共查询到20条相似文献,搜索用时 15 毫秒
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(50):16244-16247
The direct observation of amorphous barium carbonate (ABC), which transforms into a previously unknown barium carbonate hydrate (herewith named gortatowskite) within a few hundred milliseconds of formation, is described. In situ X‐ray scattering, cryo‐, and low‐dose electron microscopy were used to capture the transformation of nanoparticulate ABC into gortatowskite crystals, highly anisotropic sheets that are up to 1 μm in width, yet only about 10 nm in thickness. Recrystallization of gortatowskite to witherite starts within 30 seconds. We describe a bulk synthesis and report a first assessment of the composition, vibrational spectra, and structure of gortatowskite. Our findings indicate that transient amorphous and crystalline precursors can play a role in aqueous precipitation pathways that may often be overlooked owing to their extremely short lifetimes and small dimensions. However, such transient precursors may be integral to the formation of more stable phases. 相似文献
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(43):13625-13629
Macromolecular crystallization has many implications in biological and materials science. Similar to the crystallization of other molecules, macromolecular crystallization conventionally considers a critical nucleus, followed by crystallographic packing of macromolecules to drive further crystal growth. Herein, we discover a distinctive macromolecular crystallization pathway by developing the concept of a macromolecular mesocrystal. This nonclassical polymer crystallization occurs through the mesoscale self‐assembly of (bio)macromolecular nanocrystals. The new concept for macromolecular crystallization presented herein is fundamental and relevant to many fields, including materials science, chemistry, biomimetics, nanoscience, and structural biology. 相似文献
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(39):11902-11905
Early‐stage reaction mechanisms for aragonite‐promoting systems are relatively unknown compared to the more thermodynamically stable calcium carbonate polymorph, calcite. Using cryoTEM and SEM, the early reaction stages taking place during aragonite formation were identified in a highly supersaturated solution using an alcohol–water solvent, and an overall particle attachment growth mechanism was described for the system. In vitro evidence is provided for the solid‐state transformation of amorphous calcium carbonate to aragonite, demonstrating the co‐existence of both amorphous and crystalline material within the same aragonite needle. This supports non‐classical formation of aragonite within both a synthetic and biological context. 相似文献
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Hongbin Zhang Yang Zhao Hongxia Zhang Peicheng Wang Zhangping Shi Jianjiang Mao Prof. Yahong Zhang Prof. Yi Tang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(21):7141-7151
Diffusion limitation in micropores of zeolites leads to a demand for optimization of zeolite morphology and/or porosity. However, tailoring crystallization processes to realize targeted morphology/porosity is a major challenge in zeolite synthesis. On the basis of previous work on the salt‐aided, seed‐induced route, the template effect of seeds on the formation of micropores, mesopores and even macropores was further explored to selectively achieve desired hierarchical architectures. By carefully investigating the crystallization processes of two typical samples with distinct crystal morphologies, namely, 1) nanocrystallite‐oriented self‐assembled ZSM‐5 zeolite and 2) enriched intracrystal mesoporous ZSM‐5 zeolite, a detailed mechanism is proposed to clarify the role of silicalite‐1 seeds in the formation of diverse morphologies in a salt‐rich heterogeneous system, combined with the transformation of seed‐embedded aluminosilicate gel. On the basis of these conclusions, the morphologies/porosities of products were precisely tailored by deliberately adjusting the synthesis parameters (KF/Si, tetrapropylammonium bromide/Si and H2O/Si ratios and type of organic template) to regulate the kinetics of seed dissolution and seed‐induced recrystallization. This work may not only provide a practical route to control zeolite crystallization for tailoring crystal morphology, but also expands the knowledge of crystal growth mechanisms in a heterogeneous system. 相似文献
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Seoyeon Choi Rahul Dev Mukhopadhyay Younghoon Kim In‐Chul Hwang Wooseup Hwang Suman Kr Ghosh Kangkyun Baek Kimoon Kim 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(47):17006-17009
Transient self‐assembling systems often suffer from accumulation of chemical wastes that interfere with the formation of pristine self‐assembled products in subsequent cycles. Herein, we report the transient crystallization of a cucurbit[8]uril‐based host‐guest complex, preventing the accumulation of chemical wastes. Base‐catalyzed thermal decarboxylation of trichloroacetic acid that chemically fuels the crystallization process dissolves the crystals, and produces volatile chemical wastes that are spontaneously removed from the solution. With such self‐clearance process, no significant damping in the formation of the crystals was observed. The morphology and structural integrity of the crystals was also maintained in subsequent cycles. The concept may be further extended to obtain other temporally functional materials, quasicrystals, etc., based on stimuli‐responsive guest molecules. 相似文献
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Zhi Cai Lidong Li Youwei Zhang Zhao Yang Jie Yang Yingjie Guo Lin Guo 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(13):4233-4238
Electrochemical water splitting requires efficient, low‐cost water oxidation catalysts to accelerate the sluggish kinetics of the water oxidation reaction. A rapid photocorrosion method is now used to synthesize the homogeneous amorphous nanocages of Cu‐Ni‐Fe hydr(oxy)oxide as a highly efficient electrocatalyst for the oxygen evolution reaction (OER). The as‐fabricated product exhibits a low overpotential of 224 mV on a glassy carbon electrode at 10 mA cm?2 (even lower down to 181 mV when supported on Ni foam) with a Tafel slope of 44 mV dec?1 for OER in an alkaline solution. The obtained catalyst shows an extraordinarily large mass activity of 1464.5 A g?1 at overpotential of 300 mV, which is the highest mass activity for OER. This synthetic strategy may open a brand new pathway to prepare copper‐based ternary amorphous nanocages for greatly enhanced oxygen evolution. 相似文献
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Shawn J. Tan Jason S. Kahn Thomas L. Derrien Michael J. Campolongo Mervin Zhao Detlef‐M. Smilgies Dan Luo 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2014,126(5):1340-1343
The multiparametric nature of nanoparticle self‐assembly makes it challenging to circumvent the instabilities that lead to aggregation and achieve crystallization under extreme conditions. By using non‐base‐pairing DNA as a model ligand instead of the typical base‐pairing design for programmability, long‐range 2D DNA–gold nanoparticle crystals can be obtained at extremely high salt concentrations and in a divalent salt environment. The interparticle spacings in these 2D nanoparticle crystals can be engineered and further tuned based on an empirical model incorporating the parameters of ligand length and ionic strength. 相似文献
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(1):236-240
The mechanism of isopropanol dehydration on amorphous silica–alumina (ASA) was unraveled by a combination of experimental kinetic measurements and periodic density functional theory (DFT) calculations. We show that pseudo‐bridging silanols (PBS‐Al) are the most likely active sites owing to the synergy between the Brønsted and Lewis acidic properties of these sites, which facilitates the activation of alcohol hydroxy groups as leaving groups. Isopropanol dehydration was used to specifically investigate these PBS‐Al sites, whose density was estimated to be about 10−1 site nm−2 on the silica‐doped alumina surface under investigation, by combining information from experiments and theoretical calculations. 相似文献
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Benjamin M. Tansi Matthew L. Peris Oleg E. Shklyaev Anna C. Balazs Ayusman Sen 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(8):2317-2321
The field of active matter holds promise for applications in particle assembly, cargo and drug delivery, and sensing. In pursuit of these capabilities, researchers have produced a suite of nanomotors, fluid pumps, and particle assembly strategies. Although promising, there are many challenges, especially for mechanisms that rely on chemical propulsion. One way to circumvent these issues is by the use of external energy sources. Herein, we propose a method of using freely suspended nanoparticles to generate fluid pumping towards desired point sources. The pumping rates are dependent on particle concentration and light intensity, making it highly controllable. Using these directed flows, we further demonstrate the ability to reversibly construct and move colloidal crystals. 相似文献
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Alexander Aerts Dr. Mohamed Haouas Dr. Tom P. Caremans Lana R. A. Follens Dr. Titus S. van Erp Dr. Francis Taulelle Dr. Jan Vermant Prof. Johan A. Martens Prof. Christine E. A. Kirschhock Prof. 《Chemistry (Weinheim an der Bergstrasse, Germany)》2010,16(9):2764-2774
Colloidal silicalite‐1 zeolite was crystallized from a concentrated clear sol prepared from tetraethylorthosilicate (TEOS) and aqueous tetrapropylammonium hydroxide (TPAOH) solution at 95 °C. The silicate speciation was monitored by using dynamic light scattering (DLS), synchrotron small‐angle X‐ray scattering (SAXS), and quantitative liquid‐state 29Si NMR spectroscopy. The silicon atoms were present in dissolved oligomers, two discrete nanoparticle populations approximately 2 and 6 nm in size, and crystals. On the basis of new insight into the evolution of the different nanoparticle populations and of the silicate connectivity in the nanoparticles, a refined crystallization mechanism was derived. Upon combining the reagents, different types of nanoparticles (ca. 2 nm) are formed. A fraction of these nanoparticles with the least condensed silicate structure does not participate in the crystallization process. After completion of the crystallization, they represent the residual silicon atoms. Nanoparticles with a more condensed silicate network grow until approximately 6 nm and evolve into building blocks for nucleation and growth of the silicalite‐1 crystals. The silicate network connectivity of nanoparticles suitable for nucleation and growth increasingly resembles that of the final zeolite. This new insight into the two classes of nanoparticles will be useful to tune the syntheses of silicalite‐1 for maximum yield. 相似文献