Water structure at solid surfaces and its implications for biomolecule adsorption

Jena, Kailash C.; Hore, Dennis K.

doi:10.1039/c0cp00260g

Cited by 65 publications

(73 citation statements)

References 176 publications

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“…71 The interfacial water structure plays a major role in dictating the orientation and conformation of the adsorbed peptides and has been reported by previous simulation results. [72][73][74][75] In this sense, the interfacial water structure may also serve as a sensitive probe of adsorption events and adsorbed structure.…”

Section: Interfacial Water Behaviorsmentioning

confidence: 88%

Lipase adsorption on different nanomaterials: a multi-scale simulation study

Zhao

Chen

Jian

2015

Phys. Chem. Chem. Phys.

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Candida antarctica lipase B (CalB) is an efficient biocatalyst for hydrolysis and esterification, which plays an important role in the production of biodiesel in the bioenergy industries. The ordered immobilisation of lipases on different supports would be significant for its enzymatic catalysis in some biodiesel production processes; however, the underlying mechanisms and the preferred lipase orientation are not well understood yet. In this work, a fundamental understanding of the orientation and adsorption mechanism of lipase on four different nanomaterial surfaces with different surface chemistry are explored in detail by a combination of parallel tempering Monte Carlo (PTMC) and molecular dynamics (MD) simulations. Simulation results show that lipase is strongly adsorbed onto the hydrophobic graphite surface, as reflected by the large contact area and interaction energy; while the adsorption onto the hydrophilic TiO2 surface is weak due to two strongly adhered water layers; meanwhile lipase undergoes desorption and reorientation processes. For CalB adsorption on positively and negatively charged surfaces (NH2-SAM and COOH-SAM), the orientation distributions of lipase are narrow, and opposite orientations are obtained. CalB adsorbed on NH2-SAM has its catalytic centre oriented towards the surface, which is not conducive to the substrate binding; while the catalytic centre faces toward the solution when it is adsorbed on the COOH-SAM. Besides, the native structures of CalB adsorbed on different surfaces are preserved, which indicates lipase as a robust enzyme. The simulation results will promote our understanding on how surface properties of nanomaterials, such as charge or hydrophobicity, will affect lipase immobilisation, and help us in the rational design and development of immobilised lipase carriers.

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Section: Interfacial Water Behaviorsmentioning

confidence: 88%

Lipase adsorption on different nanomaterials: a multi-scale simulation study

Zhao

Chen

Jian

2015

Phys. Chem. Chem. Phys.

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“…The possible HA surface influence on the structure of the first shells of liquid water in physiological fluids [32,55,56], was witnessed by the influence of the HA surface electric field extended up to the multi-layers of physisorbed water. In fact, the presence at the HA/water interface of several strongly ordered hydration layers, originated from a network of strong electrostatic/hydrogen bonds, was revealed by means of molecular dynamics simulation [33].…”

Section: Discussionmentioning

confidence: 99%

“…As a consequence, from the present data, it was not possible to infer whether the multi-layer arrangement of physisorbed water is less dense at the HA/573 interface than at the HA/303 interface. As a matter of fact, in order to describe from a structural point of view the features of physisorbed water at the HA surface (both as-such and thermally activated at T = 573 K), a molecular dynamic approach should be employed [32,33].…”

Section: (A) Chemical Textural and Morphological Features Of The Invmentioning

confidence: 99%

“…In fact, water is ubiquitous in all body fluids and H 2 O molecules are expected to play a major role in the complex interplay of water-biopolymer and surface-biopolymer interactions [17,18]. The more or less ordered arrangement of H 2 O molecules at the solid biomaterial surface, which is a consequence of H bonding, electrostatic and dipolar interactions induced by the specific distribution of surface sites, is also expected to play a role in the processes occurring at the biomaterials/body fluids interface [32,33].…”

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confidence: 99%

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Coordination chemistry of Ca sites at the surface of nanosized hydroxyapatite: interaction with H₂O and CO

Bolis

Busco

Martra

et al. 2012

Phil. Trans. R. Soc. A.

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The affinity towards water of a selection of well-defined, nanostructured hydroxyapatite (HA) samples was investigated by H 2 O vapour adsorption microcalorimetry and infrared (IR) spectroscopy. A large hydrophilicity of all investigated materials was confirmed. The surface features of hydrated HA were investigated on the as-synthesized samples pre-treated in mild conditions at T = 303 K, whereas dehydrated HA features were characterized on samples activated at T = 573 K. The relatively large hydrophilicity of the hydrated surface (−D ads H ∼ 100-50 kJ mol −1 ) was due to the interaction of water with the highly polarized H 2 O molecules strongly coordinated to the surface Ca 2+ cations. At the dehydrated surface, exposing coordinatively unsaturated (cus) Ca 2+ cations, H 2 O was still molecularly adsorbed but more strongly (−D ads H ∼ 120-90 kJ mol −1 ). The use of CO adsorption to quantify the Lewis acidic strength of HA surface sites revealed only a moderate strength of cus Ca 2+ cations, as confirmed by both microcalorimetric and IR spectroscopic measurements and ab initio calculations. This result implies that the large HA/H 2 O interaction energy is due to the interplay between cus Ca 2+ sites and nearby hydrophilic PO 4 groups, not revealed by the CO probe. The lower density of cus Ca 2+ cations at the 573 K activated HA surface with respect to the *

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“…That is, if a polymer is not ordered in a polar manner (i. e., no DC fields have been applied), then no polymer response is observed except from chemical moieties at the surface (10,11). χ (2) spectroscopies such as electronic second-harmonic generation (12)(13)(14)(15)(16)(17), vibrational sum-frequency generation (SFG) (18)(19)(20)(21)(22)(23)(24)(25), or difference-frequency generation (DFG) (26,27) are therefore ideally suited to probing the interfacial structure of the polymer-water interface, including details of the polymer chains as well as the organization of the water molecules immediately adjacent to the surface. However, if the surface is dried following adsorption from solution (Figure 1d), or if the solution is rinsed away and replaced with water (Figure 1e), infrared absorption and Raman scattering may also be used.…”

Section: Introductionmentioning

confidence: 99%

IR Absorption, Raman Scattering, and IR-Vis Sum-Frequency Generation Spectroscopy as Quantitative Probes of Surface Structure

Hung

Stege

Hore

2014

Applied Spectroscopy Reviews

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Vibrational spectroscopy is a valuable quantitative tool for the determination of structure at surfaces. Various techniques may be applicable and useful, depending on what is available, the transparency of the substrates, the need for in situ probes, and the degree of interfacial specificity required. We examine and compare signals in infrared absorption, Raman scattering, and vibrational sum-frequency generation spectroscopy to the underlying molecular response. In all of these experiments, varying the beam polarizations enables the orientation of specific chemical functional groups to be determined. However, the sensitivity of each technique is directly connected to the manner in which the molecular response manifests itself in the measured signal. Starting with simple distributions of a single vibrational mode, leading up to multiple vibrational bands in more complex orientation distributions, we compare these three techniques in terms of their sensitivity to features of the molecular orientation distribution. This review is aimed at guiding planned experiments when multiple techniques are available for surface structural analysis.

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Water structure at solid surfaces and its implications for biomolecule adsorption

Cited by 65 publications

References 176 publications

Lipase adsorption on different nanomaterials: a multi-scale simulation study

Lipase adsorption on different nanomaterials: a multi-scale simulation study

Coordination chemistry of Ca sites at the surface of nanosized hydroxyapatite: interaction with H₂O and CO

IR Absorption, Raman Scattering, and IR-Vis Sum-Frequency Generation Spectroscopy as Quantitative Probes of Surface Structure

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Water structure at solid surfaces and its implications for biomolecule adsorption

Cited by 65 publications

References 176 publications

Lipase adsorption on different nanomaterials: a multi-scale simulation study

Lipase adsorption on different nanomaterials: a multi-scale simulation study

Coordination chemistry of Ca sites at the surface of nanosized hydroxyapatite: interaction with H2O and CO

IR Absorption, Raman Scattering, and IR-Vis Sum-Frequency Generation Spectroscopy as Quantitative Probes of Surface Structure

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Coordination chemistry of Ca sites at the surface of nanosized hydroxyapatite: interaction with H₂O and CO