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Guptasarma, P.

Publications and source records attributed to Guptasarma, P..

10 recordsLinked to original sources

Stationary phase KCl levels trigger changes in Dps conformation to facilitate its partitioning between reversibly-aggregated deposits and Dps-DNA condensates

In E. coli populations subjected to starvation, the transition of cells into stationary-phase is characterized by reduced KCl levels, cytoplasmic acidification, and increased production of Dps, the DNA binding protein from starved cells. Here, we show that at KCl concentrations peculiar to the stationary-phase, Dps displays greater surface hydrophobicity, lower helical content, lower stability to denaturation, greater susceptibility to proteolysis, and an intriguing ability to undergo 'reversible' deposition into liquid-solid phase separated (LSPS) aggregates, when no DNA is present. Whereas we have already previously shown that, at growth-phase KCl concentrations, Dps either remains soluble or forms liquid-liquid phase separated (LLPS) condensates with DNA, when DNA is present, here we show that the coacervation of Dps with DNA is exacerbated by stationary-phase KCl concentrations. This leads us to suggest the following interesting possibilities: (i) newly-produced Dps is reversibly kinetically-partitioned between LSPS and LLPS states, at low KCl concentrations, depending on the availability of DNA; (ii) excess Dps that is not coacervated with DNA in the LSPS state, exists in the LSPS state at low KCl concentrations; and (iii) Dps in the LSPS state dissolves to become instantaneously available for the packaging of newly-produced DNA, once nutrition becomes available, growth resumes and cytoplasmic KCl concentrations rise, before there is any production of the growth-phase DNA-packaging protein, HU.

biophysics↗

Exploring differential interactional preferences of enzyme-bearing dockarins for cohesin domains in the Clostridium thermocellum cellulosome

Using its 9 sequentially-placed cohesin (Coh) domains as bait, each CipA scaffoldin chain in a Clostridium thermocellum cellulosome binds to (and displays) some combination of 9 out of over [~]70 available dockerin (Doc) domain-bearing lignocellulose-degrading enzymes, at any time. Domains numbered Coh3 through Coh8 show over 94 % pairwise sequence identity with each other, but only [~] 61-76 % identity with Coh1, Coh2, and Coh9. Such identities are much lower ([~] 40-60 %) amongst Doc domains; however, amongst both Coh and Doc domains, polypeptide backbone folds are highly conserved, suggesting that loading preferences of enzyme-bearing Doc domains upon Coh domains must depend upon their relative abundances, and pairwise affinities. To explore this further, we used microscale thermophoresis (MST), size exclusion chromatography (SEC), native polyacrylamide gel electrophoresis (NPGE), mass spectrometry (MS) and bioinformatics-based approaches (BIBA), to examine 28 Coh-Doc pairwise interactions involving recombinant Coh [Coh1, Coh2, Coh3, Coh9] and enzyme-bearing Doc [Cel8A, Cel9F, Man26/5H, Cel9R, Xyn10C, Xyn11D, Xyn10Z] domains. Interactions were found to occur with varying affinities, suggesting that Coh1 prefers Xyn11D; Coh2 prefers Xyn10C; Coh3 prefers Cel9R; Coh9 prefers Cel9R; Coh1/Coh2 prefer Xyn partners; Coh3/Coh9 prefer Cel partners. Dual modes of binding are shown by Coh1 with Xyn10C and Xyn11D; Coh2 with Xyn10Z, Cel8A, and Cel9R; Coh3 with Cel8A, and Cel9R; and Coh9 with Xyn10C, suggesting that Doc domains use either of their two homologous helices (1 and 3) to bind to Coh domains, as earlier proposed. ImportanceBacteria such as Clostridium thermocellum use extracellular enzyme complexes called cellulosomes to degrade and use cellulose. Each complex uses a linear chain of nine cohesin (Coh) domains called a scaffoldin to bind to (and display) any nine of over seventy available xylan or cellulose-degrading enzymes that bear dockerin (Doc) domains. Understanding interactions between Coh and Doc domains facilitates an appreciation of how cellulosomes are assembled and supports the building of protein-engineered constructs that utilize such interactions for many conceivable enzymatic and other applications. The significance of the presented research lies in its demonstration of the differential modes and pairwise affinities of different Coh-Doc interactions, using recombinant protein constructs and a combination of quantitative, semi-quantitative and qualitative analytical methods.

biochemistry↗

E. coli cells advance into phase-separated (biofilm-simulating) extracellular polymeric substance containing DNA, HU, and lipopolysaccharide

We have earlier shown that HU, a nucleoid-associated protein, uses its DNA-binding surfaces to bind to bacterial outer-membrane lipopolysachharide (LPS), with this explaining how HU act as a potential glue for the adherence of bacteria to DNA, e.g., in biofilms. We have also earlier shown that HU and DNA together condense into a state of liquid-liquid phase separation (LLPS) both within, and outside, bacterial cells. Here, we report that HU and free LPS also condense into a state of phase separation, with coacervates of HU, DNA and free LPS being less liquid-like than condensates of HU and DNA alone. E. coli cells bearing surface LPS and also shedding LPS, are shown to adhere to (as well as enter into) condensates of HU and DNA. HU thus appears to play a role in maintaining both an intracellular state of phase separation involving genomic nucleoids that are phase-separated from the cytoplasm, and an extracellular state of phase separation involving coacervates of extracellular DNA, HU and LPS, in the extracellular polymeric substances (EPS) of biofilms, in which LPS content is shown to modulate liquidity. ImportanceUnderstanding biofilm genesis and nature are crucial to understanding how to deal with the bacterial resistance to antibiotics that develops eventually in persistent biofilms. This study, together with two other recent landmark studies from our group, elucidates a novel aspect of the extracellular polymeric substance (EPS) of an Escherichia coli biofilm, by creating a simulacrum of the EPS and demonstrating that its formation involves liquid-liquid phase separation (LLPS) by its component HU, DNA, and lipopolysaccharide (LPS), with LPS determining the liquidity of the EPS simulacrum. The findings provide insight into the physical nature of biofilms but also suggests that the interplay of HU, DNA, and LPS facilitates the structural integrity and functional dynamics of biofilms. These findings are a stepping stone to the eventual development of strategies to disrupt biofilm.

biochemistry↗

A glucanotransferase that uses two sub-sites and four catalytic aspartates/glutamates to disproportionate oligosaccharides ranging in length from maltotriose to starch

PF0272 (PfuAmyGT) from Pyrococcus furiosus is a 656 residues-long, homodimeric, three-domain GH57 glycoside hydrolase [homologous to TLGT from Thermococcus litoralis (PDB ID: 1K1X)]. It is proposed to be either an -amylase (EC 3.2.1.1), or a 4--glucanotransferase (EC 2.4.1.25). We demonstrate that PfuAmyGT is an exo-amylase-cum-glucanotransferase capable of transferring glucose, and dis-proportionating oligosaccharides, by excising glucose from malto-oligosaccharides (ranging in length from maltotriose to amylose/starch), and transferring it to malto-oligosaccharides (ranging in length from glucose to maltoheptaose and, possibly, even longer lengths). Convention holds that glucanotransferases transfer sugars through the serial and alternating binding of donors and acceptors to the same site, with covalent retention of excised sugars between such bindings. We present evidence of multiple behaviors in PfuAmyGT that challenge this view: (i) Production of free glucose, indicating scope for release of excised glucose; (ii) Higher activity with longer donors, indicating processivity; (iii) Accelerated activity with shorter acceptors, indicating a dependence upon rapid acceptor turnover; and (iv) Evidence of four catalytic glutamates/aspartates (E131, D222, E224, D362), indicating possible separation of excision and ligation functions. These behaviours collectively indicate the binding of donors and acceptors to separate sub-sites that have different substrate length preferences, supporting our own previous proposal regarding separate tunnel (internal) and groove (surface) binding sites. Although PfuAmyGTs mechanism of function remains to be fully elucidated, this paper definitively demonstrate coupling of exo-amylase and glucanotransferase functions involving separate sub-sites for donor and acceptor binding.

biochemistry↗

Differences in the activities of domain-swapped chimeras of two homologous GH57 glucanotransferases suggest that a glucan-binding DUF could influence donor substrate specificity

Five enzymes of the archaeal hyperthermophilic family of disproportionating GH57 4--glucanotransferases have been studied till date. Our focus here lies upon three homologous members of this family: (i) PfuAmyGT from Pyrococcus furiosus (PF0272), (ii) TonAmyGT from Thermococcus onnurenius (B6YUX8), and (iii) TliAmyGT (TLGT) from Thermococcus litoralis (O32462). The polypeptide chain of each of these enzymes is approximately 655 residues long, folded into three distinct domains (1, 2 and 3), and assembled into a homodimer. Domain 1 is a beta/alpha barrel containing an aspartate known to function as a catalytic nucleophile in TLGT. Domain 2 (which is helical) and domain 3 (made up of beta sheets) are thought to be domains of unknown function (or DUFs). In PfuAmyGT and TonAmyGT, we have recently identified a catalytically-important aspartate upon a loop in domain 2. In PfuAmyGT, we demonstrate the presence of two additional catalytically-important (glutamate) residues in domain 1, in a companion paper. In this paper, our focus lies upon domain 3 which hosts a second binding site (SBS) for a glucan, at its domain-domain interface with domain 2. Using strategies involving studies of both (a) domains (or pairs of contiguous domains) extracted from PfuAmyGT, and (b) chimeric three-domain enzymes recombining analogous domains between PfuAmyGT and TonAmyGT, we demonstrate that domain 3 determines the choice of the preferred glucan that acts as a donor in the glucan transfer reaction.

biochemistry↗

Nucleoid-Associated Proteins Undergo Liquid-Liquid Phase Separation with DNA into Multiphasic Condensates Resembling Bacterial Nucleoids

Liquid-liquid phase separation offers unique spatiotemporal control over myriad complex intracellular biochemical processes through compartmentalization of biomolecules into highly dynamic, liquid-like condensates known as membrane-less organelles. The bacterial nucleoid is thought to be one such phase-separated condensate; however, its formation, regulation, and biophysical characteristics are poorly understood. Our super-resolution imaging data suggests that nucleoids are dynamic assemblages of sub-micron-sized liquid-like droplets. We demonstrate that non-sequence-specific Nucleoid-Associated Proteins (NAPs) such as HU-A, HU-B and Dps, accrete nucleic acids and spontaneously condense with them into liquid-like, multicomponent, multiphasic, heterotypic phase-separated droplets. Upon mixing of HU-B, DNA and Dps, HU-B-enriched droplets are seen to contain demixed Dps-enriched droplets. Our findings indicate scope for the possible existence of multiphasic liquid-like compartments within nucleoids, providing insights into bacterial growth phase-dependent variations in the levels of different NAPs.

biophysics↗

Enhancing high-temperature degradation of polyethylene terephthalate through a synergistic division of enzyme labour between a solid-degrading thermostable cutinase and a reaction intermediate-degrading thermostable carboxylesterase

Cutinases degrade PET (polyethylene terephthalate) into various degradation intermediates (DIs) such as OET (oligoethylene terephthalate), BHET (bis-hydroxyethyl terephthalate), and MHET (mono-hydroxyethyl terephthalate), and eventually into TPA (terephthalic acid), which is the terminal product of degradation. Unlike PET, which is insoluble, TPA and the DIs are sparingly soluble in water. This causes both DIs and TPA to be partitioned into aqueous solution, where DIs accumulate without undergoing significant further degradation, despite being better substrates of cutinase than solid PET. This frustrates the creation of a circular economy involving PET and TPA (since TPA must be separated from DIs before re-condensation into PET). We argue that the non-degradation of DIs owes to cutinase becoming progressively depleted from solution, through binding to solid PET. This creates a conundrum, in that degradation of PET is anticipated to be inversely correlated with degradation of DIs (at least while solid PET remains available to deplete cutinase from solution), causing any improvement of the cutinases PET-binding efficiency to only further ensure non-degradation of released DIs. Here, we propose the deployment of a second DI-degrading enzyme; one that remains in solution, and acts as an assistant to the master PET-invading cutinase acting upon PETs surface. We demonstrate that one such dual-enzyme system, consisting of a thermostable Thermus thermophilus carboxylesterase (TTCE), characterized here for the first time, and the already-used thermostable leaf-branch compost cutinase (LCC), allows complete degradation of all products of PET hydrolysis into TPA in solution, at 60 {degrees}C, even in the presence of residual solid PET.

biochemistry↗

N-terminal extensions strengthen hydrophobic inter-subunit interactions between HU's C-terminal domains to frustrate heterodimer formation

HU is a nucleoid-associated protein (NAP) that helps bacterial chromosomal DNA to remain compact. Escherichia coli contains two homologs of HU that are ~ 70 % identical: HU-A and HU-B. The early log phase, late log phase, and stationary phase of E. coli growth are reported to be dominated, respectively, by HU-AA homodimers, HU-BB homo-dimers, and HU-AB heterodimers. Here, we show that the formation of HU-AB heterodimers occurs to a much lower degree in HU chains that have a displaced N-terminus, whether through addition of an N-terminal affinity (polyhistidine) tag, or fusion of a fluorescent protein. A combination of mass spectrometry, spectroscopy, chromatography, and electrophoresis (exploring glutaraldehyde crosslinking of subunits) was used to study the mixing, co-expression, unfolding and refolding of HU-AA and HU-BB homodimers. The data suggests that, in HU polypeptides with N-terminal extension, whereas inter-subunit contacts between the alpha helical N-terminal domains (NTDs) undergo facile unfolding and dissociation, inter-subunit contacts between the beta sheet- and IDR-dominated C-terminal domains (CTDs) fail to do so, due to persistence of hydrophobic inter-subunit interactions between two beta sheets. This persistence causes HU to remain nominally dimeric even after substantive unfolding, and frustrates subunit exchange and heterodimer formation.

biochemistry↗

Mechanism of bacterial adhesion and embedment in a DNA biofilm matrix:Evidence that binding of outer membrane lipopolysaccharide (LPS) to HU is key

In biofilms, bacteria are embedded within a matrix of extracellular DNA (e-DNA). Since bacterial cells and e-DNA are both negatively-charged, a positively-charged substance must act like a glue to allow bacteria to be embedded within the DNA matrix. Here we show that HU (a highly-abundant, histone-like, nucleoid-associated, DNA-binding protein) facilitates bacterium-bacterium and bacterium-DNA interactions by binding to lipopolysaccharide (LPS), a bacterial outer membrane component. We demonstrate that LPS binds to both the canonical and non-canonical DNA-binding sites on HU. We propose that the hexose sugar-terminal phosphate moieties present in the lipid A head-group of LPS bind to the same lysine/arginine residues that are involved in binding of the pentose sugar-phosphate groups in DNA. Alternate binding of LPS and DNA by HUs DNA-binding sites could allow HU to bind to bacterial cells surfaces and thus elicit bacterium-bacterium and bacterium-DNA interactions in biofilms.

microbiology↗

Sustained exposure to trypsin causes cells to transition into a state of reversible stemness that is amenable to transdifferentiation

During cell culture, trypsin, a serine protease, is applied to cells for 5-10 minutes to separate them from each other and from the underlying substratum so that they can be transferred to a different vessel, for re-plating, after growth medium containing 10 % serum has been added to the cells, in a well-known technique known as passaging. The serum in the growth medium contains alpha-1 antitrypsin, which is a potent inhibitor of trypsin, elastase and other serine proteases. Although what is used is bovine serum in which levels of proteins could be different from levels seen in humans, normal human serum contains A1AT (> 1 mg/ml; > [~]18 {micro}mol/L) as well as trypsin itself (< 460 ng/ml, or [~]0.02 {micro}mol/L), with the former in a [~]900-fold molar excess over the latter. Thus, it may be assumed there is also enough A1AT in the bovine serum added during passaging, to neutralize the trypsin ([~]100 M) present in the small volume of trypsin-EDTA solution used to separate cells. What are the consequences of not adding serum, when growth medium is added, or of maintaining cells for a few tens of hours in the presence of trypsin, in a serum-free growth medium? What does such sustained exposure to trypsin during cell culture do to cells? More generally, what are the responses of cells within an organism to the balance of trypsin and A1AT in the serum that bathes them constantly? We know that excesses and deficiencies in the levels of either trypsin or A1AT are associated with disease. We know that cellular metabolism can be influenced through signaling involving protease activated membrane GPCR receptors (PAR1-4). In particular, we know of a receptor called PAR2, which is specifically activated by trypsin, expressed by cells at baseline levels, and upregulated through some feedback involving trypsin-activation. We also know that cells at sites of injury or inflammation produce and secrete trypsin, and that this trypsin can act locally upon cells in a variety of ways, all of which have probably not yet been elucidated. Here, we show that sustained exposure to trypsin induces cells to de-differentiate into a stem-like state. We show that if serum is either not added at all, or added and then washed away (after confluency is attained), during cell culture, all cells exposed to exogenously-added trypsin undergo changes in morphology, transcriptome, secretome, and developmental potential, and transition into a state of stemness, in minimal essential medium (MEM). Regardless of their origins, i.e., independent of whether they are derived from primary cultures, cell lines or cancer cell lines, and regardless of the original cell type used, exposure to trypsin ([~]10 {micro}M; [~]250 {micro}g/ml) at a concentration 10-fold lower than that used to separate cells during passaging ([~]100 M), over a period of 24-48 hours, causes cells to (1) become rounded, (2) cluster together, (3) get arrested in the G0/G1 stage of the cell cycle, (4) display increased presence of 5-hydroxymethyl cytosine in their nuclei (indicative of reprogramming), (5) display increased levels of activated PAR2 membrane receptor, (6) become capable of very efficient efflux of drug-mimicking dyes, (7) express factors and/or markers known to be associated with induction and/or attainment of stemness, with predominant expression of Sox-2 within cell nuclei; (8) display overall transcriptomic (RNASEQ) profiles characteristic of stemness; (9) secrete stemness-associated factors such as bFGF, and IL-1{beta}, into the medium, in quantities sufficient to support autocrine function (in certain cases); and (10) display increased conversion of pro-MMPs into activated MMPs in the cells secretome. Notably, (11) inclusion of differentiating and/or transdifferentiating factors in the environment of such cells causes them to express markers associated with ectodermal, endodermal and mesodermal cell lineages and/or transdifferentiate into specific cell types, e.g., adipocytes or osteocytes.\n\nMost intriguingly of all, (12) the attained stemness appears to be reversible, i.e., withdrawal of trypsin from the medium prior to addition of any differentiating factors restores cells to their original morphology, also over a period of 24-48 hours. Further, (13) a known PAR2 agonist, and a known PAR2 antagonist, respectively, appear to mimic effects of trypsin addition and withdrawal/inhibition. In addition, (14) in experiments with a particular cancer characterized by high levels of stemness (TNBC; triple negative breast cancer), tissues of all TNBC patients express high levels of the PAR2 receptor, as do cells from a known TNBC-derived cell line. We propose that through their effects on PAR levels, and PAR activation status, the balance of trypsin and A1AT levels in organisms normally regulates cellular potential for differentiation, de-differentiation or transdifferentiation, in a local manner, with the default status being that A1AT inhibits trypsin and keeps cells differentiated, whereas sustained trypsin signaling at sites of injury through local production of trypsin helps to place cells into an intermediate state of stemness from which they can either return to their original differentiated state(s), or undergo factor-dependent differentiation, or transdifferentiation, into specific cell types or lineages. It is also possible that reduction in A1AT promotes regeneration. We present a core (RNASEQ-derived) signature for trypsin-induced stemness in human corneal fibroblasts (HCFs) and cells from a retinal pigment epithelial cell line (ARPE-19), noting that there are commonalities as well as differences between them, which suggests that this core signature will be amended with RNASEQ studies of more trypsin-exposed cell types. Our findings offer a possible explanation for the recent unexplained increase in the preference for serum-free protocols used for induction and maintenance of stemness involving iPSCs and mesenchymal stem cells. Also, our studies suggest a new approach to understanding and exploiting how organisms might use stemness, in adults. Trypsin-dominated serine protease induced reprogramming (SPIR) might offer a more natural, and suitably softer, method of reprogramming of cellular developmental potential for local regenerative requirements in animal tissues.

cell biology↗