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Comparison of extraction abilities of deep eutectic solvents and aqueous acid solutions for extraction of rare earths and transition metals

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Journal of Rare Earths 2024年第6期42卷 1157-1164,I0006页

作者： Svetlana Drogobuzhskaya Margarita Frolova Andrey Shishov Nikita Tsvetov Tananaev institute of chemistry-Subdivision of the Federal Research centre《Kola Science centre of the Russian Academy of Sciences》 18420926a AcademgorodokApatityRussia Murmansk State Technical University 183010Sportivnaja str.13MurmanskRussia Department of Analytical chemistry Institute of ChemistrySaint Petersburg State UniversitySpbSU.1990347/9 Universitetskaya embSt.Petersburg Russia

In recent years,deep eutectic solvents have attracted increasing interest as effective extractants for the separation of both organic substances and metals from various ***-based deep eutectic solvents are most often used as extractants for the extraction of *** this work,for the first time,the extraction efficiency of transition metals and rare earth elements(Y,Zr,Nb,La,Ce,Pr,Nd,Sm,Eu,Gd,Tb,Dy,Ho,Er,Tm,Yb,Lu,Hf and Ta)from mining tailings and Na,K,Ca,Mg,Cu,Fe,Mn,Pb,Ba,Ni and Sr from biodiesel samples using acidic deep eutectic solvents and saturated aqueous solutions of the same acids(malonic,malic,tartaric and citric)is *** this,deep eutectic solvents based on acids and their aqueous saturated solutions were prepared and *** prepared mixtures were analyzed by IR spectroscopy to confirm the formation of eutectic *** such as the density and viscosity of the resulting mixtures were also investigated,as this can be of key importance for the efficiency of metal *** extraction of rare earth metals from mining tailings took a long time(up to several days),while the extraction of metals from fuel took no more than 30 *** emission spectral methods were used as an analysis *** is shown that the extraction efficiency with aqueous solutions is better than that with eutectic solvents,which casts doubt on the need for deep eutectic solvents use in this area.

关键词： Deepeutectic solvent Metal separation Elemental analysis Rare earth metals Biodiesel

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Dimensional regulation in gigantic molybdenum blue wheels featuring{(W)Mo_(5)}motifs for enhanced proton conductivity

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Nano Research 2024年第9期17卷 8261-8268页

作者： Yu-Lun Wu Jing Du Hai-Ying Zhang Ming-Jun Hou Qiao-Yue Li Wei-Chao Chen Kui-Zhan Shao Bo Zhu Chao Qin Xin-Long Wang Zhong-Min Su Key Laboratory of Polyoxometalate and Reticular Material chemistry of Ministry of Education Department of ChemistryNortheast Normal UniversityChangchun 130024China Hebei Key Laboratory of organic Functional Molecules National Demonstration Center for Experimental Chemistry EducationTesting and Analysis CenterCollege of Chemistry and Materials ScienceHebei Normal UniversityShijiazhuang 050024China State Key Laboratory of Supramolecular Structure and Materials Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China

Dimensional regulation in polyoxometalates is an effective strategy during the design and synthesis of polyoxometalates-based high proton conductors,but it is not available to ***,the precise regulation of dimensionality has been realized in an unprecedented gigantic molybdenum blue wheel family featuring pentagonal{(W)Mo5}motifs through optimizing the molar ratio of Mo/W,including[Gd_(2)Mo_(124)W_(14)O_(422)(H_(2)O)62]38-(0D-{Mo_(124)W_(14)},1),[Mo_(126)W_(14)O441(H_(2)O)51]^(70-)(1D-{Mo_(126)W_(14)}n,2),and[Mo_(124)W_(14)O_(430)(H_(2)O)50]60-(2D-{Mo_(124)W_(14)}n,3).Such important{(W)Mo5}structural motif brings new reactivity into gigantic Mo blue *** are different numbers and sites of{Mo2}defects in each wheel-shaped monomer in 1-3,which leads to the monomers of 2 and 3 to form 1D and 2D architectures via Mo-O-Mo covalent bonds driven by{Mo2}-mediated H_(2)O ligands substitution process,respectively,thus achieving the controllable dimensional *** expected,the proton conductivity of 3 is 10 times higher than that of 1 and 1.7 times higher than that of *** continuous proton hopping sites in 2D network are responsible for the enhanced proton conductivity with lower activation *** study highlights that this dimensional regulation approach remains great potential in preparing polyoxometalates-based high proton conductive materials.

关键词： polyoxometalate molybdenum blue wheels Mo/W mixed-addenda polyoxometalates dimensional regulation proton conduction

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Alkyl chain modulation of asymmetric hexacyclic fused acceptor synergistically with wide bandgap third component for high efficiency ternary organic solar cells

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International Journal of Minerals,Metallurgy and Materials 2024年第7期31卷 1713-1719页

作者： Shufang Li Huilan Guan Can Zhu Chaoyuan Sun Qingya Wei Jun Yuan Yingping Zou College of chemistry and Chemical Engineering Central South UniversityChangsha 410083China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China institute of Carbon Neutrality and New Energy School of Electronics and InformationHangzhou Dianzi UniversityHangzhou 310018China

Herein,two asymmetric hexacyclic fused small molecule acceptors(SMAs),namely BP4F-HU and BP4F-UU,were *** elongated outside chains in the BP4F-UU molecule played a crucial role in optimizing the morphology of blend film,thereby improving charge mobility and reducing energy loss within the corresponding ***,the PM6:BP4F-UU device exhibited a higher open-circuit voltage(V_(oc))of 0.878 V compared to the PM6:BP4F-HU device with a V_(oc)of 0.863 ***,a new wide bandgap SMA named BTP-TA was designed and synthesized as the third component to the PM6:BP4F-UU host binary devices,which showed an ideal complementary absorption spectrum in PM6:BP4F-UU *** addition,BTP-TA can achieve efficient intermolecular energy transfer to BP4F-UU by fluorescence resonance energy transfer(FRET)pathway,due to the good overlap between the photoluminescence(PL)spectrum of BTP-TA and the absorption region of ***,ternary devices with 15wt%BTP-TA exhibits broader photon utilization,optimal blend morphology,and reduced charge recombination compared to the corresponding binary ***,PM6:BP4F-UU:BTP-TA ternary device achieved an optimal power conversion efficiency(PCE)of 17.83%with simultaneously increased V_(oc)of 0.905 V,short-circuit current density(J_(sc))of 26.14 mA/cm^(2),and fill factor(FF)of 75.38%.

关键词： asymmetric hexacyclic acceptor outside chain wide bandgap acceptor ternary organic solar cells

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Denitration of Nitroarenes Under Ambient Physiological Conditions Catalyzed by Graphdiyne-Supported Palladium

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CCS chemistry 2024年第3期6卷 641-651页

作者： Endong Zhang Yanyan Chen Fengting Lv Zicheng Zuo Feng He Yongjun Li Yiming Huang Yuliang Li Shu Wang Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190 College of chemistry University of Chinese Academy of SciencesBeijing 100049

The direct cleavage of C–NO_(2)bonds for reductive denitration of nitroarenes remains a challenging transformation in synthetic organic ***,we report a biocompatible palladium-deposited graphdiyne nanocatalyst(Pd@GDY/DSPE-PEG)that can catalyze reductive denitration of nitroarenes under ambient physiological *** studies support this transformation via the oxidative addition of nitroarenes with Pd(0)and subsequent ligand exchange to form arylpalladium *** one-step reductive denitration via Pd@GDY/DSPE-PEG successfully facilitates the repair of the nitrated proteins arising from endogenic ONOO−and restores their physiological function,including blocking the apoptosis pathway in living ***,Pd@GDY/DSPE-PEG was further successfully applied for catalytic denitration to reduce the level of 3-nitrotyrosine residues of proteins located in the mouse brain hippocampus in *** study provides an ideal strategy for designing highly active enzymatic mimicking synthetic catalysts for the regulation of the nitrated protein level and the detoxification of nitrative damage of living cells and tissues.

关键词： 3-nitrotyrosine artificial nanaocatalysts reductive denitration palladium-deposited graphdiyne repairing nitrated protein

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Confined Mn^(2+) enables effective aerobic oxidation catalysis

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Science China chemistry 2024年第5期67卷 1545-1553页

作者： Desheng Yuan Sicong Ma Xiao Kong Chi Zhang Lin Chen Chengsheng Yang Lihua Wang Zhen Liu Lin Ye Yongmei Liu Rui Ma Zhi-Pan Liu Yifeng Zhu Yong Cao Xinhe Bao Department of Chemical Physics University of Science and Technology of ChinaHefei 230026China Department of chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsCollaborative Innovation Center of Chemistry for Energy MaterialsFudan UniversityShanghai 200438China Key Laboratory of Synthetic and Self-Assembly chemistry for organic Functional Molecules Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of Materials and chemistry University of Shanghai for Science and TechnologyShanghai 200093China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China institute of Advanced Fluorine-Containing Materials Zhejiang Normal UniversityJinhua 321004China State Key Laboratory of Catalysis National Laboratory for Clean EnergyCollaborative Innovation Center of Chemistry for Energy MaterialsDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

Effective and mild activation of O_(2) is essential but challenging for aerobic oxidation. In heterogeneous catalysis, high-valence manganese oxide(e.g., +4) is known to be active for the oxidation, whereas divalent MnO is ineffective due to its limited capacity to supply surface oxygen and its thermodynamically unstable structure when binding O_(2) in reaction conditions. Inspired by natural enzymes that rely on divalent Mn^(2+), we discovered that confining Mn^(2+) onto the Mn_(2)O_(3) surface through a dedicated calcination process creates highly active catalysts for the aerobic oxidation of 5-hydroxymethylfurfural, benzyl alcohol, and *** Mn_(2)O_(3)-confined Mn^(2+) is undercoordinated and efficiently mediates O_(2) activation, resulting in 2–3 orders of magnitude higher activity than Mn_(2)O_(3) alone. Through low-temperature infrared spectroscopy, we distinguished low-content Mn^(2+) sites at Mn_(2)O_(3) surface, which are difficult to be differentiated by X-ray photoelectron spectroscopy. The combination of in-situ energydispersive X-ray absorption spectroscopy and X-ray diffraction further provides insights into the formation of the newly identified active Mn^(2+) sites. By optimizing the calcination step, we were able to increase the catalytic activity threefold *** finding offers promising frontiers for exploring active oxidation catalysts by utilizing the confinement of Mn^(2+)and oftenignored calcination skills.

关键词： confinement catalysis manganese oxide aerobic oxidation divalent Mn^(2+) operando spectroscopies

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Synergistic silver-mediated and palladium-catalyzed nondirected olefination of aryl C–H bond: quick access to multi-substituted aryl olefins

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Science China chemistry 2024年第3期67卷 882-889页

作者： Jian Yao Lili Shao Xiaohong Huo Xiaoming Wang Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs Frontiers Science Center for Transformative MoleculesSchool of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Organometallic chemistry Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 20032China School of chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China

Transition metal-catalyzed olefination of aryl C-H bond is a powerful tool for the synthesis of alkenes. While the Pd-catalyzed oxidative C-H olefination of arenes, also known as Fujiwara-Moritani reaction, has been established as one of the most efficient methods, the substrates are largely limited to terminal olefins with electron-withdrawing group(s). Herein, we report a synergistic silver-mediated and palladium-catalyzed non-directed C-H olefination of arenes with vinyl(pseudo)halides, which offers a complementary strategy to the typical Fujiwara-Moritani reaction. The reactions proceeded well for a variety of halogenated arenes, heteroarenes, and olefin substrates, providing an efficient access to various multi-substituted aryl olefins, including trisubstituted/tetrasubstituted olefins and several complex olefins derived from medicines or natural products. Mechanistic studies indicated a bimetallic Pd/Ag cooperation is operative in the catalysis, i.e., the reaction is initiated by aryl C-H bond cleavage via ligation with phosphine/Ag species, followed by transferring of the aryl moiety to a vinyl palladium intermediate,which is in turn formed by oxidative addition of vinyl(pseudo)halide to a Pd complex. This method enables the synthesis of a wide range of challenging multi-substituted vinyl products from simple arenes(directing-group free) in a streamlined and controllable fashion.

关键词： direct C–H olefination multi-substituted aryl alkenes bimetallic Pd/Ag cooperation C–H functionalization

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Combination of methylthio-chemistry with living crystallization-driven self-assembly toward uniformπ-conjugated nanostructures with antibacterial activity,surface tailorability,tunable morphology and dimension

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Science China chemistry 2024年第7期67卷 2341-2352页

作者： Chuyu Duan Binbin Xu Ruru Li Xiaoyu Huang Shaoliang Lin Chun Feng Shanghai Key Laboratory of Advanced Polymeric Materials School of Materials Science and EngineeringEast China University of Science and TechnologyShanghai 200237China School of chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China Key Laboratory of Fluorine and Nitrogen chemistry and Advanced Materials Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

Living crystallization-driven self-assembly(CDSA)provides robust access to uniformπ-conjugated nanostructures(CNSs)from block copolymers(BCPs)containing a crystallineπ-conjugated segment with controlled dimension,morphology and composition,which show appealing applications in biomedicine,photocatalysis and *** further expand the application spectrum of these CNSs,the development of facile strategies toward diverse CNSs with varying structures/functionalities is highly ***,BCPs consisting of oligo(p-phenylene ethynylene)-b-poly(polypropyl-3-methanethiol acrylate)(OPE_(9)-bPMTPA35and OPE_(9)-b-PMTPA_(58);the subscript represents the number of repeat unit of each block)consisting of a crystallineπ-conjugated core-forming OPE_(9)segment and a corona-forming PMTPA block are *** efficient“click-type”alkylation of methylthio groups,OPE_(9)-b-PMTPA with varying contents of sulfonium unit is *** ribbon-like micelles with different widths and lengths can then be generated in a controlled manner via the self-seeding approach of living ***,negatively charged polymeric and Ag nanoparticles can be immobilized on sulfonium/methylthio-containing shells by taking advantage of electrostatic attraction and coordination interaction,***,the ribbon-like micelles with positively charged shells exhibit antibacterial activity against *** the ease of modification of PMTPA-based shell and attractive opto-electronic/photocatalytic properties ofπ-conjugated units,the combination of methylthio-chemistry and living CDSA opens a new avenue to generate multi-functional CNSs for widespread applications from biomedicine to photocatalysis.

关键词： crystallization-driven self-assembly block copolymer π-conjugated nanostructure methylthio-chemistry

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High-throughput experimentation and machine learning-promoted synthesis of α-phosphoryloxy ketones via Ru-catalyzed P(O)O–H insertion reactions of sulfoxonium ylides

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Science China chemistry 2024年

作者： An Lin Jingyuan Liu Yougen Xu Haiting Wu Yating Chen Yan Zhang Lebin Su Xiaodan Zhao Kuangbiao Liao institute of organic chemistry & MOE Key Laboratory of Bioinorganic and Synthetic chemistry School of Chemistry Sun Yat-sen University Guangzhou National Laboratory Bioland Laboratory

Herein, we report a novel and highly efficient method for the synthesis of α-phosphoryloxy carbonyl compounds via Rucatalyzed P(O)O–H insertion reactions of sulfoxonium ylides and phosphinic acids, with the assistance of high-throughput experimentation(HTE) and machine learning(ML). A variety of P(O)O-H derivatives, including diarylphosphates, alkyl phosphates, and alkoxyphosphates, are competent candidates to react with sulfoxonium ylides in this transformation, and variousα-phosphoryloxy carbonyls and propylene phosphates are directly constructed. This approach utilizes readily available sulfoxonium ylide as a carbene precursor, and features mild conditions, operational simplicity, and broad functional groups tolerance, and could be used for late-stage functionalization of structurally complex bioactive molecules. Moreover, a conducive exploration of the reaction space is also conducted(756 reactions) and a machine learning model for reaction yield prediction has been developed and applied, showcasing the practical application of this newly workflow(HTE-ML) in the field of synthetic chemistry.

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Rapid and chemoselective imidation of sulfides in aqueous buffer enabled by a novel guanidine-derived N-O reagent

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Science China chemistry 2024年第6期67卷 1929-1934页

作者： Hanzheng Li Long Xu Jiajia Dong Key Laboratory of Organofluorine chemistry Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai200032China institute of Translational Medicine National Facility for Translational Medicine(Shanghai)Shanghai Jiao Tong UniversityShanghai200240China School of chemistry and Chemical Engineering Zhangjiang Institute for Advanced StudyShanghai Jiao Tong UniversityShanghai200240China Shanghai Artificial Intelligence Laboratory Shanghai200232China

Herein we report the facile synthesis of a series of novel N-O reagents and identify N′-di-Boc-N′′-[(mesitylsulfonyl)oxy]-guanidine as an efficient imidating *** reagent is synthetically scalable and bench-stable,yet it shows unprecedented reactivity and chemoselectivity towards S(II)in buffer/hexafluoroisopropanol(HFIP)system,to generate a new class of Nguanyl *** transformation of N-guanyl sulfilimines to N-guanyl sulfoximines provides us a chance to investigate these rarely reached compounds,which are shown to be versatile precursors to a variety of N-heterocyclic and *** work provides an addition to the tool box of both sulfur imidation and guanidine synthesis,especially for the need of rapid and selective modifications of sulfur(II)center under biocompatible conditions.

关键词： sulfur imidation N-O reagent

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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

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