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71.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(6):1670-1674
An area‐selective atomic layer deposition (AS‐ALD) method is described to construct oxide nanotraps to anchor Pt nanoparticles (NPs) on Al2O3 supports. The as‐synthesized catalysts have exhibited outstanding room‐temperature CO oxidation activity, with a significantly lowered apparent activation energy (ca. 22.17 kJ mol−1) that is half that of pure Pt catalyst with the same loading. Furthermore, the structure shows excellent sintering resistance with the high catalytic activity retention up to 600 °C calcination. The key feature of the oxide nanotraps lies in its ability to anchor Pt NPs via strong metal–oxide interactions while still leaving active metal facets exposed. Our reported method for forming such oxide structure with nanotraps shows great potential for the simultaneous enhancement of thermal stability and activity of precious metal NPs. 相似文献
72.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(11):3035-3039
A new strategy is described for generating strong circularly polarized luminescence with highly tunable emission bands through chiral induction in nonchiral, totally organic, low‐molecular‐weight fluorescent dyes by chiral nanotemplate systems. Our approach allows the first systematic investigation to clarify the correlation between the circular dichroism and circularly polarized luminescence intensities. As a result, a dilute solution system with the highest circularly polarized luminescence intensity achieved to date and a dissymmetry factor of over 0.1 was identified. 相似文献
73.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(18):5113-5116
A membrane‐intercalating conjugated oligoelectrolyte (COE), PTTP , was designed and synthesized with the goal of providing red‐shifted absorption spectra relative to previously synthesized COE analogs. Specifically, electron‐rich and electron‐poor subunits were introduced in the conjugated backbone to modulate the band gap. PTTP exhibits maxima of absorption at 507 nm and of emission at 725 nm. PTTP can also efficiently function to generate singlet oxygen in situ (ΦΔ≈20 %) and has appropriate topology and dimensions to interact with lipid membranes. The resulting rapid membrane insertion and sensitizing ability provide PTTP with a highly efficient antibacterial capability under a low light dose (0.6 J cm−2) toward Gram‐negative bacteria E. coli, making it a remarkably efficient optically mediated antimicrobial agent. 相似文献
74.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(15):4302-4306
A 3,7‐diazabicyclo[3.3.1]nonane linking to two melamines is a unique transmembrane H+/Cl− carrier. In the solid state, the V‐shaped compound forms a HCl‐bound zig‐zag network through cooperative protonation and hydrogen bond interactions. In the lipid membrane, the receptor forms a dimeric self‐assembly involving multiple H+ and Cl− leading to the efficient transport of the acid. The pH‐dependent Cl− efflux observed for the compound was rationalized based on a gradual protonation model that confers an active transmembrane carrier at physiological pH. 相似文献
75.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(16):4636-4639
Multicomponent reactions are excellent tools for rapid generation of small molecules with broad chemical diversity and molecular complexity. Herein, a novel one‐pot multicomponent synthesis of β‐amino amides from aldehydes, anilines, carboxylic acids and ynamides has been successfully developed. This process is practical and efficient to unravel synthetic utility and scalability. Moreover, an isotope labeling reaction was conducted to elucidate a plausible reaction mechanism. 相似文献
76.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(12):3280-3284
Internally 1,3‐phenylene‐ and 2,5‐thienylene‐bridged [46]decaphyrins 2 and 3 have been synthesized. While 2 shows modest aromatic character derived from the global 46π‐conjugated circuit, 3 displays larger aromatic character owing to the contribution of an (annuleno)annulene‐type network consisting of two twisted Möbius aromatic thia[28]hexaphyrin segments in addition to the global 46π‐network. Upon protonation, these [46]decaphyrins underwent large structural changes to acquire strong aromaticity. Protonated 3 has been revealed to take on a planar structure composed of fused two triangular thia[28]hexaphyrin segments. 相似文献
77.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(24):6871-6876
Engineering near‐infrared (NIR) light‐sensitive enzymes remains a huge challenge. A photothermal effect‐associated method is developed for tailoring the enzymatic activity of enzymes by exposure to NIR light. An ultrasmall platinum nanoparticle was anchored in an enzyme to generate local heating upon NIR irradiation, which enhanced the enzyme activity without increasing bulk temperature. Following NIR irradiation, the enzyme activity was tailored rapidly and reversibly, and was modulated by varying laser power density and irradiation time. Four enzymes were engineered, including glucoamylase, glucose oxidase, catalase, and proteinase K with NIR‐light sensitivity, and demonstrated their utility in practical applications such as photolithography and NIR light‐responsive antibacterial or anticancer actions. Our investigation suggests that this approach could be broadly used to engineer enzymes with NIR‐light sensitivity for many biological applications. 相似文献
78.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(28):8246-8250
We successfully prepared QDs incorporated into a silica/alumina monolith (QDs‐SAM) by a simple sol–gel reaction of an Al–Si single precursor with CsPbBr3 QDs blended in toluene solution, without adding water and catalyst. The resultant transparent monolith exhibits high photoluminescence quantum yields (PLQY) up to 90 %, and good photostability under strong illumination of blue light for 300 h. We show that the preliminary ligand exchange of didodecyl dimethyl ammonium bromide (DDAB) was very important to protect CsPbBr3 QDs from surface damages during the sol–gel reaction, which not only allowed us to maintain the original optical properties of CsPbBr3 QDs but also prevented the aggregation of QDs and made the monolith transparent. The CsPbBr3 QDs‐SAM in powder form was easily mixed into the resins and applied as color‐converting layer with curing on blue light‐emitting diodes (LED). The material showed a high luminous efficacy of 80 lm W−1 and a narrow emission with a full width at half maximum (FWHM) of 25 nm. 相似文献
79.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(26):7654-7658
Deprotonation of the doubly arylene‐bridged diborane(6) derivative 1 H2 with (Me3Si)3CLi or (Me3Si)2NK gives the B−B σ‐bonded species M[ 1 H] in essentially quantitative yields (THF, room temperature; M=Li, K, arylene=4,4′‐di‐tert‐butyl‐2,2′‐biphenylylene). With nBuLi as the base, the yield of Li[ 1 H] drops to 20 % and the 1,1‐bis(9‐borafluorenyl)butane Li[ 2 H] is formed as a side product (30 %). In addition to the 1,1‐butanediyl fragment, the two boron atoms of Li[ 2 H] are linked by a μ‐H bridge. In the closely related molecule Li[ 3 H], the corresponding μ‐H atom can be abstracted with (Me3Si)3CLi to afford the B−B‐bonded conjugated base Li2[ 3 ] (THF, 150 °C; 15 %). Li[ 1 H] and Li[ 2 H] were characterized by NMR spectroscopy and X‐ray crystallography. 相似文献
80.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(27):7905-7910
The aggregation of (pro)chiral/achiral molecules into crystalline structures at interfaces forms conglomerates, racemates, and solid solutions, comparable to known bulk phases. Scanning tunneling microscopy and Monte Carlo simulations were employed to uncover a distinct racemic phase, expressing 1D disordered chiral sorting through random tiling in surface‐confined supramolecularly assembled achiral 4,4′′‐diethynyl‐1,1′:4′,1′′‐terphenyl molecules. The configurational entropy of the 1D disordered racemic tiling phase was verified by analytical modeling, and found to lie between that of a perfectly ordered 2D racemate and a racemic solid solution. 相似文献