RESUMEN
Silver gallium sulfide nanocrystals were synthesized and characterized by fluorescence, TEM, EDS, and XRD to better understand the material system with an ideal band gap of 2.7 eV. The crystals were found to nucleate in the monoclinic structure, and develop two fluorescence peaks (650, 460 nm) influenced by stoichiometry.
RESUMEN
Enzymes are able to maintain remarkably high selectivity toward their substrates while still retaining high catalytic rates. By immobilizing enzymes onto surfaces we can heterogenize these biological catalysts, making it practical to study, use, and combine them in an easily controlled system. In this work, we developed a platform that allows for the simple and oriented immobilization of proteins through DNA-directed immobilization. First, we modified a glass surface with single-stranded DNA. We then site-selectively attached the complementary DNA strand to the N-terminus of a protein. Both DNA modifications were carried out using an oxidative coupling strategy, and the DNA strands served as easily tunable and reversible chemical handles to hybridize the protein-DNA conjugates onto the surface. We have used the aldolase enzyme as a model protein to conduct our studies. We characterized each step of the protein immobilization process using fluorescent reporters as well as atomic force microscopy. We also conducted activity assays on the surfaces with DNA-linked aldolase to validate that, despite being modified with DNA and undergoing subsequent immobilization, the enzyme was still able to retain its catalytic activity and the surfaces were reusable in subsequent cycles.
Asunto(s)
ADN/metabolismo , Enzimas Inmovilizadas/metabolismo , Fructosa-Bifosfato Aldolasa/metabolismo , Ácidos Nucleicos Inmovilizados/metabolismo , ADN/química , Enzimas Inmovilizadas/química , Fructosa-Bifosfato Aldolasa/química , Vidrio/química , Ácidos Nucleicos Inmovilizados/química , Microscopía de Fuerza Atómica , Modelos Moleculares , Estructura Molecular , Oxidación-Reducción , Propiedades de SuperficieRESUMEN
Colloidal chemistry is used to control the size, shape, morphology, and composition of metal nanoparticles. Model catalysts as such are applied to catalytic transformations in the three types of catalysts: heterogeneous, homogeneous, and enzymatic. Real-time dynamics of oxidation state, coordination, and bonding of nanoparticle catalysts are put under the microscope using surface techniques such as sum-frequency generation vibrational spectroscopy and ambient pressure X-ray photoelectron spectroscopy under catalytically relevant conditions. It was demonstrated that catalytic behavior and trends are strongly tied to oxidation state, the coordination number and crystallographic orientation of metal sites, and bonding and orientation of surface adsorbates. It was also found that catalytic performance can be tuned by carefully designing and fabricating catalysts from the bottom up. Homogeneous and heterogeneous catalysts, and likely enzymes, behave similarly at the molecular level. Unifying the fields of catalysis is the key to achieving the goal of 100% selectivity in catalysis.