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Journal of Wuhan University of Technology(Materials Science) 2024年第4期39卷 904-911页

作者：易卓然 DENG Haoyuan QIN Mei 孙一 LUO Guoqiang State Key laboratory of Advanced Technology for Materials synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Graphene prepared by non-covalent modification of sulfonated poly(ether-ether-ketone)(SPG)was combined with polyvinylidene fluoride(PVDF)/Al to improve the PVDF/Al thermal conductivity while reducing the effect of the thermal resistance at the graphene-polymer *** regulation rule of SPG with different contents on the energy release of fluorine-containing system was *** the content of SPG is 4%,the peak pressure and rise rate of SPG/PVDF/Al composite powder during ignition reach the maximum of 4845.28 kPa and 8683.58 kPa/*** the content of SPG is 5%,the PVDF/Al composite powder is completely coated by SPG,and the calorific value of the material reachs the maximum of 29.094 kJ/*** the design and micro-control of the composite powder,the calorific value of the material can be effectively improved,but the improvement of the mass release rate still depends on the graphene content and surface modification state.

关键词： energetic materials PVDF/Al composites graphene modification energy release combustion

Single-cell mass spectrometry studies of drug metabolism heterogeneity and primary resistance to gefitinib in non-small cell lung cancer cells

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Chinese Chemical Letters 2024年第2期35卷 436-440页

作者： Guizhen Zhu Yaoyao Zhao Wenmei Zhang Yuanyuan Wu Yuanxing Liu Guangsheng Guo Xiayan Wang Zhihong Liu Center of Excellence for Environmental Safety and Biological Effects Beijing Key Laboratory for Green Catalysis and SeparationDepartment of ChemistryBeijing University of TechnologyBeijing 100124China Minzu University of China Beijing 100081China Key laboratory for the synthesis and Application of organic Functional Molecules College of Health Science and EngineeringHubei UniversityWuhan 430062China

Patients with epidermal growth factor receptor(EGFR)wild-type non-small cell lung cancer(NSCLC)often show primary resistance to gefitinib *** is thus necessary to study the metabolism of gefitinib in NSCLC cells to comprehensively reveal the reasons for the primary resistance of ***,we develop a platform for studying drug metabolism heterogeneity based on single-cell mass spectrometry(sDMH-scMS)by integrating living-cell electrolaunching ionization MS(ILCEI-MS)and high-performance liquid chromatography-MS(HPLC-MS)analysis,and the primary resistance of NSCLC cells to gefitinib was studied using this *** ILCEI-MS analysis showed that approximately 11.9%of NSCLC single cells contained the gefitinib metabolite M11;HPLC-MS detection diluted the intensity of M11 in subpopulations and concealed the heterogeneity of drug metabolism in tumor single *** intensity of gefitinib in EGFR wild-type A549 cells was markedly lower than in mutant PC9 cells,and the intensity of gefitinib metabolites was significantly higher than in PC9 cells,suggesting that the primary resistance of NSCLC cells is related to gefitinib ***,the combination of gefitinib and the drug-metabolizing enzyme inhibitorα-naphthoflavone was shown to overcome the primary resistance of the NSCLC ***,the results of this study are expected to be applicable for clinical drug resistance diagnosis and treatment at the single-cell level.

关键词： Single-cell mass spectrometry Drug metabolism Non-small cell lung cancer Gefitinib Primary resistance

Selective nickel-electrocatalyzed benzylic C-H oxygenation of functionalized alkyl arenes

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Chinese Chemical Letters 2024年第2期35卷 396-401页

作者： Shunyao Tang Siyi Wang Dongmei Zhang Xinxing Zhang Guang Yang Yanwei Wang Youai Qiu State Key laboratory of Elemento-organic Chemistry Frontiers Science Center for New Organic MatterCollege of ChemistryNankai UniversityTianjin 300071China College of Chemistry Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education)Renewable Energy Conversion and Storage Center (RECAST)Frontiers Science Center for New Organic MatterNankai UniversityTianjin 300071China

Herein, a site-selective paired electrochemical C–H oxidation of functionalized alkyl arenes promoted by nickel catalyst is disclosed. A Ni(Ⅱ)-dioxygen species formed in situ efficiently enable the oxidation process under mild conditions with a broad substrate scope with excellent functional group compatibilities,such as free carboxylic acid, aldehyde, halogen(including aryl iodide), amide and amino acid. The use of the nickel catalyst in combination with water provides a safe, green and economical method for oxidation of a range of molecules varying in complexity and drug derivatives, demonstrating its potential application in organic synthesis and the pharmaceutical industry. Reaction outcomes and mechanistic studies revealed the key role of the in situ Ni(Ⅱ)-dioxygen species for the subsequent oxidation of C(sp^(3))–H bonds,and short-lived reactive intermediates(aryl radical cation) was rapidly captured by the combination of a bipolar ultramicroelectrode(BUME) with nano-electrospray ionization mass spectrometry.

关键词： Electrochemical C-H oxidation Functionalized alkyl arenes Paired nickel-electrocatalysis H_(2)O oxidation Ketones

Mechanism investigation of A-site doping on modulating electronic band structure and photocatalytic performance towards CO_(2) reduction of LaFeO_(3) perovskite

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Nano Research 2024年第5期17卷 3733-3744页

作者： Chi Cao Jinshuo Li Yang Hu Lin Zhang Wensheng Yang State Key laboratory of Inorganic synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China Engineering Research Center for Nanomaterials Henan UniversityKaifeng 475004China

Three kinds of metal atoms with different valence electronic configurations,Bi(6s^(2)6p^(3)),Y(4d^(1)5s^(2)),and Ce(4f^(1)5d^(1)6s^(2)),were selected to investigate the effect of A-site(La^(3+))doping on electronic band structure,photoelectric properties,and photocatalytic performance of LaFeO_(3) *** was identified that the Bi doped LaFeO_(3) presented significantly improved photocatalytic activity towards the reduction of CO_(2),while the Y or Ce doped LaFeO_(3) displayed decreased photocatalytic activity compared to the pristine LaFeO_(3).It was revealed that doping of all the three metal atoms resulted in narrowed band gap and thus extended light absorption of LaFeO_(3) by lowering its conduction band minimum(CBM).The recombination rate and mobility of the charge carriers were represented by the relative effective mass(D)between holes and electrons for pristine and A-site doped LaFeO_(3).The doping of Bi resulted in increased D value,attributed to the Bi 6s electron states at the valence band maximum(VBM),and thus promoted separation and transfer of the charge carriers and improved photocatalytic activity of LaFeO_(3).In contrast,the doping of Ce resulted in significantly decreased D value,induced by the highly localized Ce 4f hole states at the CBM,and thus higher recombination rate of the charge carriers and decreased photocatalytic activity of LaFeO_(3).Furthermore,the Y doped LaFeO_(3) with a slightly decreased D value presented slightly increased recombination rate of the charge carriers and thus decreased photocatalytic *** a work provides new insights into the A-site doping in LaFeO_(3) perovskite,which should be helpful for optimizing the electronic band structure and activity of perovskite-type photocatalysts at atomic level.

关键词： A-site doping electronic band structure charge carrier behavior photocatalytic CO_(2)reduction perovskite-type photocatalytsts

Achieving asymmetric redox chemistry for oxygen evolution reaction through strong metal-support interactions

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Journal of Energy Chemistry 2024年第9期96卷 526-535页

作者： Shihao Wang Meiling Fan Hongfei Pan Jiahui Lyu Jinsong Wu Haolin Tang Haining Zhang State Key laboratory of Advanced Technology for Materials synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina National Energy Key laboratory for New Hydrogen-Ammonia Energy Technologies Foshan Xianhu LaboratoryFoshan 528200GuangdongChina International School of Materials Science and Engineering(School of Materials and Microelectronics) Wuhan University of TechnologyWuhan 430070HubeiChina Nanostructure Research Centre Wuhan University of TechnologyWuhan 430070HubeiChina Hubei Key laboratory of Fuel Cell Wuhan University of TechnologyWuhan 430070HubeiChina

Water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)*** this study,we address this challenge by constructing asymmetric redox chemistry through elaborate surface OO–Ru–OH and bulk Ru–O–Ni/Fe coordination moieties within single-atom Ru-decorated defective NiFe LDH nanosheets(Ru@d-NiFe LDH)in conjunction with strong metal-support interactions(SMSI).Rigorous spectroscopic characterization and theoretical calculations indicate that single-atom Ru can delocalize the O 2p electrons on the surface and optimize d-electron configurations of metal atoms in bulk through ***^(18)O isotope labeling experiment based on operando differential electrochemical mass spectrometry(DEMS),chemical probe experiments,and theoretical calculations confirm the encouraged surface lattice oxygen,stabilized bulk lattice oxygen,and enhanced adsorption of oxygen-containing intermediates for bulk metals in Ru@d-NiFe LDH,leading to asymmetric redox chemistry for *** Ru@d-NiFe LDH electrocatalyst exhibits exceptional performance with an overpotential of 230 mV to achieve 10 mA cm^(−2)and maintains high robustness under industrial current *** approach for achieving asymmetric redox chemistry through SMSI presents a new avenue for developing high-performance electrocatalysts and instills confidence in its industrial applicability.

关键词： Reaction redox chemistry Strong metal-support interactions Layered double hydroxides Electrocatalysts Water electrolysis

New strategies for asymmetric photocatalysis: asymmetric organocatalytic/photoredox relay catalysis for efficient synthesis of polycyclic compounds containing vicinal amino alcohols

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Science China Chemistry 2024年第3期67卷 945-952页

作者： Jia-Lu Zhang Wen-Bo He Xiu-Qin Hu Peng-Fei Xu State Key laboratory of Applied organic Chemistry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China State Key laboratory of Veterinary Etiological Biology College of Veterinary MedicineLanzhou UniversityLanzhou Veterinary Research InstituteChinese Academy of Agricultural SciencesLanzhou 730000China MOE Frontiers Science Center for Rare Isotopes Lanzhou UniversityLanzhou 730000China

An asymmetric catalytic strategy in photocatalysis utilizing a chirality-induced approach through an organocatalytic/photoredox relay catalysis strategy is successfully achieved for the rapid construction of polycyclic compounds containing vicinal amino alcohols in a one-pot protocol. This methodology facilitates the efficient synthesis of diverse substituted polycyclic tetrahydroquinoline and benzofuran-derived vicinal amino alcohols, each containing five consecutive chiral centers, with high yields,excellent diastereoselectivities and enantioselectivities(up to 95% yield, >20:1 dr and 98% ee), under mild reaction conditions driven by sequential bifunctional squaramide organocatalyst-catalyzed [4+2] annulation and photocatalyst-catalyzed ketyl radical addition cyclization reaction process. Furthermore, investigations into the stereoselectivity mechanism and high-resolution mass spectrometry(HRMS) experiments on free radical trapping have provided evidence for elucidating the detailed mechanism of chirality-induced processes and chiral intermediate conversions in this procedure.

关键词： enantioselective photocatalysis asymmetric organocatalytic/photocatalysis relay catalysis five consecutive chiral centers chirality-induced strategy chirality vicinal amino alcohols

A H_(4)SiW_(12)O_(40)-catalyzed three-component tandem reaction for the synthesis of 3,3-disubstituted isoindolinones

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Chinese Chemical Letters 2024年第1期35卷 233-236页

作者： Yufeng Liu Guodong Zeng Yutao Cheng Lei Chen Yunhai Liu Yongge Wei Guoping Yang School of Chemistry Biology and Material ScienceJiangxi Province Key Laboratory of Synthetic ChemistryJiangxi Key Laboratory for Mass Spectrometry and InstrumentationEast China University of TechnologyNanchang 330013China Key Lab of organic Optoelectronics&Molecular Engineering of Ministry of Education Department of ChemistryTsinghua UniversityBeijing 100084China

A H_(4)SiW_(12)O_(40)-catalyzed three-component tandem reaction of 2-acylbenzoic acids,primary amines and phosphine oxides to form 3,3-disubstituted isoindolinones was *** employing A H_(4)SiW_(12)O_(40)as the catalyst and dimethyl carbonate(DMC)as the solvent,a diverse range of 2-acylbenzoic acid derivatives and primary amines worked well to give the C3-phosphinoyl-functionalized 3,3-disubstituted isoindolinones with the yield range of 61%-87%.Advantages of this transformation include green catalyst and solvent,available starting materials,broad substrate scope,high efficiency and operational simplicity with water as the sole *** strategy achieved an efficient and green molecular fragment assembly to access isoindolinones,which would provide opportunities for the synthesis of potential biologically active molecules in a green manner.

关键词： Polyoxometalates Dehydrative coupling Three-component tandem reaction 3,3-Disubstituted isoindolinones organic carbonate

Layer-by-layer fabrication of montmorillonite coating immobilizing Cu_(2)O nanoparticles for continuously catalyzing glycerol to dihydroxyacetone

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Chinese Journal of Chemical Engineering 2024年第4期68卷 263-275页

作者： Kejin Li Jiahui Liu Dajian Li Xiaolan Chen Chunhui Zhou Research Group for Advanced Materials&Sustainable Catalysis(AMSC) State Key Laboratory Breeding Base of Green Chemistry-Synthesis TechnologyCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310032China Qing Yang Institute for Industrial Minerals Qingyang 242804China Engineering Research Center of Non-metallic Minerals of Zhejiang Province Zhejiang Institute of Geology and Mineral ResourcesHangzhou 310007China

Microreactors are increasingly used for green and safe chemical processes owing to their benefits of superior mass and heat transfer,increased yield,safety,and simplicity of ***,immobilizing catalysts in microreactors remains *** this investigation,a technique for creating Cu_(2)O/montmorillonite catalyst coating,using electrostatic attraction for layer-by-layer self-assembly,was *** montmorillonite film's morphology and thickness could be efficiently regulated by adjusting the degree of exfoliation and surface charge of montmorillonite,alongside layer-by-layer coating *** Cu_(2)O nanoparticles were immobilized using the flow deposition *** resulting Cu_(2)O@montmorillonite-film-coated capillary microreactor successfully transformed glycerol into *** conversion of glycerol and product selectivity could be controlled by adjusting the molar ratio of reactants,temperature,residence time,and Cu_(2)O *** maximum glycerol conversion observed was 47.6%,with a 27%selectivity toward *** study presents a technique for immobilizing montmorillonite-based catalyst coatings in capillary tubing,which can serve as a foundation for the future application of microreactors in glycerol conversion.

关键词： Microreactor Coating Montmorillonite Glycerol Cu_(2)O

Hybrid ionic/electronic interphase enabling uniform nucleation and fast diffusion kinetics for stable lithium metal anode

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Chinese Chemical Letters 2024年第2期35卷 626-633页

作者： Lun Li Pengxia Ji Meng Huang Zixin Zhang Hong Wang Francis Verpoort Jinlong Yang Daping He State Key laboratory of Advanced Technology for Materials synthesis and Processing School of Materials Science and EngineeringWuhan University of TechnologyWuhan 430070China Guangdong Research Center for Interfacial Engineering of Functional Materials College of Materials Science and EngineeringShenzhen UniversityShenzhen 518060China Sanya Science and Education Innovation Park of Wuhan University of Technology Sanya 572000China Hubei Engineering Research Center of RF-Microwave Technology and Application Wuhan University of TechnologyWuhan 430070China State Key laboratory of Silicate Materials for Architectures Wuhan University of TechnologyWuhan 430070China

Lithium(Li)dendrite issue,which is usually caused by inhomogeneous Li nucleation and fragile solid electrolyte interphase(SEI),impedes the further development of high-energy Li metal ***,the integrated construction of a high-stable SEI layer that can regulate uniform nucleation and facilitate fast Li-ion diffusion kinetics for Li metal anode still falls ***,we designed an artificial SEI with hybrid ionic/electronic interphase to regulate Li deposition by in-situ constructing metal Co clusters embedded in LiF *** generated Co and LiF both enable fast Li-ion diffusion kinetics,meanwhile,the lithiophilic properties of Co clusters can serve as Li-ion nucleation sites,thereby contributing to uniform Li nucleation and non-dendritic *** a result,a dendrite-free Li deposition with a low overpotential(16.1 mV)is achieved,which enables an extended lifespan over 750 h under strict *** full cells with high-mass-loading LiFePO_(4)(11.5 mg/cm^(2))as cathodes exhibit a remarkable rate capacity of 84.1 mAh/g at 5 C and an improved cycling performance with a capacity retention of 96.4%after undergoing 180 cycles.

关键词： Lithium metal anode Hybrid ionic/electronic interphase Solid electrolyte interphase Fast diffusion kinetics Dendritic growth of lithium

Polysulfide modified PtCu intermetallic nanocatalyst with enrichment realizes efficient electrooxidation ethanol to CO_(2)

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Nano Research 2024年第4期17卷 2320-2327页

作者： Shuanglong Zhou Zheng Lv Liang Zhao Dan Zhang Zuocao Wang Yu Dai Bin Li Olga Starostenko Jianping Lai Lei Wang Key laboratory of Eco-chemical Engineering Ministry of EducationTaishan scholar advantage and characteristic discipline team of Eco-chemical process and technologyLaboratory of Inorganic Synthesis and Applied ChemistryCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China College of Foreign Languages Qingdao City UniversityQingdao 266106China College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042China Institute of Macromolecular Chemistry of the National Academy of Sciences of Ukraine Kyiv 02160Ukraine Shandong Engineering Research Center for Marine Environment Corrosion and Safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042China

The main problem faced by ethanol oxidation reaction(EOR)includes low activity,poor selectivity,and *** the study,we found that polysulfide modified on the surface of PtCu intermetallic(IM)/C can simultaneously enrich hydroxyl and ethanol,which could effectively improve the catalytic activity,CO_(2) selectivity,and durability of *** mass activity and the specific activity of the product in 1 M KOH electrolyte reached 17.83 A·mgPt^(-1) and 24.67 mA·cm^(-2).The CO_(2) selectivity of polysulfide modified product achieved 93.5%,which was 30 folds higher than Pt/*** addition,the catalyst showed high catalytic *** mechanism study demonstrates that the surface modified polysulfide could significantly boost the enrichment effect of ethanol and hydroxyl species,accelerating C–C bond cleavage and CO oxidation.

关键词： Pt CO_(2) selectivity enrichment effect ethanol oxidation reaction(EOR) electrocatalyst