通讯机构:
[Wang, C ; Li, WY] H;Hengyang Normal Univ, Coll Chem & Mat Sci, Hengyang 421000, Peoples R China.;Tianjin Normal Univ, Tianjin Key Lab Struct & Performance Funct Mol, Coll Chem, Tianjin 300387, Peoples R China.
摘要:
A NiH-catalyzed migratory and non-migratory gem-difluoroallylation reaction of alkenyl amines with trifluoromethyl alkenes has been developed by judicious choice of directing groups. The reaction incorporates gem-difluoroalkene motifs into aliphatic amine derivatives at multiple positions with high levels of chemo- and regioselectivity. This practical protocol features wide substrate scope, great functional group tolerance, and easy removal of the directing groups. Notably, products from these reactions possess versatile chemical reactivity because of the secondary amide and difluoroalkene functionalities, thus building a platform for synthesizing new linear and cyclic fluoro-containing amines, which would benefit drug discovery.
作者机构:
[Lin, Xiaoyang; Ren, Jun; He, Yaxin; Yang, Chunming; Liang, Yun; Xiang, Qian; Li, Zhouli] Hunan Normal Univ, Coll Chem & Chem Engn, Natl & Local Joint Engn Lab New Petro Chem Mat, Changsha 410081, Peoples R China.;[Liu, Jinlong; Qian, Dong] Cent South Univ, Coll Chem & Chem Engn, Hunan Prov Key Lab Chem Power Resources, Changsha 410083, Peoples R China.;[Liu, Jinlong] Univ Auckland, Sch Chem Sci, Auckland 1142, New Zealand.;[Li, Junhua] Hengyang Normal Univ, Coll Chem & Mat Sci, Hengyang 421008, Peoples R China.
通讯机构:
[Qian, D ] C;[Yang, CM ] H;Hunan Normal Univ, Coll Chem & Chem Engn, Natl & Local Joint Engn Lab New Petro Chem Mat, Changsha 410081, Peoples R China.;Cent South Univ, Coll Chem & Chem Engn, Hunan Prov Key Lab Chem Power Resources, Changsha 410083, Peoples R China.
摘要:
In this work, N-doped biomass-char (N-BC) was adopted to fill and coat the commercial nickel foam (NF) achieved by the calcination of gelatin in air atmosphere. Subsequently, the Ni0.33Co0.67MoO4 nanosheet arrays were hydrothermally in-site grown on the N-BC-filled/coated NF (denoted as Ni0.33Co0.67MoO4/NF@N-BC). Served directly as a self-supporting electrode for supercapacitors, Ni0.33Co0.67MoO4/NF@N-BC holds an areal specific capacitance of 1162.5 mF cm(-2) at a corresponding 1 mA cm(-2) current density, much higher than that of Ni0.33Co0.67MoO4/NF (748.8mF cm(-2)) without the introduction of N-BC. Moreover, Ni0.33Co0.67MoO4/NF@N-BC shows excellent rate capability and durability. Additionally, the assembled two-electrode (Ni0.33Co0.67MoO4/NF@N-BC vs. active carbon (AC)@NF) all-solid-state flexible asymmetric supercapacitor is capable of reaching an energy density of 33.7 Wh kg(-1) at 347.8 W kg(-1). The significantly enhanced supercapacitive performance of Ni0.33Co0.67MoO4/NF with N-BC filling and coating emanates from the reduction of void space for NF and the improvement of electroconductivity.
摘要:
Six novel coordination polymers (CPs) based on a rigid tridentate ligand, 4 & PRIME;-(4-(imidazol-1-yl)phenyl)-4,2 & PRIME;:6 & PRIME;,4 & PRIME;'-terpyridine (imphtpy), namely {[Zn2(imphtpy)2(p-bdc)2].(H2O)}n (1), [Zn(imphtpy)(m-bdc)]n (2), {[Zn (imphtpy)(qda)1.5].(H2O)}n (3), [Cd2(imphtpy)2(m-bdc)2]n (4), [Cd(imphtpy)(abtc)0.5]n (5) and [Cd(imphtpy) (qda)]n (6), (p-H2bdc = 1,4-benzenedicarboxylic acid, m-H2bdc = 1,3-benzenedicarboxylic acid, H2qda = hy-droquinone-o,o'-diacetic acid and H4abtc = 3,3 & PRIME;,5,5 & PRIME;-azobenzenetetracarboxylic acid), have been solvothermally synthesized and characterized by elemental analysis, IR spectroscopy, powder X-ray diffraction (PXRD), ther-mogravimetric (TG) analysis and single-crystal X-ray diffraction. Complex 1 displays a pseudo four-fold inter-penetration of dia network in a [2 + 2] mode. Complex 2 exhibits a 2D-* 2D polycatenane of two-fold interpenetrated network with the sql topology. Complex 3 shows a interdigitated 2D layer with the sql topol-ogy, which is further extended into a 3D supramolecular framework through 7L-7L interactions and hydrogen bonds. Complex 4 features a two-fold interpenetrated (4,4)-connected 3D + 3D-* 3D framework with the bbf topology. Complex 5 reveals a 2D network constructed by binuclear Cd2(CO2)4 secondary building unit (SBU) with the sql topology which is further packed into a 3D supramolecular framework through 7L-7L interactions. Complex 6 is a 3D network constructed by binuclear Cd2(CO2)2O2 SBU with the uninodal 6-c pcu topology. These results indicate that the versatile coordination networks of imphtpy and various polycarboxylate ligands play crucial roles in modulating the structural topologies of coordination networks. In addtion, photo-luminescence properties have been explored for complexes 1-6 in the solid state at room temperature, which are derived from metal perturbed intraligand charge transfer (ICT) or ligand-to-ligand charge transfer.
作者:
Yang Ting-Ying;Guo Dan;Hu Yu-Qiong;Yi Si-Jia;Gu Shu-Qi;...
期刊:
无机化学学报,2023年39(1):117-126 ISSN:1001-4861
作者机构:
[Hu Yu-Qiong; He Xia; Yang Ting-Ying; Yi Si-Jia; Gu Shu-Qi; Zhang Fu-Xing; Guo Dan; Zhu Xiao-Ming] Hengyang Normal Univ, Coll Chem & Mat Sci,Key Lab Organometall New Mat, Coll Hunan Prov,Key Lab Funct Met Organ Cpds Huna, Hunan Engn Res Ctr Monitoring & Treatment Heavy M, Hengyang 421008, Hunan, Peoples R China.
期刊:
Environmental Science and Pollution Research,2023年30(47):104505-104519 ISSN:0944-1344
通讯作者:
Liu, J
作者机构:
[Liu, Jian; Zhao, Yi; Yi, Zhengji; Xu, Yue] Hengyang Normal Univ, Coll Chem & Mat Sci, Hengyang 421008, Peoples R China.;[Liu, Jian; Yi, Zhengji] Key Lab Funct Met Organ Cpds Hunan Prov, Hengyang 421008, Peoples R China.;[Liu, Jian; Yi, Zhengji] Hunan Engn Res Ctr Monitoring & Treatment Heavy M, Hengyang 421008, Peoples R China.
通讯机构:
[Liu, J ] H;Hengyang Normal Univ, Coll Chem & Mat Sci, Hengyang 421008, Peoples R China.;Key Lab Funct Met Organ Cpds Hunan Prov, Hengyang 421008, Peoples R China.;Hunan Engn Res Ctr Monitoring & Treatment Heavy M, Hengyang 421008, Peoples R China.
期刊:
Journal of Energy Storage,2023年58:106338 ISSN:2352-152X
通讯作者:
Chunming Yang<&wdkj&>Dong Qian
作者机构:
[Ren, Jun; Liang, Yun; Wang, Qing; Yang, Chunming; Xiang, Qian] Hunan Normal Univ, Coll Chem & Chem Engn, Natl & Local Joint Engn Lab New Petro Chem Mat & F, Changsha 410081, Peoples R China.;[Ren, Jun; Liang, Yun; Wang, Qing; Yang, Chunming; Xiang, Qian] Hunan Normal Univ, Coll Chem & Chem Engn, Key Lab Chem Biol & Tradit Chinese Med Res, Minist Educ China, Changsha 410081, Peoples R China.;[Liu, Jinlong; Qian, Dong] Cent South Univ, Coll Chem & Chem Engn, Hunan Prov Key Lab Chem Power Resources, Changsha 410083, Peoples R China.;[Li, Junhua] Hengyang Normal Univ, Coll Chem & Mat Sci, Key Lab Funct Met Organ Cpds Hunan Prov, Hengyang 421008, Peoples R China.
通讯机构:
[Chunming Yang] N;[Dong Qian] H;Hunan Provincial Key Laboratory of Chemical Power Resources, College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, PR China<&wdkj&>National and Local Joint Engineering Laboratory for New Petro-chemical Materials and Fine Utilization of Resources & Key Laboratory of Chemical Biology and Traditional Chinese Medicine Research (Ministry of Education of China), College of Chemistry and Chemical Engineering, Hunan Normal University, Changsha 410081, PR China
关键词:
Ni(pyrithione)(2);FeNiCo oxides;FeNi foam;High voltage window;Symmetrical supercapacitors
摘要:
The low decomposition voltage (similar to 1.23 V) of water enormously restricts the workable voltage of aqueous symmetrical supercapacitors (SSCs), which correspondingly limits the energy densities and frustrates the commercialization of aqueous SSCs. Herein, the voltage window of an all-solid-state symmetrical supercapacitors (ASSC) can be extended via employing a novel self-supporting hybrid electrode constructed by coupling FeNiCo oxides with Ni(pyrithione)(2) on FeNi foam (denoted as NiPT@FeNiCo oxides/FNF) as both cathode and anode, which was synthesized using two-step hydrothermal processes. Primarily due to the introduction of redox-active pyrithione ligand chelating Ni ions supplemented by multiple pairs of reversible redox reactions to suppress water splitting, the assembled ASSC device exhibits an extra-wide workable voltage window up to 3.2 V with ultrahigh energy exporting densities (69.9 Wh kg(-1) at 173.9 W kg(-1), and 29.1 Wh kg(-1) even at an elevated 2437.6 W kg(-1)). The energy density feature of this assembled ASSC device is superior to most existing transition metal oxide-based supercapacitors and even asymmetric or hybrid devices heretofore reported. After 10,000 cycles, this assembled ASSC device records a 92.5 % retention of initial area specific capacity. Our work offers a robust combination strategy to design high-potential electrode materials for constructing high-voltage ASSCs.
期刊:
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY,2023年300:122951 ISSN:1386-1425
通讯作者:
Gu, B
作者机构:
[Zhang, Keyang; Dai, Cong; Gu, Biao; Tang, Can; Zhao, Jingjun; Li, Xinyu; Gu, B] Hengyang Normal Univ, Coll Chem & Mat Sci, Hunan Prov Engn Res Ctr Monitoring & Treatment Hea, Key Lab Organomet New Mat, Hengyang 421008, Peoples R China.
通讯机构:
[Gu, B ] H;Hengyang Normal Univ, Coll Chem & Mat Sci, Hunan Prov Engn Res Ctr Monitoring & Treatment Hea, Key Lab Organomet New Mat, Hengyang 421008, Peoples R China.
关键词:
AIE;Bioimaging;Continuous detection;Cu(2+) and H(2)S;Fluorescent sensor
摘要:
The development of effective methods for tracking Cu(2+) and H(2)S in living organisms is urgently required due to their vital function in a variety of pathophysiological processes. In this work, a new fluorescent sensor BDF with excited-state intramolecular proton transfer (ESIPT) and aggregation-induced emission (AIE) features for the successive detection of Cu(2+) and H(2)S was constructed by introducing 3,5-bis(trifluoromethyl)phenylacetonitrile into the benzothiazole skeleton. BDF showed a fast, selective and sensitive fluorescence "turn off" response to Cu(2+) in physiological media, and the situ-formed complex can serve as a fluorescence "turn on" sensor for highly selective detection of H(2)S through the Cu(2+) displacement approach. In addition, the detection limits of BDF for Cu(2+) and H(2)S were determined to be 0.05 and 1.95μM, respectively. Encouraged by its favourable features, including strong red fluorescence from the AIE effect, large Stokes shift (285nm), high anti-interference ability and good function at physiological pH as well as a low toxicity, BDF was successfully applied for the consequent imaging of Cu(2+) and H(2)S in both living cells and zebrafish, making it an ideal candidate for detecting and imaging of Cu(2+) and H(2)S in live systems.
作者机构:
[Tang, Yinheng; Wang, Chao; Li, Wenyi; Han, Jian] Hengyang Normal Univ, Key Lab Funct Organometall Mat Hunan Prov Univ, Coll Chem & Mat Sci, Key Lab Funct Met Organ Cpds Hunan Prov, Hengyang 421008, Hunan, Peoples R China.;[Zhang, Lanlan; Wang, Chao; Huang, Jie; Luo, Chun] Tianjin Normal Univ, Coll Chem, Tianjin Key Lab Struct & Performance Funct Mol, Tianjin 300387, Peoples R China.;[Han, Jian] Nanjing Univ, Sch Chem & Chem Engn, Jiangsu Key Lab Adv Organ Mat, Nanjing 210023, Jiangsu, Peoples R China.
通讯机构:
[Chao Wang] C;College of Chemistry and Materials Science, Hengyang Normal University, Key Laboratory of Functional Metal-Organic Compounds of Hunan Province, Key Laboratory of Functional Organometallic Materials of Hunan Province Universities, Hengyang, Hunan, 421008 China<&wdkj&>Tianjin Key Laboratory of Structure and Performance for Functional Molecules;College of Chemistry, Tianjin Normal University, Tianjin, 300387 China
摘要:
We disclose a Ni‐catalyzed remote arylalkylation of picolinamide tethered alkenyl amines with readily available aryl boronic acids and alkyl halides via six‐ or seven‐membered nickelacycles, providing a facile access to valuable δ,ε‐ and ε,ζ‐difunctionalized aliphatic amines. Comprehensive Summary Directing group‐assisted, transition metal‐catalyzed three‐component difunctionalization of alkenes has emerged as a powerful tool to drive molecular complexity. However, this strategy generally works with the substrates bearing directing groups in close proximity to the alkene moieties, due to the preference for formation of kinetically stable five‐membered metallacycles. Herein, we have disclosed a complementary strategy to accomplish a nickel‐catalyzed remote arylalkylation of alkenyl amines with excellent regioselectivity and diastereofidelity, involving rare six‐ or seven‐membered metallacycles. This general protocol is compatible with a series of δ‐ and ε‐alkenyl amines, providing corresponding valuable δ,ε‐ and ε,ζ‐difunctionalized aliphatic amines that would be difficult to synthesize. The coordination of the bidentate picolinamide auxiliary and the facile oxidative addition of alkyl halides to Ni(I) species are the key to the success of the developed remote olefin dicarbofunctionalization.
作者:
Tan, Y. X.;Jiang, W. J.;Feng, Y. L.;Yu, J. X.;Kuang, D. Z.
期刊:
Russian Journal of General Chemistry,2023年93(6):1504-1512 ISSN:1070-3632
通讯作者:
Kuang, DZ
作者机构:
[Kuang, D. Z.; Jiang, W. J.; Yu, J. X.; Tan, Y. X.; Feng, Y. L.; Kuang, DZ] Hengyang Normal Univ, Coll Hunan Prov, Coll Chem & Mat Sci,Key Lab Organometall New Mat, Hunan Prov Engn Res Ctr Monitoring & Treatment Hea, Hengyang 421008, Peoples R China.
通讯机构:
[Kuang, DZ ] H;Hengyang Normal Univ, Coll Hunan Prov, Coll Chem & Mat Sci,Key Lab Organometall New Mat, Hunan Prov Engn Res Ctr Monitoring & Treatment Hea, Hengyang 421008, Peoples R China.
摘要:
Two organotin aryloxyacetate were synthesized by the reaction of 1,2-phenylenedioxydiacetic acid with dibutyltin oxide and tricyclohexyltin hydroxide. The structures were characterized by IR, H-1, C-13 NMR, and X-ray crystal diffraction. Herbicidal activity of the prepared organotin aryloxyacetate was evaluated.
期刊:
Journal of Organometallic Chemistry,2023年993:122708 ISSN:0022-328X
通讯作者:
Ya-Ping Ou
作者机构:
[Kong, Lingqiao; Ou, Ya-Ping; Xia, Yonglin; Li, Ziteng; Zhu, Xiaoming; Xu, Jingwen; Zhang, Fuxing; Lin, Zishun; Xiao, Wenbo] Hengyang Normal Univ, Coll Chem & Mat Sci, Hengyang 421008, Hunan, Peoples R China.;[Ou, Ya-Ping; Zhu, Xiaoming; Zhang, Fuxing] Hengyang Normal Univ, Hunan Prov Key Lab Funct Met Organ Cpds, Hengyang 421008, Peoples R China.;[Ou, Ya-Ping; Zhang, Fuxing] Hengyang Normal Univ, Coll Hunan Prov, Key Lab Organometall New Mat, Hengyang 421008, Hunan, Peoples R China.;[Ou, Ya-Ping; Zhang, Fuxing] Hunan Engn Res Ctr Monitoring & Treatment Heavy Me, Hengyang 421001, Hunan, Peoples R China.
通讯机构:
[Ya-Ping Ou] C;College of Chemistry and Material Science, Hengyang Normal University, Hengyang, Hunan 421008, PR China<&wdkj&>Hunan Provincial Key Laboratory of Functional Metal-Organic Compounds, Hengyang Normal University, Hengyang 421008, PR China<&wdkj&>Key Laboratory of Organometallic New Materials, College of Hunan Province, Hengyang Normal University, Hengyang, Hunan 421008, PR China<&wdkj&>Hunan Engineering Research Center for Monitoring and Treatment of Heavy Metals Pollution in the Upper Reaches of Xiangjiang River, Hengyang, Hunan 421001, PR China
摘要:
A series of asymmetrical terpyridine ruthenium-TAA redox-active organometallic complexes was pre-pared and characterized. The bonding and electronic properties of these complexes were investigated by spectro-electrochemistry and theoretical calculations. Electrochemical results revealed that four com-plexes exhibited two successive single-electron redox processes, in which the first-step electrochemical behavior of tpyRu-ethynyl-TAA complexes occurred at the triarylamine moiety, the first-step based-metal oxidation of Cl-tpyRu-TAA complex was decided, and their half-wave potential difference AE decreased gradually. The near-infrared (NIR) spectroscopic results of mixed-valence states obtained by spectro-electrochemistry showed that they all have NIR multiple absorption characteristics. The maximum ab-sorption wavelength of singly-oxidized tpyRu-ethynyl-TAA molecules redshifted with bridge conjugate extension, whereas Cl-tpyRu-TAA mixed-valence state only displayed weak absorption at high-energy re-gion, as later confirmed by TDDFT calculation. The electron coupling parameters Hab obtained from the inter-valence charge transfer analysis of mixed-valence states by the Marcus-Hush theory decreased grad-ually with the extension of the bridge chain, consistent with the electrochemical results. In addition, DFT calculation reflected that the HOMO contribution in bridge chain of neutral molecules increased with the conjugate bridge extension, and the spin density distribution of mixed-valence states was mainly localized on the aryl bridge and NAr2 and featured the less metal character and hence less charge de-localization. The above results concluded that the degree of electronic coupling and the order of redox processes are greatly affected by conjugated bridge and the coordination model between terpyridine and ruthenium.(c) 2023 Elsevier B.V. All rights reserved.
期刊:
Dyes and Pigments,2023年208:110769 ISSN:0143-7208
通讯作者:
Haitao Li<&wdkj&>Biao Gu
作者机构:
[Zhang, Youyu; Fang, Cong; Pang, Xiao; Li, Haitao; Zhou, Zile] Hunan Normal Univ, Coll Chem & Chem Engn, Key Lab Chem Biol & Tradit Chinese Med Res, Minist Educ, Changsha 410081, Peoples R China.;[Gu, Biao] Hengyang Normal Univ, Coll Chem & Mat Sci, Key Lab Chem Sensing & Catalysis, Hengyang 421008, Peoples R China.
通讯机构:
[Haitao Li; Biao Gu] K;Key Laboratory of Chemical Biology and Traditional Chinese Medicine Research (Ministry of Education), College of Chemistry and Chemical Engineering, Hunan Normal University, Changsha, 410081, PR China<&wdkj&>Key Laboratory of Chemical Sensing and Catalysis, College of Chemistry and Materials Science, Hengyang Normal University, Hengyang, 421008, PR China
摘要:
fl-Galactosidase is closely related to primary ovarian cancer and highly expressed in metastatic ovarian cancer. Therefore, the development of effective tool for in situ detecting fl-gal is urgently needed for further studies in ovarian cancer. Inspired by the advantages of near-infrared (NIR) fluorescence imaging, a NIR fluorescent probe (DCM-CHO-beta gal) with improved near-infrared fluorescence emission and detection performance was reasonably designed for the quantification and visualization of fl-gal, employing structurally modified dicyanobenzopyran derivative (DCM-CHO-OH) as fluorophore. DCM-CHO-beta gal showed a rapid response (<20 min) towards fl-gal accompanied by nearly 40-fold fluorescence enhancement at 665 nm. DCM-CHO-beta gal can quantitatively detect fl-gal ranging from 0.2 to 3 U/mL with a low detection limit (3.15 x 10-5 U/mL), and can selectively detect fl-gal in the presence of other possible interferences. In view of excellent optical, analytical performance and good biocompatibility, DCM-CHO-beta gal was applied to the visualization of endogenous fl-gal in ovarian cancer cells and zebrafish, which provided a powerful tool for the in-depth study of the role of beta-gal in beta-gal-related diseases.
期刊:
Surface and Coatings Technology,2023年467:129679 ISSN:0257-8972
通讯作者:
Wang, Jinshuang;Jing, QS
作者机构:
[Jing, Qiangshan; Hu, Mengqiu; Wang, Jinshuang; Sun, Jiarui; Liu, Bing; Lu, Xianjun; Chen, Mengdi; Wang, JS; Wang, Yinghui; Jing, QS] Xinyang Normal Univ, Henan key Lab Utilizat Nonmet Mineral south Henan, Xinyang 464000, Peoples R China.;[Shu, Chaoxi] Wuhan Univ Technol, State Key Lab Silicate Mat Architectures, Wuhan 430070, Peoples R China.;[Zhang, Hao] Jiangxi Sci & Technol Normal Univ, Jiangxi Key Lab Surface Engn, Nanchang 330013, Peoples R China.;[Sun, Junbin] Hengyang Normal Univ, Hunan Prov Univ Key Lab Funct Organomet Mat, Key Lab Funct Met Organ Cpds Hunan Prov, Coll Chem & Mat Sci, Hengyang 421008, Peoples R China.
通讯机构:
[Wang, JS; Jing, QS ] X;Xinyang Normal Univ, Henan key Lab Utilizat Nonmet Mineral south Henan, Xinyang 464000, Peoples R China.
关键词:
High -temperature phase stability;Thermo -physical properties;Thermal shock;CMAS resistance
摘要:
In this study, 16 mol% CeO2-2 mol% Sc2O3 co-stabilized ZrO2 (4S16CZ) coating was prepared by atmospheric plasma spraying (APS) technology. Parameters related to the application of 4S16CZ as a thermal barrier coatings (TBCs) were studied, including high-temperature stability, thermal insulation performance, coefficient of thermal expansion (CTE), thermal shock behavior and CaO-MgO-Al2O3-SiO2 (CMAS) resistance. After heat treatment at 1400 degrees C for 100 h, the 4S16CZ coating maintained a single non-transformable tetragonal phase (t'), exhibiting excellent high-temperature stability. Additionally, at the test temperatures (25 degrees C-1000 degrees C), the thermal conductivity of the 4S16CZ coating ranged from 0.79 W/(m & BULL;K) to 1.02 W/(m & BULL;K), lower than that of the ZrO2 coating stabilized by 7.6 wt% Y2O3 (YSZ, 0.88-1.13 W/(m & BULL;K)), The CTE of the 4S16CZ coating was from 8.3 x 10-6 K-1 to 11.2 x 10-6 K-1, which was comparable to the YSZ. Moreover, the thermal shock behaviors of 4S16CZ TBCs and 4S16CZ/YSZ TBCs were evaluated at 1050 degrees C. The thermal durability of the 4S16CZ/YSZ TBCs was higher than that of 4S16CZ TBCs due to the buffering effect of the YSZ layer. The main reasons for the failure of both TBCs were the oxidation of the bond coat, thermal mismatch stress, low fracture toughness and sintering effects. In CMAS isothermal corrosion tests, CMAS exhibited low wettability on the 4S16CZ coating. Compared with the YSZ coating, the 4S16CZ coating showed better resistance to CMAS attacks.
期刊:
JOURNAL OF ENVIRONMENTAL SCIENCE AND HEALTH PART A-TOXIC/HAZARDOUS SUBSTANCES & ENVIRONMENTAL ENGINEERING,2023年58(6):515-524 ISSN:1093-4529
通讯作者:
Zhifeng Xu
作者机构:
[Deng, Peihong; Xu, Zhifeng; Li, Junhua; Li, Lizhen] Hengyang Normal Univ, Coll Chem & Mat Sci, Hengyang, Peoples R China.;[Deng, Peihong; Xu, Zhifeng; Li, Junhua; Li, Lizhen] Key Lab Organometall New Mat Hunan Prov, Hengyang, Peoples R China.;[Deng, Peihong; Xu, Zhifeng; Li, Junhua; Li, Lizhen] Engn Res Ctr Monitoring & Treatment Heavy Met Poll, Hengyang, Peoples R China.;[Xu, Zhifeng] Hengyang Normal Univ, Coll Chem & Mat Sci, Hengyang 421008, Peoples R China.
通讯机构:
[Zhifeng Xu] C;College of Chemistry and Materials Science, Hengyang Normal University, Hengyang, PR China<&wdkj&>Key Laboratory of Organometallic New Materials of Hunan Province, Hengyang, PR China<&wdkj&>Engineering Research Center for Monitoring and Treatment of Heavy Metals Pollution in the Upper Reaches of Xiangjiang River, Hengyang, PR China
摘要:
Molecularly imprinted polymers (MIPs) are synthetic polymers with predetermined selectivity for a given analyte. One major problem associated with MIPs is the inaccessibility of a large fraction of the recognition sites that remain buried within the polymeric matrix. To address this problem, the high selectivity imparted by the imprinting technique and the porosity of three-dimensional (3D) graphene oxide (GO)-based porous materials were utilized in this work to prepare a 3D GO-based Cu(II)-ion-imprinted material (hereafter denoted as IIM) via one-pot reactions of GO, chitosan (CS), and glutaraldehyde in the presence of Cu(II). Results of equilibrium binding experiments show that IIM has a high template-ion binding capacity (1.75 mmol g(-1)) and good imprinting factor (2.19). Further, results of selectivity tests indicate that IIM has a high Cu(II)-recognition ability. IIM also has a fast binding rate and satisfactory reusability. In addition, the Langmuir isotherm model was well fitted with the experimental data, indicating the monolayer adsorption of Cu(II) ions. The present work provided a convenient approach to prepare 3D GO-based imprinted materials that are promising for enrichment or recycling of target compounds from wastewater.
作者机构:
[Liu, Xing; Feng, Hao; Li, Junhua; Cui, Ying; Wu, Qian; Wang, Fan] Hengyang Normal Univ, Hunan Prov Univ Key Lab Funct Organometall Mat, Coll Chem & Mat Sci, Key Lab Funct Met Organ Cpds Hunan Prov, Hengyang 421008, Peoples R China.;[Li, Junhua; Qian, Dong] Cent South Univ, Coll Chem & Chem Engn, Hunan Prov Key Lab Efficient & Clean Utilizat Mang, Changsha 410083, Peoples R China.;[He, Lingzhi] Sch Med, Hunan Polytech Environm & Biol, Hengyang 421008, Peoples R China.;[Tong, Haixia; He, Lingzhi] Changsha Univ Sci & Technol, Inst Chem & Biol Engn, Changsha 410114, Peoples R China.;[Liu, Zeng] Cangzhou Dahua Grp Co Ltd, Cangzhou 061000, Peoples R China.
通讯机构:
[Junhua Li] K;[Dong Qian] H;Hunan Provincial Key Laboratory of Efficient and Clean Utilization of Manganese Resources, College of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, PR China<&wdkj&>Key Laboratory of Functional Metal-Organic Compounds of Hunan Province, Hunan Province Universities Key Laboratory of Functional Organometallic Materials, College of Chemistry and Material Science, Hengyang Normal University, Hengyang, 421008, PR China<&wdkj&>Hunan Provincial Key Laboratory of Efficient and Clean Utilization of Manganese Resources, College of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, PR China
关键词:
Prussian blue analogue;Synthesis;Electrochemical sensing;5-Hydroxytryptamine
摘要:
Lack of highly efficient, inexpensive, and easily available catalysts severely limits the practical applicability of electrochemically sensing assay towards 5-hydroxytryptamine (5-HT). Herein, four kinds of Fe-Co bimetallic Prussian blue analogues (FeCo-PBAs) with different molar ratios of Fe to Co were prepared using a simple coprecipitation method. Interestingly, Fe(III) in K3 [Fe(CN)6] can be reduced to Fe(II) by adding trisodium citrate dehydrate, which could offer a new clue to synthesize PBAs with Fe(II) core ions. With the optimizational FeCo-PBA synthesized at a 0.5/1 M ratio of Fe to Co as an electrocatalyst, the constructed sensor shows excellent comprehensive performance for the 5-HT assay with a high sensitivity of 0.856 mu A mu M-1 and an ultralow detection limit of 8.4 nM. Under the optimum conditions, linearity was obtained in the ranges of 0.1-10.0 mu M and 10.0-200.0 mu M and preferable recoveries ranged from 97.8% to 103.0% with relative standard deviation (RSD) < 4.0%. The integrated properties of FeCo-PBA can be comparable to previously reported electrocatalysts for the 5-HT assay including noble metal-based and expensive carbon (graphene and carbon nanotubes)-based electrocatalysts. The proposed sensor also exhibits outstanding selectivity, reproducibility, and practicality for real sample analyses. This work is the first report on the PBA-based sensor for the 5-HT assay, verifying the practicability of this high-performance sensor for the 5-HT assay.
作者:
Yi Si-Jia;He Xia;Gu Shu-Qi;Deng Zhe-Yu;Li Jia-Hong;...
期刊:
无机化学学报,2023年39(5):874-882 ISSN:1001-4861
通讯作者:
Zhu, XM
作者机构:
[He Xia; Li Jia-Hong; Zhu Xiao-Ming; Deng Zhe-Yu; Yi Si-Jia; Gu Shu-Qi; Zhang Fu-Xing; Yu Jiang-Xi] Hengyang Normal Univ, Coll Hunan Prov,Key Lab Organomet New Mat, Coll Chem & Mat Sci,Key Lab Funct Metal Organ Cpd, Hunan Engn Res Ctr Monitoring & Treatment Heavy M, Hengyang 421008, Hunan, Peoples R China.
通讯机构:
[Zhu, XM ] H;Hengyang Normal Univ, Coll Hunan Prov,Key Lab Organomet New Mat, Coll Chem & Mat Sci,Key Lab Funct Metal Organ Cpd, Hunan Engn Res Ctr Monitoring & Treatment Heavy M, Hengyang 421008, Hunan, Peoples R China.