Abstract:
:To understand design principles for assembling photosynthetic biohybrids that incorporate precisely-controlled sites for electron injection into redox enzyme cofactor arrays, we investigated the influence of chirality in assembly of the photosensitizer ruthenium(II)bis(2,2'-bipyridine)(4-bromomethyl-4'-methyl-2,2'-bipyridine), Ru(bpy)2(Br-bpy), when covalently conjugated to cysteine residues introduced by site-directed mutagenesis in the triheme periplasmic cytochrome A (PpcA) as a model biohybrid system. For two investigated conjugates that show ultrafast electron transfer, A23C-Ru and K29C-Ru, analysis by circular dichroism spectroscopy, CD, demonstrated site-specific chiral discrimination as a factor emerging from the close association between [Ru(bpy)3]2+ and heme cofactors. CD analysis showed the A23C-Ru and K29C-Ru conjugates to have distinct, but opposite, stereoselectivity for the Λ and Δ-Ru(bpy)2(Br-bpy) enantiomers, with enantiomeric excesses of 33.1% and 65.6%, respectively. In contrast, Ru(bpy)2(Br-bpy) conjugation to a protein site with high flexibility, represented by the E39C-Ru construct, exhibited a nearly negligible chiral selectivity, measured by an enantiomeric excess of 4.2% for the Λ enantiomer. Molecular dynamics simulations showed that site-specific stereoselectivity reflects steric constraints at the conjugating sites and that a high degree of chiral selectivity correlates to reduced structural disorder for [Ru(bpy)3]2+ in the linked assembly. This work identifies chiral discrimination as means to achieve site-specific, precise geometric positioning of introduced photosensitizers relative to the heme cofactors in manner that mimics the tuning of cofactors in photosynthesis.
journal_name
Photosynth Resjournal_title
Photosynthesis researchauthors
Ponomarenko NS,Kokhan O,Pokkuluri PR,Mulfort KL,Tiede DMdoi
10.1007/s11120-019-00697-8subject
Has Abstractpub_date
2020-02-01 00:00:00pages
99-113issue
2eissn
0166-8595issn
1573-5079pii
10.1007/s11120-019-00697-8journal_volume
143pub_type
杂志文章abstract::For maximal rates of CO2 assimilation in isolated intact spinach chloroplasts the generation of the adequate NADPH/ATP ratio is achieved either by cyclic electron flow around photosystem I or by linear electron transport to oxaloacetate, nitrite or oxygen (Mehler-reaction). The interrelationships between these poising...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/BF00019060
更新日期:1994-10-01 00:00:00
abstract::Using 77 K chlorophyll a (Chl a) fluorescence spectra in vivo, the development was studied of Photosystems II (PS II) and I (PS I) during greening of barley under intermittent light followed by continuous light at low (LI, 50 mumol m(-2) s(-1)) and high (HI, 1000 mumol m(-2) s(-1)) irradiances. The greening at HI inte...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1023/A:1020943107318
更新日期:2002-01-01 00:00:00
abstract::A correlated influence of cation concentration and excitation energy level on PS II Abbreviations: AMPD = 2-amino-2-methyl-1,3-propanediol; DCIP = 2-6 dichlorophenol indophenol; DCIPH2 = DCIP in reduced state; DCIPr = rate of DCIP-reduction; DCMU = 3-(3,4 dichlorophenyl)1-1 dimethyl-urea; Fv = variable fluorescence; F...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/BF00018228
更新日期:1980-06-01 00:00:00
abstract::Earlier mass spectrometric measurements, in which oxygen evolution was measured following short saturating light flashes, indicated that with a time resolution of about 30 s no form of bound water and/or an oxidation product exists up to the redox state S3 of the oxygen evolving center (R. Radmer and O. Ollinger, 1986...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/BF00046761
更新日期:1993-01-01 00:00:00
abstract::The crystallization of a given protein is a hard task being even more complicated when the protein shows a hydrophobic behavior. In the case of photosynthetic proteins, the difficulty of the experiments increased due to the high light sensitivity. Aqueous solutions of photosystem II core complex (OEC PSII) of Pisum sa...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/s11120-007-9131-y
更新日期:2006-12-01 00:00:00
abstract::DCMU (3-(3,4-dichlorophenyl)-1,1-dimethylurea) at concentrations higher than 10 μM suppresses the second time range delayed fluorescence (DF) of pea chloroplasts, due to inhibition of the oxidizing side of photosystem II (PS II). The inhibition of the reducing side of PS II resulting in the suppression of millisecond ...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/BF00054986
更新日期:1988-01-01 00:00:00
abstract::When CO(2) supply is limited, aquatic photosynthetic organisms induce a CO(2)-concentrating mechanism (CCM) and acclimate to the CO(2)-limiting environment. Although the CCM is well studied in unicellular green algae such as Chlamydomonas reinhardtii, physiological aspects of the CCM and its associated genes in multic...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/s11120-010-9614-0
更新日期:2011-09-01 00:00:00
abstract::The Soret absorption spectra of six synthetic rigid porphyrin dimers whose crystal structures have been determined are simulated using simple exciton theory. The objective is to test the validity of the point dipole and associated approximations; the electronic interaction parameters are thus calculated using data obt...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/BF00048299
更新日期:1989-12-01 00:00:00
abstract::It had been proposed that a loop, typically containing 26 or 27 amino acids, which is only present in monomeric, ferredoxin-dependent, "plant-type" glutamate synthases and is absent from the catalytic α-subunits of both NADPH-dependent, heterodimeric glutamate synthases found in non-photosynthetic bacteria and NADH-de...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/s11120-014-0044-2
更新日期:2015-02-01 00:00:00
abstract::Polyamines (PAs) are small metabolites that are produced and oxidized in chloroplasts with an obscure mode of action. Recently, we showed that qE is stimulated by PAs in higher plants (Nicotiana tabacum) and in genetically modified plants with elevated thylakoid-associated PAs (Ioannidis and Kotzabasis Biochim Biophys...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/s11120-010-9617-x
更新日期:2011-02-01 00:00:00
abstract::The photosynthetic sulfur bacterium, Chromatium vinosum, was cultured in inorganic photographic processing solutions containing silver thiosulfate complex salt (AgNa3(S2O3)2) under light. It was found that Chromatium was resistant to Ag and accumulated granular silver in the membrane during growth. The amount of Ag ac...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/BF00118318
更新日期:1986-01-01 00:00:00
abstract::This contribution gives a brief survey of the short history since the discovery of the aerobic phototrophic bacteria to focus on a general evolutionary scenario. Most of the citations are of reviews that have covered the earlier literature and to which the reader is directed at appropriate places in the following text...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1023/A:1020493518379
更新日期:2002-01-01 00:00:00
abstract::The linear, four-step oxidation of water to molecular oxygen by photosystem II requires cooperation between redox reactions driven by light and a set of redox reactions involving the S-states within the oxygen-evolving complex. The oxygenevolving complex is a highly ordered structure in which a number of polypeptides ...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/BF00037001
更新日期:1985-01-01 00:00:00
abstract::The thylakoid membrane protein PsbS is critical for quenching excessive excitation energy in mechanisms that involve the light-harvesting complexes of photosystem II. Liposomes of thylakoid lipids have been shown to be a very good platform to study photosynthetic membrane proteins and their interactions. In this study...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/s11120-015-0176-z
更新日期:2016-01-01 00:00:00
abstract::Inorganic phosphate participates in many fundamental processes within the plant cell. Its broad influence on plant metabolism is related to such key operations as metabolite transport, enzyme regulation and carbohydrate metabolism in general. This review discusses these topics with special emphasis on the role assigne...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/BF00016551
更新日期:1993-03-01 00:00:00
abstract::I provide here a personal perspective on (i) the awards that were given to young investigators at the 2008 and 2009 Gordon Research Conferences on Biochemistry/Biophysics of Photosynthesis; and (ii) the ambiance at these conferences through some photographs, particularly of the 2009 conference. ...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/s11120-009-9479-2
更新日期:2009-10-01 00:00:00
abstract::Time-resolved (TR) infrared (IR) spectroscopy in the nanosecond to second timescale has been extensively used, in the last 30 years, in the study of photosynthetic systems. Interesting results have also been obtained at lower time resolution (minutes or even hours). In this review, we first describe the used technique...
journal_title:Photosynthesis research
pub_type: 杂志文章,评审
doi:10.1007/s11120-016-0305-3
更新日期:2017-02-01 00:00:00
abstract::Far-red light photoacclimation (FaRLiP) is a mechanism that allows some cyanobacteria to utilize far-red light (FRL) for oxygenic photosynthesis. During FaRLiP, cyanobacteria remodel photosystem (PS) I, PS II, and phycobilisomes while synthesizing Chl d, Chl f, and far-red-absorbing phycobiliproteins, and these change...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/s11120-016-0309-z
更新日期:2017-02-01 00:00:00
abstract::Chlorophyll f is a photosynthetic pigment that was discovered in 2010. In this study, we present investigations on spectral and dynamic characteristics of singlet-excited and triplet states of Chl f with the application of ultrafast time-resolved absorption and fluorescence spectroscopies. The pigment was studied at r...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/s11120-014-9981-z
更新日期:2014-07-01 00:00:00
abstract::Electron transfer pathways in photosynthesis involve interactions between membrane-bound complexes such as reaction centres with an extrinsic partner. In this study, the biological specificity of electron transfer between the reaction centre-light-harvesting 1-PufX complex and its extrinsic electron donor, cytochrome ...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/s11120-013-9812-7
更新日期:2014-05-01 00:00:00
abstract::The polypeptide composition of thylakoid membranes of the red alga Cyanidium caldarium was studied by PAGE in the presence of lithium dodecyl sulfate. The thylakoid membranes were shown to contain 65 polypeptides with mol wt from 110 to 10 kDa. PS I isolated from C. caldarium cells is composed of at least 5 components...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/BF00035678
更新日期:1991-10-01 00:00:00
abstract::The previous work in our lab showed that the spinach chloroplast ATP synthase epsilon mutant with 3 amino acid residues deleted from the N-terminus had much lower ability to inhibit ATP hydrolysis and block proton leakage in comparison to a mutant with 1 or 2 residues deleted from the N-terminus. The present study aim...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/s11120-004-6554-6
更新日期:2005-01-01 00:00:00
abstract::Optically detected magnetic resonance of chlorosome-containing membranes from the green filamentous bacterium Chloroflexus aurantiacus has been performed both by fluorescence and absorption detection. Triplet states localized in the chlorosomes and in the B808-866 complex have been characterized. After chemical reduct...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1023/A:1014947412940
更新日期:2002-01-01 00:00:00
abstract::Heliobacteria are a recently discovered group of anoxygenic phototrophic bacteria, first described in 1983. Heliobacteria contain bacteriochlorophyll g, a pigment unique to species of this group, and synthesize the simplest photosynthetic complexes of all known phototrophs. Also, unlike all other phototrophs, heliobac...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/s11120-009-9516-1
更新日期:2010-06-01 00:00:00
abstract::The effect of nitrate and nitrite on long-term chlorophyll fluorescence has been studied in filamentous blue-green algae. Cells grown autotrophically with nitrate as nitrogen source show, under argon atmosphere, a high level of fluorescence. The addition of either nitrete or nitrite induces a significant fluorescence ...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/BF00032356
更新日期:1981-09-01 00:00:00
abstract::Illumination of the dark-incubated cells of Synechocystis PCC6803 caused recovery of both respiratory activity of oxygen uptake and PS I-cyclic electron flow, which was monitored by the dark reduction of P700(+) in the presence of DCMU after a 50 ms pulse light (MT) under background far-red light, but the effects were...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1023/A:1017946524199
更新日期:2001-01-01 00:00:00
abstract::By recording leaf transmittance at 820 nm and quantifying the photon flux density of far red light (FRL) absorbed by long-wavelength chlorophylls of Photosystem I (PS I), the oxidation kinetics of electron carriers on the PS I donor side was mathematically analyzed in sunflower (Helianthus annuus L.), tobacco (Nicotia...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1023/A:1026070612022
更新日期:2003-01-01 00:00:00
abstract::Cyanobacteria are photosynthetic prokaryotes and widely used for photosynthetic research as model organisms. Partly due to their prokaryotic nature, however, estimation of photosynthesis by chlorophyll fluorescence measurements is sometimes problematic in cyanobacteria. For example, plastoquinone pool is reduced in th...
journal_title:Photosynthesis research
pub_type: 杂志文章,评审
doi:10.1007/s11120-017-0367-x
更新日期:2017-09-01 00:00:00
abstract::Cassava, bean and maize leaves were fed with(14)CO2 in light and the primary products of photosynthesis identified 5 and 10 seconds after assimilation. In maize, approximately three quarters of the labelled carbon was incorporated in C4 acids, in beans about two thirds in PGA, and in cassava approximately 40-60% in C4...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1007/BF00055123
更新日期:1987-01-01 00:00:00
abstract::The effect of acetate metabolism on the light energy distribution between the two photosystems, on the PS II/PS I stoichiometry and on the expression of psbA and psbB and psaA genes was investigated in the green alga, Chlamydobotrys stellata during autotrophic (CO(2)), mixotrophic (CO(2) plus acetate) and photoheterot...
journal_title:Photosynthesis research
pub_type: 杂志文章
doi:10.1023/A:1010650532693
更新日期:2000-01-01 00:00:00