Growth of organic crystals via attachment and transformation of nanoscopic precursors

Jiang, Yuan; Kellermeier, Matthias; Gebauer, Denis; Lu, Zihao; Rosenberg, Rose; Moise, Adrian; Przybylski, Michael; Cölfen, Helmut

doi:10.1038/ncomms15933

Cited by 43 publications

(49 citation statements)

References 44 publications

(73 reference statements)

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“…The exact nature of this high binding affinity is unknown, although the exceedingly high binding force revealed in our AFM analysis of CC interaction with cholesterol-containing lipid domain may offer some clue. The extraction of cholesterol from the membrane may mimic the precursor condensation onto the crystalline surface in the typical growth of organic crystals ( 57 ), which may be translated into a force exerted on the plasma membrane. This notion, however, requires vigorous experimental verification, as alternative explanation may exist.…”

Section: Discussionmentioning

confidence: 99%

Cholesterol Crystal-Mediated Inflammation Is Driven by Plasma Membrane Destabilization

Shu

Chen

et al. 2018

Front. Immunol.

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Atherosclerosis is driven by an inflammatory milieu in the walls of artery vessels. Initiated early in life, it progresses to plaque formation and form cell accumulation. A culprit in this cascade is the deposition of cholesterol crystals (CC). The involvement of smaller crystals in the early stage of atherosclerotic changes may be critical to the long-term pathological development. How these small crystals initiate the pro-inflammatory events is under study. We report here an unexpected mechanism that microscopic CC interact with cellular membrane in a phagocytosis-independent manner. The binding of these crystals extracts cholesterol from the cell surface. This process causes a sudden catastrophic rupture of plasma membrane and necrosis of the bound cells independent of any known cell death-inducing pathways, releasing inflammatory agents associated with the necrotic cell death. Our results, therefore, reveal a biophysical aspect of CC in potentially mediating the inflammatory progress in atherosclerosis.

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Section: Discussionmentioning

confidence: 99%

Cholesterol Crystal-Mediated Inflammation Is Driven by Plasma Membrane Destabilization

Shu

Chen

et al. 2018

Front. Immunol.

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“…When LCPs are applied for controlling the organization of organic and inorganic materials, liquid‐solid and liquid‐liquid interfaces are crucial factors. Recently, crystallization studies of D,L‐glutamic acid identify the attachment of hydrated nanoscopic assemblies to pre‐formed crystals, followed by the release of hydration water, structural relaxation and transformation to 2D crystals . However, on silica surface, the nanoscopic assemblies do not transform easily.…”

Section: Pathways To Complex Organizations Of Mattermentioning

confidence: 98%

From Solute, Fluidic and Particulate Precursors to Complex Organizations of Matter

Rao

Cölfen

2018

The Chemical Record

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The organization of matter from its constitutive units recruits intermediate states with distinctive degrees of self-association and molecular order. Existing as clusters, droplets, gels as well as amorphous and crystalline nanoparticles, these precursor forms have fundamental contributions towards the composition and structure of inorganic and organic architectures. In this personal account, we show that the transitions from atoms, molecules or ionic species to superstructures of higher order are intertwined with the interfaces and interactions of precursor and intermediate states. Structural organizations distributed across different length scales are explained by the multistep nature of nucleation and crystallization, which can be guided towards functional hybrid materials by the strategic application of additives, templates and reaction environments. Thus, the non-classical pathways for material formation and growth offer conceptual frameworks for elucidating, inducing and directing fascinating material organizations of biogenic and synthetic origins.

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“…Traditionally, crystallization is considered to follow the classical theory based on monomer-bymonomer addition. However, it has recently been shown that nonclassical crystallization occurs in many systems: 21,48,50,[77][78][79][80][81][82] Nucleation can have a two-step mechanism that differs from that described by classical nucleation theory; 77,83-87 particles larger than monomers / ions can participate in the growth of crystals; 30,39,40 an oriented attachment (OA) mechanism has also been identified, in which nanocrystals coalesce to form the bulk crystal. 34,[36][37][38]88 The term "crystallization by particle attachment (CPA)" is now used to denote crystallization processes that are dominated by particles other than monomers / ions.…”

Section: Nonclassical Crystallization Of Cof-5mentioning

confidence: 99%

Nucleation and Growth of Covalent Organic Frameworks from Solution: The Example of COF-5

et al. 2017

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The preparation of two-dimensional covalent organic frameworks (2D COFs) with large crystalline domains and controlled morphology is necessary for realizing the full potential of their atomically precise structures and uniform, tailorable porosity. Currently 2D COF syntheses are developed empirically, and most materials are isolated as insoluble and unprocessable powders with typical crystalline domain sizes smaller than 50 nm. Little is known about their nucleation and growth processes, which involve a combination of covalent bond formation, degenerate bond exchange, and noncovalent stacking processes. A deeper understanding of the chemical processes that lead to COF polymerization and crystallization is key to achieving improved materials quality and control. Here, we report a kinetic Monte Carlo (KMC) model that describes the formation of a prototypical boronate-ester linked 2D COF known as COF-5 from its 2,3,6,7,10,11-hexahydroxytriphenylene and 1,4-phenylene bis(boronic acid) monomers in solution. The key rate parameters for the KMC model were derived from experimental measurements when possible and complemented with reaction pathway analyses, molecular dynamics simulations, and binding free-energy calculations. The essential features of experimentally measured COF-5 growth kinetics are reproduced well by the KMC simulations. In particular, the simulations successfully captured a nucleation process followed by a subsequent growth process. The nucleating species are found to be relatively small, multilayer structures that form through multiple pathways. During the growth of COF-5, extensions in the lateral (in-plane) and vertical (stacking) directions are both seen to be linear with respect to time and are dominated by monomer addition and oligomer association, respectively. Finally, we show that the experimental observations of increased average crystallite size with the addition of water are modeled accurately by the simulations. These results will inform the rational development of 2D COF polymerizations by controlling the rate of nucleation, thereby increasing their materials quality.

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Growth of organic crystals via attachment and transformation of nanoscopic precursors

Cited by 43 publications

References 44 publications

Cholesterol Crystal-Mediated Inflammation Is Driven by Plasma Membrane Destabilization

Cholesterol Crystal-Mediated Inflammation Is Driven by Plasma Membrane Destabilization

From Solute, Fluidic and Particulate Precursors to Complex Organizations of Matter

Nucleation and Growth of Covalent Organic Frameworks from Solution: The Example of COF-5

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