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Zinc oxide nano-enabled microfluidic reactor for water purification and its applicability to volatile organic compounds

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Microsystems & Nanoengineering 2018年第1期4卷 450-456页

作者： Imadeddine Azzouz Yamina Ghozlane Habba Martine Capochichi-Gnambodoe Frédéric Marty Jérôme Vial Yamin Leprince-Wang Tarik Bourouina UniversitéParis-Est ESIEE-ParisESYCOM EA 25522 Boulevard Blaise Pascal93162 Noisy-le-GrandFrance UniversitéParis-Est UPEMESYCOM EA 25525 Boulevard Descartes77420 Champs sur MarneFrance LSABM CNRS UMR 8231ESPCI ParisTech-PSL Research University10 Rue Vauquelin75005 ParisFrance

This paper reports fast and efficient chemical decontamination of water within a tree-branched centimeter-scale microfluidic *** microreactor integrates Zinc oxide nanowires(ZnO NWs)in situ grown acting as an efficient photocatalytic nanomaterial *** growth of ZnO NWs within the microfluidic chamber brings this photocatalytic medium at the very close vicinity of the water flow path,hence minimizing the required interaction time to produce efficient purification *** demonstrate a degradation efficiency of 95%in o5 s of residence time in one-pass *** to our estimates,it becomes attainable using microfluidic reactors to produce decontamination of merely 1 l of water per day,typical of the human daily drinking water *** conduct our experiments,we have chosen a laboratory-scale case study as a seed for addressing the health concern of water contamination by volatile organic compounds(VOCs),which remain difficult to remove using alternative decontamination techniques,especially those involving water *** contaminated water sample contains mixture of five pollutants:Benzene;Toluene;Ethylbenzene;m–p Xylenes;and o-Xylene(BTEX)diluted in water at 10 *** of *** was analytically monitored in a selective manner until it falls below 1 *** each of the five pollutants,corresponding to the maximum contaminant level(MCL)established by the US Environmental Protection Agency(EPA).We also report on a preliminary study,investigating the nature of the chemical by-products after the photocatalytic VOCs degradation process.

关键词： microfluidic reactor water purification zinc oxide nanowires volatile organic compounds(VOCs) Benzene,Toluene,Ethylbenzene,m-p Xylenes,o-Xylene(BTEX)

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Accelerating water dissociation at carbon supported nanoscale Ni/NiO heterojunction electrocatalysts for high-efficiency alkaline hydrogen evolution

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Nano Research 2023年第4期16卷 4742-4750页

作者： Cong Li Jiang-Yan Xue Wei Zhang Fei-Long Li Hongwei Gu Pierre Braunstein Jian-Ping Lang College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of Chemistry and Materials Engineering Changshu Institute of TechnologyChangshu 215500China Universitéde Strasbourg-CNRS Institut de Chimie(UMR 7177 CNRS)4 rue Blaise Pascal-CS 90032Strasbourg 67081France

The synergistic catalysis of heterojunction electrocatalysts for the multi-step process in hydrogen evolution reaction(HER)is a promising approach to enhance the kinetics of alkaline ***,we proposed a strategy to form nanoscale Ni/NiO heterojunction porous graphitic carbon composites(Ni/NiO-PGC)by reduction-pyrolysis of the preformed Ni-metal-organic framework(MOF)under H2/N2 *** from low electron transfer resistance,increased number of active sites,and unique hierarchical micro-mesoporous structure,the optimized Ni/NiO-PGC_(10-1-400)exhibited excellent electrocatalytic performance and robust stability for alkaline HER(η10=30 mV,65 h).Density functional theory(DFT)studies revealed that the redistribution of electrons at the Ni/NiO interface enables the NiO phase to easily initiate the dissociation of alkaline H_(2)O,and shifts down the d-band center of Ni and optimizes the H*adsorption-desorption process of Ni,thereby leading to extremely high HER *** work contributes to a further understanding of the synergistic promotion of the multi-step HER processes by heterojunction electrocatalysts.

关键词： water dissociation Ni/NiO heterojunction metal-organic frameworks(MOFs)derivatives hydrogen evolution reaction reduction pyrolysis

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Electronic engineering of Co-Ru diatomic sites and Ru nanoparticles for synergistic promotion of hydrogen evolution

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Nano Research 2024年第5期17卷 3714-3723页

作者： Wei Zhang Cong Li Yongyong Cao Jun-Yang Ji Zhao-Chen Li Zheng Niu Hongwei Gu Pierre Braunstein Jian-Ping Lang College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China College of Biological Chemical Science and EngineeringJiaxing UniversityJiaxing 314001China Universitéde Strasbourg-CNRS Institut de Chimie(UMR 7177 CNRS)4 rue Blaise Pascal-CS 9003267081 StrasbourgFrance

The coexistence of multi-component active sites like single-atom sites,diatomic sites(DAS)and nanoclusters is shown to result in superior performances in the hydrogen evolution reaction(HER).Metal diatomic sites are more complex than single-atom sites but their unique electronic structures can lead to significant enhancement of the HER *** the synthesis and identification of DAS is usually challenging,we report a simple access to a diatomic catalyst by anchoring Co-Ru DAS on nitrogen-doped carbon supports along with Ru nanoparticles(NPs).Experimental and theoretical results revealed the atomic-level characteristics of Co-Ru sites,their strong electronic coupling and their synergy with Ru NPs within the *** unique electronic structure of the catalyst resulted in an excellent HER activity and stability in alkaline *** work provides a valuable insight into a widely applicable design of diatomic catalysts with multi-component active sites for highly efficient HER electrocatalysis.

关键词： Co-Ru diatomic sites Ru nanoparticles multiple active sites synergistic effect hydrogen evolution reaction

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Tetraolefin stereospecific photodimerization and photopolymerization in coordination polymers

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Science China Chemistry 2022年第10期65卷 1867-1872页

作者： Wei-Jie Gong Zhan-Yong Yang Yu-Xuan Hong Dong Liu Zheng Niu Pierre Braunstein Jian-Ping Lang College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China Jiangsu Key Laboratory for Chemistry of Low-Dimensional Materials School of Chemistry and Chemical EngineeringHuaiyin Normal UniversityHuaian 223300China Universitéde Strasbourg-CNRS Institut de Chimie(UMR 7177 CNRS)4 rue Blaise Pascal-CS 90032Strasbourg 67081France

In the context of the highly desirable design and preparation of smart materials with adjustable properties based on photoreactive compounds,we report two unique photoreactive coordination polymers(CPs),{[Zn(4-Iba)_(2)(4-tkpvb)]·H_()2O}_(n)(1,4-HIba=4-iodobenzoic acid,4-tkpvb=1,2,4,5-tetrakis(4-pyridylvinyl)benzene)and[Cd(1,4-bdc)(4-tkpvb)]_(n)(2,1,4-H_(2)bdc=1,4-benzenedicarboxylic acid).Depending on the metal ions and auxiliary carboxylate ligands used,the 4-tkpvb ligands in 1 and 2 adopt different mutual arrangements,which facilitate the photodimerization and photopolymerization reactions in single crystal to single crystal(SCSC)*** UV light irradiation which results in the dimerization of the 4-tkpvb ligands,the one-dimensional(1D)zigzag chainsof 1 are transformed into a two-dimensional(2D)network of{[Zn(4-Iba)_(2)(bpbtpvcb)_(0.5)]·H_(2)O}_(n)(1a,bpbtpvcb=1,3-bis(4-pyridyl)-2,4-bis(2,4,5-tri(2-(4-pyridyl)vinyl)phenylcyclobutane).Similarly,in the crystals of 2,all 4-tkpvb ligands experience a photopolymerization reaction to form an unprecedented 1D linear organic polymer,poly-1,3-bis(4-pyridyl)-2,5-bis(2-(4-pyridyl)-vinyl)phenyl)cyclobutane(poly-bpbpvpcb).Furthermore,the 2D network of 2 is converted into a three-dimensional(3D)framework of[Cd_(n)(1,4-bdc)_(n)(poly-bpbpvpcb)](2a).This work not only offers a new protocol to selectively synthesize new supramolecular cyclic compounds,but also expands the application of photopolymerization to the synthesis of macromolecules.

关键词： coordination polymers single-crystal to single-crystal transformation photodimerization photopolymerization cycloaddition

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In-situ evolution process understanding from a salan-ligated manganese cluster to supercapacitive application

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Nano Research 2022年第1期15卷 346-351页

作者： Xu Zhang Kai Zhao Xu Peng Mohamedally Kurmoo Ming-Hua Zeng Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials Ministry-of-Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules&College of Chemistry&Chemical EngineeringHubei UniversityWuhan 430062China Key Laboratory for the Chemistry and Molecular Engineering of Medicinal Resources School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541004China Institut de Chimie de Strasbourg CNRS-UMR7177Universite de Strasbourg4 rue Blaise Pascal67070 Strasbourg CedexFrance

The goal of material chemistry is to study the relationship among hierarchical structure,chemical reaction and precision preparation for materials,yet tracking pyrolysis process on multi-dimensional scale is still at primary *** we propose packing mode analysis to understand evolution process in high temperature *** a proof of concept,we first design a salan-ligated Mn3(Mn3(3-MeOsalophen)_(2)(Cl)_(2))cluster and pyrolyze it under an inert atmosphere directly to a mixed valence MnOx embedded in a porous N-doped carbon skeleton(MnOx/C).Meanwhile,combining thermogravimetry-mass spectrometry(TG-MS)with other characterization techniques,its pyrolysis process is precisely tracked real-time and Mn^(2+)/Mn^(3+)ratios in the resulting materials are deduced,ensuring excellent electrochemical *** a result,the as-preferred MnOVC-900 sample reaches 943 F/g at 1 A/g,maintaining good durability under 5,000 cycles with 90%*** highlight of packing mode analysis strategy in this work would provide a favorable approach to explore the potential relationship between structure and performance in the future.

关键词： evolution process understanding thermogravimetry-mass spectrometry salan-ligated manganese cluster packing mode analysis supercapacitive performance

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Arylazopyrazole-functionalized photoswitchable octanuclear Zn(Ⅱ)-silsesquioxane nanocage

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Science China Chemistry 2021年第3期64卷 419-425页

作者： Kai Sheng Ya-Nan Liu Rakesh Kumar Gupta Mohamedally Kurmoo Di Sun School of Aeronautics Shandong Jiaotong UniversityJi'nan 250037China School of Chemistry and Chemical Engineering State Key Laboratory of Crystal MaterialsShandong UniversityJi'nan 250100China Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology School of Chemistry and Chemical Engineering厶iaocheng UniversityLiaocheng 252000China Institut de Chimie de Strasbourg Universite de StrasbourgCNRS-L/MR 71774 rue Blaise PascalStrasbourg Cedex 67008France

Photoswitchable organic materials have shown significant advancement for photonic applications,however,the polynuclear metal clusters conjugated with photoswitching properties are still ***,a novel octanuclear Zn(Ⅱ) nanocage{[Zn_(8)-(Me_(4)Si_(4)O_(8))_(2)(azopz)_(8)]·4CH_(2)Cl_(2)·MeOH·MeCN}(SD/Zn8)(Hazopz=3,5-dimethyl-4-(phenyldiazenyl)-1H-pyrazole),based on multidentate silsesquioxane and pyrazole modified by photoisomerizable azo group has been designed and synthesized to realize the reversible photoswitching behavior.X-ray crystallographic study reveals that the unique metal core consists of two annular Me_(4)Si_(4)O_(8)^(4-)sandwiching a ring of eight Zn atoms where the pyrazole end of azopz-bridges them *** azopz-ligands diverge above and below the plane defined by eight Zn ***,SD/Zn8 shows quick trans-to-cis transformation upon 365 nm light irradiation,which can be easily changed back by 450 nm light,but slow cis-to-trans reversibility at room temperature as confirmed by UV-V is and 1H NMR *** process,which presumably regulates the spaces,acts like a pump and is completely *** such,it can be considered as a molecular pump energized by ***,the molecule is an energy reservoir where it absorbs the light energy and releases it slowly with time.

关键词： silsesquioxane metal-organic nanocage photochromism X-ray single-crystal structure

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Tracking the multiple-step formation of an iron(Ⅲ) complex and its application in photodynamic therapy for breast cancer

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Science China Chemistry 2019年第6期62卷 719-726页

作者： Zhong-Hong Zhu Qian Hu Hui-Ling Pan Yuexing Zhang Haibing Xu Mohamedally Kurmoo Jin Huang Ming-Hua Zeng Key Laboratory for the Chemistry and Molecular Engineering of Medicinal Resources School of Chemistry and Pharmaceutical SciencesGuangxi Normal University Shanghai Key Laboratory of New Drug Design School of Pharmacy East China University of Science and Technology Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials Ministry of Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules College of Chemistry and Chemical Engineering Hubei University Université de Strasbourg Institut de Chimie de Strasbourg CNRS-UMR7177 4 rue Blaise Pascal

A tandem reaction of pyridin-2-ylmethanamine(L1′) with 8-hydroxyquinoline-2-carbaldehyde(HL1) assisted by FeCl_3 was observed to give the new nitrogen heterocycle HL3(HL3=2-(imidazo[1,5-a]pyridin-3-yl)quinolin-8-ol) as its Fe(Ⅲ) complex,[Fe(L3)Cl_2](Fe1). Electrospray ionization mass spectrometry(ESI-MS) reveals its formation involves three steps:(1) coordination of both HL1 and L1′ to Fe,(2) aldehyde-amine coupling, and(3) ring closure. The results of electronic absorption spectroscopy, cyclic voltammetry, and density functional theory(DFT) calculations show the proximity of the optical transition energy to that of the excitation of ~3O_2 to ~1O_2, which prompted us to explore its application as a photosensitizer for photodynamic therapy(PDT). Photo-toxicity studies show that Fe1 exhibits the highest anti-proliferation efficiency in human breast cancer MDA-MB-231 cells under light irradiation. Moreover, studies with orthotopic models of breast cancer further expounded the anti-tumor activity of Fe1 with no significant toxicity to other organs and low retention in the body.

关键词： tandem formation iron(Ⅲ) complex DFT calculation photodynamic therapy breast cancer

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An equivalence result for moment equations when data are missing at random

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Statistical Theory and Related Fields 2019年第2期3卷 199-207页

作者： Marian Hristache Valentin Patilea Univ Rennes EnsaiCNRSCREST–UMR9194F–35000 RennesFrance Center for Research in Economics and Statistics(CREST) Ecole Nationale de la Statistique et de l’Analyse de l’Information(Ensai)Campus de Ker-Lannrue Blaise PascalBP 3720335172 Bruz cedexFrance

We consider general statistical models defined by moment equations when data are missing atrandom. Using the inverse probability weighting, such a model is shown to be equivalent with amodel for the observed variables only, augmented by a moment condition defined by the missing mechanism. Our framework covers a large class of parametric and semiparametric modelswhere we allow for missing responses, missing covariates and any combination of them. Theequivalence result is stated under minimal technical conditions and sheds new light on variousaspects of interest in the missing data literature, as for instance the efficiency bounds and theconstruction of the efficient estimators, the restricted estimators and the imputation.

关键词： Efficiency bounds imputation inverse probability weighting semiparametric regression restricted estimators

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Flexible Vertex Engineers the Controlled Assembly of Distorted Supramolecular Tetrahedral and Octahedral Cages

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Research 2022年第2期2022卷 333-344页

作者： Shu-Jin Bao Ze-Ming Xu Tian-Chen Yu Ying-Lin Song Heng Wang Zheng Niu Xiaopeng Li Brendan F.Abrahams Pierre Braunstein Jian-Ping Lang Collge of Chemistry Chemical Enginering and Materias ScienceSoochow UniversitySuzhou 215123China State Key Laboratory of rgnomallic Chemistry Shanghai Jnstitute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of Plysical Science and Techmology Soochow UinversitySuzhou 215006China College of Chemistry and Enwironmenrial Engineering Shenzhen UniversilyShenzhen 518071China School of Chemistry University of MelbourneVictoria 3010Australia Universite de Strasbourg-CNRS Institut de Chimie(UMR 7177 CNRS)4 Rue Blaise Pascal CS 9003267081 StrasbourgFrance

Designing and building unique cage asemblies atrat increasing interet from supramolecular chemists but remain synthetically ***,we propose the use of a flexible vertex with adjustable angles to selectively form highly distorted tetrahedral and octahedral cages,for the first time,in which the flexible ve rtex forms from the synergistic eft of coordination and covalent *** inherent interligand angle of the vertex can be modulated by guest anions present,which allows for the fine-tuning of diferent cage ***,the reversible structural transformation between tetrahedral and octahedral cages was achieved by anion exchange monitored by mass spectrometric technique,the smaller anions favoring tetrahedral cages,while the larger anions supporting octahedral ***,the KBr-based cage thin films exhibited prominent enhancement of their third-order NLO responses in two or three orders of magnitude compared to those obtained for their corresponding *** work not only provides a new methodology to build irregular polyhedral structures in a controlled and tunable way but also provides access to new kinds of promising functional optical materials.

关键词： vertex tetrahedral synergistic

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Mesorif Gabbros(External Rif, North Morocco): Ophiolitic Suture Witness or a “Newly Discovered” Manifestation of the Central Atlantic Magmatic Province?

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Acta Geologica Sinica(English Edition) 2020年第S01期94卷 11-12页

作者： Faouziya HAISSEN Oriol GIMENO-Vives Geoffroy MOHN Valérie BOSSE Mohamed Najib ZAGHLOUL Achraf ATOUABAT Dominique FRIZON DE LAMOTTE UniversitéHassan II de Casablanca Facultédes Sciences Ben MsikDépartement de GéologieB.P.5366MaarifCasablancaMorocco UniversitéCergy-Pontoise Département Géosciences et Environnement 5GEG1 rue Descartes950000 Neuville/Oise CedexFrance Universitéblaise pascal Laboratoire Magmas et Volcans(UMR 6524)CNRS5 rue Kessler63038Clermont-FerrandFrance UniversitéAbdelmalek Essaadi Facultédes Sciences et Techniques de TangerBP 41990000 TangerMorocco

The Rif Mountain located in Northern Morocco represents the westernmost extremity of the Peri-Mediterranean Alpine orogenic *** belt is classically subdivided into:1)Internal zones(or Internal Rif which is an allochthonous metamorphic domain known worldwide thanks to the presence of large peridotite outcrops);2)flysch zones(sediments corresponding to the original cover of the Maghrebian Tethys);and 3)External zones(or External Rif representing the North African margin remnants).The External Rif is itself subdivided into Prerif,Mesorif and Intrarif domains from the South to the North and is composed by Upper Triassic to Cenozoic sediments structured in a nappe *** rock intrusions were reported in this External Rif since the preliminary geological studies even if they were wrongly mapped as"granites".Later careful fieldwork and mapping studies specified nevertheless their gabbroic nature.A more recent petrological and geochemical study of a few outcrops of those gabbroic intrusions conducted the corresponding authors,encouraged by the presence of ultramafic rocks(Beni Malek serpentines)in the eastern part of the External Rif to consider those gabbros as oceanic and so,associated to"an ophiolitic suture".Nevertheless,a recent and extended survey on the architecture and the rifting history of the Mesozoic margin of the Maghrebian Tethys focusing mainly on the Mesorif domain favor another *** detailed petrography of those mafic intrusions(mainly gabbros+dolerites and rarely extrusive rocks);their geochemical fingerprints and mainly their geochronological data(ages around 200 Ma based on U-Pb zircon LA-ICP dating)all together indicate clearly that those mafic intrusions are rather a"newly discovered"manifestation of the Central Atlantic Magmatic Province activity"CAMP"in the External Rif *** CAMP magmatism has been largely well described and characterized in all the other geological domains of Morocco(Anti-Atlas,High Atlas,Middle Atlas

关键词： external Rif Mesorif gabbro ophiolitic suture CAMP(the Central Atlantic Magmatic Province)

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