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High donor-number and low content electrolyte additive for stabilizing zinc metal anode

Journal of Energy chemistry 2024年第8期95卷 626-635,I0014页

作者： Yuxin Gong Ruifan Lin Bo Wang Huaizheng Ren Lei Wang Han Zhang Jianxin Wang Deyu Li Yueping Xiong Dianlong Wang Huakun Liu Shixue Dou MIIT key {1. of Critical Materials Technology for New Energy Conversion and Storage State Key Laboratory of Urban Water Resource and EnvironmentSchool of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangChina key {1. of Advanced Energy Materials chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China Institute of Energy Material science University of Shanghai for Science and TechnologyShanghai 200093China

The aqueous zinc ion batteries(AZIBs)are thought as promising competitors for electrochemical energy storage,though their wide application is curbed by the uncontrollable dendrite growth and gas evolution side ***,to stabilize both zinc anodes and water molecules,we developed a modified electrolyte by adding a trace amount of N,N-diethylformanmide(DEF)into the ZnSO_(4)electrolyte for the first time in zinc ion *** effectiveness of DEF is predicted by the comparison of donor number and its preferential adsorption behavior on the zinc anode is further demonstrated by several spectroscopy characterizations,electrochemical methods,and molecular dynamics *** modified electrolyte with 5%*** content can ensure a stable cycling life longer than 3400 h of Zn‖Zn symmetric cells and an ultra-reversible Zn stripping/plating process with a high coulombic efficiency of 99.7%.The Zn‖VO_(2)full cell maintains a capacity retention of 83.5%and a 1.4 mA h g^(-1.mass capacity after *** work provides insights into the role of interfacial adsorption behavior and the donor number of additive molecules in designing low-content and effective aqueous electrolytes.

关键词： Aqueous zinc ion batteries Zinc anode Electrolyte additives Donor number Zinc dendrites

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“Three-in-one” strategy of trifluoromethyl regulated blood-brain barrier permeable fluorescent probe for peroxynitrite and antiepileptic evaluation of edaravone

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Chinese Chemical Letters 2024年第10期35卷 360-363页

作者： Lei Shen Hongmei Liu Ming Jin Jinchao Zhang Caixia Yin Shuxiang Wang Yutao Yang key {1. of Medicinal chemistry and Molecular Diagnosis of the Ministry of Education Chemical Biology Key Laboratory of Hebei ProvinceState Key Laboratory of New Pharmaceutical Preparations and ExcipientsCollege of Chemistry and Materials ScienceHebei UniversityBaoding 071002China key {1. of Chemical Biology and Molecular Engineering of Ministry of Education Institute of Molecular ScienceShanxi UniversityTaiyuan 030006China

Epilepsy,as a chronic neurological disease of the brain,is closely related to oxidative stress,and the peroxynitrite(ONOO-)significantly rise up in this ***,ONOO-is considered as a potential biomarker for early prediction of ***,some potential diagnostic reagents for epilepsy are hindered by the blood-brain barrier(BBB).Meanwhile,“drug repurposing”is attracting a growing ***(EDA),as a first-line drug in the clinical treatment of cerebral ischemia,plays antioxidant roles in scavenging free radicals,promising potential antiepileptic ***,it is imperative to develop fluorescent probes for monitoring ONOO-fluctuations in the epileptic ***,we proposed a novel fluorescent probe with the thiocarbonate as the promising recognition unit for ONOO-and dicyanoisophorone derivative as the ***,by the“three-in-one”strategy,the introduction of trifluoromethyl into DCI-ONOO-3 can extend the emission wavelength of the fluorophore,shorten the response and increase ***,DCI-ONOO-3 was used for monitoring ONOO-fluxes in brain of epileptic mice and evaluating the antiepileptic efficacy of *** opens up a new way for the design of BBB permeable fluorescent probes,and provides a convincing new method for the diagnosis and treatment of epilepsy.

关键词： Fluorescent probe Blood-brain barrier Peroxynitrite Epilepsy Drug repurposing

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Post-treatment of Ti-MWW zeolite with potassium fluoride for propylene epoxidation

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Frontiers of Chemical science and Engineering 2024年第8期18卷 37-47页

作者： Xintong Li Xianchen Gong Jilong Wang Shengbo Jin Hao Xu Peng Wu state {1. laboratory of Petroleum Molecular&Process Engineering Shanghai Key Laboratory of Green Chemistry and Chemical ProcessesSchool of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062China

Epoxidation of propylene to propylene oxide(PO)with hydrogen peroxide(HPPO)is an environmentally friendly and cost-efficient process in which titanosilicates are used as ***-MWW is a potential industrial catalyst for this process,which involves the addition of HPPO to *** silanol groups generated during secondary crystallization unavoidably result in ring-opening of PO and inefficient decomposition of HPPO,which diminish the PO selectivity and the lifespan of *** address this issue,we conducted post-treatment modifications of the structured Bf-Ti-MWW catalyst with potassium fluoride aqueous *** quenching the silanol groups with potassium fluoride and implanting electron-withdrawing fluoride groups into the Ti-MWW framework,both the catalytic activity and HPPO utilization efficiency were ***,the ring opening reaction of PO was *** a continuous fixed-bed liquid-phase propylene epoxidation reaction,the KF-treated structured Ti-MWW catalyst displayed an exceptionally long lifespan of 2700 h,with a PO yield of 590 g·kg^(-1.·h^(-1..

关键词： titanosilicates Ti-MWW propylene epoxidation structured catalyst KF modification

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Catalytically generated noncovalent ammonium dienolate:a versatile platform for the development of organocatalytic asymmetric cascade reactions

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science China {1. 2024年第8期67卷 2524-2546页

作者： Jun-Bing Lin Dong-Sheng Ji Peng-Fei Xu state {1. laboratory of Applied Organic chemistry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China Shaanxi key {1. of Chemical Reaction Engineering College of Chemistry and Chemical EngineeringYan’an UniversityYan’an 716000China

Organocatalytic cascade reactions represent a powerful strategy for the rapid construction of complex chiral molecules with multiple stereocenters from simple substrates under mild conditions. The intriguing structural feature and diverse reactivity of catalytically generated dienolate species render them competent and versatile intermediates for the development of practical and valuable cascade reactions. Over the past years, a plethora of innovative and pioneering noncovalent ammonium dienolatemediated cascade reactions have been designed and implemented under the catalysis of chiral organocatalysts, making dienolate activation a general, robust, and complementary method for the functionalization of unsaturated carbonyl compounds and related substances. This review illustrates the recent advances in organocatalytic noncovalent ammonium dienolate-mediated cascade reactions(mainly from 201. to 2023), including the cascade transformations of ammonium dienolates directly generated from unsaturated ketone/aldehyde, ester/lactone/azlactone, amide/lactam/pyrazolone/oxindole, and alkylidene nitrile compounds. The contents are arranged based on the reaction types of the ammonium dienolates, with an emphasis on cascade 2,5-, 3,5-, and 4,5-difunctionalizations of these intermediates. Furthermore, other cascade reactions involving the 1.3-, 2,3-, and even more complex 3,4,5-reactivities of ammonium dienolates were also discussed. The reaction pathway, reaction stereoinduction, and synthetic applications of the ammonium dienolate-mediated cascade reactions were highlighted throughout the article. As a stimulating and ever-growing research area, the organocatalytic noncovalent ammonium dienolate-mediated cascade reactions are expected to continue demonstrating their magic power for constructing chiral targets in the future and further expanding the boundaries of asymmetric catalysis.

关键词： organocatalysis asymmetric catalysis ammonium dienolate cascade reaction difunctionalization

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Efficient and Fast X-Ray Luminescence in Organic Phosphors Through High-Level Triplet-Singlet Reverse Intersystem Crossing

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CCS chemistry 2024年第2期6卷 334-341页

作者： Yang Zhang Minghong Chen Xiaoze Wang Miao Lin Hongyu Wang Weihong Li Fuhai Chen Qing Liao Hongming Chen Qiushui Chen Meijin Lin Huanghao Yang key {1. of Molecule Synthesis and Function Discovery College of ChemistryFuzhou UniversityFuzhouFujian 350116 New Cornerstone science {1. MOE Key Laboratory for Analytical Science of Food Safety and BiologyCollege of ChemistryFuzhou UniversityFuzhouFujian 350108 College of Materials science and Engineering Fuzhou UniversityFuzhouFujian 350116

Organic scintillators that efficiently generate bright triplet excitons are of critical importance for highperformance X-ray-excited luminescence in radiation ***,the nature of triplet-singlet spinforbidden transitions in these materials often result in long-lived phosphorescence,which is undesirable for ultrafast X-ray detection and *** we demonstrate that the effect of hybridized local and charge-transfer(HLCT)excited states enables organic scintillators to exhibit highly efficient and fast radioluminescence(RL)in response to X-ray *** experimental and theoretical investigation shows that the oxidized 1.8-naphthalimide-phenothiazine dyad(OMNI-PTZ 2)with HLCT-excited states has an enhanced overlap integral of the highest occupied molecular orbital(HOMO)and lowest unoccupied molecular orbital(LUMO)on MNIπ-orbitals,and moderate donor–acceptor electron *** a result,the RL of these crystals exhibits a 61.fold increase and its monoexponential decay lifetime is three orders of magnitude faster compared to its corresponding thermally activated delayed fluorescence(TADF)molecule MNI-PTZ *** further demonstrate the practical utility of the OMNI-PTZ 2(G)in high-performance X-ray detection and imaging,achieving an X-ray dose sensitivity of 97 nGy s−1.and an exceptional spatial resolution of 20 lp/*** study provides a promising molecular design principle for utilizing triplet excitons to develop high-efficiency and fast X-ray scintillators for the development of next-generation flexible and stretchable X-ray imaging detectors.

关键词： organic scintillators X-ray imaging hybridized local and charge transfer excited state triplet-singlet reverse intersystem crossing high exciton utilization

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Revealing the Regulation Effect of Surface Charge at Aromatic Interface to Dynamic Conformational Changes of α-Synuclein at Early Aggregation Stage

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Chinese Journal of chemistry 2024年第16期42卷 1867-1876页

作者： Yuqi Zhang Lie Wu Xiue Jiang state {1. laboratoryof Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun Jilin 130022China Schoolof Applied chemistry and Engineering University of Science and Technology of ChinaHefei Anhui 230026China Research Center for analytical {1. College of ChemistryNankai UniversityTianjin 300071China

The aggregation ofα-synuclein(α-syn)is strongly influenced by membrane interfaces,but the mechanism of transition from monomers to oligomers at early aggregation stage is not ***,we investigate the adsorption and structure changes ofα-syn on oppositely charged aromatic interfaces through in-situ surface-enhanced infrared absorption(SEIRA)spectroscopy and nano-IR *** results show that the synergy of electrostatic and hydrophobic interactions leads to a“fast-slow”two-step aggregation pathway on negatively charged *** adsorption induces the formation of an extended helix structure and subsequently partial helix unwinding in NAC region,which enables the hydrophobic stacking between nearby NAC *** antiparallel β-sheet rich aggregates are gradually emerging as further interactions of monomers with the fast formed“first layer”.Monomers electrostatically adsorb on positively charged interface by C-terminus with NAC region and N-terminus stretched in solvent,which serve as an aggregation core and induce further adsorption and gradual formation of aggregates with C-terminus *** results demonstrate the modulation of surface charge and synergy of electrostatic and hydrophobic interactions on the interaction modes and aggregation pathways,which provide insights into dynamic conformation changes ofα-syn at early aggregation stage and imply the important role of spatial-temporal heterogeneity of membranes inα-synucleinopathies.

关键词： α-Synuclein Interface Early aggregation IR spectroscopy Surface analysis analytical methods Proteins Dynamic monitoring

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Physiological,transcriptome and gene functional analysis provide novel sights into cadmium accumulation and tolerance mechanisms in kenaf

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Journal of Environmental sciences 2024年第3期137卷 500-514页

作者： Shan Cao Meng Wang Jiao Pan Dengjie Luo Samavia Mubeen Caijin Wang Jiao Yue Xia Wu Qijing Wu Hui Zhang Canni Chen Muzammal Rehman Sichen Xie Ru Li Peng Chen Guangxi key {1. of Agro-environment and Agric-products safety Key Laboratory of Plant Genetics and BreedingCollege of AgricultureGuangxi UniversityNanning 530004China state {1. laboratory for Conservation and Utilization of Subtropical Agro-bioresources College of Life Science and TechnologyGuangxi UniversityNanning 530004China

Kenaf is considered to have great potential for remediation of heavy metals in ***,studies on molecular mechanisms of root Cd accumulation and tolerance are still *** this study,two differently tolerant kenaf cultivars were selected as materials and the physiological and transcriptomic effects were evaluated under Cd *** study showed that 200μmol/L CdCl_(2) treatment triggered the reactive oxygen species(ROS)explosion and membrane lipid *** with the Cd-sensitive cultivar‘Z',the Cd-tolerant cultivar‘F'was able to resist oxidative stress in cells by producing higher antioxidant enzyme activities and increasing the contents of ascorbic acid(AsA)and glutathione(GSH).The root cell wall of‘F'exhibited higher polysaccharide contents under Cd treatment,providing more Cd-binding *** were 3,439 differentially expressed genes(DEGs)that were co-regulated by Cd treatment in two *** biosynthesis and plant hormone signal transduction pathways were significantly enriched by functional annotation *** associated with pectin,cellulose,and hemi-cellulose metabolism were involved in Cd chelation of root cell wall;V-ATPases,ABCC3 and Narmp3 could participated in vacuolar compartmentalization of Cd;PDR1.was responsible for Cd effux;the organic acid transporters contributed to the absorption of Cd in *** genes might have played key roles in kenaf Cd tolerance and Cd ***,HcZIP2 was identified to be involved in Cd uptake and transport in *** findings provide a deeper understanding of the molecular pathways underlying Cd accumulation and detoxification mechanisms in kenaf.

关键词： Kenaf Cd stress Physiological Transcriptome HcZIP2

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Heterostructured Pt-Ni_(3)Mo_(3)N formed via ammonia-containing polyoxometalates for highly efficient electrocatalytic hydrogen evolution in acid medium

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Journal of Energy chemistry 2024年第5期92卷 698-704页

作者： Bianqing Ren Xue Gong Jing Cao Dezheng Zhang Zizhun Wang Ping Song Ce Han Weilin Xu state {1. laboratory of Electroanalytical chemistry Jilin Province Key Laboratory of Low Carbon Chemical PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026AnhuiChina key {1. of Automobile Materials MOE School of Materials Science&EngineeringJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsElectron Microscopy Centerand International Center of Future ScienceJilin UniversityChangchun 130012JilinChina

Constructing heterostructured nanohybrid is considered as a prominent route to fabricate alternative electrocatalysts to commercial Pt/C for hydrogen evolution reaction(HER).In this work,(NH_(4))_(4)[NiH_(6)Mo_(6)O_(4)]·5H_(2)O polyoxometalates(NiMo_(6))are adopted as the cluster precursors for simple fabrication of heterostructured Pt-Ni_(3)Mo_(3)N nanohybrids supported by carbon black(Pt-Ni_(3)Mo_(3)N/C)without using additional N *** improved porosity and enhanced electronic interaction of Pt-Ni_(3)Mo_(3)N/C should be attributed to the integration of Pt with NiMo_(6),which favors the mass transport,promotes the formation of exposed catalytic sites,and benefits the regulation of intrinsic ***,the as-obtained Pt-Ni_(3)Mo_(3)N/C exhibits impressive and durable HER performance as indicated by the low overpotential of 1..7 mV at the current density of 1. mA cm^(-2) and the stable overpotential during continuous working at 1.0 mA cm^(-2) for 1.0 *** work provides significant insights for the synthesis of new highly active heterostructured electrocatalysts for renewable energy devices.

关键词： Polyoxometalates Cluster precursors Heterostructured nanohybrids Hydrogen evolution reaction Electrocatalysis

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Supramolecular polymer network constructed by a functionalized polyimidazolium salt derived from metal-carbene template approach

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science China {1. 2024年第4期67卷 1224-1228页

作者： Ming-Ming Gan Zi-En Zhang Yi-Fan Zhang Heng Zhang Li-Ying Sun Ying-Feng Han key {1. of Synthetic and Natural Functional Molecule chemistry of the Ministry of Education Xi’an Key Laboratory of Functional Supramolecular Structure and MaterialsCollege of Chemistry and Materials ScienceNorthwest UniversityXi’an 710127China

In this study,we present a supramolecular templating approach for constructing polyimidazolium salt containing crown ether and cyclobutane *** strategy involves the formation of metal-carbene templates,photochemical cycloaddition,and subsequent demetallation of metal *** by the host-guest chemistry between crown ether units and ammonium salts,we successfully fabricated a supramolecular polymer SPN1.which features imidazolium receptors and cyclobutane *** obtained SPN1.demonstrates outstanding reversible stimulus-response,antibacterial behavior and conductivity.

关键词： metal-carbene template crown ether polyimidazolium salt host-guest chemistry

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Mn incorporated RuO_(2) nanocrystals as an efficient and stable bifunctional electrocatalyst for oxygen evolution reaction and hydrogen evolution reaction in acid and alkaline

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Chinese Chemical Letters 2024年第10期35卷 194-200页

作者： Jing Cao Dezheng Zhang Bianqing Ren Ping Song Weilin Xu state {1. laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of science and Technology of China Hefei 230026China

The development of efficient and stable bifunctional overall water-splitting is a crucial goal for clean and renewable energy,which is a challenging ***,we report an Mn-incorporated RuO_(2)(MnRuO_(2))catalyst for highly efficient electrocatalytic oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)in acid and alkaline *** from a more electrochemical active area with the incorporation of Mn,the Mn-RuO_(2)required an overpotential of 200 mV to attain a current density of 1. mA/cm^(2)for OER in *** result indicates that the doping of Mn into RuO_(2)can enhance the OER *** acidic overall water-splitting electrolyzer with good stability constructed by bifunctional Mn-RuO_(2)only requires a cell voltage of 1.50 V to afford 1. m A/cm^(2)and can operate stably for 50 h at50 mA/cm^(2),which is better than the state-of-the-art Ru-based ***,the Mn-Ru O_(2)exhibits excellent HER and OER activity in alkaline media,and it shows superior activity and durability for overall water-splitting,only needing a cell voltage of 1.49 V to attain 1. m A/cm^(2).The present work provides an efficient approach to designing and constructing efficient Ru-based electrocatalysts for overall water-splitting.

关键词： RuO_(2)-based solid solution electrocatalysts Oxygenevolution reaction Hydrogen evolution reaction Overall watersplitting Acid andalkaline

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