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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(30):8842-8846
Lithium hydride (LiH) has a strong effect on iron leading to an approximately 3 orders of magnitude increase in catalytic ammonia synthesis. The existence of lithium–iron ternary hydride species at the surface/interface of the catalyst were identified and characterized for the first time by gas‐phase optical spectroscopy coupled with mass spectrometry and quantum chemical calculations. The ternary hydride species may serve as centers that readily activate and hydrogenate dinitrogen, forming Fe‐(NH2)‐Li and LiNH2 moieties—possibly through a redox reaction of dinitrogen and hydridic hydrogen (LiH) that is mediated by iron—showing distinct differences from ammonia formation mediated by conventional iron or ruthenium‐based catalysts. Hydrogen‐associated activation and conversion of dinitrogen are discussed. 相似文献
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(31):9205-9209
We rationally engineered an elegant entropy‐driven DNA nanomachine with three‐dimensional track and applied it for intracellular miRNAs imaging. The proposed nanomachine is activated by target miRNA binding to drive a walking leg tethered to gold nanoparticle with a high density of DNA substrates. The autonomous and progressive walk on the DNA track via the entropy‐driven catalytic reaction of intramolecular toehold‐mediated strand migration leads to continuous disassembly of DNA substrates, accompanied by the recovery of fluorescence signal due to the specific release of a dye‐labeled substrate from DNA track. Our nanomachine outperforms the conventional intermolecular reaction‐based gold nanoparticle design in the context of an improved sensitivity and kinetics, attributed to the enhanced local effective concentrations of working DNA components from the proximity‐induced intramolecular reaction. Moreover, the nanomachine was applied for miRNA imaging inside living cells. 相似文献
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(39):11988-11992
A general anion‐sensing platform is reported based on a portable and cost‐effective ion‐selective optode and a smartphone detector equipped with a color analysis app. In contrast to traditional anion‐selective optodes using a hydrophobic polymer and/or plasticizer to dissolve hydrophobic sensing elements, the new optode relies on hydrophilic cellulose paper. The anion ionophore and a lipophilic pH indicator are inkjet‐printed and adsorbed on paper and form a “dry” hydrophobic sensing layer. Porous cellulose sheets also allow the sensing site to be modified with dried buffer that prevents any sample pH dependence of the observed color change. A highly selective fluoride optode using an AlIII‐porphyrin ionophore is examined as an initial example of this new anion sensing platform for measurements of fluoride levels in drinking water samples. Apart from Lewis acid–base recognition, hydrogen bonding recognition is also compatible with this sensing platform. 相似文献
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