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Recent progress on the functionalization of white phosphorus in China

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national Science Review 2024年第6期11卷 308-320页

作者： Xinlei Huangfu Zhongzhen Wang Yu Chen Junnian Wei Wei Liu Wen-Xiong Zhang Beijing national laboratory for Molecular Sciences(BNLMS) State Key Laboratory of Rare-Earth Materials Chemistry and Applications & Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular Engineering Peking University

Direct synthesis of organophosphorus compounds from white phosphorus represents a significant but challenging subject, especially in the context of ongoing efforts to comprehensively improve the phosphorus-derived chemical industry driven by sustainability and safety concerns. China is the world's largest producer of white phosphorus, creating a significant demand for the green transformation of this crucial feedstock. This review provides an overview of advancements in white phosphorus activation by Chinese research teams, focusing on the direct construction of P–C/N/O/S/M bonds from white phosphorus. Additionally, we offer some insights into prospective directions for the activation and transformation of white phosphorus in the future. This review paper aims to attract more researchers to engage in this area, stimulating follow-up exploration and fostering enduring advances.

关键词： white phosphorus organophosphorus compound activation selectivity efficiency

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

Electrostatically connected nanoarchitected electrocatalytic films for boosted water splitting

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Nano Research 2024年第3期17卷 1114-1122页

作者： Chao-Peng Wang Hao Sun Gang Bian Jia-Xi Wang Xixi Pang Guoqi Wang Jian Zhu Xian-He Bu School of materials Science and Engineering National Institute for Advanced MaterialsNankai UniversityTianjin 300350China Tianjin key laboratory of Metal and Molecule-Based Material chemistry Nankai UniversityTianjin 300350China Tianjin key laboratory for rare earth materials and applications Nankai UniversityTianjin 300350China

Active sites of two-dimensional(2D)electrocatalysts are often partially blocked owing to their inevitable stacking and hydrophobic polymeric binders in macroscale electrodes,therefore impeding their applications in efficient ***,using layered double hydroxide(LDH)nanosheets as a model 2D electrocatalyst,we demonstrate that their performance toward water splitting can be boosted when they are electrostatically assembled into an organized structure pillared by hydrophilic polyelectrolytes or nanoparticles in a layer-by-layer(LbL)*** particular,their mass activity on a planar electrode can be as large as 2.267 mA·μg^(-1) toward oxygen evolution reaction(OER),when NiFe-LDH nanosheets are electrostatically connected by poly(sodium 4-styrenesulfonate)(PSS),while drop-casted NiFe-LDH nanosheets only have a mass activity of 0.116 mA·μg^(-1).In addition,these homogeneous NiFe-LDH nanofilms can be easily deposited on three-dimensional(3D)surfaces with high areas,such as carbon cloths,to serve as practical electrodes with overpotentials of 328 mV at a current density of 100 mA·cm^(-2),and stability for 40 ***,Pt nanoparticles can be LbL assembled with NiFe-LDH as bifunctional electrodes for synergistically boosted oxygen and hydrogen evolution reactions(HER),leading to successful overall water splitting powered by a 1.5 V *** study heralds the spatial control of 2D nanomaterials in nanoscale precision as an efficient strategy for the design of advanced electrocatalysts.

关键词： layer-by-layer(LbL)assembly layered double hydroxides(LDH) two-dimensional(2D)electrocatalysts oxygen evolution reaction(OER) water splitting

Metal-metal bonds in Zintl clusters:Synthesis,structure and bonding in[Fe_(2)Sn_(4)Bi_(8)]^(3-)and[Cr_(2)Sb_(12)]^(3-)

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Chinese Chemical Letters 2024年第8期35卷 558-566页

作者： Ya-Nan Yang Zi-Sheng Li Sourav Mondal Lei Qiao Cui-Cui Wang Wen-Juan Tian Zhong-Ming Sun John E.McGrady state key laboratory of Element-Organic chemistry Tianjin Key Lab for Rare Earth Materials and ApplicationsSchool of Materials Science and EngineeringNankai UniversityTianjin 300350China Department of chemistry University of OxfordInorganic Chemistry LaboratoryOxfordOX13QRUnited Kingdom

We report here the synthesis and characterization of two new members of the M2 E 12 family of endohe-dral Zintl clusters,[Fe_(2)Sn_(4)Bi_(8)]^(3-)and[Cr_(2)Sb_(12)]^(3-),both of which contain open-shell metal dimers encap-sulated inside a triple-decker cluster of main-group *** 75-electron[Fe_(2)Sn_(4)Bi_(8)]^(3-)cluster has a D4h-symmetric structure,while[Cr_(2)Sb_(12)]^(3-),despite having the same 75-electron count,is strongly dis-torted to a geometry that resembles a CrSb_(8)crown capped by a CrSb_(4)*** structural differences between the two are driven by the increasing availability of 3d electron density in the earlier transi-tion metal,which leads,ultimately,to different electronic configurations in the two *** trends precisely mirror those observed in the ME_(10)and ME_(12)families containing a single transition metal ion.

关键词： Zintl anions Endohedral clusters Metal-metal bond Second-order Jahn-Teller effect DFT calculation

The first chiral cerium halide towards circularly-polarized luminescence in the UV region

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Science China chemistry 2024年第6期67卷 1961-1968页

作者： Xinyi Niu Zhichao Zeng Zhaoyu Wang Haolin Lu Bing Sun Hao-Li Zhang Yongsheng Chen Yaping Du Guankui Long Tianjin key Lab for rare earth materials and applications Renewable Energy Conversion and Storage CenterSmart Sensing Interdisciplinary Science CenterSchool of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin300350China Tianjin key Lab for rare earth materials and applications Center for Rare Earth and Inorganic Functional MaterialsHaihe Laboratory of Sustainable Chemical TransformationsSmart Sensing Interdisciplinary Science CenterSchool of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin300350China state key laboratory of Applied Organic chemistry Key Laboratory of Special Function Materials and Structure Design(Ministry of Education)College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000China The Centre of Nanoscale Science and Technology and state key laboratory of Elemento-Organic chemistry Frontiers Science Center for New Organic MatterCollege of ChemistryNankai UniversityTianjin300071China

Chiral organic-inorganic hybrid metal halides(OIHMHs)have attracted broader scientific community recently in spin lightemitting diodes,and circularly polarized light-emitting ***,the emission peaks of the reported chiral OIHMHs mainly locate in the visible region,and chiral OIHMH with ultraviolet(UV)circularly polarized luminescence(CPL)has been rarely *** fill this gap,cerium,a unique rare-earth(RE)element with tunable luminescence from UV to the visible region owing to the 4 f-related electronic transition,was introduced to construct the first RE-based chiral OIHMHs,R/*** chirality is successfully transferred from the chiral organic cations to the inorganic cerium chloride framework in R/S-MCC,as confirmed by the single crystal structures,circular dichroism,and *** emission spectra of R/S-MCC are in the UV region,originating from the characteristic d-f transition of Ce^(3+),which making the Ce-based metal halides are ideal candidates towards CPL light sources in the UV ***,R-and S-MCC are the first RE-based OIHMHs,also the first chiral metalhalides with UV *** work opens a new avenue for the development of the chiral OIHMH family towards RE-based chiral *** RE-based chiral metal halides couple the unique and superior optical,electrical,magnetic,and spintronic properties of RE elements with chirality could accelerate the development of chiral optoelectronics and spintronics toward real applications.

关键词： chiral rare-earth halide ultraviolet circularly-polarized luminescence d-f transition rare-earth halide perovskite chiral perovskite

Facile and effective synthesis strategy for terbium-doped hydroxyapatite toward photoelectric devices and flexible functional fibers

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rare Metals 2024年第4期43卷 1713-1723页

作者： Xiao-Dong Zhang Kun Nie Zi-Yao Hu Ran-Ran Zhou Xiu-Qiang Duan Wu-Bin Dai Song-Song Nie Song-Jun Yao Luo-Xin Wang Le-Fu Mei Hua Wang Yi-Yi Yao Xiao-Xue Ma Hubei key laboratory for New Textile materials and applications and state key laboratory of New Textile materials and Advanced Processing Technology School of Materials Science and EngineeringWuhan Textile UniversityWuhan430200China key laboratory of Testing and Tracing of rare earth Products for state Market Regulation Jiangxi University of Science and TechnologyGanzhou341000China Hubei key laboratory of Plasma chemistry and Advanced materials and key laboratory of Green Chemical Engineering Process of Ministry of Education Wuhan Institute of TechnologyWuhan430205China

As a material with good biocompatibility,hydroxyapatite(HAP)can have optical properties after doping with various rare earth *** a biocompatible fluorescent material,doped HAP could have broad applications in biological probes,drug delivery,optoelectronic materials,fluorescence anti-counterfeiting,and other *** this paper,we put forward the preparation of HAP doped with terbium(Ⅲ)ions(Tb^(3+))by hydrothermal *** controlling the Tb^(3+)doping content in reaction and the reaction time,the changes in HAP's structure,morphology,and luminescence properties under different conditions were *** the doping amount of Tb^(3+)reached an optimal value,the dipole-quadrupole would occur and the concentration would be *** control experiment showed that the optimal Tb3+content was 7.5×10^(-5)mol,which showed the best fluorescence ***,a non-luminous material,was rarely used in the field of fluorescent anti-counterfeiting and photoelectric *** proposed to prepare a luminescent aramid/polyphenylene sulfide(ACFs/PPS)fiber paper and a new light-emitting diode(LED)using the Tb-doped HAP *** composite sample exhibited an excellent stability and fluorescence performance,which also demonstrated a possibility of HAP applications in anticounterfeiting and *** introduction of Tb3+dopant HAP was done to give HAP optical properties and broaden the application range of HAP.

关键词： Hydroxyapatite rare earth luminescence Photoelectric device Aramid Polyphenylene sulfide fiber paper Luminescent fiber

Synthesis,Structure and Chemical Bonding of Polyantimony Clusters Containing Coinage Metals[M_(2)Sb_(14)]^(4-)(M=Cu,Ag)

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Chinese Journal of chemistry 2024年第6期42卷 617-622页

作者： Wei-Xing Chen Yu-He Xu Cui-Cui Wang Lei Qiao Zi-Yan Guo Wen-Juan Tian Zhong-Ming Sun state key laboratory of Element-Organic chemistry Tianjin Key Lab for Rare Earth Materials and ApplicationsSchool of Materials Science and EngineeringNankai UniversityTianjin300350 China Institute of Molecular Science Shanxi UniversityTaiyuanShanxi030006 China

Binary polyantimony clusters,namely[Cu_(2)Sb_(14)]^(4–) and [Ag_(2)Sb_(14)]^(4–),containing coinage metals,were successfully synthesized and characterized,in which two homoatomic Sb73–subunits are bridged by two coinage metals in η^(4):η^(1) and η^(1):η^(1) coordination modes,***[M_(2)Sb_(14)]^(4-),two bridging Cu ions and two Sb atoms form a planar rhombic unit,which was revealed to have antiaromatic properties by theoretical *** electron structure and bonding analysis confirmed the presence of delocalized bonds in the rhombic unit and the metallophilic interaction between two formal M^(+) ions.

关键词： Polyantimony cluster Copper Silver Antiaromaticity Metallophilic interaction Quantum chemical calculations

Lanthanide-based microlasers:Synthesis,structures,and biomedical applications

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Nano Research 2024年第1期17卷 97-111页

作者： Qian Zhang Yawei Liu Kai Liu Hongjie Zhang Engineering Research Center of Advanced rare earth materials(Ministry of Education) Department of ChemistryTsinghua UniversityBeijing 100084China state key laboratory of rare earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Xiangfu laboratory Jiaxing 314102China

The large size of lasers limits their applications in confined spaces,such as in biosensing and in vivo brain tissue *** this regard,micron-sized lasers have been *** exhibit great potential for biological detecting,remote sensing,and depth tracking due to their small sizes,sensitive properties of their spectral fingerprints,and flexible positional modulation in the ***-based luminescent materials that possess long excited-state lifetime,narrow emission bandwidth,and upconversion behaviors are promising as gain mediums for novel *** addition,lanthanide-based microlasers could be generated under natural ambient conditions with pumped or continuous light sources,which significantly promotes the practical applications of *** progress in the design,synthesis,and biomedical applications of lanthanide-based microlasers has been outlined in this *** ions doped and upconverted lanthanide-based microlasers are highlighted,which exhibit advantageous structures,miniaturized dimensions,and high lasing *** applications of lanthanide-based microlasers are further discussed,the upconverted microlasers show great advantages for biological applications owing to their tunable excitation and emission characteristics and excellent environmental ***,perspectives and challenges in the field of lanthanide-based microlasers are presented.

关键词： microlasers lanthanide-based luminescent materials upconversion nanoparticles biological applications

Boosting ammonia production in electrocatalytic NO_(x)reduction on a robust Fe/FeMoO_(4)catalyst

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Nano Research 2024年第7期17卷 5801-5806页

作者： Dong-Xue Liu Xin Deng Yong-Fu Zhu Zhe Meng Xue-Feng Sun Miao-Miao Shi Hai-Xia Zhong Jun-Min Yan key laboratory of Automobile materials Ministry of EducationSchool of Materials Science and EngineeringJilin UniversityChangchun 130022China state key laboratory of rare earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Electrocatalytic reduction of nitrate(NO_(3)^(−))and nitride(NO_(2)^(−))to ammonia(NH3)is of wide interest as a promising alternative to the energy-intensive Haber-Bosch route for mitigating the vast energy consumption and the accompanied carbon dioxide emission,as well as benefiting for the relevant sewage ***,exploring an efficient and low-cost catalyst with high atomic utilization that can effectively facilitate the slow multi-electron transfer process remains a grand ***,we present an efficient hydrogenation of NO_(3)^(−)/NO_(2)^(−)species to NH3 in both alkaline and neutral environments over the Fe_(2)(MoO_(4))_(3)derived hybrid electrocatalyst with the metallic Fe site on FeMoO_(4)(Fe/FeMoO_(4)).The Mo ingredient can play a synergistically positive role in further promoting the NH_(3) production on *** a result,Fe/FeMoO_(4)behaves well in the electrochemical NH_(3) generation from NO_(2)^(−)with a maximum NH_(3) Faradaic efficiency(FE)of 96.53%and 87.68%in alkaline and neutral electrolyte,corresponding to the NH_(3) yield rate of 640.68 and 302.56 mg·h^(−1)·mg_(cat.)^(−1),respectively,which outperforms the Fe and Mo counterpart and other similar catalyst,showing the robust catalytic capacity of each active site.

关键词： ammonia synthesis NO_(x)reduction synergistic effect alkaline/neutral electrolyte