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排序方式: 共有51条查询结果,搜索用时 31 毫秒
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2.
Patrick Shelton Toby J. Ligon Jennifer M. Dell Loagan Yarbrough James R. Vyvyan 《Tetrahedron letters》2017,58(35):3478-3481
Cananodine is a guaipyridine alkaloid with activity against liver cancer. Cananodine was synthesized using a remarkable intramolecular opening of a trisubstituted epoxide as the key step in construction of the seven-membered carbocycle of the target. The epoxide opening strategy allows all four stereoisomers of cananodine to be prepared. 相似文献
3.
Using the approach of Rulla (1996 SIAM J. Numer. Anal. 33, 68-87)for analysing the time discretization error and assuming moreregularity on the initial data, we improve on the error boundderived by Barrett and Blowey (1996 IMA J. Numer. Anal. 16,257-287) for a fully practical piecewise linear finite elementapproximation with a backward Euler time discretization of amodel for phase separation of a multi-component alloy. 相似文献
4.
Li Y Al-Eryani R Yarbrough ML Orth K Ball HL 《Journal of the American Society for Mass Spectrometry》2011,22(4):752-761
Recent studies have suggested that adenosine 5'-monophosphate (AMP) post-translational modification of proteins could represent
a novel molecular signaling pathway. Mass spectrometric fragmentation characteristics of this modification have not previously
been described and studied systematically. In this work, we therefore examined the fragmentation pattern of chemically synthesized
peptides containing AMPylated Thr, Ser, and Tyr. The formation of characteristic ions and the influence of collision energy
(CE) on the detection of characteristic ions and their relative peak intensity are reported. When peptide with AMPylated Ser/Thr
underwent collision induced dissociation (CID), peaks at m/z 348.1, 136.1, and 250.1, fragments with AMP group attached, and fragments consistent with neutral loss of 347 Da were major
characteristic ions; fragments consistent with neutral loss of 135 Da or 249 Da were weaker and not always detectable. The
observations for Tyr AMPylation followed the same general patterns as those for Ser/Thr modification, with the exception that
the ions detected for Tyr AMPylation did not include either the peak at m/z 348.1, or fragments with a mass shift of –347 Da. The results described in this paper highlight a series of diagnostic ions,
which can be used not only to confidently identify the AMPylation site based on MS and MS/MS data, but also to selectively
scan AMPylated peptides in complex protein mixtures. 相似文献
5.
For toxicological-based structure-activity relationships to advance, will require a better understanding of molecular reactivity. A rapid and inexpensive spectrophotometric assay for determining the reactive to glutathione (GSH) was developed and used to determine GSH reactivity (reactGSH) data for 21 aliphatic derivatives of esters, ketones and aldehydes. From these data, a series of structure-activity relationships were evaluated. The structure feature associated with reactGSH was an acetylenic or olefinic moiety conjugated to a carbonyl group (i.e. polarized alpha,beta-unsaturation). This structure conveys the capacity to undergo a covalent interaction with the thiol group of cysteine (i.e. Michael- addition). Quantitatively reactGSH of the alpha,beta-unsaturated carbonyl compounds is reliant upon the specific molecular structure with several tendencies observed. Specifically, it was noted that for alpha,beta-unsaturated carbonyl compounds: (1) the acetylenic-substituted derivatives were more reactive than the corresponding olefinic-substituted ones; (2) terminal vinyl-substituted derivatives was more reactive than the internal vinylene-substituted ones; (3) methyl substitution on the vinyl carbon atoms diminishes reactivity and methyl-substitution on the carbon atom farthest from the carbonyl group causes a larger reduction; (4) derivatives with carbon-carbon double bond on the end of the molecule (i.e. vinyl ketone) were more reactive than one with the carbon-oxygen bond at the end of the molecule (i.e. aldehyde) and (5) the ester with an additional unsaturated vinyl groups were more reactive than the derivative having an unsaturated ethyl group. 相似文献
6.
Gabrielle A. Leith Allison M. Rice Brandon J. Yarbrough Anna A. Berseneva Richard T. Ly Charles N. Buck III Dr. Denis Chusov Amy J. Brandt Prof. Dr. Donna A. Chen Benjamin W. Lamm Prof. Dr. Morgan Stefik Kenneth S. Stephenson Dr. Mark D. Smith Prof. Dr. Aaron K. Vannucci Dr. Perry J. Pellechia Prof. Dr. Sophya Garashchuk Prof. Dr. Natalia B. Shustova 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(15):6056-6062
The effect of donor (D)–acceptor (A) alignment on the materials electronic structure was probed for the first time using novel purely organic porous crystalline materials with covalently bound two- and three-dimensional acceptors. The first studies towards estimation of charge transfer rates as a function of acceptor stacking are in line with the experimentally observed drastic, eight-fold conductivity enhancement. The first evaluation of redox behavior of buckyball- or tetracyanoquinodimethane-integrated crystalline was conducted. In parallel with tailoring the D-A alignment responsible for “static” changes in materials properties, an external stimulus was applied for “dynamic” control of the electronic profiles. Overall, the presented D–A strategic design, with stimuli-controlled electronic behavior, redox activity, and modularity could be used as a blueprint for the development of electroactive and conductive multidimensional and multifunctional crystalline porous materials. 相似文献
7.
Stack the Bowls: Tailoring the Electronic Structure of Corannulene‐Integrated Crystalline Materials 下载免费PDF全文
Allison M. Rice Ekaterina A. Dolgopolova Brandon J. Yarbrough Gabrielle A. Leith Corey R. Martin Kenneth S. Stephenson Rebecca A. Heugh Amy J. Brandt Prof. Dr. Donna A. Chen Dr. Stavros G. Karakalos Dr. Mark D. Smith Prof. Dr. Kelsey B. Hatzell Dr. Perry J. Pellechia Prof. Dr. Sophya Garashchuk Prof. Dr. Natalia B. Shustova 《Angewandte Chemie (International ed. in English)》2018,57(35):11310-11315
We report the first examples of purely organic donor–acceptor materials with integrated π‐bowls (πBs) that combine not only crystallinity and high surface areas but also exhibit tunable electronic properties, resulting in a four‐orders‐of‐magnitude conductivity enhancement in comparison with the parent framework. In addition to the first report of alkyne–azide cycloaddition utilized for corannulene immobilization in the solid state, we also probed the charge transfer rate within the Marcus theory as a function of mutual πB orientation for the first time, as well as shed light on the density of states near the Fermi edge. These studies could foreshadow new avenues for πB utilization for the development of optoelectronic devices or a route for highly efficient porous electrodes. 相似文献
8.
Grace C. Thaggard Dr. Gabrielle A. Leith Daniil Sosnin Dr. Corey R. Martin Kyoung Chul Park Margaret K. McBride Dr. Jaewoong Lim Brandon J. Yarbrough Buddhima K. P. Maldeni Kankanamalage Gina R. Wilson Austin R. Hill Dr. Mark D. Smith Prof. Dr. Sophya Garashchuk Prof. Dr. Andrew B. Greytak Prof. Dr. Ivan Aprahamian Prof. Dr. Natalia B. Shustova 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2023,135(2):e202211776
Confinement-imposed photophysics was probed for novel stimuli-responsive hydrazone-based compounds demonstrating a conceptual difference in their behavior within 2D versus 3D porous matrices for the first time. The challenges associated with photoswitch isomerization arising from host interactions with photochromic compounds in 2D scaffolds could be overcome in 3D materials. Solution-like photoisomerization rate constants were realized for sterically demanding hydrazone derivatives in the solid state through their coordinative immobilization in 3D scaffolds. According to steady-state and time-resolved photophysical measurements and theoretical modeling, this approach provides access to hydrazone-based materials with fast photoisomerization kinetics in the solid state. Fast isomerization of integrated hydrazone derivatives allows for probing and tailoring resonance energy transfer (ET) processes as a function of excitation wavelength, providing a novel pathway for ET modulation. 相似文献
9.
Michael Beck Eric Pine Wayne Tarrant Kim Yarbrough Jensen. 《Mathematics of Computation》2007,76(259):1683-1690
We describe a new algorithm for finding integer solutions to for specific values of . We use this to find representations for values of for which no solution was previously known, including and .
10.
Stimuli-responsive temporary adhesives constitute a rapidly developing class of materials defined by the modulation of adhesion upon exposure to an external stimulus or stimuli. Engineering these materials to shift between two characteristic properties, strong adhesion and facile debonding, can be achieved through design strategies that target molecular functionalities. This perspective reviews the recent design and development of these materials, with a focus on the different stimuli that may initiate debonding. These stimuli include UV light, thermal energy, chemical triggers, and other potential triggers, such as mechanical force, sublimation, electromagnetism. The conclusion discusses the fundamental value of systematic investigations of the structure–property relationships within these materials and opportunities for unlocking novel functionalities in future versions of adhesives.Stimuli-responsive temporary adhesives emerge as next-generation multifunctional materials with advantages that include strong temporary adhesion, debonding on demand, and tunable reactivity. 相似文献