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Metallaphotoredox-Catalyzed Three-Component Couplings for Practical Synthesis of Ureas and Carbamates

Chinese Journal of chemistry 2024年第3期42卷 264-270页

作者： Ernest Koranteng Zhen-Cao Shu Yi-Yin Liu Qian Yang Bin Shi Qiang-Xian Wu Fen Tan Liang-Qiu Lu Wen-Jing Xiao Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction Ministry of EducationCollege of ChemistryCentral China Normal University152 Luoyu RoadWuhanHubei430079 China Wuhan Youji Industries Co. LtdNo.1 2nd Chemical Rd.WuhanHubei430082 China Hubei Key Laboratory of Purification and Application of Plant Anti-cancer Active Ingredients School of Chemistry and Life SciencesHubei University of EducationWuhanHubei430205 China State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhouGansu730000 China School of chemistry and Chemical Engineering Henan Normal UniversityXinxiangHenan453007 China Wuhan institute of Photochemistry and Technology WuhanHubei430082 China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai200032 China

Ureas are widely used in drugs,materials and catalysts because of their diamide structure,which can form strong hydrogen ***,it is of great scientific significance to develop efficient and green methods for the synthesis of urea compounds,especially unsymmetrical ***,we have disclosed novel and highly efficient three-component coupling reactions of organic halides,sodium cyanate and amines enabled by nickel/photoredox dual catalysis for the preparation of unsymmetrical *** reaction features simple and safe operations,broad substrate scopes,and product *** allows the facile synthesis of N-aryl/vinyl ureas from readily available,user-friendly feedstocks under mild conditions(27 examples,36%—98%yields).In addition,this method is further derived to alcohols as nucleophiles to synthesize a series of carbamates(15 examples,40%—95%yields).The mechanism experiment shows that the isocyanate produced by the coupling of halide and sodium cyanate may be the key intermediate in this reaction.

关键词： Cross-coupling Nickel Photoredox catalysis Three-component reaction Ureas Carbamates

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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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The 2^(nd)Asian Conference on Porphyrins,Phthalocyanines and Related Materials

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Chinese Chemical Letters 2024年第7期35卷 1-3页

作者： Gaojie Zhu Zhen Yang Shijun Li Weihua Zhu Rui Cao Junlong Zhang Jianzhang Zhao Jonathan L.Sessler Xunjin Zhu Jianxin Song Yongshu Xie Jianzhuang Jiang Key Laboratory for Advanced Materials and institute of Fine Chemicals School of Chemistry and Molecular EngineeringEast China University of Science&TechnologyShanghai 200237China College of Material Chemistry and Chemical EngineeringKey Laboratory of Organosilicon Chemistry and Material Technology of Ministry of EducationHangzhou Normal UniversityHangzhou 311121China School of chemistry and Chemical Engineering Jiangsu UniversityZhenjiang 212013China Key Laboratory of Applied Surface and Colloid chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi'an 710119China Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China State Key Laboratory of Fine Chemicals Frontier Science Center for Smart MaterialsSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China Department of chemistry The University of TexasAustinTexas 78712-1224United States Department of chemistry and institute of Advanced Materials Hong Kong Baptist UniversityHong Kong 999077China Key Laboratory of Chemical Biology and Traditional Chinese Medicine(Ministry of Educational of China) Key Laboratory of the Assembly and Application of Organic Functional Molecules of Hunan ProvinceCollege of Chemistry and Chemical EngineeringHunan Normal UniversityChangsha 410081China Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China

In the past decades,porphyrins,phthalocyanines and related materials have attracted significant attention due to their diverse and brilliant structures[1,2],as well as their unique electronic structures and photophysi... 详细信息

关键词： cyanine phthalocyanine Porphyrin

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Visible-light-induced synthesis of phosphorylated N-heterocycles through proton-coupled electron transfer

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Science China chemistry 2021年第5期64卷 681-683页

作者： Vera A.Vil’ Igor B.Krylov Alexander O.Terent’ev N.D.zelinsky institute of organic chemistry of the Russian Academy of Sciences Moscow 119991Russia

Phosphorus-containing organic compounds are important feedstock for the synthesis of value-added bioactive ***,the development of highly efficient synthetic methods for the construction of phosphorus-element bonds has drawn huge attention in the past decades[1].Particularly,the formation of P–C bonds from phosphoruscentered radicals has been demonstrated to be one of the most efficient and convenient strategies,which has been widely applied for the synthesis of organic phosphorus compounds in recent years.

关键词： synthesis bonds phosphorus

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Theoretical probe into universal tetrad effect for complexation discrepancy between lanthanide elements and organophosphoric extractant diethyl phosphoric acid

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Journal of Rare Earths 2024年第6期42卷 1142-1148,I0006页

作者： Haifeng Zheng Yanling Li Xuyi Zhang Jinglu Han Songsong Li Guolong Wu Qingshi Liu Xiaojuan Liu Wuping Liao State Key Laboratory of Rare Earth Resources Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China University of Science and Technology of China Hefei230026China School of chemistry and Chemical Engineering Nanchang UniversityNanchang330031China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou341000China

The deep understanding of 4f-correlated electron motion behavior is experimentally limited due to similar physicochemical properties of rare earth elements(REEs).While the solvent extraction behavior originating from the continuous occupation of 4f electrons along the lanthanide family provides a particular platform to probe the 4f electrons motion behavior and its correlations to their versatile ***,the complexation between REEs and the prototypical extractant of diethyl phosphoric acid(DEP)was substantially studied based on quantum mechanical *** results firstly show that the average bond lengths between Ln and six coordinated oxygen atoms are consistent with lanthanide contraction phenomenon,and gadolinium break effect is also obviously ***,the"tetrad effect"is figured out based on the subtle discrepancy of 4f electrons occupation,namely La-nd,Sm-Eu,Gd-Dy and ***,the main composition is 4f5d6p for La-nd,while the discrepancy is due to the increasing electrons in the 5d shell,while it is 4f5d for *** Gd-Dy,their 4f orbitals accept little electrons and the donating electrons flow into 6s5d subshells due to the half-filled stability and the enhancement of shielding *** electrons donate into 5d6p subshells due to multiply electrons occupation of 4f orbitals for *** detailed analyses obviously clarify the"tetrad effect"along the lanthanide family due to the different variation of 4f orbital *** is expected that these microscopic understandings provide important guidance for the separation of REEs and the design of new extractants.

关键词： Theoretical calculation Rare earths 4f electron Tetrad effect Gadolinium break

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Semitransparent organic photovoltaics enabled by transparent p-type inorganic semiconductor and near-infrared acceptor

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Journal of Energy chemistry 2024年第9期96卷 351-358页

作者： Xue Yan Jiayu Wang Wei He Top Archie Dela Peña Can Zhu Hailin Yu Yingyue Hu Cenqi Yan Shengqiang Ren Xingyu Chen Zhe Wang Jiaying Wu Mingjie Li Jianlong Xia Lei Meng Shirong Lu Dewei Zhao Mikhail Artemyev Yongfang Li Pei Cheng College of Polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065SichuanChina Department of Applied Physics The Hong Kong Polytechnic UniversityKowloonHong Kong 999077China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China College of Materials Science and Engineering&Engineering Research Center of Alternative Energy Materials&Devices Ministry of EducationSichuan UniversityChengdu 610065SichuanChina Department of Material Science and Technology Taizhou UniversityTaizhou 318000ZhejiangChina Advanced Materials Thrust Function HubThe Hong Kong University of Science and Technology(Guangzhou)Guangzhou 511400GuangdongChina State Key Laboratory of Advanced Technology for Materials Science and Processing Center of Smart Materials and DevicesWuhan University of TechnologyWuhan 430070HubeiChina Department of Civil1nd Environmental Engineering The Hong Kong University of Science and TechnologyHong Kong 999077China Research institute for Physical Chemical Problems Belarusian State UniversityMinsk 220006Belarus

Semitransparent organic photovoltaics(STOPVs)have gained wide attention owing to their promising applications in building-integrated photovoltaics,agrivoltaics,and floating *** semiconductors with high charge carrier mobility usually have planar and conjugated structures,thereby showing strong absorption in visible *** this work,a new concept of incorporating transparent inorganic semiconductors is proposed for high-performance ***(I)thiocyanate(CuSCN)is a visible-transparent inorganic semiconductor with an ionization potential of 5.45 eV and high hole *** transparency of CuSCN benefits high average visible transmittance(AVT)of *** energy levels of CuSCN as donor match those of near-infrared small molecule acceptor BTP-eC9,and the formed heterojunction exhibits an ability of exciton *** mobility of CuSCN contributes to a more favorable charge transport channel and suppresses charge *** control STOPVs based on PM6/BTP-eC9 exhibit an AVT of 19.0%with a power conversion efficiency(PCE)of 12.7%.Partial replacement of PM6 with CuSCN leads to a 63%increase in transmittance,resulting in a higher AVT of 30.9%and a comparable PCE of 10.8%.

关键词： Copper(I)thiocyanate Inorganic semiconductor Semitransparent organic photovoltaics Charge dissociation

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Construction of Naphthalenediimide Lanthanide(Ⅲ)-MOFs and Composites Incorporated Electron-Rich Pyrene Derivative as Multifunctional Fluorescence Sensing for Nitro Aromatic Compounds and Aldehydes

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Chinese Journal of chemistry 2024年第3期42卷 283-293页

作者： Rong Huo Ting Zhang Guang Zeng Chen Wang Yong Heng Xing Feng Ying Bai College of chemistry and Chemical Engineering Liaoning Normal UniversityDalianLiaoning116029 China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianLiaoning116023 China

The development of host-guest MOF luminescent composites has attracted considerable attention. However,it is still a challenge to reasonably design large scale conjugated polycarboxylic acids metal-organic framework (MOF) and modulate donor-acceptor interaction. Herein,a series of isostructural 3D porous lanthanide MOF [Ln_(2)(BIndI)0.5(NO_(3))(DMA)(H_(2)O)]∙DMA∙2.5H_(2)O (Ln = La (1),Ce (2),Pr (3) and nd (4);H_(4)BIndI (N,N’-bis(5-isophthalic acid)-1,4,5,8-naphthalenediimide) were synthesized. Considering the electron-deficient performances of Ln-BIndI MOFs,D-A type composites Ln-MOFs (1—4@H_(4)TBAPy) were prepared via the incorporation of electron-rich H_(4)TBAPy (1,3,6,8-tetrakis(p-benzoic acid) pyrene),which more improved the luminescence performance of complexes 1—4 and can be used as fluorescence sensors for the detection of nitro compounds and aldehydes. High sensitivity of 1@H_(4)TBAPy towards pNBA,pNA PNP,DNP,and TNP could be achieved through hydrogen bond interactions between MOF and analytes,as well as the π-π interaction between H_(4)TBAPy and the naphthalene ring of BIndI,thus the fluorescence quenching efficiency of 1@H_(4)TBAPy was better than that of the complex 1. In addition,it is found that 1@H_(4)TBAPy has high selectivity and sensitivity to aromatic aldehyde SA,5-Mesal and HMBA. Such strategy to enhance the emission of ndI based Ln-BIndI MOFs,will open up an avenue to obtain more fluorescent MOFs for sensing.

关键词： Ln-MOF Pyrene molecule NACs Aldehydes Fluorescence sensing Carboxylate ligands Charge transfer Donor-acceptor systems

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Residual levels and health risk assessment of trace metals in Chinese resident diet

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Journal of Environmental Sciences 2024年第2期136卷 451-459页

作者： Yubing Dai Shuai Sun Rong Cao Haijun Zhang Jiping Chen Ningbo Geng CAS Key Laboratory of Separation Science for Analytical chemistry Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Shenyang Pharmaceutical University Shenyang 110016China University of Chinese Academy of Sciences Beijing 100049China

Large-scale metal contamination across the food web is an intractable problem due to increasing pollutant emissions,atmospheric transport,and dry and wet deposition of *** present study focus on several trace metals that are rarely studied but have special toxicity,including tin(Sn),antimony(Sb),gold(Au),hafnium(Hf),palladium(Pd),platinum(Pt),ruthenium(Ru),tellurium(Te)and iridium(Ir).We investigated trace metals residues and distribution characteristics,and further evaluated the potential health risks from major daily food intakes in 33 cities in ***,Sb,Ir,Hf,and Au were frequently detected in food samples with the concentrations ranged from nd(not detected)to 24.78μg/kg ww(wet weight).Eggs exhibited the highest residual level of all detected metals(13.70±14.70μg/kg ww in sum),while the lowest concentrations were observed in vegetables(0.53±0.17μg/kg ww in sum).Sn accounting for more than 50%of the total trace metals concentration in both terrestrial and aquatic animal origin *** terrestrial plant origin foods,Sn and Ir were the most abundant *** and Au were the most abundant elements in egg *** addition,Sb and Ir showed a clear trophic dilution effect in terrestrial environments,while in aquatic ecosystems,Sn,Hf,and Au exhibited obvious trophic amplification *** calculated average estimated daily intake(EDI)via food consumption in five regions of China was 0.09μg/(kg·day),implying the health risk of aforementioned elements was acceptable.

关键词： Trace metals Accumulation characteristics Dietary exposure Estimated daily intake(EDI)

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Phytoremediation Strategies for Heavy Metal Contamination: A Review on Sustainable Approach for Environmental Restoration

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Journal of Environmental Protection 2024年第4期15卷 450-474页

作者： Mariam Salifu Matthew Abu John Murtala Abubakar Ibukunoluwa Abimbola Bankole Nneka Damola Ajayi Olawumi Amusan Department of chemistry and Biochemistry University of Mississippi Olemiss MS USA Department of Biochemistry Ahmadu Bello University Zaria Nigeria Department of Plant Pathology North Dakota State University Fargo ND USA Directorate of Research and Development Nigerian Institute of Leather and Science Technology (NILEST) Zaria Nigeria Department of chemistry University of Akron Akron OH USA

Current globalization trends and important breakthroughs globally need a complete study of heavy metal contamination, its causes, its impacts on human and environmental health, and different remediation strategies. Heavy metal pollution is mostly produced by urbanization and industry, which threatens ecosystems and human health. Herein, we discuss a sustainable environmental restoration strategy employing phytoremediation for heavy metal pollution, the carcinogenic, mutagenic, and cytotoxic effects of heavy metals such as cadmium, copper, mercury, selenium, zinc, arsenic, chromium, lead, nickel, and silver, which may be fatal. Phytoremediation, which was prioritized, uses plants to remove, accumulate, and depollute pollutants. This eco-friendly method may safely collect, accumulate, and detoxify toxins using plants, making it popular. This study covers phytostabilization, phytodegradation, rhizodegradation, phytoextraction, phytovolatilization, and rhizofiltration. A phytoremediation process’s efficiency in varied environmental circumstances depends on these components’ complex interplay. This paper also introduces developing phytoremediation approaches including microbe-assisted, chemical-assisted, and organic or bio-char use. These advancements attempt to overcome conventional phytoremediation’s limitations, such as limited suitable plant species, location problems, and sluggish remediation. Current research includes machine learning techniques and computer modeling, biostimulation, genetic engineering, bioaugmentation, and hybrid remediation. These front-line solutions show that phytoremediation research is developing towards transdisciplinary efficiency enhancement. We acknowledge phytoremediation’s promise but also its drawbacks, such as site-specific variables, biomass buildup, and sluggish remediation, as well as ongoing research to address them. In conclusion, heavy metal pollution threatens the ecology and public health and must be reduced. Phytoremediation

关键词： Phytoremediation Heavy-Metal Contamination Sustainability Restoration

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MnO_(2)-coated nanodiamond-driven photodynamic therapy for enhanced antitumor effect by addressing hypoxia and glutathione depletion

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Particuology 2024年第9期92卷 305-315页

作者： Jicheng Cui Dongmei Zhang Hui Qiao Zeyu Yan Wenxia Zhang Yingqi Li Key Laboratory of Chemical Biology and Molecular Engineering of Ministry of Education Institute of Molecular ScienceShanxi UniversityTaiyuan030006China Taiyuan Central Hospital Taiyuan030009China School of chemistry and Chemical Engineering Shanxi UniversityTaiyuan030006China

The generation of reactive oxygen species(ROS)at the tumor site to induce destruction is emerging as a novel strategy for cancer treatment,which involves photodynamic therapy(PDT).Nevertheless,tumors typically create a hypoxic environment and are equipped with an endogenous antioxidant defense system that could potentially impede the efficiency of the therapeutic *** overcome these drawbacks,herein,a tumor microenvironment-responsive the nd-PAA-CD-Ce6@MnO_(2)(NPCC@M)delivery system was fabricated by disulfide bond coupling chlorin e6(Ce6)to nanodiamond(nd)and further wrapped by MnO_(2)nanosheets to facilitate *** use of disulfide bond not only stabilizes Ce6 in the blood circulation to prevent premature leakage,but also destroys the antioxidant barrier of overexpressed glutathione(GSH)in tumor ***,the outer MnO_(2)was rapidly degraded by the endogenous hydrogen peroxide(H_(2)O_(2))in the acidic pH and GSH within the tumor cells,which leads to an abundance of O_(2)and while increases the level of 1O_(2)under laser *** results eventually broke the redox homeostasis and attenuate hypoxia,thereby inducing apoptosis and necrosis of tumor *** in vitro and in vivo biological effect has revealed a good biosafety profile and a high tumor suppression *** a novel nd-based system with tumor microenvironment-modulating capability to elevate oxygen content and promote GSH consumption in tumor cells opens new opportunities for enhanced ROS treatment paradigms.

关键词： Nanodiamond Photodynamic Chlorin e6 MnO_(2) Tumor suppression

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