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Catalysis by subsurface metal atoms in Al(001) through electron transfer

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National Science Review 2024年第4期11卷 12-13页

作者： Bo Sun Ding Ma Beijing National Laboratory for molecular Science New Cornerstone Science Laboratory College of Chemistry and Molecular Engineering Peking University

Heterogeneous catalysis plays a crucial role in the chemical industry, which has evolved from the investigation of chemisorption to an electronic structure[1]. Diverse strategies, such as alloying,doping, and confining, have been applied to enhance the catalytic properties of active sites through electronic modulation. The electron transfer between active sites and substrates profoundly influences catalytic activity [2].

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Strong metal-support interactions between highly dispersed Cu^(+) species and ceria via mix-MOF pyrolysis toward promoted water-gas shift reaction

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Journal of Energy chemistry 2024年第4期91卷 475-483页

作者： Xiao-Chen Sun Xing-Chi Li Ze-Wei Xie Chen-Yue Yuan De-Jiu Wang Qian Zhang Xiao-Yu Guo Hao Dong Hai-Chao Liu Ya-Wen Zhang Beijing National Laboratory for molecular Sciences(BNLMS) State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Beijing National Laboratory for molecular Sciences(BNLMS) College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Beijing National Laboratory for molecular Sciences(BNLMS) State Key Laboratory for Structural Chemistry of Stable and Unstable SpeciesCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

The modulation of metal-support interfacial interaction is significant but challenging in the design of high-efficiency and high-stability supported ***,we report a synthetic strategy to upgrade Cu-CeO_(2)interfacial interaction by the pyrolysis of mixed metal-organic framework(MOF)*** obtained highly dispersed Cu/CeO_(2)-MOF catalyst via this strategy was used to catalyze water-gas shift reaction(WGSR),which exhibited high activity of 40.5μmolCOgcat^(-1).s^(-1)at 300℃and high stability of about 120 *** on comprehensive studies of electronic structure,pyrolysis strategy has significant effect on enhancing metal-support interaction and then stabilizing interfacial Cu^(+)species under reaction *** Cu^(+)species and generated oxygen vacancies over Cu/CeO_(2)-MOF catalyst played a key role in CO molecule activation and H2O molecule dissociation,*** collaborated closely and then promoted WGSR catalytic performance in comparison with traditio nal supported *** study shall offer a robust approach to harvest highly dispersed catalysts with finely-tuned metal-support interactions for stabilizing the most interfacial active metal species in diverse heterogeneous catalytic reactions.

关键词： Cu-based catalyst MOF derivative Water-gas shift reaction Metal-support interaction

Efficient and stable PtFe alloy catalyst for electrocatalytic methanol oxidation with high resistance to CO

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Journal of Energy chemistry 2024年第3期90卷 327-336,I0008页

作者： Qian Yang Sifan Zhang Fengshun Wu Lihua Zhu Guang Li Mingzhi Chen An Pei Yingliang Feng Jiangxi Provincial Key Laboratory of Functional molecular Materials chemistry College of Chemistry and Chemical EngineeringFaculty of Materials Metallurgy and ChemistryJiangxi University of Science and TechnologyGanzhou 341000JiangxiChina college of chemistry and Chemical engineering Xiamen UniversityXiamen 361005FujianChina

Direct methanol fuel cells(DMFC) are widely considered to be an ideal green energy conversion device but their widespread applications are limited by the high price of the Pt-based catalysts and the instability in terms of surface CO toxicity in long-term ***,the PtFe alloy nanoparticles(NPs) with small particle size(~4.12 nm) supported on carbon black catalysts with different Pt/Fe atomic ratios(Pt_(1)Fe_(2)/C,Pt_(3)Fe_(4)/C,Pt_(1)Fe_(1)/C,and Pt_(2)Fe_(1)/C) are successfully prepared for enhanced anti-CO poisoning during methanol oxidation reaction(MOR).The optimal atomic ratio of Pt/Fe for the MOR is 1:2,and the mass activity of Pt_(1)Fe_(2)/C(5.40 A mg_(Pt)^(-1)) is 13.5 times higher than that of conventional commercial Pt/C(Pt/C-JM)(0.40 A mg_(Pt)^(-1)).The introduction of Fe into the Pt lattice forms the PtFe alloy phase,and the electron density of Pt is reduced after forming the PtFe ***-situ Fourier transform infrared results indicate that the addition of oxyphilic metal Fe has reduced the adsorption of reactant molecules on Pt during the *** doping of Fe atoms helps to desorb toxic intermediates and regenerate Pt active sites,promoting the cleavage of C-O bonds with good selectivity of CO_(2)(58.1%).Moreover,the Pt_(1)Fe_(2)/C catalyst exhibits higher CO tolerance,methanol electrooxidation activity,and long-term stability than other Pt_(x)Fe_(y)/C catalysts.

关键词： Alloy catalyst PtFe Methanol oxidation In-situ FTIR CO resistance

Nanomaterial Assisted Exosome Analysis Using Mass Spectrometry

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Chemical Research in Chinese Universities 2024年第2期40卷 237-254页

作者： ZHANG Yi ZHOU Bokai LI Qiuning JIN Mingshi BAI Yu Beijing National Laboratory for molecular Sciences Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871P.R.China Department of chemistry Yanbian UniversityYanji133002P.R.China

Exosomes,extracellular vesicles(EVs)that play crucial roles in biological processes,have emerged as attractive targets for noninvasive disease diagnosis and *** spectrometry(MS)offers high sensitivity,high throughput,and excellent qualification and quantification capacity,which is the ideal approach for exosome ***’unique physiochemical properties,controllable morphology,and large surface area make them promising in biological sample pretreatment and *** contributed diverse functions to the exosome MS analysis,encompassing substrates for exosome isolation and cargos enrichment,matrices for laser desorption/ionization(LDI),read-out signals and supporters for signal amplification strategies,*** this review,recent progress in the applications of nanomaterial in the exosome MS analysis was summarized and a comprehensive discussion on the challenges and perspectives was proposed for the development of an advancing analysis approach of exosomes for the accurate diagnosis and monitoring of diseases.

关键词： Exosome Nanomaterial Enrichment Matrix Mass spectrometry

NIR-IIb-triggered photodynamic therapy combined with chemotherapy platform based on rare-earth-doped nanoparticles

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Rare Metals 2024年第7期43卷 3220-3231页

作者： Zhuo Tu Yong Wan Juan Ge Chen-Chen Li Tao Liang Zhen Li college of Health Science and engineering College of Chemistry and Chemical EngineeringHubei University

Photodynamic therapy（PDT）,with high spatiotemporal selectivity,minimal side effects and less drug resistance,has emerged as a promising approach for the treatment of ***,inadequate penetration depth and poor efficacy seriously restrict its practical *** address these challenges,we developed a combined therapy platform（RENP@C/D-FA） based on rare-earth-doped nanoparticles（RENPs） with a structure of NaErF4:Tm（0.5%）@NaYF4,on which photosensitizer Ce6（chlorin e6） and chemo-therapeutic drug（DOX）(doxorubicin) were loaded by encapsulating with an amphiphilic polymer distearoyl phosphatidylethanolamine-polyethylene glycol-folic acid（DSPE-PEG-FA）.RENPs with NaErF4as the matrix possess multiple excitation/emission peaks,enabling activation of PDT under near-infrared-Ⅱb（NIR-Ⅱb,1500-1700 nm） excitation and luminescence imaging in NIR-Ⅱb region by absorbing 808 nm near-infrared ***,DOX can be selectively released in the acidic microenvironment of *** from the tumor targeting capability of folic acid,this platform can successfully ablate tumor cells and inhibit tumor growth by combining PDT and *** innovative approach holds great promise as a powerful tool for cancer treatment,showing the potential to revolutionize PDT.

关键词： Photodynamic therapy Rare-earth-doped nanoparticles NIR-IIb Chemotherapy Combined therapy

Comparison of Measurements for Enhanced Diffusion Problem in Chemical Reaction Systems

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Chinese Journal of chemistry 2024年第14期42卷 1659-1664页

作者： Ah-Young Jee Ziyang Wen Huan Wang Beijing National Laboratory for molecular Sciences College of Chemistry and Molecular EngineeringBeijing Key Laboratory of Polymer Chemistry&Physics of Ministry of EducationPeking UniversityBeijing100871 China

The problem of molecular diffusion in the soup of chemical reactions attracts mounting interest across fields ranging from chemistry to biophysics to material *** reactions involve bond breakup and formation,whose time scale is typically on the orders of fs to ps,while molecular diffusion occurs at time scales ofμs to *** two processes are often considered orthogonal,given the vastly different *** serial results show that the enzyme's diffusion is enhanced in a substrate-dependent manner,which was further extended to small molecule reaction systems,challenging this classical ***,the results from different groups using different techniques do not quantitatively agree,and a general mechanism is yet to be *** summarize experimental studies on diffusion problems and seek to reconcile the interpretation with understanding the limits of measurement tools and the chemical nature of reaction *** molecular diffusion in chemical reactions will provide fresh thoughts in designing chemical systems such as molecular machines that harvest work at the nanoscale in a controllable manner.

关键词： molecular diffusion Chemical reactions Enzyme reactions Active matter Diffusion measurements Single-molecule studies Fluorescence Time-resolved spectroscopy

Bright InP quantum dots by Ga-doping for red emitters

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Nano Research 2024年第7期17卷 6721-6733页

作者： Kai-Zheng Song Xiao-Hang He Zhe-Yong Chen Ge Tang Jin-Zhao Huang Feng-Lei Jiang college of chemistry and molecular Sciences Wuhan UniversityWuhan 430072China

Environment-friendly indium phosphide(InP)-based quantum dots(QDs)with efficient red-emitting properties are sufficiently needed to satisfy the requirement of burgeoning display and lighting ***,the syntheses of InP QDs using tris(trimethylsilyl)phosphine as the precursor are highly toxic and ***,we successfully introduced gallium(Ga)ions into tris(dimethylamino)phosphine-based red InP cores through thermally-promoted cation exchange,and the obtained Ga-doped InP cores exhibited significantly increased photoluminescence quantum yields(PLQY)of up to 26%.The existence of Ga was directly confirmed by energy-dispersive X-ray spectroscopy and X-ray photoelectron spectroscopy,and the functions of Ga were systematically *** subsequent coating of Ga-doped InP cores with ZnSeS and ZnS shells,the resulting Ga-InP/ZnSeS/ZnS QDs achieved a high PLQY of 62%with an emission maximum at 640 *** contrast,without Ga-doping,the PLQY only attained 36%using the same synthetic *** indicated an approximate 1.7-fold increase in *** enhancement of photoluminescence was related to the Ga^(3+),as it not only passivated surface defects of InP cores but also reduced core–shell interface *** Ga-InP/ZnSeS/ZnS QDs exhibited good stability towards heat treatment and ultraviolet(UV)***,the red light-emitting diode(LED)based on Ga-InP/ZnSeS/ZnS QDs performed well in a wide injected current range of 2 to 200 mA,with a maximum power efficiency of 0.68 lm/*** work showcases Ga-doping through cation exchange as a promising strategy for enhancing the efficiency of InP-based red emitters.

关键词： indium phosphide gallium doping optical properties light emitting diode

Increase of chiral sensing ability in host-guest chemistry by magnetic anisotropy

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Science China chemistry 2024年第8期67卷 2775-2782页

作者： Jia-Liang Chen Bin Li Feng Yang Tiesheng Shi Xun-Cheng Su State Key Laboratory of Elemento-organic chemistry Tianjin Key Laboratory of Biosensing and Molecular RecognitionCollege of ChemistryNankai UniversityTianjin 300071China college of chemistry Chemical Engineering and Materials ScienceZaozhuang UniversityZaozhuang 277160China

Enantiomeric molecules generally play distinct functions in chemistry,biology,and *** physical and chemical properties of chiral analytes lay difficulty in discrimination and quantification of the *** report herein an efficient approach of increasing the chiral sensing ability ofβ-cyclodextrin(β-CD),a widely used host molecule,in the hostguest chemistry by magnetic anisotropy.A rigid and chiral lanthanide binding tag was attached to theβ-CD to amplify the changes of nuclear magnetic resonance(NMR)signals in the host-guest recognition *** installation of the paramagnetic lanthanide ion inβ-CD greatly enhances the enantiomeric discrimination up to 30-fold in comparison with the diamagneticβ-CD *** addition,the magnitude of the paramagnetic effects is tunable according to the diverse range of paramagnetic strength of the lanthanide *** reported method significantly increases the chiral sensing ability ofβ-CD,which can be applied to other host *** transferred paramagnetic effects,pseudocontact shifts(PCSs)and paramagnetic relaxation enhancements(PREs),from the host to the guest molecules,are valuable structural restraints to determine the absolute stereochemistry of the chiral *** strategy does not need modification of the analytes and is complementary to the reported analytical methods that rely on the functionalization of the chiral analytes.

关键词： chiral recognition nuclear magnetic resonance host-guest chemistry magnetic anisotropy lanthanide ions

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Capturing metal clusters at the strong-interaction region to reverse Ostwald ripening

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Science China Materials 2024年第4期67卷 1363-1364页

作者： Shuheng Tian Ding Ma Beijing National Laboratory for molecular Sciences New Cornerstone Science LaboratoryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

High-temperature interactions induce sintering of metal nanoparticles(NPs) on heterogeneous catalyst surfaces, leading to reduced surface area and active site loss through Ostwald ripening [1]. This irreversible deactivation necessitates costly catalyst replacement, notably impacting metals like copper in hydrogenation and reforming reactions [2].

关键词： catalyst reforming irreversible

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