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991.
Dong Cao Huogao Huang Ming Hu Lin Cui Fanglan Geng Ziyu Rao Hongyun Niu Yaqi Cai Yuehui Kang 《Analytica chimica acta》2015
Natural organic matter (NOM) is a complex and non-uniform mixture of organic compounds which plays an important role in environmental processes. Due to the complexity, it is challenging to obtain fully detailed structural information about NOM. Although Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) has been demonstrated to be a powerful tool for providing molecular information about NOM, multiple ionization methods are needed for comprehensive characterization of NOM at the molecular level considering the ionizing selectivity of different ionization methods. This paper reports the first use of matrix assisted laser desorption/ionization (MALDI) method coupled with FT-ICR-MS for molecular characterization of NOM within a mass range of 200–800 Da. The mass spectral data obtained by MALDI were systematically compared with data generated by electrospray ionization (ESI). It showed that complementary molecular information about NOM which could not be detected by ESI, were provided by MALDI. More unsaturated and aromatic constituents of NOM with lower O/C ratio (O/C ratio < 0.5) were preferentially ionized in MALDI negative mode, whereas more polar constituents of NOM with higher O/C ratio were preferentially ionized in ESI negative mode. Molecular anions of NOM appearing at even m/z in MALDI negative ion mode were detected. The results show that NOM molecules with aromatic structures, moderate O/C ratio (0.7 > O/C ratio > 0.25) and lower H/C ratio were liable to form molecular anions at even m/z, whereas those with higher H/C ratio are more likely to form deprotonated ions at odd m/z. It is speculated that almost half of the NOM molecules identified by MALDI may be aromatic or condensed aromatic compounds with special groups which are liable to absorb electron from other molecules to generate free radical anions during MALDI ionization. 相似文献
992.
993.
In this work, a novel sandwich-type electrochemical immunosensor based on host-guest interaction was fabricated for the detection of alpha-fetoprotein (AFP). Due to the large specific surface area of multiwalled carbon nanotubes and the unique supramolecular recognition ability of β-cyclodextrins, ferrocenecarboxylic acid (Fc) was incorporated into this sensor platform by host-guest interaction to generate an electrochemical signal. And β-cyclodextrins functionalized silver supported adamantine-modified glucose oxidase (GOD-CD-Ag), was used as a label to improve the analytical performance of the immunosensor by the dual amplification strategy. The obtained GOD-CD-Ag conjugates could convert glucose into gluconic acid with the formation of hydrogen peroxide (H2O2). And then silver nanoparticles could in situ catalyze the reduction of the generated H2O2, dramatically improving the oxidation reaction of Fc. The developed immunosensor shows a wide linear calibration range from 0.001 to 5.0 ng/mL with a low detection limit (0.2 pg/mL) for the detection of AFP. The method, with ideal reproducibility and selectivity, has a wide application prospect in clinical research. 相似文献
994.
Xi Dai Tao Zhang Zhi-Fang Du Xiang-Jian Cao Ming-Yu Chen Sheng-Wen Hu Jun-Ying Miao Bao-Xiang Zhao 《Analytica chimica acta》2015
We have developed the first two-photon colorimetric and ratiometric fluorescent probe, BICO, for the detection of bisulfite (HSO3−) in aqueous solution. The probe contains coumarin and benzimidazole moieties and can detect HSO3− based on the Michael addition reaction with a limit of detection 5.3 × 10−8 M in phosphate-buffered saline solution. The probe was used to detect bisulfite in tap water, sugar and dry white wine. Moreover, test strips were made and used easily. We successfully applied the probe to image living cells, using one-photon fluorescence imaging. BICO overcomes the limitations in sensitivity of previously reported probes and the solvation effect of bisulfite, which demonstrates its excellent value in practical application. 相似文献
995.
Paecilomycines A and B,Novel Diterpenoids,Isolated from Insect‐Pathogenic Fungi Paecilomyces sp. ACCC 37762 下载免费PDF全文
Kun Zhou Xiao‐Ling Zhao Li‐Ping Han Meng‐Meng Cao Chuan Chen Bao‐Zhong Shi Du‐Qiang Luo 《Helvetica chimica acta》2015,98(5):642-649
Two new diterpenoids, named paecilomycine A ( 1 ) and paecilomycine B ( 2 ), including a novel skeleton with a five‐membered lactone ring, together with three known labdane diterpenoids, rel‐(1R,3S,4aS,5R,8aS)‐5‐[(3E)‐4‐carboxy‐3‐methylbut‐3‐en‐1‐yl]decahydro‐3‐hydroxy‐1,4a‐dimethyl‐6‐methylidenenaphthalene‐1‐carboxylic acid ( 3 ), botryosphaerin E ( 4 ), and agathic acid ( 5 ), were isolated from solid culture of the insect pathogenic fungi strain Paecilomyces sp. The structures of all compounds were established on the basis of comprehensive spectroscopic studies. The relative configurations of 1 and 2 were determined by single‐crystal X‐ray diffraction analyses. 相似文献
996.
997.
采用两步法将不同尺寸的silicalite-1分子筛纳米晶种通过自组装合成了一系列有序介孔silicalite-1分子筛。首先将强碱性的silicalite-1前驱体分别加热不同时间得到纳米晶种,然后在类似合成SBA-15的强酸性条件下组装成有序的介孔材料。合成条件的剧烈变化阻止了分子筛晶种的继续长大,并在三嵌段共聚物模板的诱导下组装成有序介孔材料。这种“自下而上”的方法制备有序介孔分子筛同时包含微孔和介孔。氮气吸脱附结果表明所制备的介孔分子筛材料均表现了很大的比表面积(730 m2/g以上)。 相似文献
998.
From Polymer to Monomer: Cleavage and Rearrangement of Si‐O‐Si Bonds after Oxidation Yielded an Ordered Cyclic Crystallized Structure 下载免费PDF全文
Yujing Zuo Zhiming Gou Jinfeng Cao Zhou Yang Haifeng Lu Prof. Shengyu Feng 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(31):10972-10977
Polymerization reactions are very common in the chemical industry, however, the reaction in which monomers are obtained from polymers is rarely invesitgated. This work reveals for the first time that oxone can break the Si‐O‐Si bond and induce further rearrangement to yield an ordered cyclic structure. The oxidation of P1 , which is obtained by reaction of 2,2′‐1,2‐ethanediylbis(oxy)bis(ethanethiol) (DBOET) with 1,3‐divinyl‐1,1,3,3‐tetramethyldisiloxane (MMVi), with oxone yielded cyclic crystallized sulfone–siloxane dimer ( P1‐ox ) after unexpected cleavage and rearrangement of the Si‐O‐Si bond. 相似文献
999.
Dr. Dongdi Zhang Fan Cao Pengtao Ma Chao Zhang Prof. Dr. You Song Zhijie Liang Xiaojing Hu Prof. Jingping Wang Prof. Dr. Jingyang Niu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(49):17683-17690
By deliberately using a metastable polyanion [(NbO2)6P2W12O56]12? ( 1 ), which was formed in situ, we have discovered the unprecedented hexameric cluster {Mn15(Nb6P2W12O62)6} ( 2 ), in which the six polyanions [Nb6P2W12O61]10? are alternately connected by four intriguing trinuclear {MnIII3} moieties and four {MnII} linkers. This discovery is the first in which the phosphoniobotungstate has been made accessible by using transition‐metal ions; furthermore, polyanion 2 represents the largest niobotungstate cluster reported to date. Analysis by means of electrospray ionization mass spectrometry (ESI‐MS ) provides insight into the self‐assembly process, and the peaks observed relate to the different charge states of the parent cluster, thus confirming the stability of 2 . In addition, magnetic‐susceptibility measurements reveal that each {MnIII3} subunit is a separate single‐molecule magnet (SMM). This discovery results from the exploration of the reverse effect of metastable polyanion 1 possessing high reactivity, thereby turning a disadvantage into an advantage. This finding could define a new synthetic strategy for the design and synthesis of magnetic polyoxometalate (POM) clusters. 相似文献
1000.
Mesoporous Carbon Nanofibers Embedded with MoS2 Nanocrystals for Extraordinary Li‐Ion Storage 下载免费PDF全文
Dr. Shan Hu Prof. Wen Chen Dr. Evan Uchaker Prof. Jing Zhou Prof. Guozhong Cao 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(50):18248-18257
MoS2 nanocrystals embedded in mesoporous carbon nanofibers are synthesized through an electrospinning process followed by calcination. The resultant nanofibers are 100–150 nm in diameter and constructed from MoS2 nanocrystals with a lateral diameter of around 7 nm with specific surface areas of 135.9 m2 g?1. The MoS2@C nanofibers are treated at 450 °C in H2 and comparison samples annealed at 800 °C in N2. The heat treatments are designed to achieve good crystallinity and desired mesoporous microstructure, resulting in enhanced electrochemical performance. The small amount of oxygen in the nanofibers annealed in H2 contributes to obtaining a lower internal resistance, and thus, improving the conductivity. The results show that the nanofibers obtained at 450 °C in H2 deliver an extraordinary capacity of 1022 mA h g?1 and improved cyclic stability, with only 2.3 % capacity loss after 165 cycles at a current density of 100 mA g?1, as well as an outstanding rate capability. The greatly improved kinetics and cycling stability of the mesoporous MoS2@C nanofibers can be attributed to the crosslinked conductive carbon nanofibers, the large specific surface area, the good crystallinity of MoS2, and the robust mesoporous microstructure. The resulting nanofiber electrodes, with short mass‐ and charge‐transport pathways, improved electrical conductivity, and large contact area exposed to electrolyte, permitting fast diffusional flux of Li ions, explains the improved kinetics of the interfacial charge‐transfer reaction and the diffusivity of the MoS2@C mesoporous nanofibers. It is believed that the integration of MoS2 nanocrystals and mesoporous carbon nanofibers may have a synergistic effect, giving a promising anode, and widening the applicability range into high performance and mass production in the Li‐ion battery market. 相似文献