scholarly journals Ordered colloidal clusters constructed by nanocrystals with valence for efficient CO2 photoreduction

2019 ◽  
Vol 5 (12) ◽  
pp. eaax5095 ◽  
Author(s):  
Jianwei Nai ◽  
Sibo Wang ◽  
Xiong Wen (David) Lou
Keyword(s):  
Building Blocks ◽  
Molecular Clusters ◽  
Oriented Attachment ◽  
Porous Structures ◽  
Interparticle Interactions ◽  
Ordered Structures ◽  
Atomic Orbitals ◽  
Colloidal Clusters ◽  
Prussian Blue Analog ◽  
Directional Bonding

The ability to construct discrete colloidal clusters (CCs) as complex as molecular clusters is limited due to the lack of available colloidal building blocks and specific directional bonds. Here, we explore a strategy to organize anisotropic Prussian blue analog nanocrystals (NCs) toward CCs with open and highly ordered structures, experimentally realizing colloidal analogs to zeolitic clathrate structures. The directional interactions are derived from either crystallographic or morphological anisotropy of the NCs and achieved by the interplay of epitaxial growth, oriented attachment, and local packing. We attribute these interparticle interactions to enthalpic and entropic valences that imitate hybridized atomic orbitals of sp3d2 octahedron and sp3d3f cube. Benefiting from the ordered multilevel porous structures, the obtained CCs exhibit greatly enhanced catalytic activity for CO2 photoreduction. Our work offers some fundamental insights into directional bonding among NCs and opens an avenue that promises access to unique CCs with unprecedented structures and applications.

scholarly journals DNA-mediated engineering of multicomponent enzyme crystals

2015 ◽  
Vol 112 (15) ◽  
pp. 4564-4569 ◽  
Author(s):  
Jeffrey D. Brodin ◽  
Evelyn Auyeung ◽  
Chad A. Mirkin
Keyword(s):  
Gold Nanoparticles ◽  
Protein Interactions ◽  
Building Blocks ◽  
Inorganic Nanoparticles ◽  
Protein Protein Interactions ◽  
Dna Interactions ◽  
Interparticle Interactions ◽  
Crystalline Materials ◽  
Catalytically Active ◽  
Surface Chemistries

The ability to predictably control the coassembly of multiple nanoscale building blocks, especially those with disparate chemical and physical properties such as biomolecules and inorganic nanoparticles, has far-reaching implications in catalysis, sensing, and photonics, but a generalizable strategy for engineering specific contacts between these particles is an outstanding challenge. This is especially true in the case of proteins, where the types of possible interparticle interactions are numerous, diverse, and complex. Herein, we explore the concept of trading protein–protein interactions for DNA–DNA interactions to direct the assembly of two nucleic-acid–functionalized proteins with distinct surface chemistries into six unique lattices composed of catalytically active proteins, or of a combination of proteins and DNA-modified gold nanoparticles. The programmable nature of DNA–DNA interactions used in this strategy allows us to control the lattice symmetries and unit cell constants, as well as the compositions and habit, of the resulting crystals. This study provides a potentially generalizable strategy for constructing a unique class of materials that take advantage of the diverse morphologies, surface chemistries, and functionalities of proteins for assembling functional crystalline materials.

Sequential dynamic structuralisation by in situ production of supramolecular building blocks

2017 ◽  
Vol 53 (61) ◽  
pp. 8553-8556 ◽  
Author(s):  
Hirohiko Yuasa ◽  
Kouichi Asakura ◽  
Taisuke Banno
Keyword(s):  
Building Blocks ◽  
Ordered Structures ◽  
In Situ Production

We demonstrate an example of sequential dynamic higher structuralisation from disordered droplets into higher-ordered structures, resulting in the formation of a hydrogel.

scholarly journals Nonclassical nucleation of protein mesocrystals via oriented attachment

2020 ◽  
Author(s):  
Alexander E.S. Van Driessche ◽  
Nani Van Gerven ◽  
Rick R.M. Joosten ◽  
Wai Li Ling ◽  
Maria Bacia ◽  
...  
Keyword(s):  
Self Assembly ◽  
Protein Crystallization ◽  
Building Blocks ◽  
Oriented Attachment ◽  
Great Promise ◽  
Inorganic Systems ◽  
Maturation Stages ◽  
Designer Proteins ◽  
Rate Limit ◽  
Classical Mechanism

AbstractSelf-assembly of proteins holds great promise for the bottom-up design and production of synthetic biomaterials. In conventional approaches, designer proteins are pre-programmed with specific recognition sites that drive the association process towards a desired organized state. Although proven effective, this approach poses restrictions on the complexity and material properties of the end-state. An alternative, hierarchical approach that has found wide adoption for inorganic systems, relies on the production of crystalline nanoparticles which in turn become the building blocks of a next-level assembly process driven by oriented attachment (OA). As it stands, OA has not been observed for proteins. Here we employ cryoEM in the high nucleation rate limit of protein crystals and map the self-assembly route at molecular resolution. We observe the initial formation of facetted nanocrystals that merge lattices by means of OA alignment well before contact is made, satisfying non-trivial symmetry rules in the process. The OA mechanism yields crystal morphologies that are not attainable through conventional crystallization routes. Based on these insights we revisit a system of protein crystallization that has long been classified as non-classical, but our data is in direct conflict with that conclusion supporting a classical mechanism that implicates OA. These observations raise further questions about past conclusions for other proteins and illustrate the importance of maturation stages after primary nucleation has taken place.

scholarly journals 15N NMR Shifts of Eumelanin Building Blocks in Water: A Combined Quantum Mechanics/Statistical Mechanics Approach

Molecules ◽  
2020 ◽  
Vol 25 (16) ◽  
pp. 3616
Author(s):  
Leonardo Bruno Assis Oliveira ◽  
Tertius L. Fonseca ◽  
Benedito J. C. Cabral
Keyword(s):  
Quantum Mechanics ◽  
Statistical Mechanics ◽  
Gas Phase ◽  
Marked Effect ◽  
Complex Structure ◽  
Building Blocks ◽  
15N Nmr ◽  
Magnetic Shielding ◽  
Atomic Orbitals ◽  
Theoretical Results

Theoretical results for the magnetic shielding of protonated and unprotonated nitrogens of eumelanin building blocks including monomers, dimers, and tetramers in gas phase and water are presented. The magnetic property in water was determined by carrying out Monte Carlo statistical mechanics sampling combined with quantum mechanics calculations based on the gauge-including atomic orbitals approach. The results show that the environment polarization can have a marked effect on nitrogen magnetic shieldings, especially for the unprotonated nitrogens. Large contrasts of the oligomerization effect on magnetic shielding show a clear distinction between eumelanin building blocks in solution, which could be detected in nuclear magnetic resonance experiments. Calculations for a π-stacked structure defined by the dimer of a tetrameric building block indicate that unprotonated N atoms are significantly deshielded upon π stacking, whereas protonated N atoms are slightly shielded. The results stress the interest of NMR experiments for a better understanding of the eumelanin complex structure.

The evaluation of van der Waals interaction in the oriented-attachment growth of nanotubes

2014 ◽  
Vol 1705 ◽  
Author(s):  
Weixuan Jin ◽  
Weidong He ◽  
Kechun Wen ◽  
Xiao Lin ◽  
Yuqian Zhang ◽  
...  
Keyword(s):  
Growth Mechanism ◽  
Side Effect ◽  
Growth Parameters ◽  
Van Der Waals ◽  
Van Der Waals Interaction ◽  
Oriented Attachment ◽  
Interparticle Interactions ◽  
Fundamental Understanding ◽  
First Time

AbstractTaking the advantage of nanomaterials to protect the environment and avoiding the side effect need a fundamental understanding of the growth mechanism of the nanomaterials. Here, the van der Waals interaction between a nanoparticle and a nanotube in the oriented-attachment growth of nanotubes is quantitatively evaluated for the first time. In particular, the correlation between van der Waals interaction and the growth parameters is investigated in depth. Our work opens up the opportunity of studying the important interparticle interactions in the oriented attachment growth of nanotubes.

scholarly journals Patchy Nanoparticle Synthesis and Self-Assembly

2020 ◽  
Author(s):  
Ahyoung Kim ◽  
Lehan Yao ◽  
Falon Kalutantirige ◽  
Shan Zhou ◽  
Qian Chen
Keyword(s):  
Self Assembly ◽  
Nanoparticle Synthesis ◽  
Building Blocks ◽  
Design And Synthesis ◽  
Patchy Particles ◽  
Living Organisms ◽  
Directional Bonding ◽  
Patchy Nanoparticles ◽  
Assembly Pathways ◽  
Physical Principles

Biological building blocks (i.e., proteins) are encoded with the information of target structure into the chemical and morphological patches, guiding their assembly into the levels of functional structures that are crucial for living organisms. Learning from nature, researchers have been attracted to the artificial analogues, “patchy particles,” which have controlled geometries of patches that serve as directional bonding sites. However, unlike the abundant studies of micron-scale patchy particles, which demonstrated complex assembly structures and unique behaviors attributed to the patches, research on patchy nanoparticles (NPs) has remained challenging. In the present chapter, we discuss the recent understandings on patchy NP design and synthesis strategies, and physical principles of their assembly behaviors, which are the main factors to program patchy NP self-assembly into target structures that cannot be achieved by conventional non-patched NPs. We further summarize the self-assembly of patchy NPs under external fields, in simulation, and in kinetically controlled assembly pathways, to show the structural richness patchy NPs bring. The patchy NP assembly is novel by their structures as well as the multicomponent features, and thus exhibits unique optical, chemical, and mechanical properties, potentially aiding applications in catalysts, photonic crystals, and metamaterials as well as fundamental nanoscience.

Post-synthetic oriented attachment of CsPbBr3 perovskite nanocrystal building blocks: from first principle calculation to experimental demonstration of size and dimensionality (0D/1D/2D)

2020 ◽  
Vol 5 (6) ◽  
pp. 960-970 ◽  
Author(s):  
Sanghyun Jeon ◽  
Myung-Chul Jung ◽  
Junhyuk Ahn ◽  
Ho Kun Woo ◽  
Junsung Bang ◽  
...  
Keyword(s):  
Building Blocks ◽  
Oriented Attachment ◽  
First Principle ◽  
Experimental Demonstration ◽  
Solvent Treatment ◽  
Principle Calculation ◽  
First Principle Calculation

Immiscible solvent treatment induced oriented attachment of perovskite nanocrystal, resulting in change of size and dimensionality (0D/1D/2D).

HYDROGEN-BONDED STRUCTURES OF TRIMESIC AND MELAMINE ON HIGHLY ORIENTED PYROLYTIC GRAPHITE

2014 ◽  
Vol 21 (03) ◽  
pp. 1450035 ◽  
Author(s):  
LING ZHU ◽  
XUMING XU ◽  
YAN WANG ◽  
SHUYI LIU ◽  
JIE LING ◽  
...  
Keyword(s):  
Scanning Tunneling Microscopy ◽  
Functional Groups ◽  
Guest Molecule ◽  
Pyrolytic Graphite ◽  
Building Blocks ◽  
Scanning Tunneling ◽  
Porous Structures ◽  
Highly Oriented Pyrolytic Graphite ◽  
Tunneling Microscopy ◽  
Trimesic Acid

The assembled structures of triangular symmetrically shape molecules with three functional groups, trimesic acid (TMA) and melamine, have been investigated by scanning tunneling microscopy on Highly Oriented Pyrolytic Graphite (HOPG) in ambient. Hexagonal porous structures are formed by these molecules and the cavity of the assembled structure becomes bigger when larger molecules are used as building blocks. The cavity within the assembled structure formed by TMA is bigger enough to host guest molecule.

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