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Atmospheric chemistry of 2-nitrobenzaldehyde:Initiated by photo-excitation,OH-oxidation,and small TiO_(2) clusters adsorption catalysis

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Journal of environmental Sciences 2024年第5期139卷 123-137页

作者： Feng-Yang Bai Xiang-Huan Liu Ting-Ting Meng Zhou Yu Yi-Chen Wang Shuang Ni Zhen Zhao institute of Catalysis for Energy and environment College of Chemistry and Chemical EngineeringShenyang Normal UniversityShenyang 110034China

The fate of 2-nitrobenzaldehyde(2-NBA)is of interest in atmospheric chemistry as it is a semi-volatile organic compound with high *** study presents a quantum chemical study of the gas-phase reactions of 2-NBA photo-excitation and OH-oxidation in the absence and presence of small TiO_(2) *** further understand the unknown photolysis mechanism,the photo-reaction pathways of ground singlet state and the lying excited triplet state of 2-NBA were investigated including the initial and subsequent reactions of proton transfer,direct CO,NO_(2),and HCO elimination routes in the presence of O_(2) and ***,the OH-mediated degradation of 2-NBA proceeded via five H-extraction and six OH-addition channels by indirect mechanism,which follows a succession of reaction steps initiated by the formation of weakly stable intermediate *** H-extraction from the-CHO group was the dominant pathway with a negative activation energy of-1.22 kcal/*** calculated rate coefficients at 200–600 K were close to the experimental data in literature within 308-352 K,and the kinetic negative temperature independence was found in both experimental literature and computational ***,2-NBA was favored to be captured onto small TiO_(2) clusters via six adsorption configurations formed via various combination of three types of bonds of Ti…O,Ti…C,and O…H between the molecularly adsorbed 2-NBA and TiO_(2) *** indicted that the chemisorptions of aldehyde oxygen have largest *** results suggested adsorption conformations have a respectable impact on the catalysis *** study is significant for understanding the atmospheric chemistry of 2-nitrobenzaldehyde.

关键词： 2-nitrobenzaldehyde OH radical oxidation Rate coefficient Photolysis mechanism Adsorption catalysis

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Design of dual-functional protic porous ionic liquids for boosting selective extractive desulfurization

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Petroleum Science 2024年第4期21卷 2817-2829页

作者： Jin-Rui Zhang Jie Yin Jing He Hong-Shun Ran Wei Jiang Hong-Ping Li Wen-Shuai Zhu Hua-Ming Li Ming Zhang School of the environment and Safety Engineering & institute for Energy Research Jiangsu University School of Chemistry and chemical Engineering Jiangsu University

Porous ionic liquids have demonstrated excellent performance in the field of separation, attributed to their high specific surface area and efficient mass transfer. Herein, task-specific protic porous ionic liquids(PPILs) were prepared by employing a novel one-step coupling neutralization reaction strategy for extractive desulfurization. The single-extraction efficiency of PPILs reached 75.0% for ***, adding aromatic hydrocarbon interferents resulted in a slight decrease in the extraction efficiency of PPILs(from 45.2% to 37.3%, 37.9%, and 33.5%), indicating the excellent extraction selectivity of PPILs. The experimental measurements and density functional theory calculations reveal that the surface channels of porous structures can selectively capture dibenzothiophene by the stronger electrophilicity(Eint(HS surface channel/DBT)=-39.8 kcal mol-1), and the multiple extraction sites of ion pairs can effectively enrich and transport dibenzothiophene from the oil phase into PPILs through π...π, C-H...π and hydrogen bonds interactions. Furthermore, this straightforward synthetic strategy can be employed in preparing porous liquids, offering new possibilities for synthesizing PPILs with tailored functionalities.

关键词： Protic porous ionic liquids Extractive desulfurization Selectivity Density functional theory

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A systematic understanding of microbial reductive dechlorination towards an improved “one health” soil bioremediation: A review and perspective

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Science China Technological Sciences 2024年第10期67卷 3009-3031页

作者： HE Yan LI ShuYao YUAN Jing CHENG Jie DOU JiBo YANG XueLing XU JianMing Zhejiang Provincial Key Laboratory of Agricultural Resources and environment Institute of Soil and Water Resources and Environmental ScienceCollege of Environmental and Resource SciencesZhejiang University Key Laboratory of environment Remediation and Ecological Health Ministry of Education Microbiome Network and Department of Agricultural biology Colorado State University Departments of Chemistry and chemical & Biomolecular Engineering Institute for Functional Intelligent Materials (I-FIM)National University of Singapore

Chlorinated organic pollutants(COPs), both emerging and traditional, are typical persistent pollutants that harm soil health worldwide. Dechlorinators mediated reductive dechlorination is the optimal way to completely remove COPs from anaerobic soil through a redox reaction driven by electron transfer during microbial anaerobic respiration. Generally, the dechlorinated depletion of COPs in situ often interacts with multiple element biogeochemical activities, e.g., methanogenesis, sulfate reduction, iron reduction, and denitrification. Elucidating the relevance of biogeochemical cycles between COPs and multiple elements and the coupled mechanisms involved, thus, helps to develop effective pollution control strategies with the balance between pollution degradation and element cycles in heterogeneous soil, ultimately contributing to “one health” goal. In this review, we summarized the microbial-chemical coupling redox processes and the driving factors, elucidated the interspecies metabolites exchange and electron transfer mechanisms within COP-dechlorinating communities, and further proposed a detailed design, construction, and analysis framework of engineering COP-dechlorinating microbiomes via “top-down” selfassembly and “bottom-up” synthesis to pave the way from laboratory to practical field application. Especially, we delve into the major challenges and perspectives surrounding the design of state-of-the-art synthetic microbial communities. Our goal is to improve the understanding of the microbial-mediated coupling between reductive dechlorination and element biogeochemical cycling, with a particular focus on the implications for health-integrated soil bioremediation under the “one health” concept.

关键词： reductive dechlorination biogeochemical redox processes interspecies interaction synthetic microbiomes, anaerobic soils

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Effect of yttrium and manganese addition on catalytic soot combustion activity and anti-high-temperature stability of CeO_(2) catalyst

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Journal of Rare Earths 2024年第2期42卷 334-344,I0004页

作者： Yi Zhu Xingyu Liu Wei Shi Jia Li Changbing Ye Ruimei Fang Huifeng Zhu Shanhu Chen Li Lan College of Chemistry biology and environment Yuxi Normal UniversityYuxi 653100China institute of biology and environmental Engineering Yuxi Normal UniversityYuxi 653100China College of environment and Resources Chongqing Technology and Business UniversityChongqing 400067China College of Chemistry and chemical Engineering Jiangxi Science and Technology Normal UniversityNanchang 330013China College of Materials and Mechatronics Jiangxi Science and Technology Normal UniversityNanchang 330013China

In order to analyze the influence of the addition of yttrium and manganese on the soot combustion performance and high temperature stability of CeO_(2) catalyst,a series of Y/Mn-modified CeO_(2) catalysts were *** effects of structural properties,textural properties,oxygen vacancies,Ce^(3+),surface adsorbed oxygen species,reduction properties and desorption properties of oxygen species on the activity were analyzed by various characterization *** results of the activity test show that the addition of manganese is beneficial to enhancement of the activity,while the addition of yttrium increases the amount of reactive oxygen species,but decreases the *** aging at 700℃,the activity of the CeMn catalyst decreases most sharply,while the catalytic activity of the CeY catalyst can be maintained to a certain ***,the addition of yttrium and manganese at the same time can stabilize the *** fundamental reason is that yttrium and manganese move to the surface of the solid solution after aging,which increases the reduction performance of the catalyst,thus contributing to the increase of *** the activity of CeYMn catalyst decreases after aging at 800℃,it is still higher than that of other catalysts aged at 700℃.

关键词： CeO_(2)catalyst Soot catalytic combustion Diesel pollution control Rare earths High temperature stability Low temperature reduction performance

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Effective peroxydisulfate activation by CQDs-MnFe_(2)O_(4)@ZIF-8 catalyst for complementary degradation of bisphenol A by free radicals and non-radical pathways

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Chinese chemical Letters 2024年第5期35卷 371-379页

作者： Shuo Li Xinran Liu Yongjie Zheng Jun Ma Shijie You Heshan Zheng College of Chemistry and chemical Engineering Qiqihar UniversityQiqihar 161006China State Key Laboratory of Urban Water Resource and environment School of EnvironmentHarbin Institute of TechnologyHarbin 150090China

The present study reported fabrication of novel carbon quantum dots-MnFe_(2)O_(4)@ZIF-8(CQDs-MFO@ZIF-8)by using co-precipitation hydrothermal method for activation of peroxydisulfate(PDS)to degrade bisphenol A(BPA),one of important emerging organic pollutants in water ***-MFO@ZIF-8 served as a highly efficient thermal activated PDS catalyst with high catalytic degradation efficiency,reusability and *** catalyst achieved almost completely removal of 20.0 mg/L BPA within 5.0 min,and the degradation efficiency remained higher than 83%after 5 consecutive *** radicals(^(·)OH,SO_(4)^(·-)and^(·)O_(2)^(-))and non-free radicals((1)O_(2))were generated in the thermal PDS-activation system,in which singlet oxygen((1)O_(2))played a dominant role in the degradation of *** potential toxicity of BPA degradation intermediates was analyzed upon the culture of *** and Chlorella sorokiniana by using Ecological Structure-Activity Relationship Model(ECOSAR)*** catalytic performances of BPA degradation by CQDs-MFO@ZIF-8 were evaluated for treatment of different practical water samples to further verify the feasibility of practical *** study provides proof-in-concept demonstration of new nanomaterials for enhanced catalytic water decontamination.

关键词： Bisphenol A Degradation Peroxydisulfate ^(1)O_(2) Toxicity analysis

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Activatable photoacoustic bioprobe for visual detection of aging in vivo

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Chinese chemical Letters 2024年第4期35卷 324-329页

作者： Zihong Li Jie Cheng Ping Huang Guoliang Wu Weiying Lin institute of Optical Materials and chemical biology Guangxi Key Laboratory of Electrochemical Energy MaterialsSchool of Chemistry and Chemical EngineeringGuangxi UniversityNanning 530004China

Aging is a natural physiological process with various challenges, related to the loss of homeostasis within the organism, which is not a disease, but a significantly strong risk factor for multiple diseases, including myocardial infarction, stroke, some age-related cancers, macular degeneration, osteoarthritis, neurodegeneration, and many others. In the body, the main manifestation of aging is cellular aging, which exists within tissues and has a local or global impact on tissue function. However, the lack of effective aging detection tools has always been an issue that cannot be ignored in the field of aging research. Therefore,it is necessary to construct a non-invasive tool for in vivo detection of aging. Here, we show that the photoacoustic probe(LGAL), which has peak excitation and emission wavelengths in the near-infrared optical window, binds in vivo and at high contrast to the hallmark of aging, and allows for the microscopic imaging of aging through the intact mice. Firstly, this tool LGAL has been successfully applied to detect senescence in cells, displaying stronger photoacoustic signals than normal cells. Then, by using the photoacoustic probe, the blood vessels and tissues inside the mice can be visualized. Young and elderly mice exhibit varying intensities of photoacoustic signals, marking the first time a probe has been used to explore the aging of blood vessels and tissues inside the mice. Finally, we monitored the changes in the degree of aging during tumor treatment under photoacoustic(PA) imaging for the first time. As the treatment time increased, the degree of aging of the tumor gradually deepened. We expect the powerful tool could be a noninvasive and powerful tool for the study of aging biology.

关键词： Near-infrared Photoacoustic Aging Senescence Tumor Sa-β-gal

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Strong metal-support interaction between AuPd nanoparticles and oxygen-rich defect ZrO_(2) for enhanced catalytic 5-hydroxymethylfurfural oxidation

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Chinese chemical Letters 2024年第2期35卷 507-511页

作者： Yunlei Zhang Yiran Liu Wen Guan Mengxue Cao Yao Chen Pengwei Huo institute of Green Chemistry and chemical Technology School of Chemistry and Chemical EngineeringJiangsu UniversityZhenjiang 212013China School of the environment and Safety Jiangsu UniversityZhenjiang 212013China

The unique properties of metal oxide surfaces,crystal surfaces and defects play vital roles in biomass upgrading *** this work,hierarchical porous bowl-shaped ZrO_(2)(HB-ZrO_(2))with mixed crystal phase was designed and employed as the support for loading AuPd bimetal with different proportions to synthesize AuPd/HB-ZrO_(2) *** effects of surface chemistry,oxygen defects,bimetal interaction and metal-support interaction of AuPd/HB-ZrO_(2) on catalytic performance for the selective oxidation of 5-hydroxymethylfurfural(HMF)to 2,5-furandicarboxylic acid(FDCA)were systematically *** Au 2 Pd1/HB-ZrO_(2) catalyst afforded a satisfactory FDCA yield of 99.9%from HMF oxidation using O_(2) as the oxidant in water,accompanied with an excellent FDCA productivity at 97.6 mmol g^(−1) h^(−1).This work offers fresh insights into rationally designing efficient catalysts with oxygen-rich defects for the catalytic upgrading of biomass platform chemicals.

关键词： 5-Hydroxymethylfurfural oxidation 2,5-Furandicarboxylic acid Oxygen-rich defect ZrO_(2) AuPd bimetal Bowl-shaped structure

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Evaluating the tumor stratification with a lysosomal pH sensitive-probe by fluorescence lifetime imaging

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Chinese chemical Letters 2024年第3期35卷 262-267页

作者： Jun Yan Xing Liang Qian Zhang Luolin Wang Weiying Lin Guangxi Key Laboratory of Electrochemical Energy Materials Institute of Optical Materials and Chemical BiologySchool of Chemistry and Chemical EngineeringGuangxi UniversityNanning 530004China

Owing to the anaerobic metabolism in the tumor,abundant acidic metabolites are produced and accumulated in the ***,the cells in different tumor layers are directly linked to the pH ***,due to the lack of robust tools,the high-efficient evaluation of the acidic micro-environment of tumor stratification faces the challenge of accurate *** designed a new pH sensitive fluorescent lifetime probe target to *** we expected,the fluorescence lifetime of PLN possesses a good linear fit to the pH value,which could detect the pH change at a single lysosome level in real time,and then evaluate the different acidity of tumor *** probe PLN is successfully used to evaluate the tumor stratification by fluorescence lifetime imaging microscopy(FLIM)for the first time,which is of great significance in the preoperative diagnosis of clinical tumor treatment or evaluation of drug delivery effect.

关键词： FLIM pH Fluorescence imaging Lysosome Tumor imaging

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The short and long-term effect of polystyrene nanoplastics on nitrifying sludge at high nitrite concentrations

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Journal of environmental Sciences 2024年第1期135卷 222-231页

作者： Xiaolong Wang Jialu Huang Zhiqiang Qi Ruiqin Kang Chao Du Da Li School of chemical and environmental Engineering Anyang Institute of TechnologyAnyang 455000China Henan Licheng environmental Technology Co. Ltd.Anyang 455000China State Key Laboratory of Urban Water Resource and environment School of EnvironmentHarbin Institute of TechnologyHarbin 150090China

The effect of nanoplastics(NPs)on nitrite oxidation bacteria(NOB)community in treating high-strength wastewater remains unclear,which seriously affects the stability of nitrogen removal *** this study,highly active nitrifying sludge was enriched and exposed to 50nm polystyrene NPs(PS-NPs)for short-term(1,100,500,and 1000 mg/L,1.5 hr)and long-term(1,10,100 mg/L,40 days)at high nitrite *** contrast to previous studies,our results showed that the exposures to PS-NPs had little effect on nitrifying *** long-term exposure,the protein/polysaccharide ratios in extracellular polymeric substances(EPS)were positively correlated with PS-NPs concentrations(0.78–0.99).The produced reactive oxygen species(ROS)were gradually removed,and PS-NPs higher than 10 mg/L caused damage to membrane ***-term exposure for 40 days increased the community diversity and caused significant differences between the control and exposed *** control group were dominated by Nitrobacter and Exiguobacterium,while the exposure group was dominated by Bacillus,Mycobacterium,and Nitrospira.A noticeable shift in the NOB community from Nitrobacter(26.5%to 3.4%)to Nitrospira(1.61%to 14.27%)was observed.A KEGG analysis indicated a decrease in cell growth and death,cell motility and energy *** appeared that NOB could adapt to PS-NPs stress through enhanced secretion and removal of oxidative ***,this study provided new insights into the response mechanism of NOB to PS-NPs exposure.

关键词： Nanoplastics Nitrifying activity Extracellular polymeric substance(EPS) Exposure Community analysis

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TiO_(2) nanofiber-supported copper nanoparticle catalysts for highly efficient methane conversion to C1 oxygenates under mild conditions

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Nano Research 2024年第5期17卷 3844-3852页

作者： Wencui Li Yu Ren Zean Xie Yipeng Wang Hang Zhang Dianxiang Peng Hengfang Shen Hongfei Shi Jiaxin Cai Peng Wang Tongxin Zhang Zhen Zhao State Key Laboratory of Heavy Oil Processing China University of Petroleum(Beijing)Beijing 102249China institute of Catalysis for Energy and environment College of Chemistry&Chemical EngineeringShenyang Normal UniversityShenyang 110034China institute of Petrochemical Technology Jilin Institute of Chemical TechnologyJilin 132022China

The selective oxidation of methane under mild conditions remains the“Holy Grail of Catalysis”.The key to activating methane and inhibiting over-oxidation of target oxygenates lies in designing active *** nanoparticles were loaded onto TiO_(2) nanofibers using the photo-deposition *** resulting catalysts were found to effectively convert methane into C1 oxygenated products under mild *** with previously reported catalysts,it delivers a superior performance of up to 2510.7 mmol·g_(Cu)^(-1)·h^(-1) productivity with a selectivity of around 100%at 80℃for 5 *** characterizations and density functional theory(DFT)calculations indicate that TiO_(2) in the mixed phase of anatase and rutile significantly increases the Cu^(+)/CuO ratio of the supported Cu species,and this ratio is linearly related to the formation rate of oxygen-containing *** CuI site promotes the generation of active O species from H_(2)O_(2) dissociation on Cu_(2)O(111).These active O species reduce the energy barrier for breaking the C-H bond of CH_(4),thus boosting the catalytic *** methane conversion mechanism was proposed as a methyl radical pathway to form CH_(3)OH and CH_(3)OOH,and then the generated CH_(3)OH is further oxidized to HOCH_(2)OOH.

关键词： TiO_(2)nanofiber copper nanoparticles photo-deposition method methane oxidation C1 oxygenates

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