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Nucleophiles promotes the decomposition of electrophilic functional groups of tetracycline in ZVI/H_(2)O_(2) system: Efficiency and mechanism

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Chinese Chemical Letters 2024年第10期35卷 414-420页

作者： Xin Li Wanting Fu Ruiqing Guan Yue Yuan Qinmei zhong Gang Yao Sheng-Tao Yang Liandong Jing Song bai Key Laboratory of Pollution Control Chemistry and Environmental Functional Materials for Qinghai-Tibet Plateau of the National Ethnic Affairs Commission School of Chemistry and EnvironmentSouthwest Minzu UniversityChengdu 610041China Key Laboratory of General Chemistry of the National Ethnic Affairs Commission School of Chemistry and EnvironmentSouthwest Minzu University.Chengdu 610041China Institute of Environmental Engineering RWTH Aachen UniversityAachen 52062Germany

When zero-valent iron(ZVI)is prepared and applied under neutral conditions,it is easy to form oxides or hydroxides on its surface,which hinders the electron release of *** this end,a nucleophile was introduced into the ZVI system to inhibit the precipitation of iron ions,improve the conductivity of the solution,and promote the removal efficiency of electrophilic functional groups in organic *** this study,the addition of nucleophiles such as ethylenediamine,methylamine and dimethylamine to the ZVI/H_(2)O_(2)system resulted in an enhanced removal efficiency of tetracycline(TC)under neutral condition,while electrophiles such as EDTA-2Na and oxalic acid dihydrate impeded the removal of *** results demonstrated that the presence of nucleophiles could effectively promote the release of iron ions and increase the proportion of ferrous in both aqueous solution and solid surface of *** and theoretical calculation results revealed that the electrophilic functional group was eliminated in the TC molecule,and the toxicity of the treated solution was reduced ***,this work provides a selection of the conditions and pollutants applicable to ZVI under neutral pH conditions.

关键词： ZVI Nucleophiles Tetracycline Electrophilicfunctionalgroup Electronic transfer

Application of UiO-66 and its composites for remediation and resource recovery of typical environmental contaminants:a review

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Rare Metals 2024年第6期43卷 2498-2526页

作者： Hui-Min Zhang Yun-Long Wang Xin-Feng Zhu zhen-zhen Huang Dan-Dan Pang Kai Wang Chao-Hai Wang zhong-Xian Song Shi-Qiang Yin Lin-Lin Chang Jin-Hui Zhang School Infirmary Henan University of Urban ConstructionPingdingshan 467036China Faculty of Environmental and Municipal Engineering Henan Key Laboratory of Water Pollution Control and Rehabilitation TechnologyKey Laboratory of Carbon Emission Reduction and Combined Air Pollution Control TechnologyHenan University of Urban ConstructionPingdingshan 467036China School of Resources&Environment Collaborative Innovation Center of Coalbed Methane and Shale Gas for Central Plains Economic RegionHenan Polytechnic UniversityJiaozuo 454003China The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters Ministry of EducationGuangzhou Higher Education Mega CentreSouth China University of TechnologyGuangzhou 510006China

UiO-66 series metal-organic framework materials(MOFs)are typical porous materials assembled by Zr^(4+) with a large mass-to-nucleus ratio and terephthalic acid ligands,which form tetrahedral and octahedral cages arranged in a periodic triangular window *** to the strong interaction between Zr and O,UiO-66 series MOFs exhibit high thermal stability,structural stability,and chemical *** article mainly reviews the applications of UiO-66 and its composites in adsorption,photocatalysis,and resource utilization,while exploring the harm of pollutants to human health and the *** the first part,the differences in adsorption and removal mechanisms of liquid organic pollutants,heavy metals,and volatile organic compounds(VOCs)are *** results show that organic pollutants are mainly removed by physical adsorption,electrostatic interactions,hydrogen bonding,andπ-πinteractions,while heavy metals are mainly removed by chemical adsorption,electrostatic interactions,reduction,and *** are mainly removed by the pore volume and pore size structure of the *** catalysis can achieve non-toxic treatment of pollutants,and this study mainly focuses on UiO-based composite materials constructed by strategies such as semiconductor composites,ion doping,and metal/dye *** the second part,the synergistic effect between the components of UiO-based composite materials promotes the oriented and rapid separation and transfer of earriers at the material interface,thereby promoting the generation of active species such as h^(+),·O_(2)^(-) and·OH,and achieving rapid degradation of pollutants and detoxification of heavy *** the third part,heterojunctions can realize the resource utilization of pollutants in water and air,producing energy-type substances such as hydrogen and methanol while solving environmental *** addition,this article also summarizes the harm of common typical pollutants to the environment

关键词： UiO Adsorption Photocatalysis Environmental pollution Resource recovery

Bifunctional noble-metal-free cocatalyst coating enabling better coupling of photocatalytic CO_(2)reduction and H_(2)O oxidation on direct Z-scheme heterojunction

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Nano Research 2024年第6期17卷 5022-5030页

作者： Wei Zhao Weihao Mo Yan Zhang Lingxuan Hu Yiyi zheng Zhulei Chen Xiangyue Niu Yuling Zhao Lichun Liu Shuxian zhong Song bai Key Laboratory of the Ministry of Education for Advanced Catalysis Materials College of Chemistry and Materials ScienceZhejiang Normal UniversityJinhua 321004China College of Biological Chemical Sciences and Engineering and Nanotechnology Research InstituteJiaxing UniversityJiaxing 314001China College of Geography and Environmental Sciences Zhejiang Normal UniversityJinhua 321004China College of Chemical and Biological Engineering Zhejiang UniversityHangzhou 310058China School of Biological and Chemical Engineering Panzhihua UniversityPanzhihua 617000China

Selective loading of spatially separated redox cocatalysts on direct Z-scheme heterojunctions holds great promise for advancing the efficiency of artificial photosynthesis,which however is limited to the photodeposition of noble metal cocatalysts and the fabrication of hollow double-shelled semiconductor ***,the co-exposure of discrete cocatalyst and semiconductor increases the product diversity when both the exposed sites of which participate in CO_(2)***,we present a facile and versatile protocol to overcome these limitations via surface coating of Z-scheme heterojunctions with bifunctional noble-metal-free *** Cu_(2)O/Fe_(2)O_(3)(CF)as a model heterojunction and layered Ni(OH)_(2)as a model cocatalyst,it is found that Ni(OH)_(2)lying on the surfaces of Cu_(2)O and Fe_(2)O_(3)separately co-catalyzes the CO_(2)reduction and H_(2)O *** experimental and theoretical investigation reveals that the Ni(OH)_(2)outer layer:(i)mitigates the charge recombination in CF and balances their transfer and consumption;(ii)reduces the rate-determining barriers for CO_(2)-to-CO and H_(2)O-to-O_(2)conversion,(iii)suppresses the side proton reduction occurring on CF,and(iv)protects the CF from component *** expected,the redox reactions stoichiometrically proceed,and significantly enhanced photocatalytic activity,selectivity,and stability in CO generation are achieved by the stacked Cu_(2)O/Fe_(2)O_(3)@Ni(OH)_(2)in contrast to *** study demonstrates the significance of the synergy between bifunctional cocatalysts and Z-scheme heterojunctions for improving the efficacy of overall redox reactions,opening a fresh avenue for the rational design of artificial photosynthetic systems.

关键词： Z-scheme heterojunction bifunctional cocatalyst CO_(2)reduction H_(2)O oxidation stoichiometric redox reaction

Abiotic stress treatment reveals expansin like A gene OfEXLA1 improving salt and drought tolerance of Osmanthus fragrans by responding to abscisic acid

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Horticultural Plant Journal 2024年第2期10卷 573-585页

作者： Bin Dong Qianqian Wang Dan Zhou Yiguang Wang Yunfeng Miao Shiwei zhong Qiu Fang Liyuan Yang zhen Xiao Hongbo Zhao School of Landscape Architecture Zhejiang Agriculture and Forestry UniversityHangzhouZhejiang 311300China Zhejiang Provincial Key Laboratory of Germplasm Innovation and Utilization for Garden Plants HangzhouZhejiang 311300China Key Laboratory of National Forestry and Grassland Administration on Germplasm Innovation and Utilization for Southern Garden Plants HangzhouZhejiang 311300China

Sweet osmanthus(Osmanthus fragrans) is a having general approval aromatic tree in China that is widely applied to landscaping and gardening. However, the evergreen tree adaptability is limited by many environmental stresses. Currently, limited information is available regarding the genetic analysis and functional identification of expansin genes in response to abiotic stress in sweet osmanthus. In this study, a total of 29 expansin genes were identified and divided into four groups by genome-wide analysis from the sweet osmanthus genome. Transcriptome and quantitative Real-time PCR analysis showed that the cell wall-localized protein expansin-like A(OfEXLA1) gene was significantly induced by salt and drought treatment. Histochemical GUS staining of transgenic Arabidopsis lines in which GUS activity was driven with the OfEXLA1 promoter, GUS activity was significantly induced by salt, drought, and exogenous abscisic acid(ABA). In yeast, we found OfEXLA1overexpression significantly improved the population of cells compared with wild-type strains after NaCl and polyethylene glycol(PEG)treatment. Additionally, OfEXLA1 overexpression not only promoted plant growth, but also improved the salt and drought tolerance in Arabidopsis. To gain insight into the role of ABA signaling in the regulation of OfEXLA1 improving abiotic tolerance in sweet osmanthus, four differentially expressed ABA Insensitive 5(ABI5)-like genes(OfABL4, OfABL5, OfABL7, and OfABL8) were identified from transcriptome, and dualluciferase(dual-LUC) and yeast one hybrid(Y1H) assay showed that OfABL4 and OfABL5 might bind to OfEXLA1 promoter to accumulate the OfEXLA1 expression by responding to ABA signaling to improve abiotic tolerance in sweet osmanthus. These results provide the information for understanding the molecular functions of expansin-like A gene and molecular breeding of sweet osmanthus in future.

关键词： Osmanthus fragrans Abiotic tolerance Expansin Abscisic acid

Overlooked interaction between redox-mediator and bisphenol-A in permanganate oxidation

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Environmental Science and Ecotechnology 2024年第5期21卷 248-255页

作者： Honglong Zhang Qiaoqiao Zhao Kangbao zhong Ruopeng bai Jiaojiao Dong Jun Ma Jing Zhang Timothy J.Strathmann School of Environment Harbin Institute of TechnologyHarbin150090PR China Institute of Nuclear and New Energy Technology Tsinghua UniversityBeijing100084PR China School of Chemistry and Chemical Engineering Chongqing Key Laboratory of Chemical Theory and MechanismChongqing UniversityChongqing401331PR China College of Environment and Ecology Chongqing UniversityChongqing400045PR China Department of Civil and Environmental Engineering Colorado School of Mines1500 Illinois StreetGoldenCO80401United States

Research efforts on permanganate(Mn(VII))combined with redox-mediator(RM),have received increasing attention due to their significant performance for bisphenol-A(BPA)***,the mechanisms underpinning BPA degradation remain *** we show the overlooked interactions between RM and BPA during permanganate oxidation by introducing an RMdN-hydroxyphthalimide(NHPI).We discovered that the concurrent generation of MnO_(2) and phthalimide-N-oxyl(PINO)radical significantly enhances BPA oxidation within the pH range of *** detection of radical cross-coupling products between PINO radicals and BPA or its derivatives corroborates the pivotal role of radical cross-coupling in BPA ***,we observed the formation of an NHPI-BPA complex,which undergoes preferential oxidation by Mn(VII),marked by the emergence of an electronrich domain in *** findings unveil the underlying mechanisms in the Mn(VII)/RM system and bridge the knowledge gap concerning BPA transformation via *** research paves the way for further exploration into optimizing complexation sites and RM dosage,significantly enhancing the system's efficiency in water treatment applications.

关键词： Permanganate Redox-mediator Bisphenol-A Radical cross-coupling Complexation

Engineering the axial coordination of cobalt single atom catalysts for efficient photocatalytic hydrogen evolution

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Nano Research 2024年第6期17卷 5114-5121页

作者： Ning Kang Lingwen Liao Xue Zhang zhen He Binlu Yu Jiahong Wang Yongquan Qu Paul KChu Seeram Ramakrishna Xue-Feng Yu Xin Wang Licheng bai Materials Interfaces Center Shenzhen Institute of Advanced TechnologyChinese Academy of Sciences(CAS)Shenzhen 518055China Key Laboratory of Materials Physics Anhui Key Laboratory of Nanomaterials and NanotechnologyCAS Center for Excellence in NanoscienceInstitute of Solid State PhysicsChinese Academy of SciencesHefei 230031China Department of Chemistry City University of Hong KongKowloonHong Kong 999077China Hong Kong Branch of National Precious Metals Material Engineering Research Center(NPMM) City University of Hong KongKowloonHong Kong 999077China Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an 710072China Department of Physics and Department of Materials Science and Engineering City University of Hong KongKowloonHong Kong 999077China National University of Singapore(NUS)Centre for Nanofibers and Nanotechnology Department of Mechanical EngineeringNational University of SingaporeSingapore 117542Singapore

Improving the catalytic activity of non-noble metal single atom catalysts(SACs)has attracted considerable attention in materials *** optimizing the local electronic structure of single atom can greatly improve their catalytic activity,it often involves in-plane modulation and requires high ***,we report a novel strategy to manipulate the local electronic structure of SACs via the modulation of axial Co-S bond anchored onto graphitic carbon nitride(C_(3)N_(4))at room temperature(RT).Each Co atom is bonded to four N atoms and one S atom(Co-(N,S)/C_(3)N_(4)).Owing to the greater electronegativity of S in the Co-S bond,the local electronic structure of the Co atoms is available to be controlled at a relatively moderate ***,when employed for the photocatalytic hydrogen evolution reaction,the adsorption energy of intermediate hydrogen(H*)on the Co atoms is remarkably *** the presence of the Co-(N,S)/C_(3)N_(4)SACs,the hydrogen evolution rates reach up to 10 mmol/(g·h),which is nearly 10 and 2.5 times greater than the rates in the presence of previously reported transition metal/C_(3)N_(4)and noble platinum nanoparticles(PtNPs)/C_(3)N_(4)catalysts,*** to the tailorable axial Co-S bond in the SAC,the local electronic structure of the Co atoms can be further optimized for other photocatalytic *** axial coordination engineering strategy is universal in catalyst designing and can be used for a variety of photocatalytic applications.

关键词： transition metal single-atom local electronic structure photocatalytic hydrogen evolution graphitic carbon nitride axial coordination environment

Direct ink writing of multifunctional gratings with gel-like MXene/norepinephrine ink for dynamic electromagnetic interference shielding and patterned Joule heating

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Nano Research 2024年第3期17卷 1585-1594页

作者： Pei-Zhu Jiang Zhiming Deng Peng Min Lvxuan Ye Cheng-Zhang Qi Hao-Yu Zhao Ji Liu Hao-Bin Zhang zhong-zhen Yu Beijing Key Laboratory of Advanced Functional Polymer Composites Beijing University of Chemical TechnologyBeijing 100029China State Key Laboratory of Organic-Inorganic Composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China School of Chemistry CRANN and AMBERTrinity College DublinDublin D02PN40Ireland

Intelligent electromagnetic interference(EMI)shielding modulators with a wide tuning range and cyclic stability are urgently needed but their fabrication remains challenging.A gel-like MXene/norepinephrine ink is developed and multifunctional MXene gratings with wide EMI shielding effectiveness(SE)tuning range,superior reversibility,and high mechanical flexibility are constructed by direct ink writing approach for dynamic EMI shielding and patterned Joule heating *** modulable MXene/norepinephrine grating with a high conductivity of 3510 S·cm-1 can conveniently realize the seamless modulation of the EMI SE by adjusting the angle between the MXene grating filaments and the electric field of the incident electromagnetic waves,offering highly reversible switching between shielding“On”(28.0 dB)and“Off”(0.5 dB)***,due to the optimized integration of the MXene ink and the rationally designed pattern,a superior specific EMI SE of 95,688.2 dB·cm^(2)·g^(-1) is achieved in the“On”***,the MXene/norepinephrine ink can be used to fabricate many complex patterned gratings with superior stability,instant responsibility,and superb mechanical flexibility,exhibiting a unique patterned Joule heating *** writing of multifunctional gratings paves a means for developing intelligent EMI shielding materials,wearable electronic devices,and advanced thermal management materials.

关键词： MXene ink direct ink writing electromagnetic interference shielding multifunctional gratings Joule heating

HSP110 aggravates ischemia-reperfusion injury after liver transplantation by promoting NF-κB pathway

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Hepatobiliary & Pancreatic Diseases International 2024年第4期23卷 344-352页

作者： Qing-Zhi Hu zhen-Rui Cao Wei-Xiong zheng Min-Jie Zhao Jun-Hua Gong Cong Chen zhong-Jun Wu Rui Tao Department of Hepatobiliary Surgery Bishan Hospital of Chongqing Medical UniversityChongqing 402760China Department of Cardiothoracic Surgery the First Affiliated Hospital of Chongqing Medical UniversityChongqing 400016China c Department of Hepatobiliary Surgery the First Affiliated Hospital of Chongqing Medical UniversityChongqing 400016China Department of Hepatobiliary Surgery the Second Affiliated Hospital of Chongqing Medical UniversityChongqing 400010China

Background:Ischemia-reperfusion injury(IRI)poses a significant challenge to liver transplantation(LT).The underlying mechanism primarily involves overactivation of the immune *** shock protein 110(HSP110)functions as a molecular chaperone that helps stabilize protein ***:An IRI model was established by performing LT on Sprague-Dawley rats,and HSP110 was silenced using ***-eosin staining,TUNEL,immunohistochemistry,ELISA and liver enzyme analysis were performed to assess IRI following *** blotting and quantitative reverse transcription-polymerase chain reaction were conducted to investigate the pertinent molecular ***:Our findings revealed a significant increase in the expression of HSP110 at both the mRNA and protein levels in the rat liver following LT(P<0.05).However,when rats were injected with siRNAHSP110,IRI subsequent to LT was notably reduced(P<0.05).Additionally,the levels of liver enzymes and inflammatory chemokines in rat serum were significantly reduced(P<0.05).Silencing HSP110 with siRNA resulted in a marked decrease in M1-type polarization of Kupffer cells in the liver and downregulated the NF-κB pathway in the liver(P<0.05).Conclusions:HSP110 in the liver promotes IRI after LT in rats by activating the NF-κB pathway and inducing M1-type polarization of Kupffer *** HSP110 to prevent IRI after LT may represent a promising new approach for the treatment of LT-associated IRI.

关键词： Ischemia-reperfusion injury Liver transplantation Inflammation HSP110 Heat shock proteins NF-κB

Asymmetric Autotandem Palladium Catalysis forα,β-Unsaturated Lactones:Merging Olefin and Ester Hydrogenation

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CCS Chemistry 2024年第8期6卷 1987-1999页

作者： Lei Sun Han Wang Die bai Chang-Bin Yu Bo Wu Rong-zhen Liao Yong-Gui Zhou State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023Liaoning School of Chemistry and Chemical Engineering Huazhong University of Science and TechnologyWuhan 430074Hubei

Autotandem catalysis(ATC)is fascinating since a single catalyst can promote tandem reactions involving two or more mechanisms in a single reactor and is a highly desirable approach to realize multifarious transformations in organic synthetic ***,a palladium-catalyzed asymmetric autotandem hydrogenation ofα,β-unsaturated lactones is disclosed,providing chiral saturated *** this reaction,the C=C bond inα,β-unsaturated lactones was first hydrogenated to give the dihydrocoumarins with high enantioselectivity,followed by hydrogenation of the ester group with the same catalytic ***,after decreasing the reaction temperature,hydrogenation of the single C=C bond proceeded smoothly,delivering the dihydrocoumarin products with high yield and *** experiments and density functional theory calculations were carried out to elucidate the cause of this unusual asymmetric autotandem ***,the homogeneous palladium catalyst was successfully applied in the hydrogenation of esters under neutral conditions.

关键词： autotandem catalysis asymmetric hydrogenation chiral dihydrocoumarins hydrogenation of esters α β-unsaturated esters