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Access to Versatile Functionalized Cu(Ⅲ) Complexes Enabled by Direct Transmetalation to Well-Defined Copper(Ⅲ) Fluoride Complex Me_(4)N^(+)[Cu(CF_(3))_(3)F]^(-)

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Chinese Journal of chemistry 2024年第10期42卷 1107-1113页

作者： Guangyu Wang Huaiyuan Li Xuebing Leng Long Lu Qilong Shen Key Laboratory of Fluorine and Nitrogen chemistry and Advanced Materials Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of Sciences345 Lingling LuShanghai 200032China

The invention of a well-defined Cu(Ⅲ)fluoride complex Me_(4)N^(+)[Cu(CF_(3))_(3)(F)]^(-)1 enabled to access a versatile of functionalized Cu(Ⅲ)complexes[Me_(4)N]^(+)[Cu(X)(CF_(3))_(3)]^(-)(X=C_(6)F_(5),C_(6)F_(5)C≡C,CN,Cl,N_(3),^(t)BuOO,SCN,OAc,SAr),many of them for the first *** availability of these complexes allowed us to evaluate the trans-influence order of ligand in Cu(Ⅲ)complexes:Bn>CF_(3)^(-)>C_(6)F_(5)^(-)>N_(3)^(-)>py~CH_(3)^(-)~C_(6)F_(5)C≡C>NO_(2)PhO^(-)~^(t)BuOO^(-)~CH_(3)COO^(-)>F^(-).

关键词： Fluorine Copper Cu(Ⅲ) Cu(Ⅲ)fluoride Trifluoromethyl

Suppressing the lattice oxygen diffusion via high-entropy oxide construction towards stabilized acidic water oxidation

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Nano Research 2024年第3期17卷 1107-1113页

作者： Jing Ni Zhaoping Shi Yibo Wang Jiahao Yang Hongxiang Wu Pengbo Wang Kai Li Meiling Xiao Changpeng Liu Wei Xing State Key Laboratory of Electroanalytic chemistry Jilin Province Key Laboratory of Low Carbon Chemistry PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The scale-up deployment of ruthenium(Ru)-based oxygen evolution reaction(OER)electrocatalysts in proton exchange membrane water electrolysis(PEMWE)is greatly restricted by the poor *** the lattice-oxygen-mediated mechanism(LOM)has been identified as the major contributor to the fast performance degradation,impeding lattice oxygen diffusion to inhibit lattice oxygen participation is imperative,yet remains challenging due to the lack of efficient ***,we strategically regulate the bonding nature of Ru–O towards suppressed LOM via Ru-based high-entropy oxide(HEO)*** lattice disorder in HEOs is believed to increase migration energy barrier of lattice *** a result,the screened Ti_(23)Nb_(9)Hf_(13)W_(12)Ru_(43)O_(x) exhibits 11.7 times slower lattice oxygen diffusion rate,84%reduction in LOM ratio,and 29 times lifespan extension compared with the state-of-the-art RuO_(2) *** work opens up a feasible avenue to constructing stabilized Ru-based OER catalysts towards scalable application.

关键词： ruthenium-based high-entropy oxide suppressing the lattice oxygen diffusion acidic oxygen evolution reaction

Solid-state atomic hydrogen as a broad-spectrum RONS scavenger for accelerated diabetic wound healing

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National Science Review 2024年第2期11卷 196-206页

作者： Man Luo Qin Wang Gang Zhao Wei Jiang Cici Zeng Qingao Zhang Ruyu Yang Wang Dong Yunxi Zhao Guozhen Zhang Jun Jiang Yucai Wang Qing Zhu Key Laboratory of Precision and Intelligent chemistry School of Chemistry and Materials Science University of Science and Technology of China department of Radiology The First Affiliated Hospital of University of Science and Technology of China Division of Life Sciences and Medicine University of Science and Technology of China Shenzhen Senior High School Institute of Intelligent Innovation Henan Academy of Sciences

Hydrogen therapy shows great promise as a versatile treatment method for diseases associated with the overexpression of reactive oxygen and nitrogen species（RONS）. However, developing an advanced hydrogen therapy platform that integrates controllable hydrogen release, efficient RONS elimination, and biodegradability remains a giant technical challenge. In this study, we demonstrate for the first time that the tungsten bronze phase H0.53WO3（HWO） is an exceptionally ideal hydrogen carrier, with salient features including temperature-dependent highly-reductive atomic hydrogen release and broad-spectrum RONS scavenging capability distinct from that of molecular hydrogen. Moreover, its unique p H-responsive biodegradability ensures post-therapeutic clearance at pathological sites. Treatment with HWO of diabetic wounds in an animal model indicates that the solid-state atomic H promotes vascular formation by activating M2-type macrophage polarization and anti-inflammatory cytokine production, resulting in acceleration of chronic wound healing. Our findings significantly expand the basic categories of hydrogen therapeutic materials and pave the way for investigating more physical forms of hydrogen species as efficient RONS scavengers for clinical disease treatment.

关键词： atomic hydrogen RONS scavenger inflammatory regulation diabetic wound healing hydrogen therapy

Axial enantiomers with donor-regulated TADF feature for multicolor circularly polarized electroluminescence

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Science China chemistry 2024年第6期67卷 2039-2045页

作者： Chen-Hao Guo Wen-Long Zhao Ke-Ke Tan Wei-Chen Guo Liheng Feng Chuan-Feng Chen Meng Li School of chemistry and Chemical Engineering Shanxi UniversityTaiyuan030006China Beijing National Laboratory for Molecular sciences CAS Key Laboratory of Molecular Recognition and FunctionInstitute of ChemistryChinese Academy of SciencesBeijing100190China University of Chinese Academy of sciences Beijing100049China

This study optimized the TADF feature of axial chiral enantiomers through precise donor engineering,and multicolor CP-TADFwas achieved in the axial chiral *** pairs of axial enantiomers with donor-regulated TADF feature,namely(R/S)-TPCBD,(R/S)-DPCBD,and(R/S)-DPACBD,were synthesized by introducing carbazole donors with different substituents onto biphenyl cyanide *** the electron-donating ability of donors increases,the emission of these axial enantiomers ranges from 455,476 to 552 nm,their singlet-triplet energy gaps(ΔE_(ST))gradually decrease from 0.30,0.22 to 0.02 e V,accompanied by an increasement in the transition rate(k_(RISC))of RISC process,and the k_(RISC)of DPACBD could reach up to 7.16×10^(5)s^(-1).These axial enantiomers also exhibit mirror-image CD and circularly polarized luminescence(CPL)***,OLEDs based on TPCBD,DPCBD,and DPACBD as emitter were then fabricated,which displayed blue,green,and orange electroluminescence with EQE_(max)of 13.0%,16.4%,and 25.0%,*** results also exhibited a phenomenon of device efficiency increasing with the enhancement of donor ***,the CP-OLEDs using(R/S)-TPCBD,(R/S)-DPCBD and(R/S)-DPACBD as emitters displayed intense CPEL signals with g_(EL)values of 3.4×10^(-3)/-4.1×10^(-3),3.2×10^(-3)/-3.1×10^(-3)and2.3×10^(-3)/-2.1×10^(-3),*** convenient molecular engineering of donor regulation in the same molecular skeleton,CP-TADF materials with multicolor CPEL and improved device performance could be conveniently achieved.

关键词： axial chirality thermally activated delayed fluorescence circularly polarized luminescence electroluminescence organic light-emitting diodes

A Label-Free Deoxyribozyme Sensor for m^(6)A Demethylase Activity Detection

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Chinese Journal of chemistry 2024年第9期42卷 951-956页

作者： Xiuyuan Wang Shusheng Yu Yuqiu He Fuan Wang Xiaoqing Liu College of chemistry and Molecular sciences Wuhan UniversityWuhanHubei 430072China

A label-free deoxyribozyme(DNAzyme)biosensor for m^(6) demethylase activity detection is *** demethylase FTO(Fat mass and obesity-associated protein),an important m^(6) demethylase of ALKBH demethylase family is present,the m^(6) group is specifically demethylated,and the cleavage activity of DNAzyme is *** allows the cleavage product that contains G-quadruplex sequence to bind to thioflavin T(ThT)and generate fluorescence *** biosensor shows high specificity and sensitivity,and fast reaction *** study demonstrates a new design of allosteric DNAzyme for *** method represents the first label-free nucleic acid biosensor for FTO assay,providing a feasible route towards inhibitors screening.

关键词： DNAzyme Analytical methods Biosensing m^(6)A demethylation Fluorescence

Recovery and in-situ reduction of precious metals by graphdiyne and graphdiyne oxide for antibacterial use

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Rare Metals 2024年第4期43卷 1747-1757页

作者： Ming-Ji Jiang Ya-Na Zhang Ling-Shen Meng Jing Kang Yong-Jun Li Alideertu Dong College of chemistry and Chemical Engineering Inner Mongolia UniversityHohhot010021China Engineering Research Center of Dairy Quality and Safety Control Technology Ministry of EducationInner Mongolia UniversityHohhot010021China department of chemistry University of ZurichCH-8057ZurichSwitzerland Laboratory of Organic Solids and Beijing National Laboratory for Molecular sciences Institute of ChemistryChinese Academy of SciencesBeijing100190China

Based on the in-situ self-reduction and chemical stability,graphdiyne(GDY)and graphdiyne oxide(GDYO)are used as trapping agents to investigate the ability for recovering Au^(3+),Ag^+,and Pd^(2+)under different pH values and interfering *** strong acidity at pH=1,these two agents demonstrate high select recovery towards the three precious metal ions,which could be insitu reduced to nanoparticles(NPs).In addition,superparamagnetic Fe_(3)O_(4)NPs are deposited on the surfaces of GDY and *** magnetic responses enable GDYFe_(3)O_(4)to recover precious metals conveniently and efficiently by the aid of an external magnetic *** study also confirms the antibacterial activity of the as-recovered NPs deposited on GDY and GDYO against Escherichia coli and Staphylococcus aureus(1×10^(5)colony-forming unit(CFU)·mL^(-1)),and the antibacterial rates are 100%.This strategy of recovering precious metals and subsequently reusing to combat pathogens will be of great significance for environmental remediation and biomedical applications.

关键词： Graphdiyne In-situ reduction Recovery Precious metals Antibacterial

Conformational dynamics as an intrinsic determinant of prion protein misfolding and neurotoxicity

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Neural Regeneration Research 2024年第10期19卷 2095-2096页

作者： Alessandro Cembran Pedro Fernandez-Funez department of chemistry and Biochemistry University of Minnesota DuluthDuluthMNUSA department of Biomedical sciences University of Minnesota Medical SchoolDuluth CampusDuluthMNUSA

The prion protein(PrP) is the key molecular and pathological mediator of prion diseases,a heterogeneous group of brain disorders with fatal *** diseases are rare but deserve special attention because of their unique f... 详细信息

关键词： folding intrinsic dynamics

Nickel-based cerium zirconate inorganic complex structures for CO_(2)valorisation via dry reforming of methane

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Journal of Environmental sciences 2024年第6期140卷 12-23页

作者： Juan Luis Martín-Espejo Loukia-Pantzechroula Merkouri Jesús Gándara-Loe José Antonio Odriozola Tomas Ramirez Reina Laura Pastor-Pérez department of Inorganic chemistry and Material sciences Institute of Seville University of Seville-CSICSeville 41092Spain department of Chemical and Process Engineering University of SurreyGuildford GU27XHUnited Kingdom

The increasing anthropogenic emissions of greenhouse gases(GHG)is encouraging extensive research in CO_(2)*** reforming of methane(DRM)depicts a viable strategy to convert both CO_(2)and CH4into syngas,a worthwhile chemical *** the different active phases for DRM,the use of nickel as catalyst is economically favourable,but typically deactivates due to sintering and carbon *** stabilisation of Ni at different loadings in cerium zirconate inorganic complex structures is investigated in this work as strategy to develop robust Ni-based DRM *** and TPR-H2analyses confirmed the existence of different phases according to the Ni loading in these ***,superficial Ni is observed as well as the existence of a CeNiO_(3)perovskite *** catalytic activity was tested,proving that 10 wt.%Ni loading is the optimum which maximises *** catalyst was also tested in long-term stability experiments at 600and 800℃in order to study the potential deactivation issues at two different *** 600℃,carbon formation is the main cause of catalytic deactivation,whereas a robust stability is shown at 800℃,observing no sintering of the active phase evidencing the success of this strategy rendering a new family of economically appealing CO_(2)and biogas mixtures upgrading catalysts.

关键词： CO_(2)conversion Dry reforming of methane Nickel catalysts Pyrochlore Cerium zirconate

Metastable face-centered cubic ruthenium-based binary alloy for efficient alkaline hydrogen oxidation electrocatalysis

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Journal of Energy chemistry 2024年第5期92卷 207-215页

作者： Yunbo Li Jianchao Yue Chaoyi Yang Hongnan Jia Hengjiang Cong Wei Luo College of chemistry and Molecular sciences Wuhan UniversityWuhan 430072HubeiChina

Metastable nanostructured electrocatalyst with a completely different surface environment compared to conventional phase-based electrocatalyst often shows distinctive catalytic *** Ru-based electrocatalysts have been widely investigated toward hydrogen oxidation reaction(HOR)under alkaline electrolytes,these studies are mostly limited to conventional hexagonal-close-packed(hcp)phase,mainly arising from the lack of sufficient synthesis *** this study,we report the precise synthesis of metastable binary RuW alloy with face-centered-cubic(fcc)*** find that the introduction of W can serve as fcc phase seeds and reduce the formation energy of metastable fcc-RuW ***,fcc-RuW exhibits remarkable alkaline HOR performance and stability with the activity of 0.67 mA cm_(Ru)^(-2)which is almost five and three times higher than that of hcp-Ru and commercial Pt/C,respectively,which is attributed to the optimized binding strength of adsorbed hydroxide intermediate derived from tailored electronic structure through W doping and phase ***,this strategy can also be applied to synthesize other metastable fcc-RuCr and fcc-RuMo alloys with enhanced HOR performances.

关键词： Hydrogen oxidation reaction Metastable phase Face-centered cubic(fcc) Ru Phase engineering