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A novel Tb^(3+) and Eu^(3+) co-doped dual-emitting phosphate K_(3)SrBi(P_(2)O_(7))_(2) phosphor for application in FIR thermometers

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Journal of Rare Earths 2024年第3期42卷 455-463,I0001页

作者： Baochen Wang Shifeng Sun Zeqi Li Zongwang Li Weiwei Lin Chao Zeng Yan-gai Liu Ruiyu Mi School of Chemical and Environmental Engineering Anhui Polytechnic UniversityWuhu241000China State-Province Joint Engineering lab.ratory of Zeolite Membrane Materials Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of EducationInstitute of Advanced MaterialsCollege of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang330022China Beijing Key lab.ratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes National Laboratory of Mineral MaterialsSchool of Materials Science and TechnologyChina University of GeosciencesBeijing100083China

Rare earth co-doped phosphor for fluorescence intensity ratio(FIR) thermometer has gained increasing attention in recent years. Herein, the novel Tb^(3+)and Eu^(3+)co-doped K_(3)SrBi(P_(2)O_(7))_(2)(KSBP) phosphate phosphors were reported. The crystal structure of the title phosphor was determined using Rietveld refinement and proved to have a three-dimensional structure. The time-resolved spectroscopy reveals that there is almost no energy transfer between Tb^(3+)and Eu^(3+). More importantly, Tb^(3+)and Eu^(3+)emissions show different thermal quenching behaviors, which claims the potential of this material for application in optical thermometer. The FIR of the typical KSBP:0.02Tb^(3+),0.04Eu^(3+)sample demonstrates a polynomial relationship as a function of temperature and the absolute and relative sensitivity are0.025 K^(-1) and 0.59%/K, respectively. In general, our study reports a novel and potential KSBP:Tb^(3+),Eu^(3+)phosphate phosphor that is promising for use in high-sensitive FIR thermometers.

关键词： Phosphor Thermometer Fluorescence intensity ratio Thermal stability Rare earths

Ultrasound-responsive spherical nucleic acid against c-Myc/PD-L1 to enhance anti-tumoral macrophages in triple-negative breast cancer progression

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Science China(Life Sciences) 2024年第4期67卷 698-710页

作者： Runtian Wang Gaigai Li Fangyan Gao Feng Xu Xintong Li Jian Zhang Jinbo Li Xiaoxiang Guan Department of Oncology The First Affiliated Hospital of Nanjing Medical UniversityNanjing 210029China State Key lab.ratory of Analytical chemistry for Life Sciences Jiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringChemistry and Biomedicine Innovation Center(ChemBIC)Nanjing UniversityNanjing 210023China Department of Medical Oncology Fudan University Shanghai Cancer CenterDepartment of OncologyShanghai Medical CollegeFudan UniversityShanghai 200032China Jiangsu Key lab.of Cancer Biomarkers Prevention and TreatmentCollaborative Innovation Center for Cancer Personalized MedicineNanjing Medical UniversityNanjing 211166China

Triple-negative breast cancer(TNBC)is the most challenging breast cancer subtype because of its aggressive behavior and limited therapeutic targets.c-Myc is hyperactivated in the majority of TNBC tissues,however,it has been considered an“undruggable”target due to its disordered ***,we developed an ultrasound-responsive spherical nucleic acid(SNA)against c-Myc and PD-L1 in *** is a self-assembled and carrier-free system composed of a hydrophilic small-interfering RNA(si RNA)shell and a hydrophobic core made of a peptide nucleic acid(PNA)-based antisense oligonucleotide(ASO)and a *** accomplished significant enrichment in the tumor by enhanced permeability and retention(EPR)effect,the controllab.e release of effective elements by ultrasound activation,and the combination of targeted therapy,immunotherapy and *** study demonstrated significant anti-tumoral effects in vitro and in *** cytometry showed an invigorated tumor microenvironment(TME)characterized by a significant alteration in the composition of tumor-associated macrophages(TAM)and decreased proportion of PD-1-positive(PD-1+)T effector cells after appropriate treatment of the ultrasound-responsive SNA(USNA).Further experiments verified that tumor-conditioned macrophages residing in the TME were transformed into the anti-tumoral *** finding offers a novel therapeutic strategy against the“undruggable”c-Myc,develops a new targeted therapy for c-Myc/PD-L1 and provides a treatment option for the TNBC.

关键词： triple-negative breast cancer c-Myc spherical nucleic acid self-assembly

Heterointerface engineering of assembled CoP_(2) on N-modified carbon as efficient trifunctional electrocatalysts for Zn-Air batteries and overall water splitting

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Nano Research 2024年第5期17卷 3801-3809页

作者： Yan Chen Zhenrui Yang Juan Wang Yun Yang Xuedong He Yang Wang Jiadong Chen Yaqing Guo Xin Wang Shun Wang Huile Jin Wenzhou Key lab.of Advanced Energy Storage and Conversion Zhejiang Province Key Lab of Leather EngineeringCollege of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China Zhejiang Engineering Research Center for Electrochemical Energy Materials and Devices Institute of New Materials and Industrial TechnologiesWenzhou UniversityWenzhou 325035China School of Chemical and Biomedical Engineering Nanyang Technological UniversitySingapore 637459Singapore

Enhancing catalytic activity through modulating the interaction between N-doped carbon and metal phosphides clusters is an effective ***,the electronic structure modulation of CoP_(2) supported N-modified carbon(CoP_(2)/NC)has been designed and prepared as efficient electrocatalysts for oxygen reduction reaction(ORR),oxygen evolution reaction(OER),and hydrogen evolution reaction(HER).Notably,CoP_(2)/NC-1 catalyst exhibits impressive performance in alkaline media,with an ORR half-wave potential of 0.84 V,as well as OER and HER overpotentials of 290 and 129 mV(at 10 mA·cm^(−2)),*** addition,CoP_(2)/NC-1 produces a power density as high as 172.9 mW·cm^(−2),and excellent reversibility of 100 h at 20 mA·cm^(−2) in home-made Zn-air *** experimental results demonstrate that the synergistic interactions between N modified carbon substrate and CoP_(2) material significantly enhance the kinetics of ORR,OER,and *** functional theory(DFT)calculations reveal the strong electrons redistribution of CoP_(2) induced by high-density N atoms at the interface,thus optimizing the key intermediates and significantly lower the energy barrier of *** electronic adjustments of CoP_(2) greatly enhance its kinetics of ORR/OER/HER,leading to faster *** study provides profound insights into the specific modification of CoP_(2) by N-doped carbon,enabling the construction of efficient catalysts.

关键词： two-dimensional(2D)carbon metal-organic framework cobalt phosphide zinc air battery water splitting

The initial stages of Li_(2)O_(2) formation during oxygen reduction reaction in Li-O_(2) batteries:The significance of Li_(2)O_(2) in charge-transfer reactions within devices

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Journal of Energy chemistry 2024年第1期88卷 223-231,I0006页

作者： Daniela M.Josepetti Bianca P.Sousa Simone A.J.Rodrigues Renato G.Freitas Gustavo Doubek Advanced Energy Storage Division LABCenter for Innovation on New EnergiesSchool of Chemical EngineeringUniversity of CampinasAv Albert Einstein 50013083-852CampinasSPBrazil Institute of Physics&Department of chemistry Laboratory of Computational MaterialsFederal University of Mato Grosso78060-900CuiabáMTBrazil

Lithium-oxygen batteries are a promising technology because they can greatly surpass the energy density of lithium-ion ***,this theoretical characteristic has not yet been converted into a real device with high *** with air contamination,metallic lithium reactivity,and complex discharge and charge reactions are the main issues for this technology.A fast and reversible oxygen reduction reaction(ORR)is crucial for good performance of secondary batteries',but the partial knowledge of its mechanisms,especially when devices are concerned,hinders further *** this perspective,the present work uses operando Raman experiments and electrochemical impedance spectroscopy(EIS)to assess the first stages of the discharge processes in porous carbon electrodes,following their changes cycle by cycle at initial operation.A growth kinetic formation of the discharge product signal(Li_(2)O_(2))was observed with operando Raman,indicating a first-order reaction and enabling an analysis by a microkinetic *** solution mechanism in the evaluated system was ascribed for an equivalent circuit with three time *** the time constant for the anode interface reveals to remain relatively constant after the first discharge,its surface seemed to be more *** model indicated that the reaction occurs at the Li_(2)O_(2) surface,decreasing the associated resistance during the initial discharge ***,the growth of Li_(2)O_(2) forms a hetero-phase between Li_(2)O_(2)/electrolyte,while creating a more compact and homogeneous on the Li_(2)O_(2)/cathode *** methodology here described thus offers a way of directly probing changes in surface chemistry evolution during cycling from a device through EIS analysis.

关键词： Li-O_(2)battery Operando Raman analysis Equivalent circuit modeling Time-constant distribution

The configuration of Au^(δ+)-ZrO_(2)^(δ−)species induced activation enhances electrocatalytic CO_(2)to formate conversion

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Nano Research 2024年第7期17卷 6006-6015页

作者： Yongjian Jia Yadi Zhang Mengque Lin Yangyang Cheng Yanjie Xu National Engineering Research Center for Technology and Equipment of Environmental Deposition Lanzhou Jiaotong UniversityLanzhou 730070China Key lab.of Opt-Electronic Technology and Intelligent Control of Ministry of Education Lanzhou Jiaotong UniversityLanzhou 730070China School of Environmental Engineering and chemistry Luoyang Institute of Science and TechnologyLuoyang 471023China

Electrochemical CO_(2)conversion into value-added chemicals is a promising technology to solve the greenhouse effect and recycle chemical ***,the electrochemical CO_(2)reduction reaction(e-CO_(2)RR)is seriously compromised by weak CO_(2)adsorption and a rough CO_(2)activation process based on the chemical inertness of the CO_(2)molecule and the formed fragile metal–C/O *** this paper,we designed and fabricated Au particles embedded in ZrO_(2).The configuration of Au particles being of positive charge and ZrO_(2)with negative charge is induced and generated by metal–support interactions(MSIs).As a result,Au/ZrO_(2)@C presents a big difference in the CO_(2)conversion compared with the known work,affording a formate yield of 112.5μmol·cm^(−2)·h^(−1)at−1.1 V *** hydrogen electrode(RHE),and a max formate Faradaic efficiency of up to 94.1%at−0.9 V *** superior performance was attributed to the activated Au–ZrO_(2)interface to form the Au^(δ+)*** insitu Fourier transform infrared(FTIR)spectroscopy and theoretical calculations show that the MSIs configuration can be inclined to the*OCO intermediate generation on Au^(δ+)species activating CO_(2)molecules and then accelerate the formation of the*OCHO intermediate in e-CO_(2)RR,thereby favoring the CO_(2)conversion to formate.

关键词： electrochemical CO_(2)reduction reaction(e-CO_(2)RR) Au_(δ+)species formic acid *OCHO intermediate metal-support interactions

Synthesis,chemical bonding and reactivity of new medium-sized polyarsenides

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Chinese Chemical Letters 2024年第7期35卷 497-501页

作者： Xu-Hui Yue Xiang-Wen Zhang Hui-Min He Lei Qiao Zhong-Ming Sun State Key lab.ratory of Element-Organic chemistry Tianjin Key Lab for Institution Rare Earth Materials and ApplicationsSchool of Materials Science and EngineeringNankai UniversityTianjin 300350China Department of Physics Institute of Computational and Applied PhysicsTaiyuan Normal UniversityJinzhong 030619China

Gaining an understanding of the growth mechanism from single atoms to clusters and bulk materials continues to present a ***,it is important to explore the evolving trends of clusters in the structure and properties during the size *** this work,we report the synthesis and characterization of two medium-sized chain-like polyarsenic anions.[As_(21)]^(3-)represents a trimeric example of polyarsenic anion assembled through oxidative coupling of As_(7)^(3-)*** anion As_(18)^(4-)included in[As_(18)MO_(2)(CO)_(8)]^(4-)is regarded as formed by two realgar-type As_(8)subunits connected by a dinuclear AsAs *** As_(18)cluster was previously predicted by theory,and this is the first time successfully synthesized using wet chemistry ***,small-sized polyarsenides As_(2)^(2-)and As_(10)^(2-)were found in compound[K(18-crown-6)]_(3)[As_(10)]_(0.5)[As_(4){Mo(CO)_(3)}_(2)]_(0.5)·*** these,the former exhibits coordination with metal ***-crystal X-ray diffraction combined with quantum chemical calculations revealed the formation of double bonded As_(2)^(2-)stabilized by metal carbonyl *** work demonstrates a novel synthetic approach for the preparation of new polyarsenides and highlights their intriguing bonding characteristics,laying the foundation for the synthesis of such compounds and paving the way for their potential applications.

关键词： Polyarsenide Zintl anions Chain-like cluster DFT calculations AdNDP

Molecular compositions and sources of organic aerosols at a rural site on the Guanzhong Plain,Northwest China:The importance of biomass burning

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Particuology 2024年第6期89卷 44-56页

作者： Yali Liu Minxia Shen Haijiao Liu Wenting Dai Weining Qi Yifan Zhang Lu Li Yue Cao Xin Wang Xiao Guo Yingkun Jiang Jianjun Li State Key lab.ratory of Loess and Quaternary Geology Key Lab of Aerosol Chemistry and PhysicsInstitute of Earth EnvironmentChinese Academy of SciencesXi'an 710061China Xi'an Institute for Innovative Earth Environment Research Xi'an 710061China National Observation and Research Station of Regional Ecological Environment Change and Comprehensive Management in the Guanzhong Plain ShaanxiChina

The concentration of PM_(2.5)has considerably reduced in recent years,but remains relatively high in *** particular,the increasing contribution of organic compounds to PM_(2.5)generates popular pressure for further reductions,resulting in an urgent need to study organic aerosol(OA).To investigate the molecular composition and source contribution of OA in the rural area of the Guanzhong Plain,Northwest China,PM_(2.5)samples were collected during 3–23 August 2016 and 5–20 January 2017 and studied for more than 100 organic tracer *** mean concentration of total measured organic compounds is 662±296 ng/m^(3)in summer and 3258±1925 ng/m^(3)in *** is the most abundant single compound found throughout the sampling period,which is a crucial tracer for biomass burning emissions,preliminary suggesting that biomass burning is an essential source of *** summer,organic compounds such as lipid compounds,sugar compounds,and polycyclic aromatic hydrocarbons(PAHs),more come from higher plants,wood burning,vehicle exhausts,plastic waste,and other direct emission *** PAHs(OPAHs),nitrophenols,and phthalic acids more come from the atmosphere through the oxidation reaction of aromatic precursors,especially photochemical ***,in winter,most of the increases in concentrations of organic compounds are attributed to biomass *** analysis of a haze event(14–19 January 2017)during the winter sampling period shows that the increases in the concentration of organic compounds are unaccompanied by strong secondary formation under lower relative humidity(49.1%±13.5%).The main reason for the growth of OA in this haze event is the accumulation of primary OA(POA).The source apportionment by the positive matrix factorization(PMF)model shows that biomass burning(37.1%)is the primary source of OA in the rural regions of the Guanzhong Plain,especially in winter(40.6%).The contribution of secondary formation decreases from 26.0%in summer t

关键词： Organic aerosol Molecular composition Seasonal variation Source apportionment Guanzhong Plain

Suppression of Co(Ⅱ)ion deposition and hazards:Regulation of SEI film composition and structure

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Journal of Energy chemistry 2024年第2期89卷 259-265,I0007页

作者： Jiaqi Zhan Mingzhu Liu Yutian Xie Jiarong He Hebing Zhou Lidan Xing Weishan Li National and Local Joint Engineering Research Center of MPTES in High Energy and Safety LIBs Engineering Research Center of MTEES(Ministry of Education)Research Center of BMET(Guangdong Province)Key Lab.of ETESPG(GHEI)Innovative Platform for ITBMD(Guangzhou Municipality)School of ChemistrySouth China Normal UniversityGuangzhou 510006GuangdongChina

Despite the presence of Li F components in the solid electrolyte interphase(SEI)formed on the graphite anode surface by conventional electrolyte,these Li F components primarily exist in an amorphous state,rendering them incapable of effectively inhibiting the exchange reaction between lithium ions and transition metal ions in the ***,nearly all lithium ions within the SEI film are replaced by transition metal ions,resulting in an increase in interphacial impedance and a decrease in ***,we demonstrate that the SEI film,constructed by fluoroethylene carbonate(FEC)additive rich in crystalline Li F,effectively inhibits the undesired Li^(+)/Co^(2+)ion exchange reaction,thereby suppressing the deposition of cobalt compounds and metallic ***,the deposited cobalt compounds exhibit enhanced structural stability and reduced catalytic activity with minimal impact on the interphacial stability of the graphite *** findings reveal the crucial influence of SEI film composition and structure on the deposition and hazards associated with transition metal ions,providing valuable guidance for designing next-generation electrolytes.

关键词： Lithium-ion batteries Transition metal ions SEI film Composition and structure

Palladium-catalyzed multi components oxy-aminofluorination and aminofluorination of gem-difluoroalkenes

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Chinese Chemical Letters 2024年第2期35卷 420-425页

作者： Fen Wu Xin Li Junbiao Chang Dachang Bai State Key lab.ratory of Antiviral Drugs NMPA Key Laboratory for Research and Evaluation of Innovative DrugKey Laboratory of Green Chemical Media and ReactionsMinistry of EducationSchool of Chemistry and Chemical EngineeringPingyuan LaboratoryHenan Normal UniversityXinxiang 453007China State Key lab.ratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

organofluorine compounds are widely used in the realm of drug discovery and material ***,we developed palladium catalyzed intermolecular aminofluorination and oxy-aminofluorination of gem‑difluoroalkenes with N-fluorobenzenesulfonimide(NFSI),in which NFSI was used as the nitrogen source and *** reaction provides an efficient and straightforward synthesis route of a series ofα-trifluoromethyl benzylic ***,three/four components oxy-aminofluorination processes were realized to giveα-trifluoromethyl benzylic ether with a terminal amino group,which proceed through C(sp^(3))-O bond cleavage of easily availab.e ether and simultaneous introduced a fluorine,an amino and an oxy substituent in one pot with excellent *** divergent reactivity not only included the incorporation of one ether molecular,but also much more challenged two ether insertion with excellent selectivity through succession C(sp^(3))-O bonds *** protocol allows for concise synthesis of high value amines with fluoroalkyl-substituents and selectively transformation of easily availab.e ethers by high-valent palladium catalysis.

关键词： Palladium Multi components Aminofluorination Oxy-aminofluorination C(sp^(3))-O bond cleavage