Non-modular fatty acid synthases yield distinct N-terminal acylation in ribosomal peptides
Nature Chemistry
by Hengqian Ren, Chunshuai Huang, Yuwei Pan, Shravan R. Dommaraju, Haiyang Cui, Maolin Li, Mayuresh G. Gadgil, Douglas A. Mitchell, Huimin Zhao
3d ago
Nature Chemistry, Published online: 25 March 2024; doi:10.1038/s41557-024-01491-3 Ribosomally synthesized and post-translationally modified peptides (RiPPs) can have vast structural diversity and biological functions enabled by disparate post-translational modifications (PTMs). However, unconventional PTMs derived from non-RiPP biosynthesis are rarely reported. Now a class of lipopeptides featuring a distinct fatty-acyl-modified N terminus and the responsible RiPP/fatty-acid hybrid biosynthetic machinery have been characterized ..read more
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Dynamic three-dimensional structures of a metal–organic framework captured with femtosecond serial crystallography
Nature Chemistry
by Jaedong Kang, Yunbeom Lee, Seonggon Lee, Hosung Ki, Jungmin Kim, Jain Gu, Yongjun Cha, Jun Heo, Kyung Won Lee, Seong Ok Kim, Jaehyun Park, Sang-Youn Park, Sangsoo Kim, Rory Ma, Intae Eom, Minseok Kim, Jeongho Kim, Jae Hyuk Lee, Hyotcherl Ihee
3d ago
Nature Chemistry, Published online: 25 March 2024; doi:10.1038/s41557-024-01460-w Time-resolved femtosecond crystallography (TR-SFX) is a powerful technique to monitor structural transitions in protein crystals at the atomic level, but its use in non-protein synthetic materials remains limited. Now TR-SFX has been used to visualize the structural dynamics of metal–organic frameworks, showing the potential of this tool to study the dynamic motion of crystalline porous materials ..read more
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Catalyst self-assembly accelerates bimetallic light-driven electrocatalytic H2 evolution in water
Nature Chemistry
by Isaac N. Cloward, Tianfei Liu, Jamie Rose, Tamara Jurado, Annabell G. Bonn, Matthew B. Chambers, Catherine L. Pitman, Marc A. ter Horst, Alexander J. M. Miller
3d ago
Nature Chemistry, Published online: 25 March 2024; doi:10.1038/s41557-024-01483-3 Although the light-driven generation of hydrogen from water is a promising approach to renewable fuels, the H–H bond formation step represents a persistent mechanistic question. Now light-harvesting molecular catalysts have been shown to self-assemble into nanoscale aggregates that feature improved efficiency for photoelectrochemical H2 evolution ..read more
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Silicon-RosIndolizine fluorophores with shortwave infrared absorption and emission profiles enable in vivo fluorescence imaging
Nature Chemistry
by William E. Meador, Eric Y. Lin, Irene Lim, Hannah C. Friedman, David Ndaleh, Abdul K. Shaik, Nathan I. Hammer, Boqian Yang, Justin R. Caram, Ellen M. Sletten, Jared H. Delcamp
3d ago
Nature Chemistry, Published online: 25 March 2024; doi:10.1038/s41557-024-01464-6 Accessing longer-wavelength emitting organic fluorophores is critical for diagnostic imaging. Here a series of silicon-RosIndolizine fluorophores with emission maxima at 1,300 nm, 1,550 nm and 1,700 nm were synthesized. The fluorophores generate high-resolution in vivo fluorescence images in mice and establish design principles for future shortwave-infrared fluorophore designs ..read more
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Blocking and rescuing tryptophan interactions
Nature Chemistry
by Aidan K. Haney, T. Ashton Cropp
3d ago
Nature Chemistry, Published online: 25 March 2024; doi:10.1038/s41557-024-01478-0 Expansion of the genetic code can enable precise manipulation of proteins through selective functionalization of specific residues. Now, control of tryptophan interactions in proteins can be established by encoding of a vinyl-caged tryptophan analogue that can be selectively decaged to rescue protein activity ..read more
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Copper catalysed asymmetric amination
Nature Chemistry
by Joshua D. Sieber
3d ago
Nature Chemistry, Published online: 25 March 2024; doi:10.1038/s41557-024-01487-z Chiral amines possessing a stereogenic carbon atom bearing three carbon substituents and one nitrogen substituent are challenging structural motifs to prepare enantioselectively. Now, such motifs have been accessed in high enantiopurities by asymmetric Cu-catalysed propargylic amination using sterically confined ligands ..read more
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Identifying phase-separating biomolecular condensates in cells
Nature Chemistry
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5d ago
Nature Chemistry, Published online: 22 March 2024; doi:10.1038/s41557-024-01503-2 We developed a high-throughput, unbiased strategy for the identification of endogenous biomolecular condensates by merging cell volume compression, sucrose density gradient centrifugation and quantitative mass spectrometry. We demonstrated the performance of this strategy by identifying both global condensate proteins and those responding to specific biological processes on a proteome-wide scale ..read more
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Enantioselective propargylic amination and related tandem sequences to α-tertiary ethynylamines and azacycles
Nature Chemistry
by Zheng Zhang, Ying Sun, Yi Gong, Da-Liang Tang, Hui Luo, Zhi-Peng Zhao, Feng Zhou, Xin Wang, Jian Zhou
5d ago
Nature Chemistry, Published online: 19 March 2024; doi:10.1038/s41557-024-01479-z Enantioenriched α-disubstituted α-ethynylamines are valuable synthons to chiral α-tertiary amines and azacycles, but their facile access remains challenging. Now, sterically confined pyridinebisoxazoline ligands have been developed to facilitate highly enantioselective Cu(I)-catalysed propargylic amination of both aliphatic and aryl ketone-derived propargylic carbonates to give α-tertiary ethynylamines. Related tandem sequences are reported to synthesize quaternary azacycles ..read more
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Cage escape governs photoredox reaction rates and quantum yields
Nature Chemistry
by Cui Wang, Han Li, Tobias H. Bürgin, Oliver S. Wenger
1w ago
Nature Chemistry, Published online: 18 March 2024; doi:10.1038/s41557-024-01482-4 The spontaneous recombination of photogenerated radicals surrounded by solvent molecules is an important energy-wasting elementary step in photoredox reactions. Now the decisive role that cage escape plays in these reactions is shown in three benchmark photocatalytic reactions, with quantitative correlations observed between photoredox product formation rates and cage escape quantum yields ..read more
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RNA modulates hnRNPA1A amyloid formation mediated by biomolecular condensates
Nature Chemistry
by Chiara Morelli, Lenka Faltova, Umberto Capasso Palmiero, Katarzyna Makasewicz, Marcell Papp, Raphaël P. B. Jacquat, Dorothea Pinotsi, Paolo Arosio
2w ago
Nature Chemistry, Published online: 12 March 2024; doi:10.1038/s41557-024-01467-3 The underlying mechanism for how heterotypic protein–RNA interactions modulate the liquid to amyloid transition of hnRNPA1A, a protein involved in amyotrophic lateral sclerosis, has so far remained elusive. Now characterization of hnRNPA1A condensate formation and aggregation in vitro reveals that the RNA/protein stoichiometry affects the molecular pathways leading to amyloid formation ..read more
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