质子交换膜燃料电池高稳定性低铂载量膜电极的研究进展
作者:
李丹;张博雅;刘柏鸿;陶阳;熊子昂;...
期刊:
化工进展 ,2021年40(S2):89-100 ISSN:1000-6613
通讯作者:
Li, Dan(1009116307@qq.com);Hou, Sanying(tysgying@163.com)
作者机构:
[李丹; 张博雅; 刘柏鸿; 侯三英] School of Chemistry and Chemical Engineering, University of South China, Hunan, Hengyang;421001, China;[陶阳] School of Resource Environment and Safety Engineering, University of South China, Hunan, Hengyang;[熊子昂] Powder Metallurgy Research Institute, Central South University, Hunan, Changsha;410083, China
关键词:
燃料电池;稳定性;催化剂;低铂载量;高功率密度
摘要:
质子交换膜燃料电池由于高能量转化率、零污染、低温启动等优点在新能源领域备受关注,但其成本和耐久性仍是本领域的挑战性课题.本文首先回顾了近年来国内外研究者在降低燃料电池成本和提高其耐久性方面取得的成就,从催化剂制备技术、膜电极结构优化、耐久性提升三个方面介绍了近年来国内外在降低膜电极铂载量、提高膜电极功率密度和耐久性方面的发展趋势,通过构筑铂基合金、核壳结构和纳米结构等催化剂能有效地降低铂载量,从而降低燃料电池成本;通过构筑多孔结构催化层或气体扩散层可以改善膜电极的微结构,从而提高电池的功率密度;通过开发新型质子交换膜、更换催化剂载体等方法可以提高膜电极的耐久性.最后,本文针对目前研究进展阐述提高膜电极稳定性仍然是目前的研究难题,并对未来的研究方向进行了展望.
语种:
中文
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电催化4-喹诺酮和二烃基二硒醚的交叉脱氢偶联反应
作者:
Chen, Jin-Yang;Wu, Hong-Yu;Gui, Qing-Wen;Yan, Shan-Shu;Deng, Jie;...
期刊:
催化学报 ,2021年42(9):1445-1450 ISSN:0253-9837
通讯作者:
He, Wei-Min(weiminhe2016@yeah.net)
作者机构:
[He, Wei-Min; Lin, Ying-Wu; Chen, Jin-Yang] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.;[Gui, Qing-Wen; Deng, Jie; Yan, Shan-Shu] Yangtze Normal Univ, Coll Chem & Chem Engn, Chongqing 408000, Peoples R China.;[Wu, Hong-Yu; Cao, Zhong] Changsha Univ Sci & Technol, Hunan Prov Key Lab Mat Protect Elect Power & Tran, Changsha 410114, Hunan, Peoples R China.
通讯机构:
[He, W.-M.] S;School of Chemistry and Chemical Engineering, China
关键词:
Green chemistry;Cross-dehydrogenative coupling;Atom ecomnomy;Reusability;Electrochemistry
摘要:
An environmentally friendly method for the synthesis of 3-organylselenyl quinolones through the electrochemical cross-dehydrogenative coupling of 4-quinolones and diorganyl diselenides was developed. As a green, atom economic and self-separating process, the present reaction requires neither external oxidants nor electrolytes, forming a recyclable catalytic system.
语种:
英文
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Electrochemical multicomponent synthesis of 4-selanylpyrazoles under catalyst- And chemical-oxidant-free conditions
作者:
Wu, Yan;Chen, Jin-Yang;Ning, Jing;Jiang, Xue;Deng, Jie;...
期刊:
Green Chemistry ,2021年23(11):3950-3954 ISSN:1463-9262
通讯作者:
He, Wei-Min(weiminhe2016@yeah.net)
作者机构:
[Wu, Yan; He, Wei-Min; Chen, Jin-Yang] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Ning, Jing; Deng, Yu; Xu, Rui; Jiang, Xue; Deng, Jie] Yangtze Normal Univ, Coll Chem & Chem Engn, Chongqing 408000, Peoples R China.
通讯机构:
[He, W.-M.] S;School of Chemistry and Chemical Engineering, China
摘要:
An electrochemical multicomponent reaction was established under catalyst-, chemical-oxidant-free and mild conditions, which provides an eco-friendly and simple protocol for constructing 4-selanylpyrazoles. A broad range of 4-selanylpyrazole derivatives could be obtained from easily available raw materials in good to excellent yields. © The Royal Society of Chemistry 2021.
语种:
英文
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Black Phosphorus/Polymers: Status and Challenges
作者:
Zhang, Ye;Ma, Chunyang;Xie, Jianlei;Agren, Hans;Zhang, Han
期刊:
Advanced Materials ,2021年33(37):e2100113 ISSN:0935-9648
通讯作者:
Zhang, Han(hzhang@szu.edu.cn);Ågren, Hans(hans.agren@physics.uu.se)
作者机构:
[Zhang, Ye; Xie, Jianlei; Zhang, Han; Ma, Chunyang] Shenzhen Univ, Collaborat Innovat Ctr Optoelect Sci & Technol, Int Collaborat Lab 2D Mat Optoelect Sci & Technol, Minist Educ,Inst Microscale Optoelect, Shenzhen 518060, Peoples R China.;[Zhang, Ye] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Agren, Hans] Uppsala Univ, Dept Phys & Astron, Box 516, S-SE-75120 Uppsala, Sweden.
通讯机构:
[Hans Ågren] D;[Han Zhang] C;Collaborative Innovation Center for Optoelectronic Science & Technology, International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen, 518060 China<&wdkj&>Department of Physics and Astronomy, Uppsala University, Box 516, Uppsala, SE-751 20 Sweden
关键词:
applications;black phosphorus;challenges;polymers
摘要:
As a newly emerged mono-elemental nanomaterial, black phosphorus (BP) has been widely investigated for its fascinating physical properties, including layer-dependent tunable band gap (0.3–1.5 eV), high ON/OFF ratio (104), high carrier mobility (103 cm2 V−1 s−1), excellent mechanical resistance, as well as special in-plane anisotropic optical, thermal, and vibrational characteristics. However, the instability caused by chemical degradation of its surface has posed a severe challenge for its further applications. A focused BP/polymer strategy has more recently been developed and implemented to hurdle this issue, so at present BP/polymers have been developed that exhibit enhanced stability, as well as outstanding optical, thermal, mechanical, and electrical properties. This has promoted researchers to further explore the potential applications of black phosphorous. In this review, the preparation processes and the key properties of BP/polymers are reviewed, followed by a detailed account of their diversified applications, including areas like optoelectronics, bio-medicine, and energy storage. Finally, in accordance with the current progress, the prospective challenges and future directions are highlighted and discussed. © 2021 Wiley-VCH GmbH
语种:
英文
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Divergent functionalization of alpha,beta-enones: catalyst-free access to beta-azido ketones and beta-amino alpha-diazo ketones dagger
作者:
Tu, Youshao* ;Dong, Honglin;Wang, Huamin* ;Ao, Yuhui;Liu, Yu
期刊:
Chemical Communications ,2021年57(37):4524-4527 ISSN:1359-7345
通讯作者:
Tu, Youshao;Wang, Huamin
作者机构:
[Tu, Youshao; Ao, Yuhui; Liu, Yu; Dong, Honglin] Changchun Univ Technol, Coll Chem & Life Sci, Adv Inst Mat Sci, 2055 N Yanan Ave, Changchun 130012, Peoples R China.;[Wang, Huamin] Univ South China, Coll Chem & Chem Engn, 28 N Changsheng West Rd, Hengyang 421001, Peoples R China.
通讯机构:
[Tu, Youshao; Wang, Huamin] C;College of Chemistry and Life Science, Advanced Institute of Materials Science, Changchun University of Technology, 2055 N. Yan'an Avenue, Changchun 130012, P. R. China.;College of Chemistry and Chemical Engineering, University of South China, 28 N Changsheng West Road, Hengyang 421001, P. R. China.
摘要:
A simple and practical method for the azidation of β-fluoroalkyl α,β-unsaturated ketones to access a wide variety of fluorinated nitrogenous carbonyl compounds is developed. Different from existing precedents, neither a metallic nor an organic catalyst was involved in our strategy. Judicious choice of solvents allows for the modulation of the reaction outcomes, delivering β-azido ketones or β-amino α-diazo ketones. The reaction system features environmental friendliness, mild conditions, simplicity and excellent functional group tolerance. © The Royal Society of Chemistry.
语种:
英文
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Designing of 0D/2D mixed-dimensional van der waals heterojunction over ultrathin g-C3N4 for high-performance flexible self-powered photodetector
作者:
Zhang, Ye;Xu, Yiguo;Guo, Jia;Zhang, Xiuwen;Liu, Xinling;...
期刊:
Chemical Engineering Journal ,2021年420:129556 ISSN:1385-8947
通讯作者:
Zhang, Ye(yezhang@usc.edu.cn)
作者机构:
[Liu, Xinling; Zhang, Ye; Fu, Yushuang] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Cao, Rui; Zhang, Xiuwen; Xu, Yiguo; Zhang, Han; Shi, Zhe; Guo, Jia; Zhang, Feng; Ma, Chunyang] Shenzhen Univ, Collaborat Innovat Ctr Optoelect Sci & Technol, Int Collaborat Lab 2D Mat Optoelect Sci & Technol, Minist Educ,Inst Microscale Optoelect, Shenzhen 518060, Peoples R China.
通讯机构:
[Ye Zhang] S;[Han Zhang] C;School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, PR China<&wdkj&>Collaborative Innovation Center for Optoelectronic Science & Technology, International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen 518060, PR China
关键词:
Flexible;g-C3N4@Bi;Mixed-dimensional;Photodetector;Self-powered
摘要:
Mixed-dimensional van der Waals heterojunctions have attracted a great deal of attention due to their excellent photoelectric conversion capability, which have been widely applied for self-powered photoelectrochemical (PEC)-type devices as the growing demands of clean energy, environmental governance and protection, and the underwater communications. In this work, 0D Bismuth quantum dots (Bi QDs) encapsulated 2D g-C3N4 nanosheets (g-C3N4@Bi) mixed-dimensional heterojunctions were prepared and spined on ITO-coated polyethylene terephthalate (PET) substrate for working as self-powered PEC-type photodetector (PD). Density functional theory calculations evidenced the successful construction of a type II van der Waals heterojunction between g-C3N4 and Bi as well as its enhanced optoelectronic characteristics. Benefiting from the superior properties of g-C3N4@Bi, the as-prepared PD exhibits a high photocurrent of 5.02 μA cm−2, a responsivity of 2843.14 μA W−1, and a specific detectivity of 2.25 × 1011 Jones at 0 V. Furthermore, the PD exhibits self-powered capability after 1000 cycles of bending, and the stable and repeatable ON/OFF signals can be detected over 90 days, indicating the excellent long-term stability and the potential of g-C3N4@Bi-based PD in practical applications. © 2021 Elsevier B.V.
语种:
英文
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Synergistic cooperative effect of CF3SO2Na and bis(2-butoxyethyl)ether towards selective oxygenation of sulfides with molecular oxygen under visible-light irradiation
作者:
Liu, Kai-Jian;Wang, Zheng;Lu, Ling-Hui;Chen, Jin-Yang;Zeng, Fei;...
期刊:
Green Chemistry ,2021年23(1):496-500 ISSN:1463-9262
通讯作者:
He, Wei-Min
作者机构:
[Zeng, Fei; Liu, Kai-Jian; Wang, Zheng; He, Wei-Min; Lu, Ling-Hui] Hunan Univ Sci & Engn, Dept Chem & Bioengn, Yongzhou 425100, Peoples R China.;[Lin, Ying-Wu; Chen, Jin-Yang] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Cao, Zhong] Changsha Univ Sci & Technol, Hunan Prov Key Lab Mat Protect Elect Power & Duns, Changsha 410114, Peoples R China.;[Yu, Xianyong] Hunan Univ Sci & Technol, Sch Chem & Chem Engn, Xiangtan 411201, Peoples R China.
通讯机构:
[He, Wei-Min] H;Hunan Univ Sci & Engn, Dept Chem & Bioengn, Yongzhou 425100, Peoples R China.
摘要:
A safe, practical and eco-friendly method for the switchable synthesis of sulfoxides and sulfones through visible-light-initiated oxygenation of sulfides at ambient temperature under transition-metal-, additives-free and minimal solvent conditions. The synergistic catalytic efforts between CF3SO2Na and 2-butoxyethyl ether represents the key promoting factor for the reaction. This journal is © The Royal Society of Chemistry.
语种:
英文
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用于铀酰离子检测的光化学分析传感器研究新进展
作者:
郦瑜杰;张迪;刘陈;王志梅;廖力夫;...
期刊:
化工进展 ,2021年40(1):477-486 ISSN:1000-6613
通讯作者:
Xiao, Xilin(xiaoxl2001@163.com)
作者机构:
[郦瑜杰; 王志梅; 肖锡林] School of Resource & Environment and Safety Engineering, University of South China, Hengyang;421001, China;[张迪; 刘陈; 廖力夫] School of Chemistry and Chemical Engineering, University of South China, Hengyang;Key Laboratory of Hengyang for Health Hazard Factors Inspection and Quarantine, University of South China, Hengyang;[郦瑜杰; 张迪; 刘陈; 王志梅; 廖力夫; 肖锡林] 421001, China
关键词:
铀酰;紫外可见分光光度法;荧光;拉曼散射法
摘要:
随着全球变暖和能源问题的出现,对于核能这种清洁能源的开发和应用越发深入和广泛。铀作为一种核原料非常宝贵,然而以铀为主的核废料因其高放射性和生物毒性对人类的生命健康产生了威胁,因此如何实现对其痕量检测成为了人们关注的焦点。光化学传感器由于分析迅速、灵敏度高,能够及时检测排查铀等放射性元素。因此,研发拥有高选择性、高灵敏度和可重复使用的铀酰光化学检测传感器就显得尤为重要。本文主要阐述了近年来基于光化学技术的铀酰检测传感器的前沿进展,其中光化学技术主要包括紫外可见分光光度法(UV-vis)、荧光(fluorescence)分光光度法、表面增强拉曼散射法(SERS)等,并讨论了其各自检测特性,分析了优势与不足之处,初步探讨了光化学传感技术测铀的发展趋势及方向,为进一步设计铀酰光化学检测传感器提供了参考。
语种:
中文
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Selective oxidation of (hetero)sulfides with molecular oxygen under clean conditions
作者:
Liu, Kai-Jian;Deng, Ji-Hui;Yang, Jie;Gong, Shao-Feng;Lin, Ying-Wu;...
期刊:
Green Chemistry ,2020年22(2):433-438 ISSN:1463-9262
通讯作者:
He, Wei-Min
作者机构:
[Liu, Kai-Jian; He, Wei-Min; Yang, Jie; Gong, Shao-Feng; Deng, Ji-Hui] Hunan Univ Sci & Engn, Dept Chem, Yongzhou 425100, Peoples R China.;[Lin, Ying-Wu] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[He, Jun-Yi; Cao, Zhong] Changsha Univ Sci & Technol, Hunan Prov Key Lab Mat Protect Elect Power & Tran, Changsha 410114, Peoples R China.
通讯机构:
[He, Wei-Min] H;Hunan Univ Sci & Engn, Dept Chem, Yongzhou 425100, Peoples R China.
摘要:
The development of eco-friendly and switchable catalytic systems for the conversion of a sole raw-material into distinct high-value products is a particularly attractive concept and a daunting synthetic challenge. In the present work, the first example of efficient and selective oxidation of sulfides to sulfones and sulfoxides using molecular oxygen under clean conditions was established. © The Royal Society of Chemistry.
语种:
英文
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Rational designing an azo colorimetric sensor with high selectivity and sensitivity for uranium environmental monitoring
作者:
Wu, Xumeng;Yin, Qiang;Huang, Qiuxiang;Mao, Yu;Hu, Qinghua;...
期刊:
Analytica Chimica Acta ,2020年1140:153-167 ISSN:0003-2670
通讯作者:
Wang, Hongqing
作者机构:
[Wang, Hongqing; Huang, Qiuxiang; Wu, Xumeng; Hu, Qinghua] Univ South China, Hunan Key Lab Design & Applicat Actinide Complexe, Hengyang 421001, Hunan, Peoples R China.;[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:
Environmental detection;PADAP derivatives;Rational design;Sensor;Uranyl ion
摘要:
Uranium, a double-edged sword with high-efficiency energy and radioactive toxicity, attracts people to enjoy the advantages by generating power, but at the same time brings potential harm by nuclide migration. Therefore, it is necessary to develop a highly-efficient sensor to monitor uranyl ions in the field. However, the designed processes of the reported sensors are random, time-consuming and difficulty. It is urgent to find a new strategy to rationally, quickly and effectively screen out the required molecule for efficient uranium detection. Herein, with the guidance from the rational design method, the parameter, Egap , was applied to judge the chromatic aberration between the designed PADAP derivate and its uranyl complex. And the optimized structure sensor, 2-((3-bromo-5-(9,9-dioctyl-7-(4,4,5,5tetramethyl-1,3,2-dioxaborolan-2-yl)-9H-fluoren-2-yl)-2-pyridylazo)-5-(diethylamino)phenol (abbr. W1H), was screened and successfully synthesized. W1H exhibited significant color change (red to blue) after binding uranyl ions, and its detection limit for uranium was as low as nanomolar. More meaningfully, the coordination mechanism of W1H toward uranium was clarified by theoretical calculation of the electron cloud density distribution, E-bind, and H-1 NMR, IR and MS for the first time. With the more excellent uranyl sensitivity, selectivity, and recyclability, W1H and its colorimetric test strip have been applied to the detection of low-concentration uranium in environmental samples around the uranium tailings, providing a useful on-site method to monitor trace uranium in actual samples. (c) 2020 Elsevier B.V. All rights reserved.
语种:
英文
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An AIE+TICT activated colorimetric and ratiometric fluorescent sensor for portable, rapid, and selective detection of phosgene
作者:
Hu, Qinghua* ;Huang, Qiuxiang;Liang, Kexin;Wang, Yuyuan;Mao, Yu;...
期刊:
Dyes and Pigments ,2020年176:108229 ISSN:0143-7208
通讯作者:
Hu, Qinghua;Wang, Hongqing
作者机构:
[Wang, Hongqing; Huang, Qiuxiang; Hu, Qinghua; Mao, Yu; Wang, HQ; Liang, Kexin; Wang, Yuyuan; Yin, Qiang] Univ South China, Sch Chem & Chem Engn, Hunan Key Lab Design & Applicat Actinide Complexe, 28 Changsheng West Rd, Hengyang 42001, Hunan, Peoples R China.
通讯机构:
[Hu, QH; Wang, HQ] U;Univ South China, Sch Chem & Chem Engn, Hunan Key Lab Design & Applicat Actinide Complexe, 28 Changsheng West Rd, Hengyang 42001, Hunan, Peoples R China.
关键词:
Fluorescent sensors;AIE plus TICT;Phosgene;Colorimetric;Ratiometric
摘要:
Colorless and highly toxic phosgene has long been considered to be a great menace to human health and national security. Excellent AIE + TICT characteristic ratiometric and colorimetric fluorescent sensor TPE-CI was constructed with the combination of the TICT based 3-benzo[d]imidazole-chromen-2-imine unit and AIE based tetraphenylethene (TPE) unit. TPE-CI can detect phosgene not only in organic solvent through a change from the TICT process to the AIE process, but also in solid-state through a new change from the AIE + TICT process to the AIE process. TPE-CI exhibited convenient to use as a test strip, rapid response (less than 6 s in solvent and 2 min in air atmosphere), excellent selectivity and fair sensitivity for visual inspection of trace phosgene in the organic solvent and in the gas phase. The limit of detection (LOD) was calculated and derived as 0.36 μM in solvent and 0.27 ppm in the air atmosphere, which was far below the acute phosgene exposure level of human response. The satisfactory results indicate that this AIE + TICT strategy may offer valuable thinking to develop convenient solid-state optical sensors with dual ratiometric and colorimetric fluorescence response for gaseous phosgene identification. © 2020 Elsevier Ltd
语种:
英文
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Theoretical insights into selective separation of trivalent actinide and lanthanide by ester and amide ligands based on phenanthroline skeleton
作者:
Wang, Cui;Wu, Qun-Yan* ;Wang, Cong-Zhi;Lan, Jian-Hui;Nie, Chang-Ming* ;...
期刊:
DALTON TRANSACTIONS ,2020年49(13):4093-4099 ISSN:1477-9226
通讯作者:
Nie, Chang-Ming;Wu, Qun-Yan;Shi, Wei-Qun
作者机构:
[Nie, Chang-Ming; Wang, Cui] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Wu, Qun-Yan; Shi, Wei-Qun; Chai, Zhi-Fang; Wang, Cong-Zhi; Lan, Jian-Hui; Wang, Cui] 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;[Wu, QY; Shi, WQ] 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:
Phenanthroline based ligands have shown potential performance for partitioning trivalent actinides from lanthanides. In this work, we have explored four ester and amide ligands based on the phenanthroline skeleton and elucidated the separation mechanism between Am(iii) and Eu(iii) ions. The molecular geometries and extraction reactions of the metal-ligand complexes were modeled by using scalar-relativistic density functional theory. The results show that the amide based ligands have stronger coordination ability with the metal ions than the corresponding ester based ligands. According to the thermodynamic results, ligands N,N′-diethyl-N,N′-ditolyl-2,9-diamide-1,10-phenanthroline (L2) and N,N′-(1,10-phenanthroline-2,9-diyl)bis(N-ethyl-P-methyl-N-(p-tolyl)phosphinic amide) (L4) appear to have the strongest complexing ability, which is supported by the result of electrostatic potential (ESP) and the M-OL bond orders. Moreover, ligand L2 has excellent selectivity for Am(iii)/Eu(iii) among the four ligands. Additionally, the bonding properties between the metal ions and the ligands reveal that the Am(iii)/Eu(iii) selectivity stems from the Am-N bonds with more covalent character, which is supported by the analysis of the hardness of the ligands and the bond orders. This work provides useful information for understanding the Am(iii)/Eu(iii) selectivity of phenanthroline derived ligands bearing ester and amide groups. This journal is © The Royal Society of Chemistry.
语种:
英文
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Aryl Diazonium-Assisted Amidoximation of MXene for Boosting Water Stability and Uranyl Sequestration via Electrochemical Sorption
作者:
Zhang, Pengcheng;Wang, Lin;Huang, Zhiwei;Yu, Jipan;Li, Zijie;...
期刊:
ACS Applied Materials & Interfaces ,2020年12(13):15579-15587 ISSN:1944-8244
通讯作者:
Shi, Weiqun
作者机构:
[Huang, Zhiwei; Yuan, Liyong; Shi, Weiqun; Yu, Jipan; Zhang, Pengcheng; Mei, Lei; Yin, Taiqi; Deng, Hao; Li, Zijie; Wang, Lin] Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.;[Wang, Hongqing; Zhang, Pengcheng] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Gibson, John K.] Lawrence Berkeley Natl Lab, Chem Sci Div, Berkeley, CA 94720 USA.;[Zheng, Lirong] Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China.;[Chai, Zhifang] Chinese Acad Sci, Ningbo Inst Ind Technol, Engn Lab Adv Energy Mat, Ningbo 315201, Peoples R China.
通讯机构:
[Shi, Weiqun] C;Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.
关键词:
MXene;amidoxime group;diazonium salt;uranium capture;electrosorption
摘要:
Despite that two-dimensional transition metal carbides and carbonitrides (MXenes) are burgeoning candidates for remediation of environmental pollutants, the construction of robust functionalized MXene nanosheets with a high affinity for target heavy metal ions and radionuclides remains a challenge. Here we report the successful placement of amidoxime chelating groups on Ti3C2Tx MXene surface by diazonium salt grafting. The introduction of amidoxime functional groups significantly enhances the selectivity of Ti3C2Tx nanosheets for uranyl ions and also greatly improves their stability in aqueous solution, enabling efficient, rapid, and recyclable uranium extraction from aqueous solutions containing competitive metal ions. Benefiting from the excellent conductivity of MXenes, the amidoxime functionalized Ti3C2Tx nanosheets show outstanding electrochemical performance such that when loaded on carbon cloth the application of an electric field increases the uranium adsorption capacity from 294 to 626 mg/g, outperforming all organic electrochemical sorption materials reported previously. The present work provides an effective strategy to functionalize MXene nanosheets with fundamental implications for the design of MXene-based selective electrosorption electrode materials. Copyright © 2020 American Chemical Society.
语种:
英文
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Visible-light-induced decarboxylative acylation of quinoxalin-2(1: H)-ones with α-oxo carboxylic acids under metal-, strong oxidant- And external photocatalyst-free conditions
作者:
Xie, Long-Yong;Bai, You-Shu;Xu, Xiang-Qin;Peng, Xia;Tang, Hai-Shan;...
期刊:
Green Chemistry ,2020年22(5):1720-1725 ISSN:1463-9262
通讯作者:
He, Wei-Min
作者机构:
[Bai, You-Shu; He, Wei-Min; Tang, Hai-Shan; Xu, Xiang-Qin; Peng, Xia; Xie, Long-Yong] Hunan Univ Sci & Engn, Dept Chem, Yongzhou 425100, Peoples R China.;[Huang, Ying; Cao, Zhong] Changsha Univ Sci & Technol, Hunan Prov Key Lab Mat Protect Elect Power & Tran, Changsha 410114, 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] H;Hunan Univ Sci & Engn, Dept Chem, Yongzhou 425100, Peoples R China.
摘要:
A mild and eco-friendly visible-light-induced decarboxylative acylation of quinoxalin-2(1H)-ones and α-oxo carboxylic acids with ambient air as the sole oxidant at room temperature was established. The reaction proceeded efficiently without any metal catalysts, strong oxidants or external-photosensitizers, ultimately reducing the generation of waste. This journal is © The Royal Society of Chemistry.
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英文
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Ag-Bi/BiVO4 chain-like hollow microstructures with enhanced photocatalytic activity for CO2 conversion
作者:
Duan, Zeyu;Zhao, Xiaojun;Wei, Chuanwan;Chen, Limiao*
期刊:
Applied Catalysis A: General ,2020年594:117459 ISSN:0926-860X
通讯作者:
Chen, Limiao
作者机构:
[Duan, Zeyu; Zhao, Xiaojun; Chen, Limiao] Cent South Univ, Coll Chem & Chem Engn, Hunan Prov Key Lab Micro & Nano Mat Interface Sci, Changsha 410083, Peoples R China.;[Wei, Chuanwan] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
通讯机构:
[Chen, Limiao] C;Cent South Univ, Coll Chem & Chem Engn, Hunan Prov Key Lab Micro & Nano Mat Interface Sci, Changsha 410083, Peoples R China.
关键词:
Ag-Bi/BiVO4;CO2 reduction;Heterojunction;Hollow structure;Photocatalytic activity
摘要:
Developing semiconductor-based photocatalysts with high activity and stability to reduce CO2 into valuable solar fuels is of great significance because of the increasingly serious energy crisis and global warming. Here, metallic Ag and Bi nanoparticles co-decorated BiVO4 (Ag-Bi/BiVO4) chain-like hollow microstructures were prepared via construction of Bi/BiVO4 hollow microstructures followed by coupling with Ag through a galvanic replacement reaction between Bi and AgNO3. The characterization results demonstrated that as-fabricated Ag-Bi/BiVO4 composites possess unique features such as extended visible-light response, rich oxygen vacancies (OVs), elevated conduction band, and high separation efficiency of photoexcited electron-hole pairs, which endow the Ag-Bi/BiVO4 composites with a surprising photocatalytic performance toward CO2 conversion to CO under visible light irradiation. The present work develops a feasible and effective strategy for developing BiVO4-based photocatalysts with suitable electronic band structure to improve the efficiency of CO2 conversion under the irradiation of visible-light. © 2020 Elsevier B.V.
语种:
英文
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Fabrication of hypoxia-responsive and uperconversion nanoparticles-modified RBC micro-vehicles for oxygen delivery and chemotherapy enhancement
作者:
Wang, Peiyuan;Jiang, Suhua;Li, Yang;Luo, Qiang;Lin, Jinyan;...
期刊:
BIOMATERIALS SCIENCE ,2020年8(16):4595-4602 ISSN:2047-4830
通讯作者:
Fan, Lingling;Zhu, Jun
作者机构:
[Jiang, Suhua; Luo, Qiang; Lin, Jinyan; Wang, Peiyuan; Li, Yang] Chinese Acad Sci, Fujian Inst Res Struct Matter, Key Lab Design & Assembly Funct Nanostruct, Fuzhou 350002, Peoples R China.;[Luo, Qiang; Fan, Lingling; Xu, Congjian; Wang, Peiyuan] Fudan Univ, Obstet & Gynecol Hosp, Shanghai 200011, Peoples R China.;[Jiang, Suhua; Luo, Qiang; Lin, Jinyan; Wang, Peiyuan; Li, Yang] Fujian Med Univ, Mengchao Hepatobiliary Hosp, United Innovat Mengchao Hepatobiliary Technol Key, Fuzhou 350025, Peoples R China.;[Jiang, Suhua; Lin, Jinyan; Wang, Peiyuan; Li, Yang] Chinese Acad Sci, Xiamen Inst Rare Earth Mat, Dept Translat Med, Xiamen 361024, Peoples R China.;[Hu, Lidan] Univ South China, Dept Biochem & Mol Biol, Hunan Prov Cooperat Innovat Ctr Mol Target New Dr, Hengyang 421001, Peoples R China.
通讯机构:
[Fan, Lingling] F;[Zhu, Jun] T;Fudan Univ, Obstet & Gynecol Hosp, Shanghai 200011, Peoples R China.;Tongji Univ, Sch Med, Shanghai Pulm Hosp, Dept Oncol, Shanghai, Peoples R China.
摘要:
Solid tumor cells in hypoxic regions resist chemotherapy treatment with conventional antitumor drugs (such as paclitaxel, PTX) because the inadequate O2 attenuates the intracellular generation of reactive oxygen species (ROS) and upregulates multidrug resistance protein expression. Hyperbaric O2 therapy concentrates on improving O2 delivery to the hypoxic tumor area, thereby enhancing the sensitivity of cancer cells to chemotherapy drugs. However, the implementation of this therapy often elicits immune response or potentiates toxicity of the drugs toward normal cells. In this work, we successfully fabricated RBC-based micro-vehicles for precise hypoxia-activated O2 delivery under the 980 nm laser irradiation. Interestingly, the subsequent chemotherapy of PTX for ovarian tumors was significantly enhanced owing to the alleviation of hypoxia tumor microenvironment. Meanwhile, the RBC-based micro-vehicles have low side tissue effects, superior biocompatibility, and ultra-low immune response. Overall, the RBC-based drug delivery system holds a fascinating perspective towards O2 delivery for chemotherapy enhancement in other clinical solid malignancies. This journal is © The Royal Society of Chemistry.
语种:
英文
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Amidoxime-Functionalized Covalent Organic Nanosheets for Sequestration of Uranium in Vivo
作者:
Chen, Long;Bai, Ru;Wang, Xiaomei;Zhang, Yijing;He, Linwei;...
期刊:
ACS Applied Bio Materials ,2020年3(12):8731-8738 ISSN:2576-6422
通讯作者:
Diwu, Juan(diwujuan@suda.edu.cn)
作者机构:
[Chen, Long; Bai, Ru; Wang, Xiaomei; Zhang, Yijing; He, Linwei; Zhang, Mingxing; Chong, Yu; Chai, Zhifang; Diwu, Juan] State Key Laboratory of Radiation Medicine and Protection, School for Radiological and Interdisciplinary Sciences (RAD-X), Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University, Suzhou;215123, China;[Wang, Xiao-Feng] School of Chemistry and Chemical Engineering, Hunan Key Laboratory for the Design and Application of Actinide Complexes, University of South China, Hengyang;421001, China;[Chen, Long; Wang, Xiaomei; Zhang, Yijing; He, Linwei; Zhang, Mingxing; Chong, Yu; Chai, Zhifang; Diwu, Juan] 215123, China
通讯机构:
[Diwu, J.] S;State Key Laboratory of Radiation Medicine and Protection, China
关键词:
amidoxime;covalent organic nanosheets;post-modifications;sequestration;uranyl
摘要:
Finding efficient actinide decorporation agents is crucial for public health and the development of the nuclear industry. The current inventory of decorporation agents is predominately limited to a handful of ligands. In this work, a two-dimensional (2D) covalent organic nanosheet (CON) material was rationally designed and tested for in vivo uranium decorporation. This material is extensively grafted with amidoxime (AO), a classic uranium-recognition ligand, which not only provides selective binding sites for uranyl but also expands the interlayer spacing of CON, making the active sites more accessible. Significantly, the results of in vivo experiments demonstrate that, in both prophylactic and prompt administration groups, CON-AO exhibits a higher excretion ratio of uranium from kidneys than that of ZnNa3-diethylenetriamine pentaacetate (DTPA), while presenting a similar level of cytotoxicity. These results suggest that functionalized CONs may emerge as a promising type of actinide in vivo decorporation agent. ©
语种:
英文
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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
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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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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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