The hydrogenation of $AlB_2$-type BaGaGe exhibits a metal to insulator (MI) transition, inducing a puckering distortion of the original hexagonal [GaGe] layers. We investigate the electronic structure changes associated with the hydrogen-induced MI transition, using extended H$\ddot{u}$ckel tight-binding band calculations. The results indicate that hydrogen incorporation in the precursor BaGaGe is characterized by an antibonding interaction of $\pi$ on GaGe with hydrogen 1s and the second-order mixing of the singly occupied antibonding $\pi^*$ orbital into it, through Ga-H bond formation. As a result, the fully occupied bonding $\pi$ band in BaGaGe changes to a weakly dispersive band with Ge pz (lone pair) character in the hydride, which becomes located just below the Fermi level. The Ga-Ge bonds within a layered polyanion are slightly weakened by hydrogen incorporation. A rationale for this is given.
Molecular orbital calculations at the extended Huckel level have been carried out for $Cp_2TiSiHPh(1),\;[Cp_2Ti]_2[{\mu}-HSi(HPh)][{\mu}-H] (2),\;and\;[Cp_2TiSiH_2Ph]_2$ (3) complexes which are important intermediates in organosilane polymerization. Stable geometry of complex 1 is not $C_{2V}$, but Cs symmetry and the rotational energy barrier of $SiH_2$ unit is computed to be 14 kcal/mol. The orbital interaction diagrams are studied to characterize the chemical bonding for the electron deficient systems, 2 and 3. It is possible for Si-H to be coordinated to the Ti metal using $\sigma$ bonding.
The 70 kDa heat-shock protein (Hsp70) involved in various cellular functions, such as protein folding, translocation and degradation, regulates apoptosis in cancer cells. Recently, it has been reported that the green tea flavonoid (−)-epigallocatechin 3-gallate (EGCG) induces apoptosis in numerous cancer cell lines and could inhibit the anti-apoptotic effect of human Hsp70 ATPase domain (hATPase). In the present study, docking model between EGCG and hATPase was determined using automated docking study. Epi-gallo moiety in EGCG participated in hydrogen bonds with side chain of K71 and T204, and has metal chelating interaction with hATPase. Hydroxyl group of catechin moiety also participated in metal chelating hydrogen bond. Gallate moiety had two hydrogen bondings with side chains of E268 and K271, and hydrophobic interaction with Y15. Based on this docking model, we determined two pharmacophore maps consisted of six or seven features, including three or four hydrogen bonding acceptors, two hydrogen bonding donors, and one lipophilic. We searched a flavonoid database including 23 naturally occurring flavonoids and 10 polyphenolic flavonoids with two maps, and myricetin and GC were hit by map I. Three hydroxyl groups of B-ring in myricetin and gallo moiety of GC formed important hydrogen bonds with hATPase. 7-OH of A-ring in myricetin and OH group of catechin moiety in GC are hydrogen bond donors similar to gallate moiety in EGCG. From these results, it can be proposed that myricetin and GC can be potent inhibitors of hATPase. This study will be helpful to understand the mechanism of inhibition of hATPase by EGCG and give insights to develop potent inhibitors of hATPase.
Proceedings of the Korean Society of Near Infrared Spectroscopy Conference
/
2001.06a
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pp.1181-1181
/
2001
Robinson with ${coworkers}^{1}$ have introduced two-state outer-neighbor bonding model to explain the anomalies of water. The studies on the properties of water as a function of temperature and pressure revealed that, unlike other ideas, all $H_2O$ molecules in liquid are tetrabonded. On the average they are forming two different bonding types. One type is the regular tetrahedral water-water bonding similar to that found in the ordinary ice Ih, whereas the other is a more dense nonregular tetrahedral bonding similar to that appearing in the ice II. The transformation between these two bonding forms is evidenced by FT-NIR experiment. The FT-NIR measurements were done for liquid water in the temperature range from $20^{\circ}C$ up to $80^{\circ}C$ in a wide extent of frequencies: 12 000 - 4000 $cm^{-1}$ /. Temperature dependent variations in the volume fraction of these two structures are directly related to the spectral changes. The absorbance variations are explored by means of the two-dimensional correlation spectroscopy (2DCOS), principal component analysis (PCA), curve fitting and second derivatives. The presence of the isosbestic points in a range of the combination and overtone transitions indicates that the experimental spectra are a superposition of two temperature independent components. One component of diminishing intensity with temperature increase, is assigned to a stronger hydrogen bonds occurred in the Ih type, whereas the second component showing an opposite behavior, one can attribute to a weaker H-bonds characteristic for the II type. The understanding of the hydrogen bonding network in the liquid water is very important in interpretation of the interaction between water and protein chain. The two-state model of water surrounding the protein surface could advance an understanding of the hydration process.
Isostric heats of adsorption of amines on paraffin and polyethyleneglycol were measured by gas chromatography. Value with polyethyleneglycol were significantly higher than those with paraffin due to the N-H...O bonding. The contribution of C-H...O bonding to the isosoteric heats of adsorption was negligible. The additional heats of adsorption observed as the sample size increased also increased as the number of amino hydrogen atoms decreased. This tendency was more significant with polyethyleneglycol indicating that strong directing force of amino hydrogen of primary and secondary amines to the surface hinder lateral attractive interaction which could be favored with free orientation.
Second-order rate constants ($k_N$) have been measured spectrophotometrically for the reactions of benzyl 2-pyridyl carbonate $\mathbf{3}$ and $t$-butyl 2-pyridyl carbonate $\mathbf{3}$ with a series of alicyclic secondary amines in MeCN at $25.0{\pm}0.1^{\circ}C$. Substrate $\mathbf{4}$ is much less reactive than $\mathbf{3}$ and the steric hindrance exerted by the bulky $t$-Bu group in $\mathbf{4}$ has been attributed to its decreased reactivity. The Br${\o}$nsted-type plots for the reactions of $\mathbf{3}$ and $\mathbf{4}$ are linear with ${\beta}_{nuc}=0.57$ and 0.45, respectively. Thus, the reactions have been concluded to proceed through a concerted mechanism, although the current reactions were expected to proceed through a stepwise mechanism with a zwitterionic tetrahedral intermediate $T^{\pm}$. It has been proposed that the rate of leaving-group expulsion is accelerated by the intramolecular H-bonding interaction in $T^{\pm}$ and the "push" provided by the RO group through the resonance interaction. Thus, the enhanced nucleofugality forces the reactions to proceed through a concerted mechanism. The reactivity-selectivity principle (RSP) is not applicable to the current reaction systems, since the reaction of the less reactive $\mathbf{4}$ results in a smaller ${\beta}_{nuc}$ than that of the more reactive $\mathbf{3}$. Steric hindrance exerted by the bulky $t$-Bu group in $\mathbf{4}$ has been suggested to be responsible for the failure of the RSP.
The antitumor antibiotic (+)-CC-1065 can alkylate N3 of guanine in certain sequences. A previous high-field $^1H$ NMR study on the$(+)-CC-1065d[GCGCAATTG*CGC]_2$ adduct ($^*$ indicates the drug alkylation site) showed that drag modification on N3 of guanine results in protonation of the cross-strand cytosine [Park, H-J.; Hurley, L. H. J. Am. Chem. Soc.1997, 119,629]. In this contribution we describe a further analysis of the NMR data sets together with restrained molecular dynamics. This study provides not only a solution structure of the (+)-CC-1065(N3- guanine) DNA duplex adduct but also new insight into the molecular basis for the sequence- specific interaction between (+)-CC-1065 and N3-guanine in the DNA duplex. On the basis of NOESY data, we propose that the narrow minor groove at the 7T8T step and conformational kinks at the junctions of 16C17A and 18A19T are both related to DNA bending in the drugDNA adduct. Analysis of the one-dimensional $^1H$ NMR (in $H_2O$) data and rMD trajectories strongly suggests that hydrogen bonding linkages between the 8-OH group of the (+)-CC-1065 A-sub-unit and the 9G10C phosphate via a water molecule are present. All the phenomena observed here in the (+)-CC-1065(N3-guanine) adduct at 5'$-AATTG^*$are reminiscent of those obtained from the studies on the (+)-CC-1065(N3-adenine) adduct at $5'-AGTTA^*$, suggesting that (+)-CC-1065 takes advantage of the conformational flexibility of the 5'-TPu step to entrap the bent structure required for the covalent bonding reaction. This study reveals a common molecular basis for (+)-CC-1065 alkylation at both $5'-TTG^*$ and $5'-TTA^*$, which involves a trapping out of sequence-dependent DNA conformational flexibility as well as sequence-dependent general acid and general base catalysis by duplex DNA.
Metal industry is one of the most representative heavy industries and the median sales volume of steel and nonferrous metal companies is over one billion dollars in the case America [Forbes 2006]. As seen in the recent business market situation, an increasing number of industrial manufacturers and suppliers are moving from adversarial to cooperative exchange attitudes that support the long-term relationships with their customers. This article presents the results of an empirical study of the antecedent factors of business relationships in metal industry of the United States. Commitment has been reviewed as a significant and critical variable in research on inter-organizational relationships (Hong et al. 2007, Kim et al. 2007). The future stability of any buyer-seller relationship depends upon the commitment made by the interactants to their relationship. Commitment, according to Dwyer et al. [1987], refers to "an implicit or explicit pledge of relational continuity between exchange partners" and they consider commitment to be the most advanced phase of buyer-seller exchange relationship. Bonds are made because the members need their partners in order to do something and this integration on a task basis can be either symbiotic or cooperative (Svensson 2008). To the extent that members seek the same or mutually supporting ends, there will be strong bonds among them. In other words, the principle that affects the strength of bonds is 'economy of decision making' [Turner 1970]. These bonds provide an important idea to study the causes of business long-term relationships in a sense that organizations can be mutually bonded by a common interest in the economic matters. Recently, the framework of structural bonding has been used to study the buyer-seller relationships in industrial marketing [Han and Sung 2008, Williams et al. 1998, Wilson 1995] in that this structural bonding is a crucial part of the theoretical justification for distinguishing discrete transactions from ongoing long-term relationships. The major antecedent factors of buyer commitment such as technology, CLalt, transaction-specific assets, and importance were identified and explored from the perspective of structural bonding. Research hypotheses were developed and tested by using survey data from the middle managers in the metal industry. H1: Level of technology of the relationship partner is positively related to the level of structural bonding between the buyer and the seller. H2: Comparison level of alternatives is negatively related to the level of structural bonding between the buyer and the seller. H3: Amount of the transaction-specific assets is positively related to the level of structural bonding between the buyer and the seller. H4: Importance of the relationship partner is positively related to the level of structural bonding between the buyer and the seller. H5: Level of structural bonding is positively related to the level of commitment to the relationship. To examine the major antecedent factors of industrial buyer's structural bonding and long-term relationship, questionnaire was prepared, mailed out to the sample of 400 purchasing managers of the US metal industry (SIC codes 33 and 34). After a follow-up request, 139 informants returnedthe questionnaires, resulting in a response rate of 35 percent. 134 responses were used in the final analysis after dropping 5 incomplete questionnaires. All measures were analyzed for reliability and validity following the guidelines offered by Churchill [1979] and Anderson and Gerbing [1988]., the results of fitting the model to the data indicated that the hypothesized model provides a good fit to the data. Goodness-of-fit index (GFI = 0.94) and other indices ( chi-square = 78.02 with p-value = 0.13, Adjusted GFI = 0.90, Normed Fit Index = 0.92) indicated that a major proportion of variances and covariances in the data was accounted for by the model as a whole, and all the parameter estimates showed statistical significance as evidenced by large t-values. All the factor loadings were significantly different from zero. On these grounds we judged the hypothesized model to be a reasonable representation of the data. The results from the present study suggest several implications for buyer-seller relationships. Theoretically, we attempted to conceptualize the antecedent factors of buyer-seller long-term relationships from the perspective of structural bondingin metal industry. The four underlying determinants (i.e. technology, CLalt, transaction-specific assets, and importance) of structural bonding are very critical variables of buyer-seller long-term business relationships. Our model of structural bonding makes an attempt to systematically examine the relationship between the antecedent factors of structural bonding and long-term commitment. Managerially, this research provides industrial purchasing managers with a good framework to assess the interaction processes with their partners and, ability to position their business relationships from the perspective of structural bonding. In other words, based on those underlying variables, industrial purchasing managers can determine the strength of the company's relationships with the key suppliers and its state of preparation to be a successful partner with those suppliers. Both the supplying and customer companies can also benefit by using the concept of 'structural bonding' and evaluating their relationships with key business partners from the structural point of view. In general, the results indicate that structural bonding gives a critical impact on the level of relationship commitment. Managerial implications and limitations of the study are also discussed.
Chiral recognition models for resolving π-basic N-acyl-α-(1-naphthyl)alkylamines and π-acidic N-(3,5-dinitrobenzoyl)-α-amino alkyl esters on a (S)-tyrosine-derived chiral stationary phase (CSP) containing both π-basic and π-acidic interaction site have been proposed. In the models, the CSP was supposed to interact with the analytes through the π-π interaction between the 3,5-dinitrophenyl or the 3,5-dimethylphenyl group of the CSP and the 1-naphthyl or the 3,5-dinitrophenyl group of the analyte, and through the hydrogen bonding interaction between the appropriate N-H hydrogen of the CSP and the appropriate carbonyl oxygen of the analyte. In this instance, the alkyl substituent of the pertinent enantiomer of the analyte was found to intercalate between the adjacent strands of the bonded phase and consequently control the trends of the separation factors.
Sato Harumi;Murakami Rumi;Zhang Jianming;Ozaki Yukihiro;Mori Katsuhito;Takahashi Isao;Terauchi Hikaru;Noda Isao
Macromolecular Research
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v.14
no.4
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pp.408-415
/
2006
Temperature-dependent, wide-angle, x-ray diffraction (WAXD) patterns and infrared (IR) spectra were measured for biodegradable poly(3-hydroxybutyrate) (PHB) and its copolymers, poly(3-hydroxybutyrate-co-3-hydroxyhexanoate) P(HB-co-HHx) (HHx=2.5, 3.4, 10.5, and 12 mol%), in order to explore their crystal and lamellar structure and their pattern of C-H...O=C hydrogen bonding. The WAXD patterns showed that the P(HB-co-HHx) copolymers have the same orthorhombic system as PHB. It was found from the temperature-dependent WAXD measurements of PHB and P(HB-co-HHx) that the a lattice parameter is more enlarged than the b lattice parameter during heating and that only the a lattice parameter shows reversibility during both heating and cooling processes. These observations suggest that an interaction occurs along the a axis in PHB and P(HB-co-HHx). This interaction seems to be due to an intermolecular C-H...O=C hydrogen bonding between the C=O group in one helical structure and the $CH_3$ group in the other helical structure. The x-ray crystallographic data of PHB showed that the distance between the O atom of the C=O group in one helical structure and the H atom of one of the three C-H bonds of the $CH_3$ group in the other helix structure is $2.63{\AA}$, which is significantly shorter than the sum of the van der Waals separation ($2.72{\AA}$). This result and the appearance of the $CH_3$ asymmetric stretching band at $3009 cm^{-1}$ suggest that there is a C-H...O=C hydrogen bond between the C=O group and the $CH_3$ group in PHB and P(HB-co-HHx). The temperature-dependent WAXD and IR measurements revealed that the crystallinity of P(HB-co-HHx) (HHx =10.5 and 12 mol%) decreases gradually from a fairly low temperature, while that of PHB and P(HB-co-HHx) (HHx = 2.5 and 3.5 mol%) remains almost unchanged until just below their melting temperatures. It was also shown from our studies that the weakening of the C-H...O = C interaction starts from just above room temperature and proceeds gradually increasing temperature. It seems that the C-H...O=C hydrogen bonding stabilizes the chain holding in the lamellar structure and affects the thermal behaviour of PHB and its copolymers.
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