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Photoinduced generation of alkyl and phthalimide nitrogen radicals from N-hydroxyphthalimide esters for the synthesis of benzophenone-type bioisosteres

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Science china chemistry 2024年第10期67卷 3389-3396页

作者： Fei Li Jianyang Dong Huijuan Liao Jiayi Dang Xuechen Zhou Yuying Wang Chenya Wang Qin Jiang Gang Li Dong Xue key laboratory of Applied Surface and colloid chemistry Ministry of Education and School of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’an 710119China

N-Hydroxyphthalimide(NHPI)esters have emerged as powerful sources of alkyl radicals generated by single-electron transfer,but homolysis of NHPI ester to produce an alkyl radical and a phthalimide nitrogen radical is still in its *** this study,we developed a light-induced method for generation of alkyl and phthalimide nitrogen radicals from NHPI esters and subsequent reactions of the radicals with[1.1.1]propellane and aryl aldehydes for rapid generation of bicycle[1.1.1]pentane *** method does not require metals or photosensitizers,features a broad substrate scope(90 examples)and excellent functional group tolerance,and can be used for the functionalization of structurally complex natural products and *** investigations indicate that the reaction involves photoinduced homolytic cleavage of the Cs_(2)CO_(3)-NHPI ester complex to produce alkyl and phthalimide nitrogen radicals and subsequent hydrogen atom transfer between the phthalimide nitrogen radical and the aldehyde to generate an acyl radical.

关键词： phthalimide nitrogen radicals aryl aldehydes hydrogen atom transfer bicycle[1.1.1]pentane ketones bioisosteres

Surfactant-metal-organic framework complexes and their derivatives:advances in electrocatalysis

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Science china chemistry 2024年第10期67卷 3209-3222页

作者： Yining Liu Mengying Wang Zuozhong Liang Haoquan Zheng key laboratory of Applied Surface and colloid chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’an 710119China

Metal-organic frameworks(MOFs)and their derivatives received more and more attention due to the diverse morphologies,rich porous structures,and tunable metal active sites,which have been widely used in energy-related electrocatalytic ***,a class of compounds with hydrophilic and hydrophobic portions in the molecular structure,are able to modulate the properties of liquid and solid *** play a crucial role in controlling the shape and size of MOFs,which helps optimize electrocatalytic performance,especially in improving the exposure and accessibility of catalytic active *** this review,we first outline the types and applications of ***,we describe the interface modulation and reaction mechanism of different surfactants during the forming of MOFs and their ***,we discuss the current applications of surfactant-modified MOFs and their derivatives in *** review provides a better understanding of surfactantassistant structure regulation and electrocatalytic activity study of MOFs and their derivatives.

关键词： metal-organic frameworks surfactants interface modulation electrocatalysis

Construction of novel P-Si/TiO_(2)/HfO_(2)/MoS_(2)/Pt heterophotocathode for enhanced photoelectrochemical water splitting

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Nano Research 2024年第5期17卷 4428-4436页

作者： Jiaru Li Jiayu Bai Songjie Hu Wenyu Yuan Yuyu Bu Xiaohui Guo key lab of Synthetic and Natural Functional Molecule chemistry of ministry of education Shaanxi Key Laboratory for Carbon Neutral TechnologyThe College of Chemistry and Materials ScienceNorthwest UniversityXi'an 710069China key lab of Wide Band-Gap Semiconductor Materials and Devices School of MicroelectronicsXidian UniversityXi’an 710071China key lab of Macromolecular Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid ChemistryMinistry of EducationSchool of Chemistry&Chemical EngineeringShaanxi Normal UniversityXi'an 710062China

Photoelectrochemical devices have been developed to enable the conversion of solar ***,their commercial potential is restricted by the limited stability of the materials *** enhance the stability of photocathode and its solar water splitting performance,a P-Si/TiO_(2)/HfO_(2)/MoS_(2)/Pt composite photocathode is developed in this *** novel TiO_(2)/HfO_(2)/MoS_(2) serial nanostructure provides excellent stability of the photocathode,and optimizes the interface energy barrier to further facilitate the transfer process of photogenerated carriers within the *** best P-Si/TiO_(2)/HfO_(2)/MoS_(2)/Pt photocathode demonstrates an initial potential of 0.5 V(***)and a photocurrent density of-29 mA/cm^(2) at 0 V(***).Through intensity modulated photocurrent spectroscopy and photoluminescence test,it is known that the enhanced water splitting performance is attributed to the optimized carrier transfer *** findings provide a feasible strategy for the stability and photon quantum efficiency enhancement of silicon-based photocathode devices.

关键词： photoelectrochemical water splitting stability surface/interface engineering HfO_(2)layer

Cationic Conjugated Oligomers for Efficient and Rapid Antibacterial Photodynamic Therapy via Both Type Ⅰ and Type Ⅱ Pathways

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Chinese Journal of chemistry 2024年第1期42卷 61-66页

作者： Huan Wang Shuwen Guo Qiong Yuan Meiqi Li Yanli Tang Country key laboratory of Analytical chemistry for Life Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid ChemistryMinistry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi'anShaanxi 710119China

Recently,photodynamic therapy(PDT)has attracted wide attention due to its less susceptibility to drug resistance,broad-spectrum biocidal activity and biosafety in normal ***,the traditional photosensitizers(Ps)face the disadvantage of poor therapeutic efficacy due to the requirement of an aerobic environment to generate ^(1)O_(2) through Type Ⅱ ***,we designed and synthesized a novel cationic conjugated oligomer oligo(phenylene vinylene)(OPV)and studied its antibacterial photodynamic activity against both Gram-negative Escherichia coli(***)and Gram-positive bacteria methicillin-resistant Staphylococcus aureus(MRSA).Importantly,the OpV can rapidly produce reactive oxygen species(ROs)through double pathways,Type Ⅰ and Ⅱ mechanism under white light irradiation,and efficiently kill *** and MRSA at a nanomolar *** dual type photosensitizing capability makes OPV promising for enhanced PDT to treat pathogens and tumors in complex environments.

关键词： Conjugated oligomers Antibacterial photodynamic therapy Oligo(phenylene vinylene) Reactive oxygen species Typelandll pathways

Rational cathode configuration with bilayer membranes to engineer current-collector-free high-areal-sulfur lithium-sulfur batteries

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Nano Research 2024年第6期17卷 5224-5232页

作者： Jianmei Han Hua Zhang Peng Wang Ning Song Xuguang An Baojuan Xi Shenglin Xiong College of chemistry and Chemical Engineering Taishan UniversityTai’an 271021China key laboratory of the colloid and Interface chemistry Ministry of Educationand School of Chemistry and Chemical EngineeringShandong UniversityJinan 250100China School of Mechanical Engineering Chengdu UniversityChengdu 610106China

The application of light-weight current collectors is preferred because of the increased energy density of the *** it in mind,the cathode is designed with self-made paperlike memberane as current collector coupled with another interlayer to enable the high-energy-density lithium-sulfur *** a facile and green step-by-step methodology,the hybrid membrane is finalized successfully,consisting of reduced graphene oxide sheets covering paper-derived carbon(GPC)bearing Fe@Fe2O3 and Fe1−xS@Fe2O3 core-shell nanoparticles(FeFeO/FeSFeO@GPC).The film works as the current collector and interlayer simultaneously considering the porous and conductive *** demonstrated by the electrochemical testing,the FeFeO/FeSFeO@GPC hybrid cell exhibits attractive cycling stability and superior rate *** cell configuration and structural/composition merits of FeFeO/FeSFeO@GPC film facilitate the faster reaction kinetics,conducive to the improvement of capacity *** view of the effective cathode design,the areal sulfur loading is increased to 10.46 mg·cm^(−2)and a reversible capacity of 6.67 mAh·cm^(−2)can be retained after 60 cycles at 0.1 C.

关键词： light-weight self-made current collector core-shell high-areal-sulfur lithium-sulfur batteries

Performance optimization of chalcogenide catalytic materials in lithium-sulfur batteries:Structural and electronic engineering

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Chinese Chemical Letters 2024年第7期35卷 147-166页

作者： Jianmei Han Peng Wang Hua Zhang Ning Song Xuguang An Baojuan Xi Shenglin Xiong College of chemistry and Chemical Engineering Taishan UniversityTai'an 271021China key laboratory of colloid and Interface chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShandong UniversityJi'nan 250100China School of Mechanical Engineering Chengdu UniversityChengdu 610106China

Lithium-sulfur batteries(LSBs)boasting remarkable energy density have garnered significant attention within academic and industrial ***,the progression of LSBs remains constrained by the languid redox kinetics intrinsic to sulfur and the pronounced shuttle effect induced by lithium polysulfides(Li PSs),which seriously affecting the energy density,cycling life and rate *** conceptualization and implementation of catalytic materials stand acknowledged as a propitious stratagem for orchestrating kinetic modulation,particularly in excavating the conversion of LiPSs and has evolved into a focal point for *** them,chalcogenide catalytic materials(CCMs)have shown satisfactory catalytic effects ascribe to the unique physicochemical properties,and have been extensively developed in recent *** the lack of systematic summary regarding the development of CCMs and corresponding performance optimization strategies,herein,we initiate a comprehensive review regarding the recent progress of CCMs for effective collaborative immobilization and accelerated transformation kinetics of Li *** that,the modulation strategies to improve the catalytic activity of CCMs are summarized,including structural engineering(morphology engineering,surface/interface engineering,crystal engineering)and electronic engineering(doping and vacancy,etc.).Finally,the application prospect of CCMs in LSBs is clarified,and some enlightenment is provided for the reasonable design of CCMs serving practical LSBs.

关键词： Lithium-sulfur batteries Chalcogenide Catalytic materials Lithium polysulfides Structural engineering Electronic engineering

Organic interfacial engineering of gold nanowires for selective glycerol electrooxidation

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Chinese Chemical Letters 2024年第3期35卷 502-507页

作者： Zhe Wang Qingling Hong Boqiang Miao Tianjiao Wang Yu Ding Pujun Jin Pei Chen Yu Chen key laboratory of Macromolecular Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education)Shaanxi Key Laboratory for Advanced Energy DevicesSchool of Materials Science and EngineeringShaanxi Normal UniversityXi'an 710062China

The selective electrochemical conversion of glycerol into value-added products is a green and sustainable strategy for the biomass *** this work,Au nanowires(Au-NW)modified with polyethyleneimine(PEI)molecule(Au-NW@PEI)is obtained by an up-bottom post-modification *** characterization,molecular dynamics simulation and density functional theory demonstrate that the loose-packed PEI monolayer firmly and uniformly distribute on the Au-NW surface due to the strong Au-N *** experiments and product analysis display that PEI modification significantly enhance the electro-activity of Au-NW for the glycerol electro-oxidation reaction(GEOR)due to the electronic ***,the steric hindrance and electrostatic effect of PEI layer make the optimizing adsorption of intermediates ***,the selectivity of C3 product glyceric acid over Au-NW@PEI is increased by nearly 20%.The work thus indicates that the rational design of metal-organic interface can effectively elevate the electro-activity and selectivity of Au nanostructures,which may have wide application in biomass development.

关键词： Glycerol electrooxidation reaction Organic interface engineering Gold-based nanomaterials Electrocatalysis Selectivity

Highly selective adsorption of rhenium by amyloid-like protein material

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Science china(Technological Sciences) 2024年第5期67卷 1417-1430页

作者： MUHAMMAD Arif YANG QingMin KANWAL Aisha ZHAO Jian NAWAZ Mohsan REN Hao YANG Peng key laboratory of Applied Surface and colloid chemistry Ministry of Education Xi’an key laboratory of Polymeric Soft Matter International Joint Research Center on Functional Fiber and Soft Smart TextileSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’an710119China School of chemistry and Chemical Engineering Northwestern Polytechnical UniversityXi’an710072China

Rhenium separation from molybdenum in molybdenite minerals and waste leachate has become an emerging *** this challenge,we prepared a set of protein-based alkylamine/alkylammonium salts complexes as extractants for selective uptake of rhenium from molybdenum,where the protein component turned into the insoluble amyloid-like structure when its internal disulfide bonds were reduced,namely phase-transition *** them,the phase-transited lysozyme and methyletrioctyleammonium chloride complex(PTL-N263)exhibited the most efficient adsorption at the alkaline condition for the electrostatic interaction between negatively charged metal ions with positively charged center(R_(4)N^(+))in N263,where negatively charged protein residues hindered the ion exchange of Cl^(-)in N263 for larger size Mo species(Mo_(7)O_(24)^(6-))than smaller size Re species(ReO^(4-)).The adsorption follows the Freundlich model and pseudo-second-order kinetics,which exhibits toplevel adsorption performance with a maximum adsorption capacity of 124 mg/g and a separation factor(β_(Re/Mo))of 2.78×10^(3)for *** adsorption capacity per unit area(57.2 mg/(g m^(2)))is 1.6–41 times higher than previously reported adsorbents,and the cost for adsorbing 1 g of Re(VII)is$1.07,indicating its industrial *** adsorption strategy can be applied to separating Re from Mo in binary solutions and industrial wastewater with other competing ions.

关键词： amyloid phase-transited lysozyme selective adsorption rhenium waste leachate solution

Molecular template derived ultrathin N-doped carbon layer on cobalt selenide nanobelts for durable and rapid sodium storage

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Nano Research 2024年第9期17卷 8145-8154页

作者： Chuanliang Wei Baojuan Xi Kangdong Tian Xinlu Zhang Quanyan Man keyan Bao Wutao Mao Jinkui Feng Shenglin Xiong key laboratory of the colloid and Interface chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringSchool of Materials Science and EngineeringShandong UniversityJinan 250100China Resource Environment and Clean Energy laboratory School of Chemical and Environmental EngineeringJiangsu University of TechnologyChangzhou 213001China

Sodium-ion batteries(SIBs)are an attractive battery system because of similar characteristics to lithium-ion batteries(LIBs)and large Na element ***,exploring stable,high-capacity and high-rate anode materials for SIBs is still challenging ***,diethylenetriamine(DETA)molecular template derived ultrathin N-doped carbon(NC)layer decorated CoSe_(2)nanobelts(CoSe_(2)/NC)are prepared by solvothermal reaction followed by calcination *** CoSe_(2)/NC exhibits large potential as an anode for *** and theoretical calculations reveal that the in situ formed conductive ultrathin NC layer can not only relieve the volume change of CoSe_(2)but also accelerate electron and ion *** addition,the nanobelt structure of CoSe_(2)/NC with abundant exposed active sites can obviously accelerate the electrochemical *** the synergistic effect of special nanobelt structure and NC layer,the rate as well as cycling performances of CoSe_(2)/NC are obviously improved.A superior capacity retention of 94.8%is achieved at 2 A·g^(-1)after 2000 *** using Na3V2(PO4)3 cathodes,the pouch full batteries can work steadily at 0.5 C,verifying the application ***_(2)/NC anodes also exhibit impressive performances in LIBs and potassium-ion batteries(PIBs).

关键词： CoSe2 nanobelts ultrathin N-doped carbon layer sodium-ion batteries anode high rate