Dual-function surface hydrogen bonds enable robust O2activation for deep photocatalytic toluene oxidation
作者：
Li, Hao;Jiang, Fuze;Drdova, Sarka;Shang, Huan;Zhang, Lizhi;...
期刊：
Catalysis Science & Technology ,2021年11(1):319-331 ISSN：2044-4753
通讯作者：
Wang, Jing
作者机构：
[Drdova, Sarka; Li, Hao; Wang, Jing; Jiang, Fuze] Swiss Fed Inst Technol, Inst Environm Engn, CH-8093 Zurich, Switzerland.;[Drdova, Sarka; Li, Hao; Wang, Jing; Jiang, Fuze] Swiss Fed Labs Mat Sci & Technol, Empa, Lab Adv Analyt Technol, CH-8600 Dubendorf, Switzerland.;[Zhang, Lizhi; Shang, Huan] Cent China Normal Univ, Coll Chem, Inst Appl & Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[Wang, Jing] S;Swiss Fed Inst Technol, Inst Environm Engn, CH-8093 Zurich, Switzerland.;Swiss Fed Labs Mat Sci & Technol, Empa, Lab Adv Analyt Technol, CH-8600 Dubendorf, Switzerland.
摘要：
Solar-driven molecular oxygen activation by semiconductor photocatalysts is a prototypical reaction manifesting complex interactions among photons, charge carriers, and reactants. In this study, we demonstrate that energetic O2 activation towards volatile organic compound control can be realized via constructing a sophisticated surface hydrogen bond (HB) network having a dual-function. The extensive HBs established between the hydroxyl-rich BiOCl surface and phosphoric acid are first shown to significantly weaken surface Bi-O bonds, enabling facile oxygen vacancy (OV) generation. OVs, which act as reliable electron capture and static O2 activation centers, reinforce the interaction between photons and excitons for rapid charge carrier separation. Moreover, dynamic O2 activation with sluggish kinetics can be surmounted by another type of HB localized between hydroxyl groups of phosphoric acid and OV-adsorbed O2. These unique localized HBs facilitate interfacial electron transfer from BiOCl to O2, displaying a unique energy coupling route between charge carriers and reactants. For simulated indoor toluene oxidation, the substantially boosted O2 activation is shown to accelerate the kinetic processes associated with the primary oxidation of toluene into benzaldehyde and benzoic acid, as well as aromatic ring opening towards deep oxidation. Undesirable intermediate accumulation and catalyst deactivation are thus avoided. The present work highlights the pivotal roles of HBs in robust photocatalytic O2 activation. It will provide novel insights into the design of high-performance catalysts for efficient and safe control of indoor volatile organic compounds. This journal is © The Royal Society of Chemistry.
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Thermo-controllable dehydrogenation of ammonia borane by luminescent and thermo-responsive catalysts based on SiO2@Pt@PABI-Tb@PNIPAM
作者：
Huang, Hui;Wang, Jun* ;Xu, Yafei;Xu, Rui;Li, Wuke
期刊：
Applied Catalysis A: General ,2020年594:117463 ISSN：0926-860X
通讯作者：
Wang, Jun
作者机构：
[Li, Wuke; Xu, Yafei; Xu, Rui; Huang, Hui; Wang, Jun] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.
通讯机构：
[Wang, Jun] C;Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.
关键词：
Ammonia borane;Dehydrogenation;Luminescence;Thermo-responsive
摘要：
In this paper, a luminescent and thermo-responsive catalyst based on SiO2@[email protected]@PNIPAM was prepared by incorporating Pt nanoparticles, luminescent material and mesoporous silica with thermo-responsive polymer. The obtained catalyst was characterized by IR, TGA, UV–vis, SEM, TEM, X-ray photoelectron spectroscopy and luminescence. The hybrid catalyst exhibits “on-off” green luminescence in solution under UV irradiation, which could be observed by eyes. The catalytic results indicate that the dehydrogenation of ammonia borane (AB) catalyzed by SiO2@[email protected]@PNIPAM is thermo-controllable and switchable. The SiO2@[email protected]@PNIPAM shows high catalytic activity for the generation of hydrogen at room temperature. However, it exhibits much lower catalytic activity at high temperature. The catalysts exhibit excellent durability because the support and polymer could prevent the aggregation and leaching of Pt nanoparticles during catalysis. The catalytic research offers a new approach to the thermo-controllable application in the generation of hydrogen from AB. © 2020 Elsevier B.V.
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Design and synthesis of novel phthalazinone derivatives as potent poly(ADP-ribose)polymerase 1 inhibitors
作者：
Xin, Minhang* ;Sun, Jiajia;Huang, Wei* ;Tang, Feng;Liu, Zhaoyu;...
期刊：
FUTURE MEDICINAL CHEMISTRY ,2020年12(19):1691-1707 ISSN：1756-8919
通讯作者：
Xin, Minhang;Huang, Wei
作者机构：
[Xin, Minhang; Sun, Jiajia] Xi An Jiao Tong Univ, Hlth Sci Ctr, Sch Pharm, Dept Med Chem, 76 Yanta West Rd, Xian 710061, Peoples R China.;[Huang, Wei] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Tang, Feng; Liu, Zhaoyu; Wang, Jia; Jin, Qiu] Jiangsu Simcere Pharmaceut Co Ltd, 699-18 Xuan Wu Dist, Nanjing 210042, Peoples R China.
通讯机构：
[Xin, Minhang] X;[Huang, Wei] C;Xi An Jiao Tong Univ, Hlth Sci Ctr, Sch Pharm, Dept Med Chem, 76 Yanta West Rd, Xian 710061, Peoples R China.;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
关键词：
lead compound;PARP-1 inhibitors;phthalazinone derivatives;potent;sensitizing effect
摘要：
Aim: The development of effective PARP-1 inhibitors has received great enthusiasm in medicinal chemistry communities. Results: A new series of novel phthalazinone derivatives were designed and synthesized. Among these, B1 and B16 displayed more potent PARP-1 inhibitory activities than olaparib. B16 gave an IC50 value of 7.8 nM against PARP-1, and a PF50 value of 3.4 in the sensitizing effect assay. The in vivo pharmacokinetic properties evaluation showed B16 displayed insufficient oral exposure, and it was also not stable in rat blood. Conclusion: The results indicated that our design phthalazinone derivatives were potent PARP-1 inhibitors, and compound B16 was a valuable lead compound with significant in vitro efficacy, deserving further optimization to develop anticancer drug candidate. © 2020 Future Medicine Ltd.. All rights reserved.
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英文
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Synthesis and Evaluation of Halogenated 5-(2-Hydroxyphenyl)pyrazoles as Pseudilin Analogues Targeting the Enzyme IspD in the Methylerythritol Phosphate Pathway
作者：
Wang, Jili;Zhou, Yaqing;Wang, Xiuwen;Duan, Lixia;Duan, Jiang;...
期刊：
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY ,2020年68(10):3071-3078 ISSN：0021-8561
通讯作者：
Li, Weiguo;Zhang, Aidong
（ 作者机构：
[Zhang, Aidong; Zhou, Yaqing; Wang, Jili; Wang, Xiuwen; Li, Weiguo; Duan, Jiang; Li, WG; Duan, Lixia] Cent China Normal Univ, Coll Chem, Key Lab Pesticides & Chem Biol, Minist Educ, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Li, WG; Zhang, AD] C;Cent China Normal Univ, Coll Chem, Key Lab Pesticides & Chem Biol, Minist Educ, Wuhan 430079, Hubei, Peoples R China.
关键词：
MEP pathway;IspD;pseudilin;analogue;5-(2-hydroxyphenyl)pyrazole;synthesis;herbicide
摘要：
This work reports halogenated 5-(2-hydroxyphenyl)pyrazoles as pseudilin analogues with the potential to target the enzyme IspD in the methylerythritol phosphate (MEP) pathway. Such analogues were designed using the bioisosteric replacement of the pseudilin core structure and synthesized via an efficient three-step route. With AtIspD-based screening and pre- and post-emergence herbicidal tests, these compounds were demonstrated to have considerable activities against AtIspD, with IC50 up to 3.27 μM, and against model plants rape and barnyard grass, with moderate to excellent activities. At a rate of 150 g/ha in the greenhouse test, three compounds exhibited higher or comparable herbicidal activities than pseudilin. Molecular docking of representative compounds into the allosteric site of AtIspD revealed a binding mode similar to that of pseudilin. The established bioisosterism and synthesis method in this work may serve as an important tool for the development of new herbicides and antimicrobials targeting IspD in the MEP pathway. © 2020 American Chemical Society.
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Efficient Ammonia Electrosynthesis from Nitrate on Strained Ruthenium Nanoclusters
作者：
Li, Jie;Zhan, Guangming;Yang, Jianhua;Quan, Fengjiao;Mao, Chengliang;...
期刊：
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY ,2020年142(15):7036-7046 ISSN：0002-7863
通讯作者：
Zhang, Lizhi;Yu, Jimmy C.
作者机构：
[Xu, Liangpang; Lei, Fengcai; Chan, Alice W. M.; Li, Lejing; Liu, Yang; Yu, Jimmy C.; Li, Jie] Chinese Univ Hong Kong, Dept Chem, Shatin, Hong Kong, Peoples R China.;[Quan, Fengjiao; Zhang, Lizhi; Shi, Yanbiao; Mao, Chengliang; Zhan, Guangming] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Minist Educ,Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.;[Wang, Jianfang; Yang, Jianhua] Chinese Univ Hong Kong, Dept Phys, Shatin, Hong Kong, Peoples R China.;[Wong, Po Keung; Wang, Bo] Chinese Univ Hong Kong, Sch Life Sci, Shatin, Hong Kong, Peoples R China.;[Du, Yi; Dou, Shi-Xue] Univ Wollongong, AIIM, ISEM, Wollongong, NSW 2500, Australia.
通讯机构：
[Zhang, Lizhi; Yu, Jimmy C.] C;Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Minist Educ,Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.;Chinese Univ Hong Kong, Dept Chem, Shatin, Hong Kong, Peoples R China.
摘要：
The limitations of the Haber-Bosch reaction, particularly high-temperature operation, have ignited new interests in low-temperature ammonia-synthesis scenarios. Ambient N-2 electroreduction is a compelling alternative but is impeded by a low ammonia production rate (mostly <10 mmol g(cat)(-1) h(-1)), a small partial current density (<1 mA cm(-2)), and a high-selectivity hydrogen-evolving side reaction. Herein, we report that room-temperature nitrate electroreduction catalyzed by strained ruthenium nanoclusters generates ammonia at a higher rate (5.56 g(cat)(-1) h(-1)) than the Haber- Bosch process. The primary contributor to such performance is hydrogen radicals, which are generated by suppressing hydrogen-hydrogen dimerization during water splitting enabled by the tensile lattice strains. The radicals expedite nitrate-to-ammonia conversion by hydrogenating intermediates of the rate-limiting steps at lower kinetic barriers. The strained nanostructures can maintain nearly 100% ammonia-evolving selectivity at >120 mA cm(-2) current densities for 100 h due to the robust subsurface Ru-O coordination. These findings highlight the potential of nitrate electroreduction in real-world, low-temperature ammonia synthesis.
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英文
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Hydrogen Spillover to Oxygen Vacancy of TiO2- xHy/Fe: Breaking the Scaling Relationship of Ammonia Synthesis
作者：
Mao, Chengliang;Wang, Jiaxian;Zou, Yunjie;Qi, Guodong;Loh, Joel Yi Yang;...
期刊：
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY ,2020年142(41):17403-17412 ISSN：0002-7863
通讯作者：
Zhang, Lizhi;Ozin, Geoffrey A.
作者机构：
[Zhang, Lizhi; Zou, Yunjie; Liu, Xiao; Ai, Zhihui; Wang, Jiaxian; Mao, Chengliang; Shang, Huan; Zhao, Jincai; Li, Jie; Li, Meiqi] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Ghoussoub, Mireille; Mao, Chengliang; Wang, Lu; Xia, Meikun; Ozin, Geoffrey A.] Univ Toronto, Dept Chem, Solar Fuels Cluster, Mat Chem & Nanochem Res Grp, Toronto, ON M5S 3H6, Canada.;[Qi, Guodong; Xu, Jun; Deng, Feng] Chinese Acad Sci, State Key Lab Magnet Resonance & Atom & Mol Phys, Natl Ctr Magnet Resonance Wuhan, Wuhan Inst Phys & Math,Innovat Acad Precis Measur, Wuhan 430071, Peoples R China.;[Loh, Joel Yi Yang; Kherani, Nazir P.] Univ Toronto, Dept Mat Sci & Engn, Toronto, ON M5S 3E4, Canada.;[Zhang, Tianhua] Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst NERC C, Sch Chem Engn, Fuzhou 350002, Fujian, Peoples R China.
通讯机构：
[Zhang, Lizhi] C;[Ozin, Geoffrey A.] U;Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;Univ Toronto, Dept Chem, Solar Fuels Cluster, Mat Chem & Nanochem Res Grp, Toronto, ON M5S 3H6, Canada.
摘要：
Optimizing kinetic barriers of ammonia synthesis to reduce the energy intensity has recently attracted significant research interest. The motivation for the research is to discover means by which activation barriers of N2 dissociation and NHz (z = 1-2, surface intermediates) destabilization can be reduced simultaneously, that is, breaking the "scaling relationship". However, by far only a single success has been reported in 2016 based on the discovery of a strong-weak N-bonding pair: transition metals (nitrides)-LiH. Described herein is a second example that is counterintuitively founded upon a strong-strong N-bonding pair unveiled in a bifunctional nanoscale catalyst TiO2-xHy/Fe (where 0.02 ≤ x ≤ 0.03 and 0 < y < 0.03), in which hydrogen spillover (H) from Fe to cascade oxygen vacancies (OV-OV) results in the trapped form of OV-H on the TiO2-xHy component. The Fe component thus enables facile activation of N2, while the OV-H in TiO2-xHy hydrogenates the N or NHz to NH3 easily. © 2020 American Chemical Society.
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英文
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Structural insights into the photoactivation of Arabidopsis CRY2
作者：
Ma, Ling;Guan, Zeyuan;Wang, Qiang;Yan, Xuhui;Wang, Jing;...
期刊：
NATURE PLANTS ,2020年6(12):1432-1438 ISSN：2055-026X
通讯作者：
Yin, Ping;Gong, Xin
作者机构：
[Yin, Ping; Yan, Xuhui; Wang, Qiang; Zhang, Delin; Ma, Ling; Wang, Jing; Guan, Zeyuan] Huazhong Agr Univ, Natl Key Lab Crop Genet Improvement, Wuhan, Peoples R China.;[Yin, Ping; Yan, Xuhui; Wang, Qiang; Zhang, Delin; Ma, Ling; Wang, Jing; Guan, Zeyuan] Huazhong Agr Univ, Natl Ctr Plant Gene Res, Wuhan, Peoples R China.;[Ma, Ling] Chinese Univ Hong Kong, Kobilka Inst Innovat Drug Discovery, Shenzhen, Peoples R China.;[Ma, Ling] Univ Sci & Technol China, Sch Life Sci, Hefei, Peoples R China.;[Wang, Zhizheng] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan, Peoples R China.
通讯机构：
[Yin, Ping] H;[Gong, Xin] S;Huazhong Agr Univ, Natl Key Lab Crop Genet Improvement, Wuhan, Peoples R China.;Huazhong Agr Univ, Natl Ctr Plant Gene Res, Wuhan, Peoples R China.;Southern Univ Sci & Technol, Dept Biol, Shenzhen, Guangdong, Peoples R China.
摘要：
The blue-light receptor cryptochrome (CRY) in plants undergoes oligomerization to transduce blue-light signals after irradiation, but the corresponding molecular mechanism remains poorly understood. Here, we report the cryogenic electron microscopy structure of a blue-light-activated CRY2 tetramer at a resolution of 3.1 Å, which shows how the CRY2 tetramer assembles. Our study provides insights into blue-light-mediated activation of CRY2 and a theoretical basis for developing regulators of CRYs for optogenetic manipulation. © 2020, The Author(s), under exclusive licence to Springer Nature Limited.
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英文
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Modulation of an intermediate layer between NiCoP and Ni foam substrate in a microwire array electrode for enhancing the hydrogen-evolution reaction
作者：
Guo, Dan;Chen, Huayu;Tian, Hanmin* ;Ouyang, Shuxin* ;Wang, Jianbo;...
期刊：
Chemical Communications ,2020年56(37):4990-4993 ISSN：1359-7345
通讯作者：
Tian, Hanmin;Ouyang, Shuxin;Lv, Jun
作者机构：
[Tian, Hanmin; Guo, Dan] Hebei Univ Technol, Sch Elect & Informat Engn, Tianjin 300400, Peoples R China.;[Chen, Huayu] China Jiliang Univ, Coll Mat & Chem, Hangzhou 310018, Peoples R China.;[Chen, Huayu] Tianjin Univ, TJU NIMS Int Collaborat Lab, Sch Mat Sci & Engn, Tianjin 300072, Peoples R China.;[Ouyang, Shuxin] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.;[Wang, Jianbo] Southeast Univ, Sch Elect Sci & Engn, Nanjing 210096, Peoples R China.
通讯机构：
[Tian, Hanmin] H;[Ouyang, Shuxin] C;[Lv, Jun] L;[Lv, Jun] S;Hebei Univ Technol, Sch Elect & Informat Engn, Tianjin 300400, Peoples R China.
摘要：
A hierarchical electrode consisting of a Ni foam substrate, an intermediate layer of a Mo-doped basic cobalt carbonate microwire array, and a surface layer of NiCoP was fabricated for hydrogen evolution. The introduction of the intermediate layer accounted for the low overpotential (45 mV, 10 mA cm-2) and high solar-to-hydrogen conversion efficiency (14.9%) in a PEC water splitting application. © The Royal Society of Chemistry 2020.
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英文
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Dual-site activation enhanced photocatalytic removal of no with Au/CeO2
作者：
Shang, Huan;Huang, Shun;Li, Hao;Li, Meiqi;Zhao, Shengxi;...
期刊：
Chemical Engineering Journal ,2020年386:124047 ISSN：1385-8947
通讯作者：
Ai, Zhihui;Zhang, Lizhi
作者机构：
[Wang, Jiaxian; Zhang, Lizhi; Shang, Huan; Li, Hao; Ai, ZH; Zhang, LZ; Zhao, Shengxi; Huang, Shun; Ai, Zhihui; Li, Meiqi] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm & Appl Chem, Wuhan 430079, Peoples R China.
通讯机构：
[Ai, ZH; Zhang, LZ] C;Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm & Appl Chem, Wuhan 430079, Peoples R China.
关键词：
Air purification;Dual-site activation;Oxygen vacancy;Photocatalytic NO removal
摘要：
Photocatalytic technology provides an effective strategy for aerobic purification of dilute gaseous NO pollutant, but suffers from its low efficiency. In this study, we demonstrate that the bicomponent Au/CeO2 photocatalyst possesses an enhanced photocatalytic NO removal performance under visible light irradiation, with a higher NO conversion efficiency (65%) and triple rate constant (0.1451 min−1) versus CeO2 (50%, 0.0448 min−1). Density function theory calculations and experimental results revealed that oxygen vacancies on the CeO2 component could favorably initiate the adsorption and activation of O2 to generate [rad]O2−, simultaneously, Au nanoparticles loaded on the CeO2 surface were active centers for adsorption and activation of NO to produce NO+ by plasmonic holes of the Au under visible light irradiation. Subsequently, these [rad]O2− and NO+ species generated via dual-site activation pathway on Au/CeO2 photocatalyst reacted spontaneously to generate the final NO3−, leading to enhanced photocatalytic removal of NO. This study sheds light on a dual-site induced photocatalytic NO oxidation and advances the design of effective air purification photocatalyst. © 2020 Elsevier B.V.
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英文
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Temperature/pH dual-responsive and luminescent drug carrier based on PNIPAM-MAA/lanthanide-polyoxometalates for controlled drug delivery and imaging in HeLa cells
作者：
Wang, Jun* ;Huang, Na;Peng, Qi;Cheng, Xiaoyan;Li, Wuke
期刊：
Materials Chemistry and Physics ,2020年239:121994 ISSN：0254-0584
通讯作者：
Wang, Jun
作者机构：
[Li, Wuke; Peng, Qi; Cheng, Xiaoyan; Wang, Jun; Huang, Na] Cent China Normal Univ, Coll Chem, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Wang, Jun] C;Cent China Normal Univ, Coll Chem, Wuhan 430079, Hubei, Peoples R China.
关键词：
Lanthanide-polyoxornetalates;Dual-responsive;Luminescence;Controlled release;Bioimaging
摘要：
In this paper, the luminescent temperature/pH dual-responsive nanoparticles based on lanthanide-polyoxometalates were fabricated as a controllable drug delivery system. In the drug delivery carrier, the mesoporous silica acted as the core, and the poly (N-isopropylacrylamide-co-methacrylic acid) and lanthanide-polyoxometalates served as the dual-responsive shell and luminescent labeling, respectively. Composite hydrogels exhibited red luminescence under UV Irradiation, which was visible to the naked eye. The releases of doxorubicin hydrochloride (DOX) from the composites were temperature/pH-dependent. DOX can be quickly released in an acidic environment and at high temperatures. Moreover, the drug delivery carrier showed minimal toxicity to HeLa cells and exhibited good biocompatibility. However, DOX loaded drug-delivery system showed the significant toxicity to HeLa cancer cells in vitro. Cell imaging has shown that lanthanide polyoxometalates composites can be used as bioimaging materials for cell monitoring. As a result, the drug delivery systems based on lanthanide-polyoxometalates have potential applications in the field of biomedical science.
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英文
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Fabrication of PNIPAM-chitosan/decatungstoeuropate/silica nanocomposite for thermo/pH dual-stimuli-responsive and luminescent drug delivery system
作者：
Huang, Na;Wang, Jun* ;Cheng, Xiaoyan;Xu, Yafei;Li, Wuke
期刊：
Journal of Inorganic Biochemistry ,2020年211:111216 ISSN：0162-0134
通讯作者：
Wang, Jun
作者机构：
[Li, Wuke; Xu, Yafei; Cheng, Xiaoyan; Wang, Jun; Huang, Na] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.
通讯机构：
[Wang, Jun] C;Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.
关键词：
Biocompatible;Dual-responsive;Chitosan;Luminescence;Drug delivery;Cells
摘要：
A luminescent and dual-stimuli-responsive nanocomposite based on mesoporous silica, poly (N-isopropylacrylamide)-chitosan and decatungstoeuropate was prepared. To fabricate the nanocomposite, the mesoporous silica nanoparticles were coated with thermo/pH dual-responsive poly (N-isopropylacrylamide)-chitosan and the luminescent decatungstoeuropate particles were grafted onto copolymers. The designed nanocarrier could show exhibit good red luminescence as well as obvious thermo/pH stimuli-responsive properties, which could be employed as a drug storage reservoir for the loading and release of anticancer drug doxorubicin (DOX). The research indicated that the releases of DOX were thermo/pH dependent and high temperatures/acidic conditions were favorable for the fast release of drug. In vitro cytotoxicity tests revealed that the drug delivery carrier displayed excellent biocompatible and the composites loaded with DOX showed significant suppression effect on HeLa cells. Luminescence spectra showed that the composite containing decatungstoeuropate displayed fine red luminescence at various temperatures and pH values, which could be utilized as a potential labeling material in field of medicine.
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英文
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A novel BODIPY-based MOF photocatalyst for efficient visible-light-driven hydrogen evolution
作者：
Yang, Heng;Wang, Jinming;Ma, Ji;Yang, Hong;Zhang, Jing;...
期刊：
Journal of Materials Chemistry A ,2019年7(17):10439-10445 ISSN：2050-7488
通讯作者：
Wen, Lili;Peng, Tianyou
作者机构：
[Yang, Hong; Zhang, Jing; Ma, Ji; Yang, Heng; Wen, Lili] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.;[Wang, Jinming; Peng, Tianyou] Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Hubei, Peoples R China.;[Lv, Kangle] South Cent Univ Nationalities, Key Lab Catalysis & Mat Sci, State Ethn Affairs Commiss, Coll Resources & Environm Sci, Wuhan 430074, Peoples R China.
通讯机构：
[Wen, Lili] C;[Peng, Tianyou] W;Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.;Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Hubei, Peoples R China.
摘要：
Considerable attention has been paid to promising applications of photoactive metal-organic frameworks (MOFs) in visible-light-enhanced hydrogen production. In this study, a pillared-paddlewheel type metal-organic framework [Zn2(BODIPY)(BPDC)2]·H2O (denoted as CCNU-1) featuring BODIPY struts, and capable of efficiently absorbing visible light from 200 to 800 nm, has been fabricated, which is thought to be the first BODIPY-based MOF decorated with Pt nanoparticles as the co-catalyst for efficient photocatalytic H2 generation under visible-light illumination. Impressively, Pt/CCNU-1 exhibited a remarkable H2 production rate as high as 4680 μmol g-1 h-1 with the use of l-ascorbic acid as a sacrificial reagent from an aqueous medium, and a high apparent quantum efficiency of 9.06% at 420 nm. To our knowledge, Pt/CCNU-1 is the most visible-light photoactive Pt/MOF composite for H2 generation from water hitherto, highlighting the promising future of MOF materials in solar-to-chemical energy conversion. This work provides significant insights into the development of MOF-based systems for visible-light-responsive photocatalysts for water reduction. © The Royal Society of Chemistry.
语种：
英文
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CRISPR/Cas Systems towards Next-Generation Biosensing
作者：
Li, Yi;Li, Shiyuan;Wang, Jin* ;Liu, Guozhen*
期刊：
Trends in Biotechnology ,2019年37(7):730-743 ISSN：0167-7799
通讯作者：
Liu, Guozhen;Wang, Jin
作者机构：
[Liu, Guozhen; Li, Yi] Univ New South Wales, Fac Engn, ARC Ctr Excellence Nanoscale Biophoton, Grad Sch Biomed Engn, Sydney, NSW 2052, Australia.;[Liu, Guozhen; Li, Yi] Univ New South Wales, Australian Ctr NanoMed, Sydney, NSW 2052, Australia.;[Li, Shiyuan] Shanghai Tolo Biotechnol Co Ltd, Shanghai 200233, Peoples R China.;[Wang, Jin] Shanghai Normal Univ, Coll Life & Environm Sci, Shanghai 200234, Peoples R China.;[Liu, Guozhen] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Liu, Guozhen] U;[Wang, Jin] S;[Liu, Guozhen] C;Univ New South Wales, Fac Engn, ARC Ctr Excellence Nanoscale Biophoton, Grad Sch Biomed Engn, Sydney, NSW 2052, Australia.;Univ New South Wales, Australian Ctr NanoMed, Sydney, NSW 2052, Australia.
关键词：
CRISPR/Cas;Cas12;Cas13;Cas9;biosensing;diagnostics;nucleic acid detection
摘要：
Beyond its remarkable genome editing ability, the CRISPR/Cas9 effector has also been utilized in biosensing applications. The recent discovery of the collateral RNA cleavage activity of the Cas13a effector has sparked even greater interest in developing novel biosensing technologies for nucleic acid detection and promised significant advances in CRISPR diagnostics. Now, along with the discovery of Cas12 collateral cleavage activities on single-stranded DNA (ssDNA), several CRISPR/Cas systems have been established for detecting various targets, including bacteria, viruses, cancer mutations, and others. Based on key Cas effectors, we provide a detailed classification of CRISPR/Cas biosensing systems and propose their future utility. As the field continues to mature, CRISPR/Cas systems have the potential to become promising candidates for next-generation diagnostic biosensing platforms.
语种：
英文
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Liposomal Antitumor Vaccines Targeting Mucin 1 Elicit a Lipid-Dependent Immunodominant Response
作者：
Du, Jing-Jing;Zou, Shi-Yao;Chen, Xiang-Zhao;Xu, Wen-Bo;Wang, Chang-Wei;...
期刊：
CHEMISTRY-AN ASIAN JOURNAL ,2019年14(12):2116-2121 ISSN：1861-4728
通讯作者：
Liu, Zheng;Guo, Jun
作者机构：
[Zhang, Lian; Wang, Jian; Du, Jing-Jing; Zou, Shi-Yao; Yin, Xu-Guang; Zhou, Shi-Hao; Chen, Xiang-Zhao; Xu, Wen-Bo; Tang, Yuan-Kai; Liu, Zheng; Guo, J; Guo, Jun; Wang, Chang-Wei] Cent China Normal Univ, Int Joint Res Ctr Intelligent Biosensing Technol, Hubei Int Sci & Technol Cooperat Base Pesticide &, Key Lab Pesticide & Chem Biol,Minist Educ,Coll Ch, Wuhan 430079, Hubei, Peoples R China.;[Gao, Xiao-Fei] East China Univ Technol, Jiangxi Key Lab Mass Spectrometry & Instrumentat, Nanchang 330013, Jiangxi, Peoples R China.
通讯机构：
[Liu, Z; Guo, J] C;Cent China Normal Univ, Int Joint Res Ctr Intelligent Biosensing Technol, Hubei Int Sci & Technol Cooperat Base Pesticide &, Key Lab Pesticide & Chem Biol,Minist Educ,Coll Ch, Wuhan 430079, Hubei, Peoples R China.
关键词：
MUC1 antigen;NKT cells;cancer;fully synthetic vaccines;liposomes;alphaGalCer
摘要：
The tumor-associated antigen mucin 1 (MUC1) has been pursued as an attractive target for cancer immunotherapy, but the poor immunogenicity of the endogenous antigen hinders the development of vaccines capable of inducing effective anti-MUC1 immunodominant responses. Herein, we prepared synthetic anti-MUC1 vaccines in which the hydrophilic MUC1 antigen was N-terminally conjugated to one or two palmitoyl lipid chains (to form amphiphilic Pam-MUC1 or Pam2-MUC1). These amphiphilic lipid-tailed MUC1 antigens were self-assembled into liposomes containing the NKT cell agonist αGalCer as an adjuvant. The lipid-conjugated antigens reshaped the physical and morphological properties of liposomal vaccines. Promising results showed that the anti-MUC1 IgG antibody titers induced by the Pam2-MUC1 vaccine were more than 30- and 190-fold higher than those induced by the Pam-MUC1 vaccine and the MUC1 vaccine without lipid tails, respectively. Similarly, vaccines with the TLR1/2 agonist Pam3CSK4 as an adjuvant also induced conjugated lipid-dependent immunological responses. Moreover, vaccines with the αGalCer adjuvant induced significantly higher titers of IgG antibodies than vaccines with the Pam3CSK4 adjuvant. Therefore, the non-covalent assembly of the amphiphilic lipo-MUC1 antigen and the NKT cell agonist αGalCer as a glycolipid adjuvant represent a synthetically simple but immunologically effective approach for the development of anti-MUC1 cancer vaccines. © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
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Discovery of potent anti-inflammatory 4-(4,5,6,7-tetrahydrofuro[3,2-c]pyridin-2-yl) pyrimidin-2-amines for use as Janus kinase inhibitors
作者：
Wang, Yazhou* ;Huang, Wei* ;Xin, Minhang;Chen, Pan;Gui, Li;...
期刊：
Bioorganic & Medicinal Chemistry ,2019年27(12):2592-2597 ISSN：0968-0896
通讯作者：
Wang, Yazhou;Huang, Wei;Liu, Fei
作者机构：
[Huang, Wei; Wang, Yazhou] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.;[Gui, Li; Chen, Pan; Zhu, Xinrong; Luo, Hongpeng; Liu, Fei; Huang, Wei; Wang, Yazhou; Wang, Jia; Cong, Xin; Liu, F; Zhao, Xinxin] Jiangsu Simcere Pharmaceut Co Ltd, Jiangsu Key Lab Mol Targeted Antitumor Drug Res, 699-18 Xuanwu Dist, Nanjing 210042, Jiangsu, Peoples R China.;[Xin, Minhang] Xi An Jiao Tong Univ, Sch Pharm, Hlth Sci Ctr, Dept Med Chem, 76 Yanta West Rd, Xian 710061, Peoples R China.;[Gui, Li; Chen, Pan; Liu, Fei; Zhao, Xinxin] Nanjing Noratech Pharmaceut Co Ltd, 9 Weidi Rd,Jiangsu Life Pk, Nanjing 210046, Jiangsu, Peoples R China.;[Wang, Yazhou] Nanjing Sanhome Pharmaceut Co Ltd, Nanjing, Jiangsu, Peoples R China.
通讯机构：
[Wang, YZ; Huang, W; Liu, F] J;Jiangsu Simcere Pharmaceut Co Ltd, Jiangsu Key Lab Mol Targeted Antitumor Drug Res, 699-18 Xuanwu Dist, Nanjing 210042, Jiangsu, Peoples R China.
关键词：
Anti-inflammatory;Furo[3,2-c]pyridine;JAK inhibitor;Rheumatoid arthritis
摘要：
The Janus kinase (JAK) family of tyrosine kinases has been proven to provide targeted immune modulation. Orally available JAK inhibitors have been used for the treatment of immune-mediated inflammatory diseases, such as rheumatoid arthritis (RA). Here, we report the design, synthesis and biological evaluation of 4-(4,5,6,7-tetrahydrofuro[3,2-c]pyridin-2-yl) pyrimidin-2-amino derivatives as JAK inhibitors. Systematic structure-activity relationship studies led to the discovery of compound 7j, which strongly inhibited the four isoforms of JAK kinases. Molecular modeling rationalized the importance of cyanoacetyl and phenylmorpholine moieties. The in vivo investigation indicated that compound 7j possessed favorable pharmacokinetic properties and displayed slightly better anti-inflammatory efficacy than tofacitinib at the same dosage. Accordingly, compound 7j was advanced into preclinical development.
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英文
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Study on student engagement in the course chemistry pedagogy based on mobile learning
作者：
Li, J.;Wang, J.* ;Wu, Z.;Xie, S.;Jiang, A.
期刊：
Journal of Science Education ,2019年20(2):1-24 ISSN：0124-5481
通讯作者：
Wang, J.
作者机构：
College of Chemistry, Central China Normal University, Wuhan, Hubei, China;Normal College, Qingdao University, Qingdao, Shandong, China;School of Foreign Language Education, Qingdao University, Qingdao, Shandong, China;School of Physics and Electronic Technology, Dalian, Liaoning, China
通讯机构：
Normal College, Qingdao University, Qingdao, Shandong, China
关键词：
Chemistry Pedagogy;Mobile learning;Student engagement;Teacher education
摘要：
The pre-service teachers admitted in 2012, 2013 and 2014 to the teacher education program in College of Chemistry in Central China Normal University who have adopted mobile learning in the course Chemistry Pedagogy were selected as the research objects, and those admitted in 2014 but have not had any experience of mobile learning in the course Chemistry Pedagogy were selected as the control group. Through questionnaires, interviews and classroom observations, student engagement in the course was studied. It was found that the pre-service teachers supported the use of mobile devices in their class and their engagement in the course Chemistry Pedagogy based on mobile learning was acceptable; their behavioral engagement, cognitive engagement and emotional engagement were mutually highly positively correlated, but their behavioral engagement was significantly higher than cognitive engagement and emotional engagement; mobile learning significantly promoted students’ course engagement; while to adopt mobile learning technology efficiently, it is necessary to design teaching carefully, trying to stimulate students’ cognitive initiative and self-control in learning to guarantee their deep cognitive engagement; overcoming the emotional barriers generated by technical exchanges and stimulating long-lasting and stable learning motivation can better promote their emotional engagement in chemistry teacher education programs. © 2019, Beijing Science Education Innovation center. All rights reserved.
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英文
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Rapid Aerobic Inactivation and Facile Removal of Escherichia coli with Amorphous Zero-Valent Iron Microspheres: Indispensable Roles of Reactive Oxygen Species and Iron Corrosion Products.
作者：
Sun, Hongwei;Wang, Jian;Jiang, Yao;Shen, Wenjuan;Jia, Falong* ;...
期刊：
Environmental Science & Technology ,2019年53(7):3707-3717 ISSN：0013-936X
通讯作者：
Jia, Falong;Zhang, Lizhi;Liao, Xiaomei
作者机构：
[Zhang, Lizhi; Sun, Hongwei; Shen, Wenjuan; Jia, Falong; Zhang, LZ] Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;[Wang, Jian; Jiang, Yao; Liao, Xiaomei; Wang, Shaohui] Cent China Normal Univ, Sch Life Sci, Hubei Key Lab Genet Regulat & Integrat Biol, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Jia, FL; Zhang, LZ; Liao, Xiaomei] C;Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;Cent China Normal Univ, Sch Life Sci, Hubei Key Lab Genet Regulat & Integrat Biol, Wuhan 430079, Hubei, Peoples R China.
摘要：
Zero valent iron (ZVI) is recently regarded as a promising alternative for water disinfection, but still suffers from low efficiency. Herein we demonstrate that amorphous zerovalent iron microspheres (A-mZVI) exhibit both higher inactivation rate and physical removal efficiency for the disinfection of Escherichia coli than conventional crystalline nanoscale ZVI (C-nZVI) under aerobic condition. The enhanced E. coli inactivation performance of A-mZVI was mainly attributed to more reactive oxygen species (ROSs), especially free •OH, generated by the accelerated iron dissolution and molecular oxygen activation in bulk solution. In contrast, C-nZVI preferred to produce surface bound •OH, and its bactericidal ability was thus hampered by the limited physical contact between C-nZVI and E. coli. More importantly, hydrolysis of dissolved iron released from A-mZVI produced plenty of loose FeOOH to wrap E. coli, increasing the dysfunction of E. coli membrane. Meanwhile, this hydrolysis process lowered the stability of E. coli colloid and caused its rapid coagulation and sedimentation, favoring its physical removal. These findings clarify the indispensable roles of ROSs and iron corrosion products during the ZVI disinfection, and also provide a promising disinfection material for water treatment. Copyright © 2019 American Chemical Society.
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英文
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Reprint of: Acid-mediated four-component tandem cyclization: Access to multifused 1,3-benzoxazine frameworks
作者：
Wang, Jungang;Zhou, Rongrong;Zhuang, Shiyi;Wu, Anxin*
期刊：
Tetrahedron ,2019年74(51):7283-7289 ISSN：0040-4020
通讯作者：
Wu, Anxin
作者机构：
[Wang, Jungang] Guizhou Minzu Univ, Sch Chem Engn, Guiyang 550025, Guizhou, Peoples R China.;[Zhou, Rongrong; Zhuang, Shiyi; Wu, Anxin] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Wu, Anxin] C;Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Hubei, Peoples R China.
关键词：
Multicomponent reaction;Benzoxazine;Multifused heterocycles;Acid-mediated
摘要：
An acid-mediated multicomponent reaction has been developed for the direct synthesis of multifused 1,3-benzoxazine derivatives from simple and readily available arylglyoxal monohydrates and 2-aminobenzyl alcohols under mild conditions. This novel protocol is proposed to proceed through intramolecular poly-heterocyclizations, thus leading to the formation of three new rings and six new chemical bonds, including four CN and two CO bonds.
语种：
英文
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Chiral galactose responsive S-phenethylamine calix [4] arene-based sensing surface
作者：
Zhang, Xujie;Yang, Yuxia;Gu, Yulin;Zhang, Jin;Cheng, Jian;...
期刊：
Sensors and Actuators B-Chemical ,2019年297:126662 ISSN：0925-4005
通讯作者：
Sun, Kunpeng;Li, Haibing
作者机构：
[Sun, Kunpeng; Zhang, Xujie; Gu, Yulin; Yang, Yuxia] Chinese Acad Sci, Natl Engn Res Ctr Fine Petrochem Intermediates, Lanzhou Inst Chem Phys, Lanzhou 730000, Gansu, Peoples R China.;[Zhang, Jin; Zhang, Xujie; Cheng, Jian; Li, Haibing; Wang, Junhua] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol CCNU, Minist Educ, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Sun, Kunpeng; Li, Haibing] C;Chinese Acad Sci, Natl Engn Res Ctr Fine Petrochem Intermediates, Lanzhou Inst Chem Phys, Lanzhou 730000, Gansu, Peoples R China.;Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol CCNU, Minist Educ, Wuhan 430079, Hubei, Peoples R China.
关键词：
Calix[4]arene;Chiral selective;Galactose enantiomer;Self-assembly;Sensing surface
摘要：
Herein, we reported a novel surface based chemosensor, a highly chiral responsive surface recognized galactose enantiomer based on the self-assembly system, which exhibits highly efficient chiral selective for D-galactose via contact angle measurements (CA). We primarily studied the interaction between S-phenethylamine-calix[4]arene (S-DPC4A) and L/D-galactose through the characterization of 1H NMR spectroscopic and UV spectroscopic, then a functional S-DPC4A-based sensing surface were constructed by click reaction and characterized by the analysis of contact angle and X-ray photoelectron spectroscopy (XPS). Interestingly, the S-DPC4A-based sensing surface exhibited highly dynamic responsive for the D-galactose on the tilted interface, realized the weak chiral-interaction signals to convert into the macroscopic properties of materials and reached visual distinction accompanying the changes of surface wettability. © 2019
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英文
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Beyond the Thermal Equilibrium Limit of Ammonia Synthesis with Dual Temperature Zone Catalyst Powered by Solar Light
作者：
Mao, Chengliang;Li, Hao;Gu, Honggang;Wang, Jiaxian;Zou, Yunjie;...
期刊：
Chem ,2019年5(10):2702-2717 ISSN：2451-9294
通讯作者：
Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Li, Hao; Shen, Wenjuan; Zou, Yunjie; Wang, Jiaxian; Mao, Chengliang; Zhao, Jincai; Li, Jie] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;[Gu, Honggang; Liu, Shiyuan] Huazhong Univ Sci & Technol, State Key Lab Digital Mfg Equipment & Technol, Wuhan 430074, Hubei, Peoples R China.;[Qi, Guodong; Xu, Jun; Deng, Feng] Chinese Acad Sci, State Key Lab Magnet Resonance & Atom & Mol Phys, CAS Key Lab Magnet Resonance Biol Syst, Wuhan Inst Phys & Math,Natl Ctr Magnet Resonance, Wuhan 430071, Hubei, Peoples R China.
通讯机构：
[Zhang, Lizhi] C;Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
关键词：
ammonia synthesis;black TiO2;equilibrium limit;Fe nanonecklace;nitrogen fixation;oxygen vacancy;photocatalysis;photothermal catalysis;plasmonic;SDG7: Affordable and clean energy;TiO2
摘要：
Plasmonic local heating effect of Fe nanonecklace endowed TiO2-xHy/Fe catalyst of hot-zone Fe and cool-zone TiO2-xHy, which were responsible for tandem N2 activation and NH3 assembly, respectively. With such dual temperature zones and the tandem kinetic mechanism, light-driven TiO2-xHy/Fe nanonecklace achieved highly efficient ammonia synthesis with NH3 yield beyond the thermodynamic equilibrium limit of thermocatalytic ammonia synthesis. © 2019 Elsevier Inc.Artificial ammonia synthesis (Haber-Bosch process) is a prototypical exothermic reaction of maximum catalytic yield restricted by the unbreakable equilibrium law. This is because bottlenecked N2 dissociation necessitates high temperature, but high temperature reversely shifts the thermal equilibrium toward NH3 decomposition. To surmount this equilibrium limit, here, we propose a new scenario of dual-temperature-zone catalysis. Powered by sunlight, the apparent temperature of TiO2-xHy/Fe hybrid reaches 495°C but with local temperature difference up to 137°C between the hot zone (Fe) and “cooling” zone (TiO2-xHy) owing to the plasmonic local heating effect. The hot Fe bearing hot carriers efficiently dissociates N2, while working-in-tandem TiO2-xHy well accommodates spilled-over N from Fe via successive hydrogenation, prominently mitigating the reverse equilibrium shift and thus delivering record NH3 concentrations of 1,939 (1 atm) and 19,620 ppm (10 atm) at 495°C, 1.55 and 1.57 times the theoretical equilibrium limits of 1,249 and 12,459 ppm, respectively. © 2019 Elsevier Inc.A key goal of contemporary ammonia synthesis is to reduce the consumption of fossil fuel by the design of more efficient thermocatalysts or “green” alternative pathways. However, the maximum NH3 yields of thermocatalysis are restricted by the thermodynamic equilibrium limit, while the catalytic efficiency of alternative pathway, like photocatalysis, is low in comparison with that of thermocatalysis. Here, we report an efficient solar light-driven N2 + 3H2 = 2NH3 via a photothermal pathway on a Fe-nanonecklace-hydrogenated titanium hybrid, generating NH3 with concentration beyond the equilibrium limit of thermocatalysis. The mechanism study reveals the reaction path of high-temperature N2 activation on Fe and low-temperature NH3 formation on TiO2-xHy, originating from the plasmonic local heating effect of Fe nanonecklace. This light-induced non-equilibrium catalysis ensures both high NH3 yield and high catalytic efficiency, and thus, it may be a promising alternative ammonia synthesis pathway. © 2019 Elsevier Inc.
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