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91.
利用原位漫反射傅里叶红外光谱(DRIFTS), 考察了室温下羰基硫(COS)在经氨气和有机胺预吸附的α-Fe2O3上的非均相反应, 并同时比较了氨气和不同有机胺(甲胺、三甲胺、三乙胺、苯胺、吡啶和吡咯)对反应活性的影响及其反应动力学. 结果表明, 经碱性物质预吸附后, COS可在α-Fe2O3表面发生氧化反应, 主要产物为气态CO2、表面HCO3-、表面CO32-和表面SO42-, 且α-Fe2O3表面预吸附的碱性物质大大提高了COS在α-Fe2O3上的反应能力, 在碱性物质的影响中, 甲胺对反应的促进能力最大, 相比纯α-Fe2O3反应的反应活性提高了约4.5倍, 然而苯胺和吡咯对COS的反应影响不是很明显.观察到的不同碱性物质对COS的转化能力依次为: 甲胺>三甲胺>氨气>三乙胺>吡啶>吡咯>苯胺≈纯样品, 受碱性物质的影响, COS的反应级数由一级转变为二级. 此外, 研究也发现碱性物质的覆盖度和表面吸附水对COS转化能力存在一定的影响. 这些实验结果表明在碱性物质存在下,表面M―O-是COS在α-Fe2O3发生氧化反应的关键活性位点, 对反应活性的贡献较大, 并在此基础上探讨碱性条件下COS的反应转化机制. 相似文献
92.
Strong Induced‐Fit Binding of Viologen and Pyridine Derivatives in Adjustable Porphyrin Cavities 下载免费PDF全文
Dr. Alexander B. C. Deutman Jan M. M. Smits Dr. René de Gelder Dr. Johannes A. A. W. Elemans Prof. Roeland J. M. Nolte Prof. Alan E. Rowan 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(36):11574-11583
The synthesis and binding properties of new porphyrin cage compounds consisting of a rigid diphenylglycoluril part, which is connected via flexible bis(ethyleneoxy) spacers to a (metallo)porphyrin “roof”, are reported. Binding of viologen guests and pyridine ligands in these porphyrin cages are accompanied by significant conformational reorganizations of the hosts. Despite these structural changes, association constants are still very high, revealing that not only receptors that bind guests according to a lock‐and‐key mechanism but also those that bind guests by an induced‐fit mechanism can exhibit strong binding. 相似文献
93.
Stijn F. M. van Dongen Madhavan Nallani Dr. Jeroen J. L. M. Cornelissen Dr. Roeland J. M. Nolte Prof. Dr. Jan C. M. van Hest Prof. Dr. 《Chemistry (Weinheim an der Bergstrasse, Germany)》2009,15(5):1107-1114
Porous polymersomes based on block copolymers of isocyanopeptides and styrene have been used to anchor enzymes at three different locations, namely, in their lumen (glucose oxidase, GOx), in their bilayer membrane (Candida antarctica lipase B, CalB) and on their surface (horseradish peroxidase, HRP). The surface coupling was achieved by click chemistry between acetylene-functionalised anchors on the surface of the polymersomes and azido functions of HRP, which were introduced by using a direct diazo transfer reaction to lysine residues of the enzyme. To determine the encapsulation and conjugation efficiency of the enzymes, they were decorated with metal-ion labels and analysed by mass spectrometry. This revealed an almost quantitative immobilisation efficiency of HRP on the surface of the polymersomes and a more than statistical incorporation efficiency for CalB in the membrane and for GOx in the aqueous compartment. The enzyme-decorated polymersomes were studied as nanoreactors in which glucose acetate was converted by CalB to glucose, which was oxidised by GOx to gluconolactone in a second step. The hydrogen peroxide produced was used by HRP to oxidise 2,2′-azinobis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS) to ABTS.+. Kinetic analysis revealed that the reaction step catalysed by HRP is the fastest in the cascade reaction. 相似文献
94.
Anthony J. Kirby Patrick Camilleri Jan B. F. N. Engberts Martin C. Feiters Roeland J. M. Nolte Olle Sderman Mark Bergsma Paul C. Bell Matthew L. Fielden Cristina L. García Rodríguez Philippe Gudat Andreas Kremer Caroline McGregor Christele Perrin Gaël Ronsin Marcel C. P. van Eijk 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2003,115(13):1486-1496
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Hoogboom J Velonia K Rasing T Rowan AE Nolte RJ 《Chemical communications (Cambridge, England)》2006,(4):434-435
By incorporating an ester-containing substrate in a self-assembled alignment layer for liquid crystal cells, the presence of a lipase (CALB) can be directly detected through its enzymatic action on the alignment layer, without the need for fluorescent labelling or enzyme assays. 相似文献