Nanostructuring of Molecular Assembly Using Electrochemical Reductive Desorption of Locally Stabilized Thiol Monolayers

2016 ◽  
Vol 120 (29) ◽  
pp. 15823-15829 ◽  
Author(s):  
Katsuyoshi Ikeda ◽  
Yuma Takeuchi ◽  
Kohei Kanamaru ◽  
Shuto Suzuki ◽  
Kohei Uosaki
Keyword(s):  
Molecular Assembly ◽  
Thiol Monolayers ◽  
Reductive Desorption

A Kinetic Model for the Reductive Desorption of Self-Assembled Thiol Monolayers

Langmuir ◽  
2001 ◽  
Vol 17 (11) ◽  
pp. 3273-3280 ◽  
Author(s):  
Willem H. Mulder ◽  
Juan José Calvente ◽  
Rafael Andreu
Keyword(s):  
Kinetic Model ◽  
Thiol Monolayers ◽  
Reductive Desorption ◽  
Self Assembled

Flavin radicals, conformational sampling and robust design principles in interprotein electron transfer: the trimethylamine dehydrogenase-electron-transferring flavoprotein complex

2004 ◽  
Vol 71 ◽  
pp. 1-14
Author(s):  
David Leys ◽  
Jaswir Basran ◽  
François Talfournier ◽  
Kamaldeep K. Chohan ◽  
Andrew W. Munro ◽  
...  
Keyword(s):  
Electron Transfer ◽  
Dimensional Space ◽  
Three Dimensional ◽  
Kinetic Studies ◽  
Molecular Assembly ◽  
Conformational Sampling ◽  
Trimethylamine Dehydrogenase ◽  
Key Residues ◽  
Electron Transferring Flavoprotein ◽  
Electron Transfer Complex

TMADH (trimethylamine dehydrogenase) is a complex iron-sulphur flavoprotein that forms a soluble electron-transfer complex with ETF (electron-transferring flavoprotein). The mechanism of electron transfer between TMADH and ETF has been studied using stopped-flow kinetic and mutagenesis methods, and more recently by X-ray crystallography. Potentiometric methods have also been used to identify key residues involved in the stabilization of the flavin radical semiquinone species in ETF. These studies have demonstrated a key role for 'conformational sampling' in the electron-transfer complex, facilitated by two-site contact of ETF with TMADH. Exploration of three-dimensional space in the complex allows the FAD of ETF to find conformations compatible with enhanced electronic coupling with the 4Fe-4S centre of TMADH. This mechanism of electron transfer provides for a more robust and accessible design principle for interprotein electron transfer compared with simpler models that invoke the collision of redox partners followed by electron transfer. The structure of the TMADH-ETF complex confirms the role of key residues in electron transfer and molecular assembly, originally suggested from detailed kinetic studies in wild-type and mutant complexes, and from molecular modelling.

Chemically Fueled Assembly of Macrocycles Comprising Multiple Transient Bonds

2019 ◽  
Author(s):  
Mohammad Mosharraf Hossain ◽  
Joshua Atkinson ◽  
Scott Hartley
Keyword(s):  
Covalent Bond ◽  
Dicarboxylic Acids ◽  
Molecular Assembly ◽  
Chemical Systems ◽  
Complex Architectures ◽  
The Creation ◽  
Dynamic Exchange

Dissipative (nonequilibrium) assembly powered by chemical fuels has great potential for the creation of new adaptive chemical systems. However, while molecular assembly at equilibrium is routinely used to prepare complex architectures from polyfunctional monomers, species formed out of equilibrium have, to this point, been structurally very simple. In most examples the fuel simply effects the formation of a single transient covalent bond. Here, we show that chemical fuels can assemble bifunctional components into macrocycles containing multiple transient bonds. Specifically, dicarboxylic acids give aqueous dianhydride macrocycles on treatment with a carbodiimide. The macrocycle is assembled efficiently as a consequence of both fuel-dependent and -independent mechanisms: it undergoes slower decomposition, building up as the fuel recycles the components, and is a favored product of the dynamic exchange of the anhydride bonds. These results create new possibilities for generating structurally sophisticated out-of-equilibrium species.

Chemically Fueled Assembly of Macrocycles Comprising Multiple Transient Bonds

2019 ◽  
Author(s):  
Mohammad Mosharraf Hossain ◽  
Joshua Atkinson ◽  
Scott Hartley
Keyword(s):  
Covalent Bond ◽  
Dicarboxylic Acids ◽  
Molecular Assembly ◽  
Chemical Systems ◽  
Complex Architectures ◽  
The Creation ◽  
Dynamic Exchange

Dissipative (nonequilibrium) assembly powered by chemical fuels has great potential for the creation of new adaptive chemical systems. However, while molecular assembly at equilibrium is routinely used to prepare complex architectures from polyfunctional monomers, species formed out of equilibrium have, to this point, been structurally very simple. In most examples the fuel simply effects the formation of a single transient covalent bond. Here, we show that chemical fuels can assemble bifunctional components into macrocycles containing multiple transient bonds. Specifically, dicarboxylic acids give aqueous dianhydride macrocycles on treatment with a carbodiimide. The macrocycle is assembled efficiently as a consequence of both fuel-dependent and -independent mechanisms: it undergoes slower decomposition, building up as the fuel recycles the components, and is a favored product of the dynamic exchange of the anhydride bonds. These results create new possibilities for generating structurally sophisticated out-of-equilibrium species.

scholarly journals Structure of mouse Mx1 protein. Molecular assembly and GTP-dependent conformational change

1993 ◽  
Vol 268 (20) ◽  
pp. 15033-15038
Author(s):  
M. Nakayama ◽  
K. Yazaki ◽  
A. Kusano ◽  
K. Nagata ◽  
N. Hanai ◽  
...  
Keyword(s):  
Conformational Change ◽  
Molecular Assembly

scholarly journals Identifying molecules as biosignatures with assembly theory and mass spectrometry

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Stuart M. Marshall ◽  
Cole Mathis ◽  
Emma Carrick ◽  
Graham Keenan ◽  
Geoffrey J. T. Cooper ◽  
...  
Keyword(s):  
Mass Spectrometry ◽  
De Novo ◽  
Outer Space ◽  
Molecular Assembly ◽  
Detection Experiment ◽  
Complex Molecules ◽  
The World ◽  
Life Detection ◽  
Molecular Complexity ◽  
The Universe

AbstractThe search for alien life is hard because we do not know what signatures are unique to life. We show why complex molecules found in high abundance are universal biosignatures and demonstrate the first intrinsic experimentally tractable measure of molecular complexity, called the molecular assembly index (MA). To do this we calculate the complexity of several million molecules and validate that their complexity can be experimentally determined by mass spectrometry. This approach allows us to identify molecular biosignatures from a set of diverse samples from around the world, outer space, and the laboratory, demonstrating it is possible to build a life detection experiment based on MA that could be deployed to extraterrestrial locations, and used as a complexity scale to quantify constraints needed to direct prebiotically plausible processes in the laboratory. Such an approach is vital for finding life elsewhere in the universe or creating de-novo life in the lab.

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