Direct Observation of Phenylalanine Orientations in Statherin Bound to Hydroxyapatite Surfaces

Weidner, Tobias; Dubey, Manish; Breen, Nicholas F.; Ash, Jason T.; Baio, Joe E.; Jaye, Cherno; Fischer, Daniel A.; Drobny, Gary P.; Castner, David G.

doi:10.1021/ja301711w

Cited by 38 publications

(53 citation statements)

References 62 publications

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“…33 However, because the nanocrystalline TiO 2 plate used in this study exhibits morphological features about 20 nm in size, 34 it is not easy to extract the orientation information directly. We therefore estimate the proportion of NCS groups in BD that interact with nanocrystalline TiO 2 based on the information from the N719 dye.…”

Section: Resultsmentioning

confidence: 99%

Investigation of the influence of coadsorbent dye upon the interfacial structure of dye-sensitized solar cells

Honda

Yanagida

et al. 2014

The Journal of Chemical Physics

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The interface between Ru(tcterpy)(NCS)3TBA2 [black dye (BD); tcterpy = 4,4′,4″-tricarboxy-2,2′:6′,2″-terpyridine, NCS = thiocyanato, TBA = tetrabutylammonium cation] and nanocrystalline TiO2, as found in dye-sensitized solar cells, is investigated by soft-X-ray synchrotron radiation and compared with the adsorption structure of cis-Ru(Hdcbpy)2(NCS)2TBA2 (N719; dcbpy = 4,4′-dicarboxy-2,2′-bipyridine) on TiO2 to elucidate the relationship between the adsorption mode of BD and the photocurrent with and without coadsorbed indoline dye D131. The depth profile is characterized with X-ray photoelectron spectroscopy and S K-edge X-ray absorption fine structure using synchrotron radiation. Both datasets indicate that one of the isothiocyanate groups of BD interacts with TiO2 via its S atom when the dye is adsorbed from a single-component solution. In contrast, the interaction is slightly suppressed when D131 is coadsorbed, indicated by the fact that the presence of D131 changes the adsorption mode of BD. Based upon these results, the number of BD dye molecules interacting with the substrate is shown to decrease by 10% when D131 is coadsorbed, and the dissociation is shown to be related to the short-circuit photocurrent in the 600–800 nm region. The design of a procedure to promote the preferential adsorption of D131 therefore leads to an improvement of the short-circuit current and conversion efficiency.

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Section: Resultsmentioning

confidence: 99%

Investigation of the influence of coadsorbent dye upon the interfacial structure of dye-sensitized solar cells

Honda

Yanagida

et al. 2014

The Journal of Chemical Physics

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“…This side chain of F14 was also found to be only ~4 Å from the surface, consistent with an interaction between the ring and the surface. In nicely complementary studies, Near Edge X-ray Absorption Fine Structure (NEXAFS) spectroscopy and sum frequency generation (SFG) provide data consistent with this interpretation [38]. The results from the study of F14 suggest that while the interaction in this region of the protein is weaker, there is still a preference, possibly entropic, for the protein to be associated with the surface.…”

Section: Studies With Hydroxyapatitementioning

confidence: 92%

“…The distance of a number of the side chain residues from HAP were studied for statherin, including phenyalanines [37,38], lysines [39], arginines [40], and glutamic acids [41]. The results from these studies begin to provide a three-dimensional view of the protein–surface complex by revealing not only distances of the side chains of these residues from the surface, but also modifications in dynamics.…”

Section: Studies With Hydroxyapatitementioning

confidence: 99%

Solid-state NMR studies of proteins immobilized on inorganic surfaces

Shaw

2015

Solid State Nuclear Magnetic Resonance

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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. These differences make it difficult to extract design principles used in nature for building materials with properties such as high strength, unusual morphologies, or uncommon phases. Consequently, design principles needed for developing synthetic materials controlled by proteins are not clear. Many biomineralization proteins are much larger than statherin and LRAP, necessitating the study of larger biomineralization proteins. More recent studies of the significantly larger full-length amelogenin (180 residues) represent a significant step forward to ultimately investigate the full diversity of biomineralization proteins. Interactions of amino acids, a silaffin derived peptide, and the model LK peptide with silica are also being studied, along with qualitative studies of the organic matrices interacting with calcium carbonate. Dipolar recoupling techniques have formed the core of the quantitative studies, yet the need for isolated spin pairs makes this approach costly and time intensive. The use of multidimensional techniques to study biomineralization proteins is becoming more common, methodology which, despite its challenges with these difficult-to-study proteins, will continue to drive future advancements in this area.

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“…Based on earlier studies showing that SFG has the capability to detect individual deuterated residues within larger proteins, we have used isotope labels to probe the orientations of individual side chains in peptides and proteins 34, 51, 54, 55, 60 . Deuterium substitution into the C–H groups leads to a red shift of ∼800 cm -1 for the C–H resonances.…”

Section: Sum Frequency Generation Spectroscopy For Protein Studiesmentioning

confidence: 99%

SFG analysis of surface bound proteins: a route towards structure determination

Weidner

Castner

2013

Phys. Chem. Chem. Phys.

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The surface of a material is rapidly covered with proteins once that material is placed in a biological environment. The structure and function of these bound proteins play a key role in the interactions and communications of the material with the biological environment. Thus, it is crucial to gain a molecular level understanding of surface bound protein structure. While X-ray diffraction and solution phase NMR methods are well established for determining the structure of proteins in the crystalline or solution phase, there is not a corresponding single technique that can provide the same level of structural detail about proteins at surfaces or interfaces. However, recent advances in sum frequency generation (SFG) vibrational spectroscopy have significantly increased our ability to obtain structural information about surface bound proteins and peptides. A multi-technique approach of combining SFG with (1) protein engineering methods to selectively introduce mutations and isotopic labels, (2) other experimental methods such as time-of-flight secondary ion mass spectrometry (ToF-SIMS) and near edge x-ray absorption fine structure (NEXAFS) to provide complementary information, and (3) molecular dynamic (MD) simulations to extend the molecular level experimental results is a particularly promising route for structural characterization of surface bound proteins and peptides. By using model peptides and small proteins with well-defined structures, methods have been developed to determine the orientation of both backbone and side chains to the surface.

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Direct Observation of Phenylalanine Orientations in Statherin Bound to Hydroxyapatite Surfaces

Cited by 38 publications

References 62 publications

Investigation of the influence of coadsorbent dye upon the interfacial structure of dye-sensitized solar cells

Investigation of the influence of coadsorbent dye upon the interfacial structure of dye-sensitized solar cells

Solid-state NMR studies of proteins immobilized on inorganic surfaces

SFG analysis of surface bound proteins: a route towards structure determination

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