Abstract:
:Photosynthetic water oxidation takes place at the Mn4CaO5 cluster in photosystem II. Around the Mn4CaO5 cluster, a hydrogen bond network is formed by several water molecules, including four water ligands. To clarify the role of this water network in the mechanism of water oxidation, we investigated the effects of the removal of Ca(2+) and substitution with metal ions on the vibrations of water molecules coupled to the Mn4CaO5 cluster by means of Fourier transform infrared (FTIR) difference spectroscopy and quantum mechanics/molecular mechanics (QM/MM) calculations. The OH stretching vibrations of nine water molecules forming a network between D1-D61 and YZ were calculated using the QM/MM method. On the the calculated normal modes, a broad positive feature at 3200-2500 cm(-1) in an S2-minus-S1 FTIR spectrum was attributed to the vibrations of strongly hydrogen-bonded OH bonds of water involving the vibrations of water ligands to a Mn ion and the in-phase coupled vibration of a water network connected to YZ, while bands in the 3700-3500 cm(-1) region were assigned to the coupled vibrations of weakly hydrogen-bonded OH bonds of water. All the water bands were lost upon Ca(2+) depletion and Ba(2+) substitution, which inhibit the S2 → S3 transition, indicating that a solid water network was broken by these treatments. By contrast, Sr(2+) substitution slightly altered the water bands around 3600 cm(-1), reflecting minor modification in water interactions, consistent with the retention of water oxidation activity with a decreased efficiency. These results suggest that the water network around the Mn4CaO5 cluster plays an essential role in the water oxidation mechanism particularly in a concerted process of proton transfer and water insertion during the S2 → S3 transition.
journal_name
Biochemistryjournal_title
Biochemistryauthors
Nakamura S,Ota K,Shibuya Y,Noguchi Tdoi
10.1021/acs.biochem.5b01120subject
Has Abstractpub_date
2016-01-26 00:00:00pages
597-607issue
3eissn
0006-2960issn
1520-4995journal_volume
55pub_type
杂志文章相关文献
BIOCHEMISTRY文献大全abstract::Malondialdehyde (MDA) and nucleobase propenals can transfer oxopropenyl groups to guanine residues of DNA to yield pyrimodopurinone (M(1)G) adducts. The DNA structural requirements for reaction with alpha,beta-unsaturated aldehydes were explored. We found that single-stranded DNA is more sensitive to oxopropenylation ...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi0113059
更新日期:2002-04-16 00:00:00
abstract::Serum paraoxonase hydrolyzes the toxic metabolites of a variety of organophosphorus insecticides. High serum paraoxonase levels appear to protect against the neurotoxic effects of organophosphorus substrates of this enzyme [Costa et al. (1990) Toxicol. Appl. Pharmacol. 103, 66-76]. The amino acid sequence accounting f...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00106a010
更新日期:1991-10-22 00:00:00
abstract::We previously reported that enzymatically modified low-density lipoprotein (E-LDL) particles obtained by LDL treatment with trypsin and then cholesterol esterase are recognized by C1q and activate the C1 complex of complement. The objective of this study was to identify the E-LDL component(s) recognized by C1q. In add...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi9021022
更新日期:2010-03-16 00:00:00
abstract::The cytochrome P450-dependent terminal desaturation of valproic acid (VPA) is of both toxicological and mechanistic interest because the product, 4-ene-VPA, is a more potent hepatotoxin than the parent compound and its generation represents a rather novel metabolic reaction for the cytochrome P450 system. In the prese...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00024a013
更新日期:1995-06-20 00:00:00
abstract::Pyridoxal 5'-phosphate at concentrations greater than 0.5 mM inhibits polymerization of deoxynucleoside triphosphate catalyzed by a variety of DNA polymerases. The requirement for a phosphate as well as aldehyde moiety of pyridoxal phosphate for inhibition to occur is clearly shown by the fact that neither pyridoxal n...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00661a033
更新日期:1976-08-10 00:00:00
abstract::Receptor tyrosine kinase (RTK) activation is associated with modulation of heptahelical receptor-stimulated adenylyl cyclase responses. The mechanisms underlying the RTK-mediated enhancement of adenylyl cyclase function remain unclear. In the present studies, we show that the tyrosine kinase-dependent enhancement of a...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi0015818
更新日期:2001-02-13 00:00:00
abstract::Sensory rhodopsin I (SRI) is a seven-transmembrane helix retinylidene protein that mediates color-sensitive phototaxis responses through its bound transducer HtrI in the archaeon Halobacterium salinarum. Deprotonation of the Schiff base attachment site of the chromophore accompanies formation of the SRI signaling stat...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi991180w
更新日期:1999-10-05 00:00:00
abstract::In vitro transcription assays have been used to study the rate of ribonucleic acid (RNA) synthesis from the Escherichia coli lactose promotor mutant lacL8UV5 contained on a 203-bp (base pair) restriction fragment. The half-life of long (63-base) RNA production from heparin-resistant RNA polymerase-promotor complexes w...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00511a003
更新日期:1981-04-14 00:00:00
abstract::Resonance Raman spectroscopy is employed to characterize heme site structural changes arising from conformational heterogeneity in deoxyMb and ligated derivatives, i.e., the ferrous CO (MbCO) and ferric cyanide (MbCN) complexes. The spectra for the reversed forms of these derivatives have been extracted from the spect...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi801779d
更新日期:2008-12-02 00:00:00
abstract::The quaternary structure stability of proteins is typically studied under conditions that accelerate their aggregation/unfolding processes on convenient laboratory time scales. Such conditions include high temperature or pressure, chaotrope-mediated unfolding, or low or high pH. These approaches have the limitation of...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi500739q
更新日期:2014-10-21 00:00:00
abstract::The first step of the kynurenine pathway for l-tryptophan (l-Trp) degradation is catalyzed by heme-dependent dioxygenases, tryptophan 2,3-dioxygenase (TDO) and indoleamine 2,3-dioxygenase. In this work, we employed stopped-flow optical absorption spectroscopy to study the kinetic behavior of the Michaelis complex of C...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/acs.biochem.0c00179
更新日期:2020-08-04 00:00:00
abstract::Bacteriophage P22 is a double-stranded DNA containing phage. Its morphogenetic pathway requires the formation of a precursor procapsid that subsequently matures to the capsid. The stability of bacteriophage P22 coat protein in both monomeric and polymeric forms under hydrostatic pressure has been examined previously [...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00004a003
更新日期:1995-01-31 00:00:00
abstract::Inhibitors of poly(ADP-ribose) polymerase (PARP, EC 2.4.2.30) are of clinical interest because they have potential for improving radiation therapy and chemotherapy of cancer. The refined binding structures of four such inhibitors are reported together with the refined structure of the unligated catalytic fragment of t...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi972383s
更新日期:1998-03-17 00:00:00
abstract::Telomeres terminate nearly exclusively in single-stranded DNA (ssDNA) overhangs comprised of the G-rich 3' end. This overhang varies widely in length from species to species, ranging from just a few bases to several hundred nucleotides. These overhangs are not merely a remnant of DNA replication but rather are the res...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/acs.biochem.6b00496
更新日期:2016-09-27 00:00:00
abstract::Adenylosuccinate synthetase catalyzes the first committed step in the de novo biosynthesis of AMP, coupling L-aspartate and IMP to form adenylosuccinate. Km values of IMP and 2'-deoxy-IMP are nearly identical with each substrate supporting comparable maximal velocities. Nonetheless, the Km value for L-aspartate and th...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi0607498
更新日期:2006-09-26 00:00:00
abstract::Pig kidney general acyl-CoA dehydrogenases forms the blue neutral radical on dithionite or photochemical reduction (Thorpe, C., Matthews, R. G., & Williams, C. H. (1979) Biochemistry 18, 331-337] in accord with its classification as a flavoprotein dehydrogenase. However, dithionite reduction of the enzyme in the prese...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00520a024
更新日期:1981-08-18 00:00:00
abstract::It is known that aconitase from mammalian mitochondria is only partially active as isolated but may be activated by incubation with iron, ascorbate, and a thiol, or with dithionite. It has been suggested that the added Fe in the activation mixture is essential for activation and that it is incorporated in the enzyme [...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00529a023
更新日期:1981-12-22 00:00:00
abstract::During cellular uptake of fluorescently labeled cell-penetrating peptides (CPPs), intense fluorescent signals are commonly observed in the nucleus of the cell, suggesting intracellular CPP relocation and potential binding to the genome of the host. We therefore investigated the interaction of the CPP HIV-1 Tat(47-57) ...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi700416h
更新日期:2007-07-10 00:00:00
abstract::Lipoprotein(a) [Lp(a)] is a unique lipoprotein consisting of a low-density lipoprotein moiety (LDL) covalently linked to apoprotein(a). Previous work has demonstrated that Lp(a) can compete with plasminogen (PGN) for binding to endothelial and mononuclear cells and can inhibit PGN activation in cell-free systems. We h...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00068a021
更新日期:1993-05-04 00:00:00
abstract::The technique of quasi-elastic light scattering was used to measure the translational diffusion coefficient, D, of purified human prothrombin in buffered aqueous solutions and to monitor for the first time the fragmentation of this protein as it is converted to thrombin. The values of D20,w, measured at two different ...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00628a016
更新日期:1977-05-03 00:00:00
abstract::Nanosecond to millisecond conformational fluctuations of Zn-substituted cytochrome c (ZnCytc) have been studied by the time-resolved transient hole-burning method. The investigation of low-temperature dynamics has been made on the ZnCytc solution sample in a water-glycerol mixture. The conformational fluctuations in t...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi981568b
更新日期:1999-02-09 00:00:00
abstract::Modification of pig kidney fructose-1,6-bisphosphatase with 2,3-butanedione in borate buffer (pH 7.8) leads to the loss of the activation of the enzyme by monovalent cations, as well as to the loss of allosteric adenosine 5'-monophosphate (AMP) inhibition. In agreement with the results obtained for the butanedione mod...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00661a017
更新日期:1976-08-10 00:00:00
abstract::Heparan sulfate (HS) proteoglycans (PGs) interact with a number of extracellular signaling proteins, thereby playing an essential role in the regulation of many physiological processes. These interactions are important for both normal signal transduction and regulation of the tissue distribution of signaling molecules...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi6025424
更新日期:2007-04-03 00:00:00
abstract::A major challenge to the study of protein folding is the fact that intermediate states along the reaction pathway are generally unstable and thus difficult to observe. Recently developed NMR relaxation dispersion experiments present an avenue to accessing such states, providing kinetic, thermodynamic, and structural i...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi051771o
更新日期:2005-11-29 00:00:00
abstract::The reduction potentials of the compound II/ferric and compound I/compound II couples have been studied, using potassium hexachloroiridate as a mediator titrant, by thin-layer spectroelectrochemistry. Compound I, which is 2 equiv more oxidized than the ferric (i.e., resting) form of the enzyme, was reversibly formed v...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00009a017
更新日期:1995-03-07 00:00:00
abstract::The aminoglycoside 6'-N-acetyltransferase AAC(6')-Ii from Enterococcus faecium is an important microbial resistance determinant and a member of the GCN5-related N-acetyltransferase (GNAT) superfamily. We report here the further characterization of this enzyme in terms of the kinetic mechanism of acetyl transfer and id...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi034148h
更新日期:2003-06-03 00:00:00
abstract::Hepatitis C virus (HCV) protease NS3 and its protein activator NS4A participate in the processing of the viral polyprotein into its constituent nonstructural proteins. The NS3/4A complex is thus an attractive target for antiviral therapy against HCV. We expressed the full-length NS3 and NS4A in insect cells as a solub...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi972010r
更新日期:1998-03-10 00:00:00
abstract::Internal fatty acylation of proteins is a recognized means of modifying biological behavior. Escherichia coli hemolysin A (HlyA), a toxic protein, is transcribed as a nontoxic protein and made toxic by internal acylation of two lysine residue epsilon-amino groups; HlyC catalyzes the acyl transfer from acyl-acyl carrie...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi990138y
更新日期:1999-07-06 00:00:00
abstract::Two mutant versions of Escherichia coli aspartate transcarbamylase were created by site-specific mutagenesis. Arg-234 of the 240s loop was replaced by serine in order to help deduce the function of the interactions that normally occur between Arg-234 and both Glu-50 and Gln-231 in the R state of the enzyme. The other ...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi00423a022
更新日期:1988-11-15 00:00:00
abstract::UreE is a homodimeric metallo-chaperone that assists the insertion of Ni(2+) ions in the active site of urease. The crystal structures of UreE from Bacillus pasteurii and Klebsiella aerogenes have been determined, but the details of the nickel-binding site were not elucidated due to solid-state effects that caused dis...
journal_title:Biochemistry
pub_type: 杂志文章
doi:10.1021/bi0601003
更新日期:2006-05-23 00:00:00