FRINK Linked Data Fragments server

Matches in SemOpenAlex for { <https://semopenalex.org/work/W2324138575> ?p ?o ?g. }

• W2324138575 endingPage "672" @default.
• W2324138575 startingPage "665" @default.
• W2324138575 abstract "Knowledge of the state of ionization and tautomerization of heteroaromatic cofactors when enzyme-bound is essential for formulating a detailed stepwise mechanism via proton transfers, the most commonly observed contribution to enzyme catalysis. In the bifunctional coenzyme, thiamin diphosphate (ThDP), both aromatic rings participate in catalysis, the thiazolium ring as an electrophilic covalent catalyst and the 4'-aminopyrimidine as acid-base catalyst involving its 1',4'-iminopyrimidine tautomeric form. Two of four ionization and tautomeric states of ThDP are well characterized via circular dichroism spectral signatures on several ThDP superfamily members. Yet, the method is incapable of providing information about specific proton locations, which in principle may be accessible via NMR studies. To determine the precise ionization/tautomerization states of ThDP during various stages of the catalytic cycle, we report the first application of solid-state NMR spectroscopy to ThDP enzymes, whose large mass (160,000-250,000 Da) precludes solution NMR approaches. Three de novo synthesized analogues, [C2,C6'-(13)C(2)]ThDP, [C2-(13)C]ThDP, and [N4'-(15)N]ThDP used with three enzymes revealed that (a) binding to the enzymes activates both the 4'-aminopyrimidine (via pK(a) elevation) and the thiazolium rings (pK(a) suppression); (b) detection of a pre-decarboxylation intermediate analogue using [C2,C6'-(13)C(2)]ThDP, enables both confirmation of covalent bond formation and response in 4'-aminopyrimidine ring's tautomeric state to intermediate formation, supporting the mechanism we postulate; and (c) the chemical shift of bound [N4'-(15)N]ThDP provides plausible models for the participation of the 1',4'-iminopyrimidine tautomer in the mechanism. Unprecedented detail is achieved about proton positions on this bifunctional coenzyme on large enzymes in their active states." @default.
• W2324138575 created "2016-06-24" @default.
• W2324138575 creator A5009378425 @default.
• W2324138575 creator A5010036955 @default.
• W2324138575 creator A5044356220 @default.
• W2324138575 creator A5045762965 @default.
• W2324138575 creator A5062717638 @default.
• W2324138575 date "2011-12-09" @default.
• W2324138575 modified "2023-09-27" @default.
• W2324138575 title "Solid-State Nuclear Magnetic Resonance Studies Delineate the Role of the Protein in Activation of Both Aromatic Rings of Thiamin" @default.
• W2324138575 cites W1640744618 @default.
• W2324138575 cites W1963881701 @default.
• W2324138575 cites W1966910457 @default.
• W2324138575 cites W1969764502 @default.
• W2324138575 cites W1979951613 @default.
• W2324138575 cites W1983268283 @default.
• W2324138575 cites W1986745697 @default.
• W2324138575 cites W1986999419 @default.
• W2324138575 cites W1987083186 @default.
• W2324138575 cites W1997738577 @default.
• W2324138575 cites W1999090137 @default.
• W2324138575 cites W2000964530 @default.
• W2324138575 cites W2007228590 @default.
• W2324138575 cites W2018779619 @default.
• W2324138575 cites W2022644397 @default.
• W2324138575 cites W2035628504 @default.
• W2324138575 cites W2036921365 @default.
• W2324138575 cites W2043078748 @default.
• W2324138575 cites W2048202808 @default.
• W2324138575 cites W2056425275 @default.
• W2324138575 cites W2060985984 @default.
• W2324138575 cites W2063701427 @default.
• W2324138575 cites W2068083144 @default.
• W2324138575 cites W2069852546 @default.
• W2324138575 cites W2076391112 @default.
• W2324138575 cites W2076538449 @default.
• W2324138575 cites W2084828445 @default.
• W2324138575 cites W2095046898 @default.
• W2324138575 cites W2104656965 @default.
• W2324138575 cites W2106471781 @default.
• W2324138575 cites W2113875939 @default.
• W2324138575 cites W2126518523 @default.
• W2324138575 cites W2136699027 @default.
• W2324138575 cites W2139797146 @default.
• W2324138575 cites W2320163706 @default.
• W2324138575 doi "https://doi.org/10.1021/ja209856x" @default.
• W2324138575 hasPubMedCentralId "https://www.ncbi.nlm.nih.gov/pmc/articles/3257386" @default.
• W2324138575 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/22092024" @default.
• W2324138575 hasPublicationYear "2011" @default.
• W2324138575 type Work @default.
• W2324138575 sameAs 2324138575 @default.
• W2324138575 citedByCount "29" @default.
• W2324138575 countsByYear W23241385752012 @default.
• W2324138575 countsByYear W23241385752013 @default.
• W2324138575 countsByYear W23241385752014 @default.
• W2324138575 countsByYear W23241385752015 @default.
• W2324138575 countsByYear W23241385752016 @default.
• W2324138575 countsByYear W23241385752017 @default.
• W2324138575 countsByYear W23241385752018 @default.
• W2324138575 countsByYear W23241385752019 @default.
• W2324138575 countsByYear W23241385752020 @default.
• W2324138575 countsByYear W23241385752021 @default.
• W2324138575 crossrefType "journal-article" @default.
• W2324138575 hasAuthorship W2324138575A5009378425 @default.
• W2324138575 hasAuthorship W2324138575A5010036955 @default.
• W2324138575 hasAuthorship W2324138575A5044356220 @default.
• W2324138575 hasAuthorship W2324138575A5045762965 @default.
• W2324138575 hasAuthorship W2324138575A5062717638 @default.
• W2324138575 hasBestOaLocation W23241385752 @default.
• W2324138575 hasConcept C111233374 @default.
• W2324138575 hasConcept C147597530 @default.
• W2324138575 hasConcept C161790260 @default.
• W2324138575 hasConcept C178790620 @default.
• W2324138575 hasConcept C180577832 @default.
• W2324138575 hasConcept C181199279 @default.
• W2324138575 hasConcept C185592680 @default.
• W2324138575 hasConcept C197957613 @default.
• W2324138575 hasConcept C2780378348 @default.
• W2324138575 hasConcept C71240020 @default.
• W2324138575 hasConceptScore W2324138575C111233374 @default.
• W2324138575 hasConceptScore W2324138575C147597530 @default.
• W2324138575 hasConceptScore W2324138575C161790260 @default.
• W2324138575 hasConceptScore W2324138575C178790620 @default.
• W2324138575 hasConceptScore W2324138575C180577832 @default.
• W2324138575 hasConceptScore W2324138575C181199279 @default.
• W2324138575 hasConceptScore W2324138575C185592680 @default.
• W2324138575 hasConceptScore W2324138575C197957613 @default.
• W2324138575 hasConceptScore W2324138575C2780378348 @default.
• W2324138575 hasConceptScore W2324138575C71240020 @default.
• W2324138575 hasIssue "1" @default.
• W2324138575 hasLocation W23241385751 @default.
• W2324138575 hasLocation W23241385752 @default.
• W2324138575 hasLocation W23241385753 @default.
• W2324138575 hasLocation W23241385754 @default.
• W2324138575 hasOpenAccess W2324138575 @default.
• W2324138575 hasPrimaryLocation W23241385751 @default.
• W2324138575 hasRelatedWork W1973544677 @default.
• W2324138575 hasRelatedWork W1983058798 @default.

• next