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Carbon-Centered Radicals in Protein Manipulation.
Methods to directly post-translationally modify proteins are perhaps the most straightforward and operationally simple ways to create and study protein post-translational modifications (PTMs). However, precisely altering or constructing the C-C scaffolds pervasive throughout biology is difficult with common two-e…
Intact nucleosomal context enables chromodomain reader MRG15 to distinguish H3K36me3 from -me2
A wealth of in vivo evidence demonstrates the physiological importance of histone H3 trimethylation at lysine 36 (H3K36me3), to which chromodomain-containing proteins, such as MRG15, bind preferentially compared to their dimethyl (H3K36me2) counterparts. However, in vitro studies using isolated H3 p…
Small molecule modulation of a redox-sensitive stress granule protein dissolves stress granules with beneficial outcomes for familial amyotrophic lateral sclerosis models
Neurodegeneràve diseases such as amyotrophic lateral sclerosis (ALS) are oten associated with mutàons in proteins that are associated with stress granules. Stress granules are condensates formed by liquid-liquid phase separàon which, when aberrant, can lead to altered condensàon behaviours and disease phe…
Direct radical functionalization of native sugars.
Naturally occurring (native) sugars and carbohydrates contain numerous hydroxyl groups of similar reactivity1,2. Chemists, therefore, rely typically on laborious, multi-step protecting-group strategies3 to convert these renewable feedstocks into reagents (glycosyl donors) to make glycans. The direct transf…
The least common multiple of consecutive arithmetic progression terms
AbstractLet k ≥ 0, a ≥ 1 and b ≥ 0 be integers. We define the arithmetic function gk,a,b for any positive integer n byIf we let a = 1 and b = 0, then gk,a,b becomes the arithmetic function that was previously introduced by Farhi. Farhi proved that gk,1,0 is periodic and that k! is a period. Hong and Yang improve…
Two-dimensional NMR lineshape analysis of single, multiple, zero and double quantum correlation experiments.
NMR spectroscopy provides a powerful approach for the characterisation of chemical exchange and molecular interactions by analysis of series of experiments acquired over the course of a titration measurement. The appearance of NMR resonances undergoing chemical exchange depends on the fre…
Synthetic Nucleosomes Reveal that GlcNAcylation Modulates Direct Interaction with the FACT Complex
AbstractTranscriptional regulation can be established by various post‐translational modifications (PTMs) on histone proteins in the nucleosome and by nucleobase modifications on chromosomal DNA. Functional consequences of histone O‐GlcNAcylation (O‐GlcNAc=O‐linked β‐N‐acetylglucosamine) are larg…
The Minimum Protein Staple? - Towards 'bio'-Baldwin's rules via inter-phosphosite linking in the MEK1 activation loop.
In small molecule organic chemistry, the heuristic insight into ring-forming processes that was enabled by Baldwin's rules some 50 years ago proved a step-change in the role of mechanistically guided synthesis. It created a lens upon and marker of fundamental stereoelectronic and conformation-guided chemic…
On matching and mismatching in protein chemistry
Post-translational protein editing methods that rely upon precise chemical alteration of sequence and hence function are of increasing utility. Whilst the role of proteins as chiral environments is functionally ubiquitous in their interaction with substrates or ligands, the influence of stereochemical ‘matching/mismat…
Late-Stage Functionalization of Living Organisms: Rethinking Selectivity in Biology.
With unlimited selectivity, full post-translational chemical control of biology would circumvent the dogma of genetic control. The resulting direct manipulation of organisms would enable atomic-level precision in "editing" of function. We argue that a key aspect that is still missing in our ability to do this (at least with…