Theoretical Insights into Modification of Nitrogen-Donor Ligands to Improve Performance on Am(III)/Eu(III) Separation
作者：
Chen, Yan-Mei;Wang, Cong-Zhi;Wu, Qun-Yan;Lan, Jian-Hui;Chai, Zhi-Fang;...
期刊：
INORGANIC CHEMISTRY ,2020年59(5):3221-3231 ISSN：0020-1669
通讯作者：
Nie, Chang-Ming;Shi, Wei-Qun
作者机构：
[Nie, Chang-Ming; Chen, Yan-Mei] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Chen, Yan-Mei; Wu, Qun-Yan; Chai, Zhi-Fang; Wang, Cong-Zhi; Lan, Jian-Hui; Shi, Wei-Qun] Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.;[Chai, Zhi-Fang] Chinese Acad Sci, Ningbo Inst Ind Technol, Engn Lab Adv Energy Mat, Ningbo 315201, Zhejiang, Peoples R China.
通讯机构：
[Nie, Chang-Ming] U;[Shi, Wei-Qun] C;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.
摘要：
Nitrogen-donor ligands have been considered to be promising agents for separating trivalent actinides (An(III)) from lanthanides (Ln(III)). Thereinto, how to decorate these ligands for better extraction performance is urgent to design "perfect" separating extractants. In this work, we systematically explored a series of heterocyclic N-donor ligands (L1 = dipyridazino[4,3-c:3′,4′-h]acridine, L2 = dipyridazino[3,4-a:4′,3′-j]phenazine, L3 = 2,6-di(cinnolin-3-yl)pyridine)), as well as their substituted derivatives, and compared their extraction and complexation ability toward An(III) and Ln(III) ions by using quasi-relativistic density functional theory (DFT). We found that the pyridazine N atoms probably play a notable role in electron donation to metal cations by molecular orbital (MO) and bond order analyses. Besides, the calculated results clearly verified that these N-donor ligands possess higher coordination affinity toward Am(III) over Eu(III). The rigid ligands (L1 and L2) exhibit higher selective abilities for the Am(III)/Eu(III) separation compared with that of the flexible ligand (L3). For each ligand, the 1:2 (metal/ligand) extraction reaction is predicted to be most probable in the separation process. The introduction of an alkyl group on the lateral chain or an electron-donating group on the main chain gives rise to a better extraction performance of the ligands, and the CyMe4 or MeO substituted ligands show higher extraction and separation ability. Simultaneous introduction of CyMe4 and MeO groups can enhance the extraction ability of the ligand to metal ions, but the separating ability depends on the differences of the extraction capacity of An(III) and Ln(III). This work can help to gain a more in-depth understanding the selectivity differences of similar N-donor ligands and provide more theoretical insights into the design of novel extractants for An(III)/Ln(III) separation. Copyright © 2020 American Chemical Society.
语种：
英文
展开
Corrigendum to “Sustainable utilization of chlorine via converting HCl to Cl2 over a robust copper catalyst” [Mol. Catal. 492 (2020) 110977–110985]
作者：
Tian, Xin;Wang, Shuai;Wang, Zhou-jun;Wang, Hongqing;Zhou, Yonghua* ;...
期刊：
Molecular Catalysis ,2020年493:111083 ISSN：2468-8231
通讯作者：
Zhou, Yonghua;Zhong, Hong;Mao, Yu
作者机构：
[Zhou, YH; Zhou, Yonghua; Zhong, Hong; Tian, Xin; Wang, Shuai] Cent South Univ, Coll Chem & Chem Engn, Hunan Prov Key Lab Efficient & Clean Utilizat Man, Changsha 410083, Peoples R China.;[Wang, Hongqing; Mao, Yu] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.;[Wang, Zhou-jun] Beijing Univ Chem Technol, Beijing Key Lab Energy Environm Catalysis, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China.
通讯机构：
[Zhou, YH; Zhong, H] C;[Mao, Yu] U;Cent South Univ, Coll Chem & Chem Engn, Hunan Prov Key Lab Efficient & Clean Utilizat Man, Changsha 410083, Peoples R China.;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.
语种：
英文
展开
Theoretical investigation into coordination and selectivity of uranyl-unilateral benzotriazole salophens (X = O/S) for R/S-triadimefons
作者：
Sun, Wei-Zhen;Dai, Lin-Lin;Kong, Xiang-He;Mao, Yu;Wu, Zhi-Lin;...
期刊：
Applied Organometallic Chemistry ,2020年34(4):e5486- ISSN：0268-2605
通讯作者：
Nie, Chang-Ming
作者机构：
[Liao, Li-Fu; Nie, Chang-Ming; Sun, Wei-Zhen; Wu, Zhi-Lin; Xiao, Xi-Lin; Kong, Xiang-He; Dai, Lin-Lin; Mao, Yu] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Liao, Li-Fu; Nie, Chang-Ming; Sun, Wei-Zhen; Xiao, Xi-Lin; Dai, Lin-Lin] Key Lab Hunan Prov Design & Applicat Nat Actinide, Hengyang 421001, Peoples R China.
通讯机构：
[Nie, Chang-Ming] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
关键词：
coordination;enantioselectivity recognition;R/S-triadimefons;uranyl-unilateral benzotriazole salophen
摘要：
The design of new uranyl-ligands (uranyl-Ls) is of great significance for the separation and utilization of uranium. In this paper, the triazole group was introduced into uranyl-salophen (uranyl-S) to form new asymmetric uranyl-unilateral benzotriazole salophen (uranyl-UBS); we further replaced two oxygen atoms of uranyl-UBS with two sulfur atoms to generate uranyl-unilateral benzotriazole thio-salophen (uranyl-UBTS) as a new receptor. Then, we comprehensively explored coordination models of uranyl-UBS and uranyl-UBTS with R/S-triadimefons (R/S-TDFs) enantiomers as the guests using density functional theory calculations at the B3LYP//RECP/6-311G** level; we then investigated enantioselectivity recognition of the new receptors to the guests R/S-TDFs. The results indicated that the uranium atoms of the receptors uranyl-S, uranyl-UBS and uranyl-UBTS could coordinate with the carbonyl oxygens in guests R/S-TDFs to form complexes of guest-receptors R/S-TDFs-uranyl-Ls that exhibited two stable V-shaped structures with quite different properties. It was found that the coordination ability to the guests R/S-TDFs is uranyl-UBTS > uranyl-UBS > uranyl-S, while the enantioselectivity for the guests is uranyl-UBTS > uranyl-S > uranyl-UBS and, when the receptor is the same, R-TDF has stronger coordination ability than S-TDF. These results provide information and theoretical supports for the experiments of asymmetric uranyl-UBS with R/S-TDFs, and produce a reference for further exploring the coordination characteristics of asymmetric uranyl-salophen with the triazole derivatives. © 2020 John Wiley & Sons, Ltd.
语种：
英文
展开
Visible-light-initiated malic acid-promoted cascade coupling/ cyclization of aromatic amines and KSCN to 2-aminobenzothiazoles without photocatalyst
作者：
He, Wei-Bao;Gao, Lan-Qing;Chen, Xin-Jie;Wu, Zhi-Lin;Huang, Ying;...
期刊：
中国化学快报：英文版 ,2020年31(7):1895-1898 ISSN：1001-8417
通讯作者：
Xu, Xin-Hua;He, Wei-Min
作者机构：
[He, Wei-Bao; Gao, Lan-Qing; Xu, Xin-Hua] Hunan Univ, Dept Chem, Changsha 410082, Hunan, Peoples R China.;[He, Wei-Min; Huang, Ying; Cao, Zhong] Changsha Univ Sci & Technol, Hunan Prov Key Lab Mat Protect Elect Power & Tran, Changsha 410114, Peoples R China.;[Chen, Xin-Jie] Hunan Univ Sci & Technol, Sch Chem & Chem Engn, Xiangtan 411201, Peoples R China.;[Wu, Zhi-Lin] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
通讯机构：
[Xu, Xin-Hua] H;[He, Wei-Min] C;Hunan Univ, Dept Chem, Changsha 410082, Hunan, Peoples R China.;Changsha Univ Sci & Technol, Hunan Prov Key Lab Mat Protect Elect Power & Tran, Changsha 410114, Peoples R China.
关键词：
Air;Photocatalysis;Cascade reaction;Photocatalyst-free;2-Aminobenzothiazoles
摘要：
By using ambient air as the oxidant and malic acid as the promoter, a practical method for the preparation of 2-aminobenzothiazoles through visible-light-initiated cascade reaction of aromatic amines and KSCN in eco-friendly bis(methoxypropy)ether under metal-, hazardous additive-, photocatalyst-free conditions was established.
语种：
英文
展开
Metal-free synthesis of 1,2,3-benzotriazines
作者：
Chen, Jin-Yang;Lin, Ying-Wu;He, Wei-Min*
期刊：
中国化学快报：英文版 ,2020年31(12):2989-2990 ISSN：1001-8417
通讯作者：
He, Wei-Min
作者机构：
[Chen, Jin-Yang] Yangtze Normal Univ, Coll Chem & Chem Engn, Chongqing 408000, Peoples R China.;[He, Wei-Min] Changsha Univ Sci & Technol, Hunan Prov Key Lab Mat Protect Elect Power & Tran, Changsha 410114, Peoples R China.;[Chen, Jin-Yang] Hunan Univ Sci & Technol, Sch Chem & Chem Engn, Xiangtan 411201, Peoples R China.;[Lin, Ying-Wu] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
通讯机构：
[He, Wei-Min] C;Changsha Univ Sci & Technol, Hunan Prov Key Lab Mat Protect Elect Power & Tran, Changsha 410114, Peoples R China.
关键词：
Iodine;Metal-free;Rearrangement reaction;1,2,3-Benzotriazines
摘要：
The recent molecular iodine catalyzed [1,2]-rearrangement of aryl amines and 3-amino-1H-indazolesfor the synthesis of 1,2,3-benzotriazines is highlighted.
语种：
英文
展开
Complexation and enantioselectivity of sulfur/selenium-substituted uranyl-salophens with R/S-chiral lactone for RRS/SSR-3, 5-Dimethyl-2-(3-fluorophenyl)-2-morpholinols
作者：
Dai Linlin;Nie Changming* ;Sun Weizhen;Xiao Yang;Mao Yu;...
期刊：
Journal of Radioanalytical and Nuclear Chemistry ,2020年324(3):993-1006 ISSN：0236-5731
通讯作者：
Nie Changming
作者机构：
[Nie Changming; Sun Weizhen; Xiao Xilin; Xiao Yang; Liao Lifu; Wu Zhilin; Dai Linlin; Mao Yu] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.;[Nie Changming; Sun Weizhen; Xiao Xilin; Xiao Yang; Liao Lifu; Wu Zhilin; Dai Linlin; Mao Yu] Key Lab Hunan Prov Design & Applicat Nat Actinide, Hengyang 421001, Hunan, Peoples R China.
通讯机构：
[Nie Changming] U;[Nie Changming] K;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.;Key Lab Hunan Prov Design & Applicat Nat Actinide, Hengyang 421001, Hunan, Peoples R China.
关键词：
Sulfur/selenium-substituted uranyl-salophens;RRS/SSR-3,5-dimethyl-2-(3-fluorophenyl) -2-morpholinols;Coordination;Enantioselectivity;Density functional theory
摘要：
In order to explore the enantioselectivity of uranyl-salophens to chiral molecules, the newly designed receptors of ?-type configuration sulfur/selenium-substituted uranyl-salophens with R/S-chiral delta-lactone were used to selectively coordinate and recognize a pair of enantiomers of RRS/SSR-3,5-dimethyl-2-(3-fluorophenyl)-2-morpholinols as guests based on the density functional theory calculations. The results indicated that the substituent effects of R/S-asymmetry sulfur/selenium-substituted uranyl-salophens significantly affected the structures and properties of coordination compounds, and the R-type receptors have higher enantioselectivity for the chiral guests than the S-type receptors both in vacuum and in solvents water, acetone and toluene except the R/S-selenium-substituted uranyl-salophen in water.
语种：
英文
展开
Understanding the Promotion Effect of Mn on CuO/Al2O3 for Catalyzed HCl Oxidation to Cl-2
作者：
Tian, Xin;Wang, Shuai;Wang, Zhou-jun;Wang, Hongqing;Zhou, Yonghua* ;...
期刊：
ChemCatChem ,2020年12(12):3240-3248 ISSN：1867-3880
通讯作者：
Zhou, Yonghua;Zhong, Hong;Mao, Yu
作者机构：
[Zhou, YH; Zhou, Yonghua; Zhong, Hong; Tian, Xin; Wang, Shuai] Cent South Univ, Hunan Prov Key Lab Efficient & Clean Utilizat Man, Coll Chem & Chem Engn, Changsha 410083, Peoples R China.;[Wang, Zhou-jun] Beijing Univ Chem Technol, Beijing Key Lab Energy Environm Catalysis, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China.;[Wang, Hongqing; Mao, Yu] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.
通讯机构：
[Zhou, YH; Zhong, H] C;[Mao, Yu] U;Cent South Univ, Hunan Prov Key Lab Efficient & Clean Utilizat Man, Coll Chem & Chem Engn, Changsha 410083, Peoples R China.;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.
关键词：
Chlorine recycling;HCl oxidation;Cl-2 evolution;CuO-MnOx;Al2O3
摘要：
HCl oxidation to Cl2 catalyzed by Cu-based catalysis is an effective way to realize the sustainable development of chlorine-involved industries. In this work, we investigated the role of promoter Mn on CuO/Al2O3 in HCl oxidation to Cl2. The X-ray diffraction (XRD), scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM) and H2-temperature programmed reduction (H2-TPR) characterizations suggested that Cu could be well dispersed in the MnOx lattice and hindered the reduction of CuO due to their strong interaction. The catalyst showed an unprecedentedly stable HCl conversion rate (xHCl) of about 79 % with space time yield (STY) of 2.14 gCl2 gcat−1 h−1 in a 1000 hours test. The results of reaction kinetics suggested that the deep chlorination of catalysts was significantly inhibited under the reaction atmosphere. Density functional theory (DFT) calculations proved that the binding energy of O on CuO−MnOx/Al2O3 ternary system was significantly strengthened that overwhelmed Cl, with ΔGO (−4.12 eV) ≪ ΔGCl (-1.75 eV), which greatly inhibited the poisoning of reactive sites by Cl*. A good correlation between experimental observations and theoretical calculations was established in this work. © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
语种：
英文
展开
Preparation of Uniform Highly Dispersed Mg-Al-LDHs and Their Adsorption Performance for Chloride Ions
作者：
Yang Pengfei* ;Xu Yuanxin;Yin Na;Ai Yong
期刊：
Industrial & Engineering Chemistry Research ,2020年59(22):10697-10704 ISSN：0888-5885
通讯作者：
Yang Pengfei
作者机构：
[Xu Yuanxin; Ai Yong; Yang Pengfei; Yin Na] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Yang Pengfei] Univ South China, Hunan Prov Engn Res Ctr Radioact Control Technol, Hengyang 421001, Peoples R China.;[Yang Pengfei] Univ South China, Hunan Prov Engn Technol Res Ctr Uranium Tailings, Hengyang 421001, Peoples R China.;[Xu Yuanxin; Ai Yong; Yang Pengfei; Yin Na] Hunan Key Lab Design & Applicat Actinide Complexe, Hengyang 421001, Peoples R China.
通讯机构：
[Yang Pengfei] U;[Yang Pengfei] H;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;Univ South China, Hunan Prov Engn Res Ctr Radioact Control Technol, Hengyang 421001, Peoples R China.;Univ South China, Hunan Prov Engn Technol Res Ctr Uranium Tailings, Hengyang 421001, Peoples R China.
摘要：
Two-dimensional flaky magnesium-aluminum hydrotalcite (Mg-Al-LDHs) with uniform particle size distribution and high dispersion was prepared using a supergravity rotating bed. The samples were characterized by scanning electron microscopy, X-ray diffraction, Brunauer-Emmett-Teller, particle size distribution analyzer (PSDA), and so forth. The morphology and particle size distribution of the Mg-Al-LDHs that were prepared by traditional hydrothermal synthesis (T-Mg-Al-LDHs) and the supergravity rotating bed (S-Mg-Al-LDHs) were compared. The adsorption performance of these Mg-Al-LDHs prepared by two methods and their calcined products (T-Mg-Al-LDOs and S-Mg-Al-LDOs) for chloride ions was also investigated. The results showed that the dispersed uniform two-dimensional Mg-Al-LDHs could be prepared using the supergravity rotating bed system, which had regularly and uniformly distributed morphology and can easily form a cross between support structures. The specific surface area of S-Mg-Al-LDHs was 142.623 m2/g, which is much larger than that of T-Mg-Al-LDHs (115.311 m2/g). The saturation absorbance of S-Mg-Al-LDHs and S-Mg-Al-LDOs toward chloride ions is 34.82 and 108.06 mg/g, respectively; the saturation absorbance of T-Mg-Al-LDHs and T-Mg-Al-LDOs toward chloride ions is 24.72 and 96.07 mg/g, respectively, which shows that S-Mg-Al-LDHs and S-Mg-Al-LDOs exhibit excellent adsorption performance. The adsorption kinetics and adsorption isotherms of S-Mg-Al-LDOs can be well-described by the pseudo-second-order kinetic and Langmuir isotherm. Copyright © 2020 American Chemical Society.
语种：
英文
展开
A Porous Aromatic Framework Functionalized with Luminescent Iridium(III) Organometallic Complexes for Turn-On Sensing of 99TcO4 -
作者：
Xu, Dongyang;Chen, Long;Dai, Xing;Li, Baoyu;Wang, Yaxing;...
期刊：
ACS Applied Materials & Interfaces ,2020年12(13):15288-15297 ISSN：1944-8244
通讯作者：
Liu, Yong;Peng, Guowen;Wang, Shuao
作者机构：
[Liu, Yong; Peng, Guowen; Xu, Dongyang] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Liu, Yong; Peng, Guowen; Xu, Dongyang] Univ South China, Sch Resource Environm & Safety Engn, Hengyang 421001, Peoples R China.;[Tao, Yi; Dai, Xing; Chai, Zhifang; Wang, Yanlong; Wang, Shuao; Wang, Yaxing; Zhou, Ruhong; Li, Baoyu; Li, Jie; Chen, Long] Soochow Univ, Sch Radiol & Interdisciplinary Sci RAD X, State Key Lab Radiat Med & Protect, Suzhou 215123, Peoples R China.;[Tao, Yi; Dai, Xing; Chai, Zhifang; Wang, Yanlong; Wang, Shuao; Wang, Yaxing; Zhou, Ruhong; Li, Baoyu; Li, Jie; Chen, Long] Soochow Univ, Collaborat Innovat Ctr Radiat Med, Jiangsu Higher Educ Inst, Suzhou 215123, Peoples R China.;[Liu, Wei] Yantai Univ, Sch Environm & Mat Engn, Yantai 264005, Peoples R China.
通讯机构：
[Liu, Y; Peng, GW] U;[Wang, Shuao] S;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;Univ South China, Sch Resource Environm & Safety Engn, Hengyang 421001, Peoples R China.;Soochow Univ, Sch Radiol & Interdisciplinary Sci RAD X, State Key Lab Radiat Med & Protect, Suzhou 215123, Peoples R China.
关键词：
iridium complex;rhenium;fluorescence detection;porous aromatic frameworks;technetium;selectivity;turn-on manner
摘要：
Contamination of 99TcO4 -, a problematic radioactive anion in the nuclear fuel cycle, in groundwater has been observed in a series of legacy nuclear sites, representing a notable radiation hazard and environmental concern. The development of convenient, rapid, and sensitive detection methods is therefore critical for radioactivity control and remediation tasks. Traditional detection methods suffer from clear demerits of either the presence of large interference from coexisting radioactive species (e.g., radioactivity counting methods) or the requirement of extensive instrumentation and analysis procedure (e.g., mass spectrometry). Here, we constructed a luminescent iridium(III) organometallic complex (Ir(ppy)2(bpy)+ ppy = 2-phenylpyridine, bpy = 2,2′-bipyridine)-grafted porous aromatic framework (Ir-PAF) for the first time, which can be utilized for efficient, facile, and selective detection of trace ReO4 -/TcO4 - in aqueous solutions. Importantly, the luminescence intensity of Ir-PAF is greatly enhanced in the presence of ReO4 -/TcO4 -, giving rise to a distinct turn-on sensor with the detection limit of 556.9 μg/L. Such a superior detection capability originates from the highly selective and strong interaction between ReO4 -/TcO4 - and Ir(ppy)2(bpy)+, leading to an efficient pre-enrichment of ReO4 -/TcO4 - during analysis and subsequently a much weaker nonradiative decay of the luminescence of Ir(ppy)2(bpy)+, as illustrated by density functional theory (DFT) calculation as well as quantum yield and fluorescence lifetime measurements. Successful quantification of trace ReO4 - in simulated Hanford low-activity waste (LAW) solution containing large excess of Cl-, NO3 -, and NO2 - was demonstrated, highlighting the bright future of luminescent PAFs in the area of chemical sensing. Copyright © 2020 American Chemical Society.
语种：
英文
展开
Copper(i)-catalyzed intermolecular cyanoarylation of alkenes: convenient access to α-alkylated arylacetonitriles
作者：
Chen, Xin-Jie;Gui, Qing-Wen;Yi, Rongnan;Yu, Xianyong* ;Wu, Zhi-Lin;...
期刊：
Organic & Biomolecular Chemistry ,2020年18(27):5234-5237 ISSN：1477-0520
通讯作者：
Yu, Xianyong;He, Wei-Min
作者机构：
[Yu, Xianyong; Chen, Xin-Jie] Hunan Univ Sci & Technol, Minist Educ, Sch Chem & Chem Engn, Key Lab Theoret Organ Chem & Funct Mol, Xiangtan 411201, Peoples R China.;[Yi, Rongnan] Hunan Univ, Dept Chem, Changsha 410082, Hunan, Peoples R China.;[Gui, Qing-Wen; He, Wei-Min; Huang, Ying; Cao, Zhong] Changsha Univ Sci & Technol, Hunan Prov Key Lab Mat Protect Elect Power & Rans, Changsha 410114, Peoples R China.;[Wu, Zhi-Lin] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
通讯机构：
[Yu, Xianyong] H;[He, Wei-Min] C;Hunan Univ Sci & Technol, Minist Educ, Sch Chem & Chem Engn, Key Lab Theoret Organ Chem & Funct Mol, Xiangtan 411201, Peoples R China.;Changsha Univ Sci & Technol, Hunan Prov Key Lab Mat Protect Elect Power & Rans, Changsha 410114, Peoples R China.
关键词：
Copper(I)-catalyzed;intermolecular cyanoarylation;α-alkylated arylacetonitriles
摘要：
A novel Cu(I)-catalyzed intermolecular cyanoarylation of alkenes with diaryliodonium salts as a radical arylating reagent and tetra-butylammonium cyanide as an electrophilic cyanating reagent was established. A broad range of α-alkylated arylacetonitriles were efficiently constructed in good to excellent yields under base- and oxidant-free and mild conditions.
语种：
英文
展开
Cholesterol in LDL receptor recycling and degradation
作者：
Yang, Hui-xian;Zhang, Min;Long, Shi-yin;Tuo, Qin-hui;Tian, Ying;...
期刊：
Clinica Chimica Acta ,2020年500:81-86 ISSN：0009-8981
通讯作者：
Zhang, Cai-ping;Liao, Duan-fang
作者机构：
[Yang, Hui-xian] Univ South China, Med Coll, Inst Cardiovasc Dis, 28 Changsheng Rd, Hengyang 421001, Hunan, Peoples R China.;[Liao, Duan-fang; Chen, Jian-xiong; Tuo, Qin-hui] Hunan Univ Chinese Med, Div Stem Cell Regulat & Applicat, State Key Lab Chinese Med Powder & Med Innovat Hu, 300 Xueshi Rd, Changsha 410208, Hunan, Peoples R China.;[Tian, Ying; Long, Shi-yin; Yang, Hui-xian; Zhang, Cai-ping; Zhang, Min; Liao, DF] Univ South China, Med Coll, Dept Biochem & Mol Biol, 28 W Changsheng Rd, Hengyang 421001, Hunan, Peoples R China.;[Chen, Jian-xiong] Univ Mississippi, Med Ctr, Dept Pharmacol & Toxicol, University, MS 38677 USA.
通讯机构：
[Zhang, CP; Liao, DF] U;Univ South China, Med Coll, Dept Biochem & Mol Biol, 28 W Changsheng Rd, Hengyang 421001, Hunan, Peoples R China.
关键词：
Dyslipidemia;IDOL;LDL-C;LDLR;PCSK9;SREBP2
摘要：
The SREBP2/LDLR pathway is sensitive to cholesterol content in the endoplasmic reticulum (ER), while membrane low-density lipoprotein receptor (LDLR) is influenced by sterol response element binding protein 2 (SREBP2), pro-protein convertase subtilisin/kexin type 9 (PCSK9) and inducible degrader of LDLR (IDOL). LDL-C, one of the risk factors in cardiovascular disease, is cleared through endocytosis recycling of LDLR. Therefore, we propose that a balance between LDLR endocytosis recycling and PCSK9-mediated and IDOL-mediated lysosomal LDLR degradation is responsible for cholesterol homeostasis in the ER. For statins that decrease serum LDL-C levels via cholesterol synthesis inhibition, the mechanism by which the statins increase the membrane LDLR may be regulated by cholesterol homeostasis in the ER.
语种：
英文
展开
Ligands modulated the variable binuclear Cd2-SBUs and structures of four layered coordination frameworks
作者：
Wang, Mengdie;Zhang, Jian;Sun, Yunkai* ;Wei, Jing* ;Tan, Chunhong;...
期刊：
CrystEngComm ,2020年22(23):3965-3974 ISSN：1466-8033
通讯作者：
Sun, Yunkai;Wang, Xiao-Feng;Wei, Jing
作者机构：
[Wang, Mengdie; Sun, Yunkai; Wang, Xiao-Feng; Zhang, Jian; Tan, Chunhong] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Sun, Yunkai; Wang, Xiao-Feng] Univ South China, Hunan Prov Engn Res Ctr Radioact Control Technol, Hengyang 421001, Peoples R China.;[Wei, Jing] Chinese Acad Sci, Fujian Inst Res Struct Matter, Fuzhou 350002, Peoples R China.
通讯机构：
[Sun, YK; Wang, XF] U;[Wei, Jing] C;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;Univ South China, Hunan Prov Engn Res Ctr Radioact Control Technol, Hengyang 421001, Peoples R China.;Chinese Acad Sci, Fujian Inst Res Struct Matter, Fuzhou 350002, Peoples R China.
摘要：
Four layered coordination polymers, namely, [Cd2(fuma)2(phen)2] (1), [Cd2(BDC)2(phen)2]·2DMF (2), [Cd2(NDC)2(phen)2]·0.5H2O (3), and [Cd2(NDC)2(bipy)2]·2DMF (4) have been synthesized under solvo-thermal conditions (fuma = fumaric acid, H2BDC = 1,4-benzenedicarboxylic acid, H2NDC = 1,4-naphthalenedicarboxylic acid, phen = 1,10-phenanthroline, bipy = 2,2′-bipyridine), which are composed of asymmetric/symmetric binuclear Cd2(RCOO)4(phen)2or Cd2(RCOO)4(bipy)2clusters as secondary building units (SBUs) linked by fuma2−, BDC2−, and NDC2−. Owing to the different steric hindrances of the di-carboxylates, the variation in Cd2(RCOO)4(phen)2SBUs showed an intriguing structural modulation, which was due to the carboxylates adopting dissimilar coordination fashions, while both the terminal phen co-ligands changed fromcis- totrans-position. Thus, this further induced twist angles (three neighbouring SBUs connected by the di-carboxylic acid) in the single layer of1-3varying from 109.7°, 132.3° to 180° (viewed along thea-axis) and correspondingly, three Cd2-SBU-based CPs exhibited structural evolution from an undulating to a lamellar layer. When the co-ligand bipy replaced phen,4also formed a lamellar layer framework based on the paddle-wheel Cd2(RCOO)4(bipy)2SBUs with bipy perpendicular to the layer rather than the slanted phen in3. The luminescence properties of1-4have also been explored, and their fluorescence emission mechanism of ligand-to-ligand charge transfer (LLCT) are confirmed by the time-dependent density functional theory (TDDFT) calculations. © The Royal Society of Chemistry 2020.
语种：
英文
展开
6π-Electrocyclization in water: microwave-assisted synthesis of polyheterocyclic-fused quinoline-2-thiones
作者：
Li, Xiao-Yun;Liu, Yan;Chen, Xiao-Lan* ;Lu, Xin-Yuan;Liang, Xing-Xing;...
期刊：
Green Chemistry ,2020年22(14):4445-4449 ISSN：1463-9262
通讯作者：
Chen, Xiao-Lan;Yu, Bing
作者机构：
[Li, Xiao-Yun; Liu, Yan; Chen, Xiao-Lan; Liang, Xing-Xing; Chen, XL; Yu, B; Qu, Ling-Bo; Lu, Xin-Yuan; Yu, Bing; Zhu, Shan-Shan] Zhengzhou Univ, Green Catalysis Ctr, Coll Chem, Zhengzhou 450001, Henan, Peoples R China.;[Liu, Yan] Xinyang Agr & Forestry Univ, Coll Biol & Pharmaceut Engn, Xinyang 464000, Peoples R China.;[Wei, Chuan-Wan] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
通讯机构：
[Chen, XL; Yu, B] Z;Zhengzhou Univ, Green Catalysis Ctr, Coll Chem, Zhengzhou 450001, Henan, Peoples R China.
摘要：
Microwave-assisted synthesis of polyheterocyclic-fused quinoline-2-thiones through the annulation of ortho-heteroaryl anilines and CS2 was realized in water without using any catalysts and additives. The desired products were obtained in high yields through simple filtration. A remarkable E-factor of 0.45 and an EcoScale score of 85.5 were obtained. © 2020 The Royal Society of Chemistry.
语种：
英文
展开
Bioinspired design of an artificial peroxidase: Introducing key residues of native peroxidases into F43Y myoglobin with a Tyr-heme cross-link
作者：
Liao, Fei;Xu, Jia-Kun;Luo, Jie;Gao, Shu-Qin;Wang, Xiao-Juan;...
期刊：
DALTON TRANSACTIONS ,2020年49(16):5029-5033 ISSN：1477-9226
通讯作者：
Lin, Ying-Wu
作者机构：
[Luo, Jie; Liao, Fei; Lin, Ying-Wu] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Xu, Jia-Kun; Wang, Xiao-Juan] Chinese Acad Fishery Sci, Minist Agr & Rural Affairs, Yellow Sea Fisheries Res Inst, Key Lab Sustainable Dev Polar Fisheries,Lab Marin, Qingdao 266071, Peoples R China.;[Gao, Shu-Qin; Lin, Ying-Wu] Univ South China, Lab Prot Struct & Funct, Hengyang 421001, Peoples R China.
通讯机构：
[Lin, Ying-Wu] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;Univ South China, Lab Prot Struct & Funct, Hengyang 421001, Peoples R China.
摘要：
Inspired by the structural features of native peroxidases, an artificial peroxidase was rationally designed using F43Y myoglobin with a Tyr-heme cross-link by further introduction of key residues, including both a distal Arg and a Trp close to the heme group, which exhibits an enhanced peroxidase activity similar to the most efficient native horseradish peroxidase. This study provides a simple approach for design of artificial heme enzymes by the combination of catalytic elements of native enzymes with the post-translational modifications of heme proteins. This journal is © The Royal Society of Chemistry.
语种：
英文
展开
The importance of Asn52 in the structure-function relationship of human cytochrome c
作者：
Lou, Dan;Liu, Xi-Chun;Wang, Xiao-Juan;Gao, Shu-Qin;Wen, Ge-Bo;...
期刊：
RSC Advances ,2020年10(73):44768-44772 ISSN：2046-2069
通讯作者：
Lin, Ying-Wu
作者机构：
[Liu, Xi-Chun; Lou, Dan; Lin, Ying-Wu; Wang, Xiao-Juan] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Gao, Shu-Qin; Wen, Ge-Bo; Lin, Ying-Wu] Univ South China, Lab Prot Struct & Funct, Med Sch, Hengyang 421001, Peoples R China.
通讯机构：
[Lin, Ying-Wu] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;Univ South China, Lab Prot Struct & Funct, Med Sch, Hengyang 421001, Peoples R China.
摘要：
The function of the highly conserved residue Asn52 in human cytochrome c (H-Cyt c) is not fully understood. Herein, we show that the naturally occurring variant N52S H-Cyt c has a perturbed secondary structure, with a small fraction of high-spin species. Remarkably, it exhibits an enhanced peroxidase activity by 3-8-fold at neutral pH, as well as self-oxidation in reaction with H2O2. This study suggests that the H-bond network mediated by Asn52 is essential to suppress the apoptotic activity of H-Cyt c under physiological conditions. © The Royal Society of Chemistry.
语种：
英文
展开
Selective Ag+Adsorption of Ureido Polymer Prepared by Cyclopolymerization Giving Large Ring Repeating Units
作者：
Sun, Yunkai;Matsumura, Yoshimasa;Ochiai, Bungo*
期刊：
ACS APPLIED POLYMER MATERIALS ,2020年2(4):1417-1421 ISSN：2637-6105
通讯作者：
Ochiai, Bungo
作者机构：
[Matsumura, Yoshimasa; Ochiai, Bungo; Sun, Yunkai] Yamagata Univ, Fac Engn, Dept Chem & Chem Engn, Yamagata 9928510, Japan.;[Sun, Yunkai] Univ South China, Coll Chem & Chem Engn, Hengyang 421001, Peoples R China.
通讯机构：
[Ochiai, Bungo] Y;Yamagata Univ, Fac Engn, Dept Chem & Chem Engn, Yamagata 9928510, Japan.
关键词：
cyclopolymerization;ureido polymer;selective adsorption;silver ion;large ring unit
摘要：
We report the synthesis of an ureido polymer containing 19-membered rings, prepared by the cyclopolymerization of a bifunctional monomer trans-1,2-bis(acryloyloxyethylureido)cyclohexane (TBAUCH) and studied for the selective adsorption of Ag+. PolyTBAUCH adsorbed Ag+ with an efficiency of 99.8%, and the maximum adsorption capacity was 39.8 mg/g. PolyTBAUCH selectively adsorbed Ag+ from an aqueous solution containing 20 different metal ions in similar concentrations. The selective adsorption depends on the controlling regioselective effect of the ring structure and the ureido groups. PolyTBAUCH could be reused at least for 5 cycles after desorption of Ag+ and maintained an Ag+ adsorption of 95.6% during the 5th cycle. Copyright © 2020 American Chemical Society.
语种：
英文
展开
Designing a colorimetric sensor containing nitrogen and oxygen atoms for uranyl ions identification: Chromatic mechanism, binding feature and on-site application
作者：
Wu, Xumeng;Mao, Yu;Wang, Dongyuan;Huang, Qiuxiang;Yin, Qiang;...
期刊：
Sensors and Actuators B-Chemical ,2020年307:127681 ISSN：0925-4005
通讯作者：
Wang, Hongqing
作者机构：
[Wang, Hongqing; Huang, Qiuxiang; Wu, Xumeng; Wang, Dongyuan; Hu, Qinghua] Univ South China, Hunan Key Lab Design & Applicat Actinide Complexe, Hengyang 421001, Hunan, Peoples R China.;[Zheng, Ming; Mao, Yu; Yin, Qiang] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.
通讯机构：
[Wang, Hongqing] U;Univ South China, Hunan Key Lab Design & Applicat Actinide Complexe, Hengyang 421001, Hunan, Peoples R China.
关键词：
Uranium;Sensor;Colorimetry;pH effect;Br-PADAP;DFT calculation;Species
摘要：
It is still a challenge for scientists to eliminate interference and improve chromatic aberration in designing colorimetric uranyl ions sensors, and it is also not clear how the species of uranium and sensor synergistically affect the coloration mechanism and coordination mode of ligands containing nitrogen or oxygen atoms at different pH. Herein, we design and synthesize 2-(5'-(p-(diphenylamino)phenyl)-2'-pyridylazo)-5-(diethylamino) phenol (abbr. S-LH) for the colorimetric detection of uranyl ions in mixed solvents. The rational introduced triphenylamine group by density functional theory (DFT) calculation enhances the chromaticity difference of the S-LH toward uranyl ions, making the detection limits of the uranyl ions approximately one order of magnitude lower than that of the present UV-vis and visual method. The species of S-LH and uranium at different pH are clarified and it well explains the reason of different color changes after adding uranyl ions. Stability constant experiments show that S-LH has excellent anti-interference to other metal ions during detecting uranium. The coordination structure of S-LH towards UO22+ is further confirmed by HRMS, H-1 NMR titration, and DFT calculation. Finally, colorimetric test strips with S-LH are prepared to detect uranium in Xiang River, providing an on-site and real-time method to detect uranyl ions in the environment.
语种：
英文
展开
The presence of mixed-valent silver in the uranyl phenylenediphosphonate framework
作者：
Bai, Ru;Chen, Lanhua;Zhang, Yugang;Chen, Long;Juan Diwu;...
期刊：
NEW JOURNAL OF CHEMISTRY ,2020年44(15):6037-6041 ISSN：1144-0546
通讯作者：
Wang, Xiao-Feng
作者机构：
[Bai, Ru; Wang, Xiao-Feng] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Bai, Ru; Wang, Xiao-Feng] Univ South China, Hunan Key Lab Design & Applicat Actinide Complexe, Hengyang 421001, Peoples R China.;[Chen, Lanhua; Chen, Long; Zhang, Yugang; Bai, Ru; Juan Diwu] Soochow Univ, State Key Lab Radiat Med & Protect, Sch Radiol & Interdisciplinary Sci RAD X, Collaborat Innovat Ctr Radiat Med Jiangsu Higher, Suzhou 215123, Peoples R China.;[Chen, Lanhua; Chen, Long; Zhang, Yugang; Bai, Ru; Juan Diwu] Soochow Univ, Sch Radiat Med & Protect, Suzhou 215123, Peoples R China.
通讯机构：
[Wang, Xiao-Feng] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;Univ South China, Hunan Key Lab Design & Applicat Actinide Complexe, Hengyang 421001, Peoples R China.
摘要：
In this work, a new 2D layered silver uranyl phosphonate compound Ag-1.51(0)[Ag-4(I)(UO2)(3)(O3PC6H4PO3)(O3PC6H4PO3H)(2)] (denoted as compound 1) was synthesized by reaction of 1,2-phenylenediphosphonic acid (H(4)PDPA) with UO2(NO3)(2)center dot 6H(2)O and AgNO3 under mild hydrothermal conditions. The uranyl layered framework consists of two types of UO8 and UO7 coordination units simultaneously connected by two kinds of phenylenediphosphonate linkers. To our surprise, the presence of both silver ions and metallic silver atoms in the free space between the layers is identified by the single crystal X-ray diffraction, EDS, and XPS techniques. The ratio of Ag+ and Ag-0 was estimated to be 2.81 : 1, based on the primary peak area of Ag 3d(5/2) from the XPS results, which corroborates with the ratio of 2.65 : 1 obtained from the XRD results. More importantly, the incorporation of the mixed-valent silver sites results in the quenching of the fluorescent emission of the uranyl phosphonate compound as evidenced by its single crystal fluorescence spectrum.
语种：
英文
展开
Synthesis of Poly(cyclotriphosphazene-co-4,4 '-diaminodiphenysulfone) Microspheres and Their Adsorption Properties for Cationic Dyes (Methylene Blue)
作者：
Zou, Jiaming;Liao, Kaifa;Xiang, Li;Liu, Mouwu;Xie, Fan;...
期刊：
Journal of Inorganic and Organometallic Polymers and Materials ,2020年30(3):976-985 ISSN：1574-1443
通讯作者：
Wang, Yanfei
作者机构：
[Xie, Fan; Liu, Mouwu; Yu, Jianglai; Zou, Jiaming; Wang, Yanfei; Xiang, Li; Liu, Xinlin; Liao, Kaifa; An, Xiaonan] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.
通讯机构：
[Wang, Yanfei] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.
关键词：
Hexachlorocyclotriphosphazene;Methylene blue;Microspheres;Adsorption
摘要：
Poly (cyclotriphosphazene-co-4,4′-diaminodiphenyl sulfone) (PZD) microspheres were prepared by precipitation polymerization with simple scheme and convenient operation, and used as a special effect adsorbent for adsorbing cationic dye, which is methylene blue (MB) in water. The synthesized PZD microspheres were characterized by SEM, TEM and XPS techniques. The influences of temperature, adsorption time, pH initial MB solution concentration and adsorbent dosage on MB adsorption were studied. The experimental results show that the adsorption of MB dye by PZD microspheres is more in line with the pseudo-second-order kinetics model than the pseudo-first-order kinetic model. In addition, the adsorption process was further resolved using Weber’s intraparticle diffusion model. Thermodynamic experiments show that the adsorption process is spontaneously carried out by endotherm. The mechanism of adsorption of MB dye by PZD microspheres may be related to the existence of a lot of electron-rich atoms N, P, S in the adsorbent, the electrostatic attraction and π–π stacking effect between PZD microspheres and MB dye.
语种：
英文
展开
One-step synthesis of an environment-friendly cyclodextrin-based nanosponge and its applications for the removal of dyestuff from aqueous solutions
作者：
Li, Liuxing;Liu, Huijun* ;Li, Wei;Liu, Kai;Tang, Ting;...
期刊：
Research on Chemical Intermediates ,2020年46(3):1715-1734 ISSN：0922-6168
通讯作者：
Liu, Huijun
作者机构：
[Tang, Ting; Liu, Juan; Liu, Huijun; Li, Wei; Jiang, Wenkang; Li, Liuxing; Liu, Kai] Univ South China, Sch Chem & Chem Engn, 28 Changsheng Rd West, Hengyang 421001, Hunan, Peoples R China.;[Liu, Huijun; Li, Liuxing] Univ South China, Hunan Key Lab Design & Applicat Actinide Complexe, Hengyang 421001, Hunan, Peoples R China.
通讯机构：
[Liu, Huijun] U;Univ South China, Sch Chem & Chem Engn, 28 Changsheng Rd West, Hengyang 421001, Hunan, Peoples R China.;Univ South China, Hunan Key Lab Design & Applicat Actinide Complexe, Hengyang 421001, Hunan, Peoples R China.
关键词：
Cyclodextrin-based nanosponge;Basic red 46;Rhodamine B;Adsorption;Environment-friendly
摘要：
Cyclodextrin-based nanosponges (CDNS) are a novel kind of polymers belonged to cross-linked derivatives of cyclodextrins, and they are safe, biodegradable materials with appreciable toxicity to the environment. In this work, CDNS were fabricated in one-step solvothermal method by beta-cyclodextrin (beta-CD) and diphenyl carbonate (DPC), for the removal of dyestuffs from wastewater using two of the familiar dyes as the model contaminant. It was systematically investigated by the influence of the amount of adsorbent, the molar ratio of beta-CD and DPC, pH, time, and initial concentration. Experimental results showed the maximum adsorption capacities of Basic red 46 and Rhodamine B were 101.43 mg/g and 52.33 mg/g, the adsorption behavior of two contaminants followed pseudo-second-order model and the Langmuir monolayer adsorption models. The differences in adsorption capacities on two model contaminants might due to the influence of dye structure. In conclusion, cyclodextrin-based nanosponges are a promising kind of environment-friendly materials in water treatment.
语种：
英文
展开
