Search results for: Wendy J. Shaw

Items from 1 to 20 out of 47 results

article

High‐yield recombinant bacterial expression of ¹³C‐, ¹⁵N‐labeled, serine‐16 phosphorylated, murine amelogenin using a modified third generation genetic code expansion protocol

Garry W. Buchko, Mowei Zhou, Cat Hoang Vesely, Jinhui Tao, more

Amelogenin constitutes ~90% of the enamel matrix in the secretory stage of amelogenesis, a still poorly understood process that results in the formation of the hardest and most mineralized tissue in vertebrates—enamel. Most biophysical research with amelogenin uses recombinant protein expressed in Escherichia coli. In addition to providing copious amounts of protein, recombinant expression allows...

article

Identification of major matrix metalloproteinase-20 proteolytic processing products of murine amelogenin and tyrosine-rich amelogenin peptide using a nuclear magnetic resonance spectroscopy based method

Garry W. Buchko, Rajith Jayasinha Arachchige, Jinhui Tao, Barbara J. Tarasevich, more

Archives of Oral Biology > 2018 > 93 > C > 187-194

The aim of this study was to identify major matrix metalloproteinase-20 (MMP20) proteolytic processing products of amelogenin over time and determine if the tyrosine-rich amelogenin peptide (TRAP) was a substrate of MMP20.Recombinant ¹⁵ N-labeled murine amelogenin and ¹³ C, ¹⁵ N-labeled TRAP were incubated with MMP20 under conditions where amelogenin self-assembles into nanospheres. Digestion products...

article

Secondary structure and dynamics study of the intrinsically disordered silica‐mineralizing peptide P₅S₃ during silicic acid condensation and silica decondensation

Christian Zerfaß, Garry W. Buchko, Wendy J. Shaw, Stephan Hobe, more

Proteins: Structure, Function, and Bioinformatics > 85 > 11 > 2111 - 2126

The silica forming repeat R5 of sil1 from Cylindrotheca fusiformis was the blueprint for the design of P₅S₃, a 50‐residue peptide which can be produced in large amounts by recombinant bacterial expression. It contains 5 protein kinase A target sites and is highly cationic due to 10 lysine and 10 arginine residues. In the presence of supersaturated orthosilicic acid P₅S₃ enhances silica‐formation whereas...

article

Carbon‐Nanotube‐Supported Bio‐Inspired Nickel Catalyst and Its Integration in Hybrid Hydrogen/Air Fuel Cells

Solène Gentil, Noémie Lalaoui, Arnab Dutta, Yannig Nedellec, more

Angewandte Chemie International Edition > 56 > 7 > 1845 - 1849

A biomimetic nickel bis‐diphosphine complex incorporating the amino acid arginine in the outer coordination sphere was immobilized on modified carbon nanotubes (CNTs) through electrostatic interactions. The functionalized redox nanomaterial exhibits reversible electrocatalytic activity for the H₂/2 H⁺ interconversion from pH 0 to 9, with catalytic preference for H₂ oxidation at all pH values. The...

article

Carbon‐Nanotube‐Supported Bio‐Inspired Nickel Catalyst and Its Integration in Hybrid Hydrogen/Air Fuel Cells

Solène Gentil, Noémie Lalaoui, Arnab Dutta, Yannig Nedellec, more

Angewandte Chemie > 129 > 7 > 1871 - 1875

article

Covalent Attachment of the Water‐insoluble Ni(P^Cy₂N^Phe₂)₂ Electrocatalyst to Electrodes Showing Reversible Catalysis in Aqueous Solution

Patricia Rodríguez‐Maciá, Nilusha Priyadarshani, Arnab Dutta, Claudia Weidenthaler, more

Electroanalysis > 28 > 10 > 2452 - 2458

Hydrogenases are a diverse group of metalloenzymes which catalyze the reversible conversion between molecular hydrogen and protons at high rates. The catalytic activity of these enzymes does not require overpotential because their active site has been evolutionarily optimized to operate fast and efficiently. These enzymes have inspired the development of molecular catalysts, which have dramatically...

article

The Role of Solvent and the Outer Coordination Sphere on H₂ Oxidation Using [Ni(P^Cy₂N^Pyz₂)₂]²⁺

Arnab Dutta, Sheri Lense, John A. S. Roberts, Monte L. Helm, more

European Journal of Inorganic Chemistry > 2015 > 31 > 5218 - 5225

Hydrogenase enzymes are reversible catalysts for H₂ production/oxidation, operating with fast rates and minimal overpotentials in water. Many synthetic catalyst mimics of hydrogenase operate in organic solvents. However, recent work has demonstrated the importance of water in the performance of some model complexes. In this work, the H₂ oxidation activity of [Ni(P^Cy₂N^{(3–pyridazyl)methyl}₂)₂]²⁺ (CyPyz)...

article

Direkter Leistungsvergleich eines bioinspirierten synthetischen Ni‐Katalysators und einer [NiFe]‐Hydrogenase, beide kovalent an eine Elektrode gebunden

Patricia Rodriguez‐Maciá, Arnab Dutta, Wolfgang Lubitz, Wendy J. Shaw, more

Angewandte Chemie > 127 > 42 > 12478 - 12482

Das aktive Zentrum von Hydrogenasen inspiriert die Entwicklung molekularer Katalysatoren zur Wasserstoffumsetzung. Ein direkter Vergleich zwischen diesen Katalysatoren und dem Enzym war jedoch bisher nicht möglich, weil verschiedene Techniken zur Bewertung der Katalysatoreigenschaften verwendet wurden. Dies macht es schwierig zu beurteilen, inwieweit die synthetisierten Katalysatoren in ihrer Leistung...

article

Direct Comparison of the Performance of a Bio‐inspired Synthetic Nickel Catalyst and a [NiFe]‐Hydrogenase, Both Covalently Attached to Electrodes

Patricia Rodriguez‐Maciá, Arnab Dutta, Wolfgang Lubitz, Wendy J. Shaw, more

Angewandte Chemie International Edition > 54 > 42 > 12303 - 12307

The active site of hydrogenases has been a source of inspiration for the development of molecular catalysts. However, direct comparisons between molecular catalysts and enzymes have not been possible because different techniques are used to evaluate both types of catalysts, minimizing our ability to determine how far we have come in mimicking the enzymatic performance. The catalytic properties of...

article

Solid-state NMR studies of proteins immobilized on inorganic surfaces

Wendy J. Shaw

Solid State Nuclear Magnetic Resonance > 2015 > 70 > C > 1-14

Solid state NMR is the primary tool for studying the quantitative, site-specific structure, orientation, and dynamics of biomineralization proteins under biologically relevant conditions. Two calcium phosphate proteins, statherin (43 amino acids) and leucine rich amelogenin protein (LRAP; 59 amino acids), have been studied in depth and have different dynamic properties and 2D- and 3D-structural features...

article

The leucine-rich amelogenin protein (LRAP) is primarily monomeric and unstructured in physiological solution

Barbara J. Tarasevich, John S. Philo, Nasib Karl Maluf, Susan Krueger, more

Journal of Structural Biology > 2015 > 190 > 1 > 81-91

Amelogenin proteins are critical to the formation of enamel in teeth and may have roles in controlling growth and regulating microstructures of the intricately woven hydroxyapatite (HAP). Leucine-rich amelogenin protein (LRAP) is a 59-residue splice variant of amelogenin and contains the N- and C-terminal charged regions of the full-length protein thought to control crystal growth. Although the quaternary...

article

Improved protocol to purify untagged amelogenin – Application to murine amelogenin containing the equivalent P70→T point mutation observed in human amelogenesis imperfecta

Garry W. Buchko, Wendy J. Shaw

Protein Expression and Purification > 2015 > 105 > Complete > 14-22

Amelogenin is the predominant extracellular protein responsible for converting carbonated hydroxyapatite into dental enamel, the hardest and most heavily mineralized tissue in vertebrates. Despite much effort, the precise mechanism by which amelogenin regulates enamel formation is not fully understood. To assist efforts aimed at understanding the biochemical mechanism of enamel formation, more facile...

article

Arginine‐Containing Ligands Enhance H₂ Oxidation Catalyst Performance

Arnab Dutta, John A. S. Roberts, Wendy J. Shaw

Angewandte Chemie International Edition > 53 > 25 > 6487 - 6491

Hydrogenase enzymes use Ni and Fe to oxidize H₂ at high turnover frequencies (TOF) (up to 10 000 s⁻¹) and low overpotentials (<100 mV). In comparison, the fastest reported synthetic electrocatalyst, [Ni^II(P^Cy₂N^tBu₂)₂]²⁺, oxidizes H₂ at 60 s⁻¹ in MeCN under 1 atm H₂ with an unoptimized overpotential of ca. 500 mV using triethylamine as a base.1 Here we show that a structured outer coordination sphere...

article

Arginine‐Containing Ligands Enhance H₂ Oxidation Catalyst Performance

Arnab Dutta, John A. S. Roberts, Wendy J. Shaw

Angewandte Chemie > 126 > 25 > 6605 - 6609

article

Enzyme Design from the Bottom Up: An Active Nickel Electrocatalyst with a Structured Peptide Outer Coordination Sphere

Matthew L. Reback, Garry W. Buchko, Brandon L. Kier, Bojana Ginovska‐Pangovska, more

Chemistry – A European Journal > 20 > 6 > 1510 - 1514

Catalytic, peptide‐containing metal complexes with a well‐defined peptide structure have the potential to enhance molecular catalysts through an enzyme‐like outer coordination sphere. Here, we report the synthesis and characterization of an active, peptide‐based metal complex built upon the well‐characterized hydrogen production catalyst [Ni(P^Ph₂N^Ph)₂]²⁺ (P^Ph₂N^Ph=1,3,6‐triphenyl‐1‐aza‐3,6‐diphosphacycloheptane)...

article

Molecular dynamics study of the proposed proton transport pathways in [FeFe]-hydrogenase

Bojana Ginovska-Pangovska, Ming-Hsun Ho, John C. Linehan, Yuhui Cheng, more

Biochimica et Biophysica Acta (BBA) - Bioenergetics > 2014 > 1837 > 1 > 131-138

Possible proton transport pathways in Clostridium pasteurianum (CpI) [FeFe]-hydrogenase were investigated with molecular dynamics simulations. This study was undertaken to evaluate the functional pathway and provide insight into the hydrogen bonding features defining an active proton transport pathway. Three pathways were evaluated, two of which consist of water wires and one of predominantly amino...

article

Electrocatalytic Oxidation of Formate with Nickel Diphosphine Dipeptide Complexes: Effect of Ligands Modified with Amino Acids

Brandon R. Galan, Matthew L. Reback, Avijita Jain, Aaron M. Appel, more

European Journal of Inorganic Chemistry > 2013 > 30 > 5366 - 5371

A series of nickel bis(diphosphine) complexes with dipeptides appended to the ligands were investigated for the catalytic oxidation of formate to carbon dioxide, a proton, and two electrons. Typical rates of approximately 7 s^–1 were found, similar to that for the parent complex (ca. 8 s^–1), with amino acid size and positioning contributing very little to the rate or operating potential. Hydroxy functionalities...

article

A solution NMR investigation into the impaired self-assembly properties of two murine amelogenins containing the point mutations T21→I or P41→T

Garry W. Buchko, Genyao Lin, Barbara J. Tarasevich, Wendy J. Shaw

Archives of Biochemistry and Biophysics > 2013 > 537 > 2 > 217-224

Amelogenesis imperfecta describes a group of inherited disorders that results in defective tooth enamel. Two disorders associated with human amelogenesis imperfecta are the point mutations T21→I or P40→T in amelogenin, the dominant protein present during the early stages of enamel biomineralization. The biophysical properties of wildtype murine amelogenin (M180) and two proteins containing the equivalent...

article

A modular, energy-based approach to the development of nickel containing molecular electrocatalysts for hydrogen production and oxidation

Wendy J. Shaw, Monte L. Helm, Daniel L. DuBois

BBA - Bioenergetics > 2013 > 1827 > 8-9 > 1123-1139

This review discusses the development of molecular electrocatalysts for H ₂ production and oxidation based on nickel. A modular approach is used in which the structure of the catalyst is divided into first, second, and outer coordination spheres. The first coordination sphere consists of the ligands bound directly to the metal center, and this coordination sphere can be used to control such...

article

The Role of a Dipeptide Outer‐Coordination Sphere on H₂‐Production Catalysts: Influence on Catalytic Rates and Electron Transfer

Matthew L. Reback, Bojana Ginovska‐Pangovska, Ming‐Hsun Ho, Avijita Jain, more

Chemistry – A European Journal > 19 > 6 > 1928 - 1941

The outer‐coordination sphere of enzymes acts to fine‐tune the active site reactivity and control catalytic rates, suggesting that incorporation of analogous structural elements into molecular catalysts may be necessary to achieve rates comparable to those observed in enzyme systems at low overpotentials. In this work, we evaluate the effect of an amino acid and dipeptide outer‐coordination sphere...

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BIOMINERALIZATION (9)
AMELOGENIN (7)
ENAMEL (5)
HOMOGENEOUS CATALYSIS (4)
OUTER COORDINATION SPHERE (4)
AMELOGENESIS (3)
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Search results for: Wendy J. Shaw

High‐yield recombinant bacterial expression of ¹³C‐, ¹⁵N‐labeled, serine‐16 phosphorylated, murine amelogenin using a modified third generation genetic code expansion protocol

Identification of major matrix metalloproteinase-20 proteolytic processing products of murine amelogenin and tyrosine-rich amelogenin peptide using a nuclear magnetic resonance spectroscopy based method

Secondary structure and dynamics study of the intrinsically disordered silica‐mineralizing peptide P₅S₃ during silicic acid condensation and silica decondensation

Carbon‐Nanotube‐Supported Bio‐Inspired Nickel Catalyst and Its Integration in Hybrid Hydrogen/Air Fuel Cells

Carbon‐Nanotube‐Supported Bio‐Inspired Nickel Catalyst and Its Integration in Hybrid Hydrogen/Air Fuel Cells

Covalent Attachment of the Water‐insoluble Ni(P^Cy₂N^Phe₂)₂ Electrocatalyst to Electrodes Showing Reversible Catalysis in Aqueous Solution

The Role of Solvent and the Outer Coordination Sphere on H₂ Oxidation Using [Ni(P^Cy₂N^Pyz₂)₂]²⁺

Direkter Leistungsvergleich eines bioinspirierten synthetischen Ni‐Katalysators und einer [NiFe]‐Hydrogenase, beide kovalent an eine Elektrode gebunden

Direct Comparison of the Performance of a Bio‐inspired Synthetic Nickel Catalyst and a [NiFe]‐Hydrogenase, Both Covalently Attached to Electrodes

Solid-state NMR studies of proteins immobilized on inorganic surfaces

The leucine-rich amelogenin protein (LRAP) is primarily monomeric and unstructured in physiological solution

Improved protocol to purify untagged amelogenin – Application to murine amelogenin containing the equivalent P70→T point mutation observed in human amelogenesis imperfecta

Arginine‐Containing Ligands Enhance H₂ Oxidation Catalyst Performance

Arginine‐Containing Ligands Enhance H₂ Oxidation Catalyst Performance

Enzyme Design from the Bottom Up: An Active Nickel Electrocatalyst with a Structured Peptide Outer Coordination Sphere

Molecular dynamics study of the proposed proton transport pathways in [FeFe]-hydrogenase

Electrocatalytic Oxidation of Formate with Nickel Diphosphine Dipeptide Complexes: Effect of Ligands Modified with Amino Acids

A solution NMR investigation into the impaired self-assembly properties of two murine amelogenins containing the point mutations T21→I or P41→T

A modular, energy-based approach to the development of nickel containing molecular electrocatalysts for hydrogen production and oxidation

The Role of a Dipeptide Outer‐Coordination Sphere on H₂‐Production Catalysts: Influence on Catalytic Rates and Electron Transfer

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