like activity benefited from physicochemical properties of gold amalgam and synergistic effect between COFs and Au NPs to oxidize chromogenic *** on highly efficient activity and distinctive color evolution,the strategy for detecting Hg^(2+)was developed and successfully applied to determine the content of Hg^(2+)in real environmental *** work manifests that a potential strategy to establish a colorimetric assay platform for environmental pollutant monitoring based on the targeted manufacturing of novel COFs with specific functions.

关键词： Covalent organic frameworks Thiazole Sulfur coordination Au nanoparticles Hg^(2+)-activated peroxidase-like activity

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Effect of Cr_(2)O_(3) on properties of CaO-SiO_(2)-Fe_(t)O-MgO system and dissolution behavior of lime

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Journal of Iron and Steel Research(International) 2024年第4期31卷 870-881页

作者： Shan-nan Li Jian-li Li Yue Yu Hang-yu Zhu The State Key laboratory of Refractories and Metallurgy Wuhan University of Science and TechnologyWuhan 430081HubeiChina Hubei Provincial Key laboratory for New Processes of Ironmaking and Steelmaking Wuhan University of Science and TechnologyWuhan 430081HubeiChina Key laboratory for Ferrous Metallurgy and Resources Utilization of Ministry of Education Wuhan University of Science and TechnologyWuhan 430081HubeiChina

The productivity of the chrome-containing semi-steel converter smelting process is directly affected by the slag-forming speed during the converter preliminary *** effects of Cr_(2)O_(3) content on the physicochemical properties of the CaO-SiO_(2)-Fe_(t)O-MgO system,such as melting temperature,solidification behavior,mineral composition,and lime dissolution rate,were *** results showed that the slag was an amorphous phase at 1500℃.When Cr_(2)O_(3) was added,Ca(Fe,Mg)Si_(2)O_(6) and spinel were formed in the *** the increase in Cr_(2)O_(3) content,the amount of spinel precipitation increased,and the dendritic FegO_(4) crystal gradually changed into the granular(Fe,Mg)(Fe,Cr)2O_(4) *** the Cr_(2)O_(3) content increased from O to 2.91 wt.%,the melting temperature of the slag rose,and the melting range of the slag expanded slightly,but the lime dissolution rate did not *** the Cr_(2)O_(3) content further increased to 9.09 wt.%,the melting temperature continued to rise,the melting range rapidly expanded,and the lime dissolution rate decreased.

关键词： Cr_(2)O_(3) Vanadium-titanium magnetite Converter Slag Lime dissolution

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Enhanced hepatic metabolic perturbation of polystyrene nanoplastics by UV irradiation-induced hydroxyl radical generation

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Journal of Environmental Sciences 2024年第8期142卷 259-268页

作者： Shiyu He Jingran Wang Lihong Zhou Zhen Mao Xiaodan Zhang Jin Cai Peili Huang School of Public Health and Beijing Key laboratory of Environmental Toxicology Capital Medical UniversityBeijing 100069China

The environmental behavior of and risks associated with nanoplastics(NPs)have attracted considerable ***,compared to pristine NPs,environmental factors such as ultraviolet(UV)irradiation that lead to changes in the toxicity of NPs have rarely been *** evaluated the changes in morphology and physicochemical properties of polystyrene(PS)NPs before and after UV irradiation,and compared their hepatotoxicity in *** results showed that UV irradiation caused particle size reduction and increased the carbonyl index(CI)and negative charge on the particle ***-aged PS NPs(aPS NPs)could induce the generation of hydroxyl radicals(·OH),but also further promoted the generation of·OH in the Fenton reaction *** pathological damage was more severe in mice exposed to aPS NPs,accompanied by a large number of vacuoles and hepatocyte balloon-like changes and more marked perturbations in blood glucose and serum lipoprotein,alanine aminotransferase and aspartate aminotransferase *** addition,exposure to PS NPs and aPS NPs,especially aPS NPs,triggered oxidative stress and significantly damaged the antioxidant capacity of mice *** with PS NPs,exposure to aPS NPs increased the number of altered metabolites in hepatic and corresponding metabolic pathways,especially glutathione *** research suggests that UV irradiation can disrupt the redox balance in organisms by promoting the production of·OH,enhancing PS NPs-induced liver damage and metabolic *** study will help us understand the health risks of NPs and to avoid underestimation of the risks of NPs in nature.

关键词： Polystyrene nanoplastics Ultraviolet-aged nanoplastics Metabolic pathway Metabolomics Hydroxyl radical

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Degradation of Rhodamine B by MnFe-LDH/PMS/O_(3) three-phase catalytic system: performance, mechanism and ecotoxicity studies

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Frontiers of Environmental Science & Engineering 2024年第1期18卷 111-127页

作者： Ying Han Ying Yang Weibao Liu Yilong Hou Ce Wang Jiangwei Shang Xiuwen Cheng Key laboratory of Pollutant Chemistry and Environmental Treatment College of Chemistry and Environmental ScienceYili Normal UniversityYining 835000China Key laboratory for Environmental Pollution Prediction and Control of Gansu Province College of Earth and Environmental SciencesLanzhou UniversityLanzhou 730000China

This study developed a novel MnFe-LDH/PMS/O3 three-phase catalytic system to degrade the organic dye RhB, which was used to address the drawbacks of persulfate oxidation and ozonation techniques. The structure, ionic and elemental composition, specific surface area, and magnetic properties of the LDHs were investigated using a variety of physicochemical characterization tools. The results showed that MnFe-LDH had a large specific surface area, a rich crystalline phase composition, and a functional group structure. The RhB degradation rate of MnFe-LDH/PMS/O3 was 0.34 min−1, which was much higher than that of other comparative systems. RhB could be completely degraded in 10 min after optimization and had a significant effect on TOC removal. The system was found to be effective over a wide pH range. Common anions were largely unaffected and humic acid acted as an inhibitor. At the same time, the system had generally effective degradation performance for different dyes. Combined with quenching experiments and EPR, it was found that SO4•−, •OH, O_(2)•−, and 1O_(2) all participated in the reaction, and •OH contributed more. The degradation pathway of RhB was derived by LC-MS, and the T.E.S.T. evaluation found that the toxicity of the intermediate product was significantly reduced. Finally, the stability and availability of LDHs were verified using cycling experiments and metal ion leaching. This work provides a theoretical basis and data support for the synergistic catalysis of PMS/O3 and the deep treatment of dye wastewater.

关键词： Rhodamine B Layered double hydroxides Peroxymonosulfate Ozonation

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The age of vanadium-based nanozymes: Synthesis, catalytic mechanisms, regulation and biomedical applications

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Chinese Chemical Letters 2024年第4期35卷 52-60页

作者： Shuaiwen Li Zihui Chen Feng Yang Wanqing Yue Department of Chemistry Key Laboratory of Biomedical Functional MaterialsSchool of ScienceChina Pharmaceutical UniversityNanjing 211198China Key laboratory of Drug Quality Control and Pharmacovigilance(China Pharmaceutical University) Ministry of EducationNanjing 211198China

Nanomaterials with enzyme-mimic(nanozyme) activity have garnered considerable attention as a potential alternative to natural enzymes, thanks to their low preparation cost, high activity, ease of preservation, and unique physicochemical properties. Vanadium(V) is a transition metal that integrates the benefits of valence-richness, low cost, and non-toxicity, making it a desirable candidate for developing a range of emerging nanozymes. In this review, we provide the first systematic summary of recent research progress on V-based nanozymes. First, we summarize the preparation of V-based nanozymes using both top-down and bottom-up synthesis methods. Next, we review the mechanism of V-based nanozymes that mimic the activity of various enzymes. We then discuss methods for regulating V-based nanozyme activity, including morphology, size, valence engineering, defect engineering, external triggering, and surface engineering. Afterward, we outline various biomedical applications, including therapeutic, anti-inflammatory, antibacterial, and biosensing. Finally, we prospect the challenges and countermeasures for V-based nanozymes based on their development. By summarizing recent research progress on V-based nanozymes, we hope to provide useful insights for researchers to further explore their potential applications and overcome their existing challenges.

关键词： Vanadium Nanozymes Catalytic mechanisms Biomedical applications Regulation

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Mitochondria-targeted nano-AIEgens as a powerful inducer for evoking immunogenic cell death

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Chinese Chemical Letters 2024年第5期35卷 338-343页

作者： Kun-Heng Li Hong-Yang Zhao Dan-Dan Wang Ming-Hui Qi Zi-Jian Xu Jia-Mi Li Zhi-Li Zhang Shi-Wen Huang Key laboratory of Biomedical Polymers of Ministry of Education Department of ChemistryWuhan UniversityWuhan 430072China

AIEgens can serve as an effective platform for the construction of photosensitizer-based immunogenic cell death(ICD)*** date,several mitochondria or endoplasmic reticulum(ER)-targeted aggregationinduced emission(AIE)molecules have been developed and have evoked massive ICD in ***,due to the complex physicochemical environment in cells,these small AIE molecules cannot maintain a stable aggregate state,which not only affects the fluorescence intensity of the photosensitizer but also decreases the generation of reactive oxygen species(ROS),and thus reducing the effect of the photosensitizer to elicit ***-based nanomicelles,which maintain a stable micellar structure,can prevent defects of AIE molecules in photodynamic therapy(PDT)***,in this study,a mitochondria-targeted AIE nanophotosensitizer was synthesized and used as a highly potent ICD inducer for vaccine preparation and tumor prevention.

关键词： Aggregation induced emission Photodynamic therapy Immunogenic cell death Reactive oxygen species Nanophotosensitizer Mitochondria

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