Periodic Dynamic Regulation of MSCs Differentiation on Redox-Sensitive Elastic Switched Substrates
作者:
Gong, Tao;Hu, Qinghua;Nie, Xiaobo;Liu, Tao;Wang, Hongqing
期刊:
ACS Applied Bio Materials ,2020年3(6):3612-3620 ISSN:2576-6422
通讯作者:
Wang, Hongqing(hqwang2001cn@126.com);Liu, Tao(lt045021@gzucm.edu.cn)
作者机构:
[Gong, Tao; Hu, Qinghua; Nie, Xiaobo; Wang, Hongqing] College of Chemistry and Chemical Engineering, University of South China, Hengyang;421001, China;[Liu, Tao] Medical College of Acu-Moxi and Rehabilitation, Guangzhou University of Chinese Medicine, Guangzhou;510006, China;[Gong, Tao; Hu, Qinghua; Nie, Xiaobo; Wang, Hongqing] 421001, China
通讯机构:
[Wang, H.] C;[Liu, T.] M;Medical College of Acu-Moxi and Rehabilitation, China;College of Chemistry and Chemical Engineering, China
关键词:
elastic substrates;hydrogel;micropattern;MSCs differentiation;redox-sensitive polymer
摘要:
The biomechanical properties of cell culture substrates can affect cell morphology, cytoskeletal structure, and cell differentiation. However, most of the elastic substrates reported to regulate the behavior of stem cells are often limited to model the static surface, such as providing a constant elasticity modulus for the substrates. In this article, we synthesized a redox-sensitive smart hydrogel with a programmed switchover of elastic substrates in response to glutathione (GSH)/oxidizided glutathione (GSSG) concentration change. The hydrogel is made up of a mixture six-arm poly(ethylene glycol)-poly(ϵ-caprolactone)-3,3′-dithiodipropionic acid gels (6A PECL-SS) and six-arm poly(ethylene glycol)-poly(ϵ-caprolactone)-acryloyl (6A PECL-AC). Under different redox stimulus (+GSH or +GSSG), the redox-sensitive substrate can act as a cross-linked switch to adjust the elasticity modulus. RT-PCR results based on cell culture evaluation indicate that the reversibly controlled elastic substrates cultured on a flat and microgroove surface exhibited good osteoinduction under different inversion frequencies. Therefore, our results indicate that this redox-responsive substrate has great potential in bone tissue engineering. Copyright © 2020 American Chemical Society.
语种:
英文
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磁性纳米材料处理含铀废水的研究进展
作者:
阳鹏飞;黎杰鑫;朱春霞
期刊:
化工进展 ,2020年39(1):206-215 ISSN:1000-6613
通讯作者:
Yang, Pengfei(ypengfei2008@126.com)
作者机构:
[阳鹏飞; 黎杰鑫; 朱春霞] School of Chemistry and Chemical Engineering, University of South China, Hengyang;Hunan;421001, China;Hunan Key Laboratory for the Design and Application of Actinide Complexes, Hengyang;[阳鹏飞; 黎杰鑫; 朱春霞] Hunan
关键词:
磁性纳米材料;分离;铀酰离子;废水;环境;吸附
摘要:
磁性纳米材料具有较强的化学稳定性、可再生回收、良好的吸附性能和易于分离等优点,在去除水溶液中的铀酰离子方面有广泛的应用前景。然而,磁性纳米材料也存在易团聚、易氧化等不足,通过表面修饰或改性等方法可改善其不足,提高其对废水中铀酰离子的去除能力,改善其吸附效果。本文通过总结近年来的相关研究资料,概括了磁性纳米材料的种类,归纳总结并比较了不同种类磁性纳米材料对含铀废水的去除能力及优势与不足,探讨了磁性纳米材料在含铀废水处理中的应用并对其机理进行了分析,阐述了磁性纳米材料去除溶液中铀酰离子的影响因素,简述了目前磁性纳米材料在处理含铀废水中有待解决的问题,并对其在分离放射性元素方面的应用前景进行了展望。
语种:
中文
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Rational design of heme enzymes for biodegradation of pollutants toward a green future
作者:
Lin, Ying-Wu*
期刊:
Biotechnology and Applied Biochemistry ,2020年67(4):484-494 ISSN:0885-4513
通讯作者:
Lin, Ying-Wu
作者机构:
[Lin, Ying-Wu] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Lin, Ying-Wu] Univ South China, Lab Prot Struct & Funct, Hengyang, Peoples R China.;[Lin, Ying-Wu] Univ South China, Hunan Key Lab Design & Applict Actinide Complexes, Hengyang, Peoples R China.
通讯机构:
[Lin, Ying-Wu] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
关键词:
biodegradation;dehaloperoxidase;dye-decolorizing peroxidase;heme enzyme;protein design
摘要:
Environmental pollutants, such as industrial dyes and halophenols, are harmful to human health, which urgently demand degradation. Bioremediation has been shown to be a cost-effective and ecofriendly approach. As reviewed herein, significant progress has been made in the last decade for biodegradation of both industrial dyes and halophenols, by engineering of native dye-decolorizing peroxidases (DyPs) and dehaloperoxidases (DHPs), and by design of artificial heme enzymes in both native and de novo protein scaffolds. The catalytic efficiency of artificial DyPs and DHPs can be rationally designed comparable to or even beyond those of natural counterparts. The enzymes are on their way from laboratory to industry and will play more crucial roles in environmental protection toward a green future. © 2019 International Union of Biochemistry and Molecular Biology, Inc.
语种:
英文
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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
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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
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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
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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
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连续反应-萃取耦合技术制备硫酸羟胺
作者:
彭超;王榆元;邓昌爱;赵方方;游奎一
期刊:
化工学报 ,2019年70(5):1842-1847 ISSN:0438-1157
通讯作者:
You, Kuiyi(youkuiyi@126.com)
作者机构:
[彭超; 王榆元; 邓昌爱] College of Chemistry and Chemical Engineering, University of South China, Hengyang;Hunan;421001, China;[赵方方; 游奎一] College of Chemical Engineering, Xiangtan University, Xiangtan;411105, China
通讯机构:
College of Chemical Engineering, Xiangtan University, Xiangtan, Hunan, China
关键词:
反应-萃取耦合;反应;平衡;水解;环己酮肟;硫酸羟胺
摘要:
以环己酮肟和硫酸为原料,研究连续反应-萃取耦合技术条件下环己酮肟水解制备硫酸羟胺。通过优化连续反应-萃取条件,将水解得到的另一产物环己酮从原有平衡体系分离,突破原反应平衡的限制,极大提高环己酮肟的转化率。结果表明,在以环己烷作为萃取剂,酸肟比1∶1,转速为2000~2500 r/min,硫酸溶液与环己烷等体积比的条件下,反应条件最佳。同时测得当原料从重相进料,通过五级串联逆流反应萃取,90 min反应基本达到平衡,经过四次循环萃取后环己酮肟转化率可达81.90%。
语种:
中文
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Metal-Carboxyl Helical Chain Secondary Units Supported Ion-Exchangeable Anionic Uranyl–Organic Framework
作者:
Mei, Lei;Liu, Kang;Wu, Si;Kong, Xiang-He;Hu, Kong-Qiu;...
期刊:
Chemistry - A European Journal ,2019年25(44):10309-10313 ISSN:0947-6539
通讯作者:
Shi, Wei-Qun
作者机构:
[Mei, Lei; Liu, Kang; Wu, Si; Kong, Xiang-He; Hu, Kong-Qiu; Yu, Ji-Pan; Chai, Zhi-Fang; Shi, Wei-Qun] Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China;[Wu, Si; Nie, Chang-Ming] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China;[Chai, Zhi-Fang] Chinese Acad Sci, Engn Lab Adv Energy Mat, Ningbo Inst Ind Technol, Ningbo 315201, Zhejiang, Peoples R China;[Liu, Kang] Univ Chinese Acad Sci, Beijing 100039, Peoples R China
通讯机构:
[Shi, Wei-Qun] C;Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China.
关键词:
actinides;anionic framework;helical chain;ion exchange;uranyl–organic compounds
摘要:
As a less explored avenue, actinide-based metal-organic frameworks (MOFs) are worth studying for the particularity of actinide nodes in coordination behaviour and assembly modes. In this work, an azobenzenetetracarboxylate-based anionic MOF supported by uranyl–carboxyl helical chain units was synthesized, incorporating linear uranyl as the metal centre. This kind of helical chain-type building unit is reported for the first time in uranyl-based MOFs. Structural analysis reveals that the formation of helical chain secondary units can be attributed to restricted equatorial coordination of rigid flat azobenzene ligand to uranyl centres. Meanwhile, this newly-synthesized anionic material has been used to remove Eu3+ ions, as a non-radioactive surrogate of Am3+ ion, through an ion-exchange process with [(CH3)2NH2]+ ions in its open channels, as evidenced by a combination of 1H NMR spectroscopy, EDS and PXRD. © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
语种:
英文
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Effective Removal of Anionic Re(VII) by Surface-Modified Ti2CTx MXene Nanocomposites: Implications for Tc(VII) Sequestration
作者:
Wang, Lin;Song, Huan;Yuan, Liyong;Li, Zijie;Zhang, Peng;...
期刊:
Environmental Science & Technology ,2019年53(7):3739-3747 ISSN:0013-936X
通讯作者:
Shi, Weiqun
作者机构:
[Zhang, Peng; Yuan, Liyong; Chai, Zhifang; Li, Zijie; Shi, Weiqun; Wang, Lin; Song, Huan] Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.;[Zhang, Peng; Yuan, Liyong; Chai, Zhifang; Li, Zijie; Shi, Weiqun; Wang, Lin; Song, Huan] Chinese Acad Sci, Inst High Energy Phys, Key Lab Biomed Effects Nanomat & Nanosafety, Beijing 100049, Peoples R China.;[Wang, Hongqing; Song, Huan] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Wang, Hongqing; Song, Huan] Univ South China, Hunan Key Lab Design & Applicat Actinide Complexe, Hengyang 421001, Peoples R China.;[Gibson, John K.] LBNL, Chem Sci Div, Berkeley, CA 94720 USA.
通讯机构:
[Shi, Weiqun] C;Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.;Chinese Acad Sci, Inst High Energy Phys, Key Lab Biomed Effects Nanomat & Nanosafety, Beijing 100049, Peoples R China.
摘要:
Environmental contamination by 99Tc(VII) from radioactive wastewater streams is of particular concern due to the long half-life of 99Tc and high mobility of pertechnetate. Herein, we report a novel MXene-polyelectrolyte nanocomposite with three-dimensional networks for enhanced removal of perrhenate, which is pertechnetate simulant. The introduction of poly(diallyldimethylammonium chloride) (PDDA) regulates the surface charge and improves the stability of Ti2CTx nanosheet, resulting in Re(VII) removal capacity of up to 363 mg g-1, and fast sorption kinetics. The Ti2CTx/PDDA nanocomposite furthermore exhibits good selectivity for ReO4- when competing anions (such as Cl- and SO42-) coexist at a concentration of 1800 times. The immobilization mechanism was confirmed as a sorption-reduction process by batch sorption experiments and X-ray photoelectron spectroscopy. The pH-dependent reducing activity of Ti2CTx/PDDA nanocomposite toward Re(VII) was clarified by X-ray absorption spectroscopy. As the pH increases, the local environment gradually changes from octahedral-coordinated Re(IV) to tetrahedral-coordinated Re(VII). The overall results suggest that Ti2CTx/PDDA nanocomposite may be a promising candidate for efficient elimination of Tc contamination. The reported surface modification strategy might result in applications of MXene-based materials in environmental remediation of other oxidized anion pollutants. Copyright © 2019 American Chemical Society.
语种:
英文
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A hydrolytically stable europium-organic framework for the selective detection of radioactive Th4+ in aqueous solution
作者:
Song, Liping;Liu, Wei;Wang, Yanlong;Chen, Lanhua;Wang, Xiao-Feng* ;...
期刊:
CrystEngComm ,2019年21(22):3471-3477 ISSN:1466-8033
通讯作者:
Wang, Xiao-Feng;Wang, Shuao
作者机构:
[Song, Liping; Wang, Xiao-Feng] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Song, Liping; Wang, Xiao-Feng] Univ South China, Hunan Prov Engn Res Ctr Radioact Control Technol, Hengyang 421001, Peoples R China.;[Chen, Lanhua; Liu, Wei; Song, Liping; Wang, Yanlong; Wang, Shuao] 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; Liu, Wei; Song, Liping; Wang, Yanlong; Wang, Shuao] Soochow Univ, Sch Radiat Med & Protect, Suzhou 215123, Peoples R China.
通讯机构:
[Wang, Xiao-Feng] U;[Wang, Shuao] S;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.;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.
摘要:
Thorium is not only a promising candidate for developing next generation nuclear fuel but also a potential radioactive contaminant. Efficient detection of thorium contamination is critically important in both nuclear science and environmental protection. We present here a 3D luminescent europium organic framework [Eu2(FDC)3(DMA)2]·4H2O (compound 1), which exhibits excellent hydrolytic stability and features highly selective detection capacity (KSV = 6.68 × 104) towards radioactive Th4+ ions among the selected monovalent, divalent and tervalent metal ions in aqueous solution. The detection limit of the material towards Th4+ is 3.49 × 10-5 mol L-1 which is close to the WHO standard. The detection capability and the sensing mechanism were demonstrated by Th4+ uptake kinetics, energy-dispersive spectroscopy mapping, absorption spectroscopy, luminescence lifetime, and competitive adsorption measurements. Compound 1 represents a rare case of a MOF based Th4+ probe. © The Royal Society of Chemistry 2019.
语种:
英文
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Insight into Coordination of Uranyl Ions with N,N′-bis(2-five-membered heterocyclidene)-1,8-anthradiamines
作者:
Long, Li-yu;Tao, Peng;Li, Tian-liang;Wu, Si;Kong, Xiang-he;...
期刊:
Applied Organometallic Chemistry ,2019年33(6):e4931- ISSN:0268-2605
通讯作者:
Nie, Chang-ming
作者机构:
[Liao, Li-fu; Wu, Si; Long, Li-yu; Li, Tian-liang; Xiao, Xi-lin; Kong, Xiang-he; Tao, Peng; Nie, Chang-ming] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Liao, Li-fu; Long, Li-yu; Xiao, Xi-lin; Tao, Peng; Nie, Chang-ming] 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;nitrogen family nonmetal elements;oxygen family nonmetal elements;uranyl;uranyl-BFHADAs
摘要:
To find new adsorbents for uranyl ions, the density functional theory (DFT) was adopted to design a series of new ligands containing an anthracene and two five-membered heterocycles with nitrogen family nonmetal elements (N, P, As) or oxygen family nonmetal elements (O, S, Se, Te), for example, ligands N,N′-bis(2-five-membered heterocyclidene)-1,8-anthradiamines (BFHADAs). Then the uranyl ions were coordinated with BFHADAs to generate five new coordination complexes (Uranyl-BFHADAs) with heteroatoms N, S, As, Se and Te, respectively. The five-membered heterocyclic rings of Uranyl-BFHADA with oxygen atoms were broken under the structural optimization and Uranyl-BFHADA with heterocyclic atoms P was not obtained. Several structures and property parameters of the ligands BFHADAs (containing heteroatoms N, S, As, Se and Te) and their uranyl complexes Uranyl-BFHADAs were theoretically investigated and analyzed. The results showed that uranyl ions could form stable coordination complexes with these five BFHADAs. The formed bonds between uranyl ions and the heteroatoms in BFHADAs were coordination bonds rather than other types of bonds. These results could provide insightful information and theoretical guidance for the coordination of uranyl with the atoms N, S, Se, As and Te in other ligands. © 2019 John Wiley & Sons, Ltd.
语种:
英文
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The Third Generation of Artificial Dye-Decolorizing Peroxidase Rationally Designed in Myoglobin
作者:
Zhang, Ping;Xu, Jiakun;Wang, Xiao-Juan;He, Bo;Gao, Shu-Qin;...
期刊:
ACS Catalysis ,2019年9(9):7888-7893 ISSN:2155-5435
通讯作者:
Lin, Ying-Wu
作者机构:
[Lin, Ying-Wu; Wang, Xiao-Juan; Zhang, Ping; He, Bo] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Xu, Jiakun] Chinese Acad Fishery Sci, Yellow Sea Fisheries Res Inst, Key Lab Sustainable Dev Polar Fisheries, Qingdao 266071, Shandong, Peoples R China.;[Xu, Jiakun] Lab Marine Drugs & Byprod Pilot Natl Lab Marine S, Qingdao 266071, Shandong, Peoples R China.;[Gao, Shu-Qin; Lin, Ying-Wu] Univ South China, Tab 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, Tab Prot Struct & Funct, Hengyang 421001, Peoples R China.
关键词:
dye-decolorizing peroxidases;artificial enzyme;protein design;myoglobin;substrate-binding;molecular docking
摘要:
Approaches to degradation of industrial dyes are desirable, of which bioremediation is more favorable. In addition to the use of native enzymes, rational design of artificial enzymes provides an alternative approach. Meanwhile, few designs can achieve a catalytic activity comparable to that of native enzymes. We have previously designed two generations of artificial dye-decolorizing peroxidases (DyPs) in myoglobin (Mb) by introduction of Tyr43 and Trp138 in the heme pocket; however, the activity is moderate. To improve the activity of the artificial DyP, we herein designed a third generation by introduction of an additional Trp (P88W) to the protein surface, named F43Y/F138W/P88W Mb. The third generation of artificial DyP was shown to exhibit a catalytic efficiency exceeding that of various native DyPs and comparable to that of the most efficient native DyPs. Titration of reactive blue 19 (RB19) and molecular docking studies revealed crucial roles of Trp88 in substrate binding and oxidation, which acts as a catalytic site. This study not only provides clues for heme protein design but also suggests that the artificial DyP has potential applications for bioremediation in the future. © 2019 American Chemical Society.
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英文
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Direct Observation of Charge Injection of Graphene in the Graphene/WSe2 Heterostructure by Optical-Pump Terahertz-Probe Spectroscopy.
作者:
Zhang, Liangliang* ;Chen, Zefeng;Zhang, Rui;Tan, Yong;Wu, Tong;...
期刊:
ACS Applied Materials & Interfaces ,2019年11(50):47501-47506 ISSN:1944-8244
通讯作者:
Zhang, Liangliang;Xu, Jianbin
作者机构:
[Shalaby, Mostafa; Tan, Yong; Zhang, Liangliang; Wu, Tong] Capital Normal Univ, Beijing Adv Innovat Ctr Imaging Theory & Technol, Beijing 100048, Peoples R China.;[Shalaby, Mostafa; Tan, Yong; Zhang, Liangliang; Wu, Tong] Capital Normal Univ, Dept Phys, Key Lab Terahertz Optoelect MoE, Beijing 100048, Peoples R China.;[Xu, Jianbin; Chen, Zefeng] Chinese Univ Hong Kong, Dept Elect Engn, Hong Kong 999077, Peoples R China.;[Zhang, Rui] Chinese Acad Sci, Shenzhen Inst Adv Technol, Shenzhen 518055, Guangdong, Peoples R China.;[Xie, Rui] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
通讯机构:
[Zhang, Liangliang; Xu, Jianbin] C;Capital Normal Univ, Beijing Adv Innovat Ctr Imaging Theory & Technol, Beijing 100048, Peoples R China.;Capital Normal Univ, Dept Phys, Key Lab Terahertz Optoelect MoE, Beijing 100048, Peoples R China.;Chinese Univ Hong Kong, Dept Elect Engn, Hong Kong 999077, Peoples R China.
关键词:
charge injection;graphene;optical-pump THz probe;photoresponse;van der Waals heterostructure
摘要:
Charge transfer across the interface and interlayer coupling in the graphene van der Waals heterostructure, which is constructed by graphene and semiconducting transition metal dichalcogenides (TMDCs), is critical for their electronic and optoelectronic applications. Photo-induced charge injection from TMDC to graphene has been studied in several heterostructure photodetectors. However, the response time significantly varies among different reports, ranging from microseconds to milliseconds. In this work, using a graphene/WSe2 heterostructure as an example, we directly observe the carrier density change in graphene by time-resolved optical-pump terahertz (THz)-probe spectroscopy and show the ultrafast picosecond photoresponse of graphene. In the absence of photoexcitation, THz time-domain spectroscopic measurements show that WSe2 can transfer holes to graphene and pull down the Fermi level of graphene. After excitation by the ultrafast laser pulse, the transient THz response shows a rapid (∼0.35 ps) increase in the graphene conductivity mainly due to the hole injection from WSe2 into graphene. Unlike previous reports on band bend as the guidance mechanism for charge transfer, our results show that the relevant mechanism is the band offset across the atomically sharp interface. © 2019 American Chemical Society.
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英文
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Artificial Enzyme Catalyzed Cascade Reactions: Antitumor Immunotherapy Reinforced by NIR-II Light.
作者:
Wen, Mei;Ouyang, Jiang;Wei, Chuanwan;Li, Hui;Chen, Wansong* ;...
期刊:
Angewandte Chemie - International Edition ,2019年58(48):17425-17432 ISSN:1433-7851
通讯作者:
Chen, Wansong;Liu, You-Nian
作者机构:
[Wen, Mei; Chen, WS; Liu, You-Nian; Chen, Wansong; Li, Hui; Ouyang, Jiang] Cent South Univ, Coll Chem & Chem Engn, Changsha 410083, Hunan, Peoples R China.;[Wen, Mei; Chen, WS; Liu, You-Nian; Chen, Wansong; Ouyang, Jiang] Cent South Univ, State Key Lab Powder Met, Changsha 410083, Hunan, Peoples R China.;[Wei, Chuanwan] Univ South China, Coll Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.
通讯机构:
[Chen, WS; Liu, YN] C;Cent South Univ, Coll Chem & Chem Engn, Changsha 410083, Hunan, Peoples R China.;Cent South Univ, State Key Lab Powder Met, Changsha 410083, Hunan, Peoples R China.
关键词:
anticancer;enzymes;immunotherapy;nanoparticles;oxidative stress
摘要:
Current cancer therapy is seriously challenged by tumor metastasis and recurrence. One promising solution to these problems is to build antitumor immunity. However, immunotherapeutic efficacy is highly impeded by the immunosuppressive state of the tumors. Here a new strategy is presented, catalytic immunotherapy based on artificial enzymes. Cu2−xTe nanoparticles exhibit tunable enzyme-mimicking activity (including glutathione oxidase and peroxidase) under near-infrared-II (NIR-II) light. The cascade reactions catalyzed by the Cu2−xTe artificial enzyme gradually elevates intratumor oxidative stress to induce immunogenic cell death. Meanwhile, the continuously generated oxidative stress by the Cu2−xTe artificial enzyme reverses the immunosuppressive tumor microenvironment, and boosts antitumor immune responses to eradicate both primary and distant metastatic tumors. Moreover, immunological memory effect is successfully acquired after treatment with the Cu2−xTe artificial enzyme to suppress tumor relapse. © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
语种:
英文
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Cooperative Capture of Uranyl Ions by a Carbonyl-Bearing Hierarchical-Porous Cu–Organic Framework
作者:
Wang, Xiao-Feng* ;Chen, Yangyang;Song, Li-Ping;Fang, Zhen;Zhang, Jian;...
期刊:
Angewandte Chemie - International Edition ,2019年58(52):18808-18812 ISSN:1433-7851
通讯作者:
Wang, Xiao-Feng;Lin, Ying-Wu;Rocha, Joao;Zhang, Yue-Biao
作者机构:
[Wang, XF; Lin, Ying-Wu; Zhang, Jian; Chen, Yangyang; Song, Li-Ping; Sun, Yunkai; Wang, Xiao-Feng] Univ South China, Sch Chem & Chem Engn, 28 Changsheng Xi Rd, Hengyang 421001, Hunan, Peoples R China.;[Wang, XF; Rocha, J; Rocha, Joao; Shi, Fanian; Wang, Xiao-Feng] Univ Aveiro, Dept Chem, CICECO, Aveiro Inst Mat, Santiago Campus, P-3810193 Aveiro, Portugal.;[Fang, Zhen] Anhui Normal Univ, Coll Chem & Mat Sci, 1 East Beijing Rd, Wuhu 241000, Anhui, Peoples R China.;[Zhang, Yue-Biao] ShanghaiTech Univ, Sch Phys Sci & Technol, 393 Middle Huaxia Rd, Shanghai, Peoples R China.
通讯机构:
[Wang, XF; Lin, YW; Rocha, J] U;[Zhang, Yue-Biao] S;Univ South China, Sch Chem & Chem Engn, 28 Changsheng Xi Rd, Hengyang 421001, Hunan, Peoples R China.;Univ Aveiro, Dept Chem, CICECO, Aveiro Inst Mat, Santiago Campus, P-3810193 Aveiro, Portugal.;ShanghaiTech Univ, Sch Phys Sci & Technol, 393 Middle Huaxia Rd, Shanghai, Peoples R China.
关键词:
adsorption mechanisms;metal-organic frameworks;porous materials;single-crystal structure;uranyl capture
摘要:
To efficiently capture the toxic uranyl ions (UO22+), a new hierarchical micro-macroporous metal–organic framework was prepared under template-free conditions, featuring interconnected multi-nanocages bearing carbonyl groups derived from a semi-rigid ligand. The material exhibits an unusually high UO22+ sorption capacity of 562 mg g−1, which occurs in an intriguing two-steps process, on the macropore-based crystal surface and in the inner nanocages. Notably, the latter is attributed to the cooperative interplay of the shrinkage of the host porous framework induced by uranyl accommodation and the free carbonyl coordination sites, as shown by both single-crystal X-ray diffraction and a red-shift of the infrared [O=UVI=O]2+ antisymmetric vibration band. © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
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英文
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Theoretical investigation into the coordination of R-/S-asymmetric uranyl–salophens containing six-membered ring lactam with cis−/trans-cyclohexylamines
作者:
Yang, Liang-Liang;Kong, Xiang-He;Wu, Zhi-Lin;Lin, Ying-Wu;Liao, Li-Fu;...
期刊:
Applied Organometallic Chemistry ,2018年32(7):e4387- ISSN:0268-2605
通讯作者:
Nie, Chang-Ming
作者机构:
[Liao, Li-Fu; Nie, Chang-Ming; Wu, Zhi-Lin; Yang, Liang-Liang; Kong, Xiang-He; Lin, Ying-Wu] Univ South China, Sch Chem & Chem Engn, 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 selectivity;density functional theory;molecular recognition;R-/S-asymmetric uranyl–salophens
摘要:
A six-membered ring lactam derivative was introduced in a parallel manner into uranyl–salophens with R/S configuration (R-/S-AUSRLs), which were used as receptors to coordinate with guests of cis−/trans-methylcyclohexylamines (cis−/trans-MCHAs). Using density functional theory calculations at the B3LYP/6-311G** level and RECP, an insight into the coordination complexes of the R-/S-AUSRLs with cis−/trans-MCHAs was obtained. The results showed that the U atoms of receptors could coordinate with the N atoms of four kinds of cis−/trans-1,2 or − 1,4 guests, but the two kinds of cis−/trans-1,3 guests could not be converged by the same method in the process of structural optimization due to steric hindrance, and thus the cis−/trans-1,3 guests could not be coordinated with the R-/S-AUSRLs. The mode of coordination of the R-/S-AUSRLs with the guests displayed a significant difference. And the change of R-AUSRL coordination ability to the cis−/trans-MCHAs was very large, but that of S-AUSRL was small. Overall, the stability of the R-series coordination complexes was higher than that of the corresponding S-series coordination complexes, and the R-AUSRL receptor had better coordination selectivity and higher molecular recognition to the cis−/trans-MCHA guests than the S-AUSRL receptor. However, the coordination ability of S-AUSRL with the cis−/trans-MCHAs was stronger than that of R-AUSRL. It was expected that these results could provide insightful information and theoretical guidance for understanding the molecular recognition of R-/S-AUSRLs for cis−/trans-type cyclohexylamine derivatives.<br/> Copyright ©2018 John Wiley & Sons, Ltd.
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英文
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Selective recognition and preliminary separation of hepatoprotective component silybin from milk thistle seeds by the prepared core-shell magnetic molecularly imprinted polymer
作者:
Gao, Yang;Tan, Ni* ;Wang, Juan;He, Dianxiong;Ji, Kang;...
期刊:
Journal of Polymer Research ,2018年25(7):1-14 ISSN:1022-9760
通讯作者:
Tan, Ni
作者机构:
[Han, Jingwen; Ji, Kang; Tan, Ni; He, Dianxiong; Gao, Yang; Yan, Xueming; Wang, Juan] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.
通讯机构:
[Tan, Ni] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.
关键词:
Silybin;Magnetic molecularly imprinted polymer;Computer simulation;Selectivity recognition;Reverse atom transfer radical precipitation polymerization
摘要:
Using hepatoprotective component silybin as the template, MAA as the functional monomer, EGDMA as the cross linker, acetonitrile as the solvent, and Fe3O4 as the magnetic substrate, the silybin magnetic molecularly imprinted polymer(S-MIP) was successfully prepared by the reverse atom transfer radical precipitation polymerization(RATRP), and non-ion imprinted polymer(NIP) was also synthesized by the same procedure only in the absence of silybin. On the basis of computer simulation and L9(34) orthogonal array design matrix, the optimal preparation conditions were finally obtained as follows that the molar ratio of silybin, MAA, and EGDMA was 1:5:60. The prepared materials were respectively characterized by SEM, XRD, FT-IR, VSM and TGA, and the kinetic analyses explored that the adsorption process of S-MIP was better describled by the pseudo-second order kinetic equation, meanwhile, scatchard analysis illustrated that the heterogeneous binding sites existed in S-MIP. Both the selectivity factor α (2.232) and the relative selectivity factor β (2.201) of S-MIP showed the aim material had the excellent specific recognition capacity and selection adsorption property to silybin. Additionally, the recycling reuse experiments explored S-MIP was of a good stability and could be used repeatedly at least five times with only 15.8% decrease of adsorption capacity when applied in the fifth experiment, and the evaluation experiments by HPLC for silybin extraction from the medicinal herb milk thistle seeds indicated that S-MIP had the potential application in separating the natural hepatoprotective component silybin from the herbal plants.
语种:
英文
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In-situ growth of hierarchical layered double hydroxide on polydopamine-encapsulated hollow Fe3O4 microspheres for efficientremoval and recovery of U(VI)
作者:
Yang, Dongxu;Wang, Xiangxue;Wang, Ning;Zhao, Guixia* ;Song, Gang;...
期刊:
Journal of Cleaner Production ,2018年172:2033-2044 ISSN:0959-6526
通讯作者:
Zhao, Guixia;Wang, Xiangke;Wang, Suhua;Wang, Hongqing
作者机构:
[Wang, Xiangke; Wen, Tao; Yang, Dongxu; Zhao, Guixia; Wang, Ning; Zhao, GX; Wang, XK; Wang, SH; Liang, Yu; Wang, Xiangxue; Wang, Suhua] North China Elect Power Univ, Coll Environm Sci & Engn, Beijing 102206, Peoples R China.;[Wang, Hongqing; Yang, Dongxu; Wang, Ning] Univ South China, Sch Chem & Chem Engn, 28 Changsheng West Rd, Hengyang 421001, Hunan, Peoples R China.;[Song, Gang; Chen, Diyun; Wang, Xiangxue] Guangdong Prov Key Lab Radionuclides Pollut Contr, Guangzhou 510006, Guangdong, Peoples R China.;[Hayat, Tasawar; Alsaedi, Ahmed; Wang, Suhua] King Abdulaziz Univ, NAAM Res Grp, Fac Sci, Jeddah 21589, Saudi Arabia.;[Wang, Xiangke] Soochow Univ, Sch Radiol & Interdisciplinary Sci, Collaborat Innovat Ctr Radiat Med, Jiangsu Higher Educ Inst, Suzhou 215123, Peoples R China.
通讯机构:
[Zhao, GX; Wang, XK; Wang, SH] N;[Wang, Hongqing] U;North China Elect Power Univ, Coll Environm Sci & Engn, Beijing 102206, Peoples R China.;Univ South China, Sch Chem & Chem Engn, 28 Changsheng West Rd, Hengyang 421001, Hunan, Peoples R China.
关键词:
Uranium (VI);Ferroferric oxide (Fe3O4);Polydopamine;Layered double hydroxides;Removal and recovery
摘要:
With the increasing demand of nuclear power plant, the depleted uranium is inevitably emitted and causes environmental risk, hence it is crucial to develop new methods to efficiently eliminate uranium compounds from water. In this work, a bifunctional material core-shell-shell layered double hydroxide (LDH) decorated hollow magnetic polydopamine (MP) microspheres (defined as MPL) were synthesized and evaluated for the cleanup of uranium (VI) from aqueous solutions through specific adsorption. The experimental results showed that the adsorption was significantly affected by pH value rather than ionic strength, reflecting that the interaction was mainly governed by inner-sphere surface complexation owing to the multiple functional groups including imine, catechol, amine, and hydroxyl groups. The adsorption kinetics can be perfectly depicted by the pseudo-second-order model with high uptake percentage of 94.8%, which was superior to the previously reported materials. Interestingly, the maximum adsorption performance can be tuned by changing the thickness of polydopamine shell and the content of LDH, in the order of MP<inf>2</inf>L<inf>2</inf>(344 mg/g) >MP<inf>2</inf>L<inf>3</inf>(291 mg/g) >MP<inf>3</inf>L<inf>2</inf>(245 mg/g) >MP<inf>2</inf>L<inf>1</inf>(211 mg/g) >ML<inf>2</inf>(142 mg/g) >MP<inf>1</inf>L<inf>2</inf>(141 mg/g) >MP<inf>2</inf>(71 mg/g) >Fe<inf>3</inf>O<inf>4</inf>(34 mg/g) at 298.15 K and pH 5.0. The adsorption mechanism has been thoroughly investigated with techniques such as transmission electron microscopy (TEM), scanning electron microscopy (SEM), vibrating sample magnetometer (VSM), X-ray diffraction (XRD), thermo-gravimetric analyses (TGA), Fourier transformed infrared spectroscopy (FT-IR) and X-ray photoelectron spectroscopy (XPS). In summary, the bifunctional material could be applied as promising building block for the enrichment and recovery of uranium (VI) from aqueous solutions in environmental pollution cleanup.<br/> ©2017 Elsevier Ltd
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英文
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A novel resonance fluorescence chemosensor based on the formation of heterobinuclear complex with a di-tetradentate macrocyclic ligand and europium (III) for the determination of uranium (VI)
作者:
Wang, Jiao;Xiao, Xilin* ;He, Bo;Jiang, Min;Nie, Changming;...
期刊:
Sensors and Actuators B-Chemical ,2018年262:359-364 ISSN:0925-4005
通讯作者:
Xiao, Xilin;Liao, Lifu
作者机构:
[Xiao, XL; Liao, Lifu; Wang, Jiao; Xiao, Xilin; Jiang, Min; Nie, Changming; Lin, Ying-Wu; He, Bo] Univ South China, Sch Chem & Chem Engn, Key Discipline Lab Natl Def Biotechnol Uranium Mi, Hengyang City 421001, Hunan, Peoples R China.
通讯机构:
[Xiao, XL; Liao, LF] U;Univ South China, Sch Chem & Chem Engn, Key Discipline Lab Natl Def Biotechnol Uranium Mi, Hengyang City 421001, Hunan, Peoples R China.
关键词:
Uranium;Resonance fluorescence chemosensor;Heterobinuclear complex;Di-tetradentate macrocyclic ligand;Europium
摘要:
In this paper, we synthesized and characterized a di-tetradentate macrocyclic ligand as a novel resonance fluorescence probe for the determination of uranium. The ligand contains two tetradentate ligand moieties and can chelate two cations to form binuclear complex. We found that when the ligand only chelates a uranyl ion or europium (III) ion, the formed complex can only produce weak resonance fluorescence. When the ligand chelates simultaneously uranyl and europium (III) to form heterobinuclear complex, the formed complex can produce strong resonance fluorescence due to the cation-cation interaction between uranyl and europium (III). Based on this finding, we established a resonance fluorescence chemosensor for the determination of uranium (VI) by utilizing the formation of the heterobinuclear complex. Under optimal conditions, the linear range for the determination of uranium (VI) is 0.008-1.2 nmol mL(-1) with a detection limit of 0.002 nmol mL(-1). The method has been applied to determine uranium (VI) in environmental water samples with the recoveries between 95.7% and 103.6%. (C) 2018 Elsevier B.V. All rights reserved.
语种:
英文
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