Mechanistic analysis of Riboswitch Ligand interactions provides insights into pharmacological control over gene expression.


Journal

Nature communications
ISSN: 2041-1723
Titre abrégé: Nat Commun
Pays: England
ID NLM: 101528555

Informations de publication

Date de publication:
17 Sep 2024
Historique:
received: 26 02 2024
accepted: 28 08 2024
medline: 18 9 2024
pubmed: 18 9 2024
entrez: 17 9 2024
Statut: epublish

Résumé

Riboswitches are structured RNA elements that regulate gene expression upon binding to small molecule ligands. Understanding the mechanisms by which small molecules impact riboswitch activity is key to developing potent, selective ligands for these and other RNA targets. We report the structure-informed design of chemically diverse synthetic ligands for PreQ

Identifiants

pubmed: 39289353
doi: 10.1038/s41467-024-52235-3
pii: 10.1038/s41467-024-52235-3
doi:

Substances chimiques

Riboswitch 0
Ligands 0
Aptamers, Nucleotide 0
RNA, Bacterial 0

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

8173

Subventions

Organisme : U.S. Department of Health & Human Services | NIH | National Cancer Institute (NCI)
ID : BC011585

Informations de copyright

© 2024. This is a U.S. Government work and not under copyright protection in the US; foreign copyright protection may apply.

Références

Ganser, L. R., Kelly, M. L., Herschlag, D. & Al-Hashimi, H. M. The roles of structural dynamics in the cellular functions of RNAs. Nat. Rev. Mol. Cell Biol. 20, 474–489 (2019).
pubmed: 31182864 pmcid: 7656661 doi: 10.1038/s41580-019-0136-0
Bose, R.; Saleem, I.; Mustoe, A. M. Causes, functions, and therapeutic possibilities of RNA secondary structure ensembles and alternative states. Cell Chem. Biol. https://doi.org/10.1016/j.chembiol.2023.12.010 (2024).
Mustoe, A. M. et al. Pervasive regulatory functions of mRNA structure revealed by high-resolution SHAPE probing. Cell 173, 181–195 (2018).
pubmed: 29551268 pmcid: 5866243 doi: 10.1016/j.cell.2018.02.034
Scull, C. E., Dandpat, S. S., Romero, R. A. & Walter, N. G. Transcriptional riboswitches integrate timescales for bacterial gene expression control. Front Mol. Biosci. 7, 607158 (2020).
pubmed: 33521053 doi: 10.3389/fmolb.2020.607158
Santner, T., Rieder, U., Kreutz, C. & Micura, R. Pseudoknot preorganization of the PreQ1 class I riboswitch. J. Am. Chem. Soc. 134, 11928–11931 (2012).
pubmed: 22775200 doi: 10.1021/ja3049964
Hewitt, W. M., Calabrese, D. R. & Schneekloth, J. S. Evidence for ligandable sites in structured RNA throughout the Protein Data Bank. Bioorg. Med. Chem. 27, 2253–2260 (2019).
pubmed: 30982658 pmcid: 8283815 doi: 10.1016/j.bmc.2019.04.010
Warner, K. D., Hajdin, C. E. & Weeks, K. M. Principles for targeting RNA with drug-like small molecules. Nat. Rev. Drug Discov. 17, 547–558 (2018).
pubmed: 29977051 pmcid: 6420209 doi: 10.1038/nrd.2018.93
Childs-Disney, J. L. et al. Targeting RNA structures with small molecules. Nat. Rev. Drug Discov. 21, 736–762 (2022).
pubmed: 35941229 pmcid: 9360655 doi: 10.1038/s41573-022-00521-4
Vicens, Q. & Kieft, J. S. Thoughts on how to think (and talk) about RNA structure. Proc. Natl. Acad. Sci. USA 119, e2112677119 (2022).
pubmed: 35439059 pmcid: 9169933 doi: 10.1073/pnas.2112677119
Corley, M. et al. An RNA structure-mediated, posttranscriptional model of human α−1-antitrypsin expression. Proc. Natl. Acad. Sci. USA 114, E10244–E10253 (2017).
pubmed: 29109288 pmcid: 5703279 doi: 10.1073/pnas.1706539114
Bernat, V. & Disney, M. D. RNA Structures as Mediators of Neurological Diseases and as Drug Targets. Neuron 87, 28–46 (2015).
pubmed: 26139368 pmcid: 4508199 doi: 10.1016/j.neuron.2015.06.012
Spitale, R. C. & Incarnato, D. Probing the dynamic RNA structurome and its functions. Nat. Rev. Genet 24, 178–196 (2023).
pubmed: 36348050 doi: 10.1038/s41576-022-00546-w
Garber, K. Drugging RNA. Nat. Biotechnol. 41, 745–749 (2023).
pubmed: 37198443 doi: 10.1038/s41587-023-01790-z
Yu, A.-M., Choi, Y. H. & Tu, M.-J. RNA Drugs and RNA targets for small molecules: Principles, progress, and challenges. Pharmacol. Rev. 72, 862–898 (2020).
pubmed: 32929000 pmcid: 7495341 doi: 10.1124/pr.120.019554
Kavita, K. & Breaker, R. R. Discovering riboswitches: the past and the future. Trends Biochem. Sci. 48, 119–141 (2023).
pubmed: 36150954 doi: 10.1016/j.tibs.2022.08.009
Sherwood, A. V. & Henkin, T. M. Riboswitch-mediated gene regulation: Novel RNA architectures dictate gene expression responses. Annu. Rev. Microbiol. 70, 361–374 (2016).
pubmed: 27607554 doi: 10.1146/annurev-micro-091014-104306
Serganov, A. & Patel, D. J. Ribozymes, riboswitches and beyond: regulation of gene expression without proteins. Nat. Rev. Genet. 8, 776–790 (2007).
pubmed: 17846637 pmcid: 4689321 doi: 10.1038/nrg2172
Roth, A. et al. A riboswitch selective for the queuosine precursor preQ1 contains an unusually small aptamer domain. Nat. Struct. Mol. Biol. 14, 308–317 (2007).
pubmed: 17384645 doi: 10.1038/nsmb1224
Eichhorn, C. D., Kang, M. & Feigon, J. Structure and function of preQ1 riboswitches. Biochim. Biophys. Acta 1839, 939–950 (2014).
pubmed: 24798077 pmcid: 4177978 doi: 10.1016/j.bbagrm.2014.04.019
Klein, D. J., Edwards, T. E. & Ferré-D’Amaré, A. R. Cocrystal structure of a class I preQ1 riboswitch reveals a pseudoknot recognizing an essential hypermodified nucleobase. Nat. Struct. Mol. Biol. 16, 343–344 (2009).
pubmed: 19234468 pmcid: 2657927 doi: 10.1038/nsmb.1563
Suddala, K. C. et al. Single transcriptional and translational preQ1 riboswitches adopt similar pre-folded ensembles that follow distinct folding pathways into the same ligand-bound structure. Nucleic Acids Res. 41, 10462–10475 (2013).
pubmed: 24003028 pmcid: 3905878 doi: 10.1093/nar/gkt798
Meyer, M. M., Roth, A., Chervin, S. M., Garcia, G. A. & Breaker, R. R. Confirmation of a second natural preQ1 aptamer class in Streptococcaceae bacteria. RNA 14, 685–695 (2008).
pubmed: 18305186 pmcid: 2271366 doi: 10.1261/rna.937308
Liberman, J. A., Salim, M., Krucinska, J. & Wedekind, J. E. Structure of a class II preQ1 riboswitch reveals ligand recognition by a new fold. Nat. Chem. Biol. 9, 353–355 (2013).
pubmed: 23584677 pmcid: 3661761 doi: 10.1038/nchembio.1231
Liberman, J. A. et al. Structural analysis of a class III preQ1 riboswitch reveals an aptamer distant from a ribosome-binding site regulated by fast dynamics. Proc. Natl. Acad. Sci. USA 112, E3485–E3494 (2015).
pubmed: 26106162 pmcid: 4500280 doi: 10.1073/pnas.1503955112
McCown, P. J., Liang, J. J., Weinberg, Z. & Breaker, R. R. Structural, functional, and taxonomic diversity of three preQ1 riboswitch classes. Chem. Biol. 21, 880–889 (2014).
pubmed: 25036777 pmcid: 4145258 doi: 10.1016/j.chembiol.2014.05.015
Lee, E. R., Blount, K. F. & Breaker, R. R. Roseoflavin is a natural antibacterial compound that binds to FMN riboswitches and regulates gene expression. RNA Biol. 6, 187 (2009).
pubmed: 19246992 doi: 10.4161/rna.6.2.7727
Langer, S. et al. The flavoenzyme azobenzene reductase AzoR from Escherichia coli binds roseoflavin mononucleotide (RoFMN) with high affinity and is less active in its RoFMN form. Biochemistry 52, 4288–4295 (2013).
pubmed: 23713585 doi: 10.1021/bi400348d
Sudarsan, N., Cohen-Chalamish, S., Nakamura, S., Emilsson, G. M. & Breaker, R. R. Thiamine pyrophosphate riboswitches are targets for the antimicrobial compound pyrithiamine. Chem. Biol. 12, 1325–1335 (2005).
pubmed: 16356850 doi: 10.1016/j.chembiol.2005.10.007
Chen, L. et al. Probing riboswitch–ligand interactions using thiamine pyrophosphate analogues. Org. Biomol. Chem. 10, 5924–5931 (2012).
pubmed: 22514012 doi: 10.1039/c2ob07116a
Traykovska, M., Popova, K. B. & Penchovsky, R. Targeting glmS Ribozyme with chimeric antisense oligonucleotides for antibacterial drug development. ACS Synth. Biol. 10, 3167–3176 (2021).
pubmed: 34734706 doi: 10.1021/acssynbio.1c00443
Schüller, A. et al. Activation of the glmS Ribozyme confers bacterial growth inhibition. ChemBioChem 18, 435–440 (2017).
pubmed: 28012261 doi: 10.1002/cbic.201600491
Stängle, D. et al. Carba-sugar analogs of glucosamine-6-phosphate: New activators for the glmS riboswitch. Chemistry 29, e202202378 (2023).
pubmed: 36326082 doi: 10.1002/chem.202202378
Flemmich, L., Moreno, S. & Micura, R. Synthesis of O (6)-alkylated preQ(1) derivatives. Beilstein J. Org. Chem. 17, 2295–2301 (2021).
pubmed: 34621392 pmcid: 8450960 doi: 10.3762/bjoc.17.147
Wu, M.-C. et al. Rational re-engineering of a transcriptional silencing PreQ1 riboswitch. J. Am. Chem. Soc. 137, 9015–9021 (2015).
pubmed: 26106809 doi: 10.1021/jacs.5b03405
Blount, K. F., Wang, J. X., Lim, J., Sudarsan, N. & Breaker, R. R. Antibacterial lysine analogs that target lysine riboswitches. Nat. Chem. Biol. 3, 44–49 (2007).
pubmed: 17143270 doi: 10.1038/nchembio842
Tran, B. et al. Parallel discovery strategies provide a basis for riboswitch ligand design. Cell Chem. Biol. 27, 1241–1249 (2020).
pubmed: 32795418 pmcid: 7709957 doi: 10.1016/j.chembiol.2020.07.021
Connelly, C. M. et al. Synthetic ligands for PreQ1 riboswitches provide structural and mechanistic insights into targeting RNA tertiary structure. Nat. Commun. 10, 1501 (2019).
pubmed: 30940810 pmcid: 6445138 doi: 10.1038/s41467-019-09493-3
Wang, Y., Parmar, S., Schneekloth, J. S. & Tiwary, P. Interrogating RNA-small molecule interactions with structure probing and artificial intelligence-augmented molecular simulations. ACS Cent. Sci. 8, 741–748 (2022).
pubmed: 35756372 pmcid: 9228567 doi: 10.1021/acscentsci.2c00149
An, J., Totrov, M. & Abagyan, R. Pocketome via comprehensive identification and classification of ligand binding envelopes. Mol. Cell Proteom. 4, 752–761 (2005).
doi: 10.1074/mcp.M400159-MCP200
Moon, M. H., Hilimire, T. A., Sanders, A. M. & Schneekloth, J. S. Jr. Measuring RNA-ligand interactions with microscale thermophoresis. Biochemistry 57, 4638–4643 (2018). From NLM.
pubmed: 29327580 doi: 10.1021/acs.biochem.7b01141
Schroeder, G. M. et al. Analysis of a preQ1-I riboswitch in effector-free and bound states reveals a metabolite-programmed nucleobase-stacking spine that controls gene regulation. Nucleic Acids Res. 48, 8146–8164 (2020).
pubmed: 32597951 pmcid: 7641330 doi: 10.1093/nar/gkaa546
Siegfried, N. A., Busan, S., Rice, G. M., Nelson, J. A. E. & Weeks, K. M. RNA motif discovery by SHAPE and mutational profiling (SHAPE-MaP). Nat. Methods 11, 959–965 (2014).
pubmed: 25028896 pmcid: 4259394 doi: 10.1038/nmeth.3029
Van Vlack, E. R., Topp, S. & Seeliger, J. C. Characterization of engineered PreQ1 riboswitches for inducible gene regulation in mycobacteria. J. Bacteriol. 199, e00656–16 (2017).
pubmed: 28069821 pmcid: 5331669
Warnasooriya, C. et al. Observation of preQ(1)-II riboswitch dynamics using single-molecule FRET. RNA Biol. 16, 1086–1092 (2019).
pubmed: 30328747 doi: 10.1080/15476286.2018.1536591
Dutta, D. & Wedekind, J. E. Nucleobase mutants of a bacterial preQ1-II riboswitch that uncouple metabolite sensing from gene regulation. J. Biol. Chem. 295, 2555–2567 (2020).
pubmed: 31659117 doi: 10.1074/jbc.RA119.010755
Kang, M., Eichhorn, C. D. & Feigon, J. Structural determinants for ligand capture by a class II preQ1 riboswitch. Proc. Natl. Acad. Sci. USA 111, E663–E671 (2014).
pubmed: 24469808 pmcid: 3926045 doi: 10.1073/pnas.1400126111
Soulière, M. F. et al. Tuning a riboswitch response through structural extension of a pseudoknot. Proc. Natl. Acad. Sci. USA 110, E3256–E3264 (2013).
pubmed: 23940363 pmcid: 3761628 doi: 10.1073/pnas.1304585110
Marinus, T., Fessler, A. B., Ogle, C. A. & Incarnato, D. A novel SHAPE reagent enables the analysis of RNA structure in living cells with unprecedented accuracy. Nucleic Acids Res. 49, e34 (2021).
pubmed: 33398343 pmcid: 8034653 doi: 10.1093/nar/gkaa1255
Busan, S. & Weeks, K. M. Accurate detection of chemical modifications in RNA by mutational profiling (MaP) with ShapeMapper 2. Rna 24, 143–148 (2018).
pubmed: 29114018 pmcid: 5769742 doi: 10.1261/rna.061945.117
Lu, J. S., Bindewald, E., Kasprzak, W. K. & Shapiro, B. A. RiboSketch: versatile visualization of multi-stranded RNA and DNA secondary structure. Bioinformatics 34, 4297–4299 (2018).
pubmed: 29912310 pmcid: 6289134 doi: 10.1093/bioinformatics/bty468
Smola, M. J., Rice, G. M., Busan, S., Siegfried, N. A. & Weeks, K. M. Selective 2’-hydroxyl acylation analyzed by primer extension and mutational profiling (SHAPE-MaP) for direct, versatile and accurate RNA structure analysis. Nat. Protoc. 10, 1643–1669 (2015).
pubmed: 26426499 pmcid: 4900152 doi: 10.1038/nprot.2015.103
Smola, M. J., Calabrese, J. M. & Weeks, K. M. Detection of RNA–protein interactions in living cells with SHAPE. Biochemistry 54, 6867–6875 (2015).
pubmed: 26544910 doi: 10.1021/acs.biochem.5b00977
Kang, M., Peterson, R. & Feigon, J. Structural insights into riboswitch control of the biosynthesis of queuosine, a modified nucleotide found in the anticodon of tRNA. Mol. Cell 33, 784–790 (2009).
pubmed: 19285444 doi: 10.1016/j.molcel.2009.02.019
Dutta, D., Belashov, I. A. & Wedekind, J. E. Coupling green fluorescent protein expression with chemical modification to probe functionally relevant riboswitch conformations in live bacteria. Biochemistry 57, 4620–4628 (2018).
pubmed: 29897738 doi: 10.1021/acs.biochem.8b00316
Johnson, J. E. Jr, Reyes, F. E., Polaski, J. T. & Batey, R. T. B12 cofactors directly stabilize an mRNA regulatory switch. Nature 492, 133–137 (2012).
pubmed: 23064232 pmcid: 3518761 doi: 10.1038/nature11607
Baba, T. et al. Construction of Escherichia coli K‐12 in‐frame, single‐gene knockout mutants: the Keio collection. Mol. Syst. Biol. 2, 2006.0008 (2006).
pubmed: 16738554 pmcid: 1681482 doi: 10.1038/msb4100050
Holmstrom, E. D., Polaski, J. T., Batey, R. T. & Nesbitt, D. J. Single-molecule conformational dynamics of a biologically functional hydroxocobalamin riboswitch. J. Am. Chem. Soc. 136, 16832–16843 (2014).
pubmed: 25325398 pmcid: 4277777 doi: 10.1021/ja5076184
Hua, B. et al. Real-time monitoring of single ZTP riboswitches reveals a complex and kinetically controlled decision landscape. Nat. Commun. 11, 4531 (2020).
pubmed: 32913225 pmcid: 7484762 doi: 10.1038/s41467-020-18283-1
Ray, S., Chauvier, A. & Walter, N. G. Kinetics coming into focus: single-molecule microscopy of riboswitch dynamics. RNA Biol. 16, 1077–1085 (2019).
pubmed: 30328748 doi: 10.1080/15476286.2018.1536594
Nafisi, S., Malekabady, Z. M. & Khalilzadeh, M. A. Interaction of β-Carboline Alkaloids with RNA. DNA Cell Biol. 29, 753–761 (2010).
Hirata, K. et al. ZOO: an automatic data-collection system for high-throughput structure analysis in protein microcrystallography. Acta Crystallogr. D. Struct. Biol. 75, 138–150 (2019).
pubmed: 30821703 pmcid: 6400253 doi: 10.1107/S2059798318017795
Yamashita, K., Hirata, K. & Yamamoto, M. KAMO: towards automated data processing for microcrystals. Acta Crystallogr D. Struct. Biol. 74, 441–449 (2018).
pubmed: 29717715 pmcid: 5930351 doi: 10.1107/S2059798318004576
Kabsch, W. XDS. Acta Crystallogr. D Biol. Crystallogr. 66, 125–132 (2010).
pubmed: 20124692 pmcid: 2815665 doi: 10.1107/S0907444909047337
McCoy, A. J. et al. Phaser crystallographic software. J. Appl. Crystallogr. 40, 658–674 (2007).
pubmed: 19461840 pmcid: 2483472 doi: 10.1107/S0021889807021206
Adams, P. D. et al. PHENIX: a comprehensive Python-based system for macromolecular structure solution. Acta Crystallogr. D Biol. Crystallogr. 66, 213–221 (2010).
pubmed: 20124702 pmcid: 2815670 doi: 10.1107/S0907444909052925
Emsley, P. & Cowtan, K. Coot: model-building tools for molecular graphics. Acta Crystallogr. D. Biol. Crystallogr. 60, 2126–2132 (2004).
pubmed: 15572765 doi: 10.1107/S0907444904019158
Spagnolli, G. et al. Pharmacological inactivation of the prion protein by targeting a folding intermediate. Commun. Biol. 4, 62 (2021).
pubmed: 33437023 pmcid: 7804251 doi: 10.1038/s42003-020-01585-x
McInnes, L., Healy, J. & Astels, S. hdbscan: Hierarchical density based clustering. J. Open Source Softw. 2, 205 (2017).
doi: 10.21105/joss.00205
Bell, G. I. Models for the specific adhesion of cells to cells. Science 200, 618–627 (1978).
pubmed: 347575 doi: 10.1126/science.347575
Jenkins, J. L., Krucinska, J., McCarty, R. M., Bandarian, V. & Wedekind, J. E. Comparison of a preQ1 riboswitch aptamer in metabolite-bound and free states with implications for gene regulation. J. Biol. Chem. 286, 24626–24637 (2011).
pubmed: 21592962 pmcid: 3137038 doi: 10.1074/jbc.M111.230375

Auteurs

Shaifaly Parmar (S)

Chemical Biology Laboratory, Center for Cancer Research, National Cancer Institute, Frederick, MD, USA.

Desta Doro Bume (DD)

Chemical Biology Laboratory, Center for Cancer Research, National Cancer Institute, Frederick, MD, USA.

Colleen M Connelly (CM)

Chemical Biology Laboratory, Center for Cancer Research, National Cancer Institute, Frederick, MD, USA.

Robert E Boer (RE)

Chemical Biology Laboratory, Center for Cancer Research, National Cancer Institute, Frederick, MD, USA.

Peri R Prestwood (PR)

Chemical Biology Laboratory, Center for Cancer Research, National Cancer Institute, Frederick, MD, USA.

Zhen Wang (Z)

Depixus SAS, Paris, France.

Henning Labuhn (H)

Depixus SAS, Paris, France.

Krishshanthi Sinnadurai (K)

Depixus SAS, Paris, France.

Adeline Feri (A)

Depixus SAS, Paris, France.

Jimmy Ouellet (J)

Depixus SAS, Paris, France.

Philip Homan (P)

Center for Cancer Research Collaborative Bioinformatics Resource, National Cancer Institute, National Institutes of Health, Bethesda, MD, USA.
Advanced Biomedical Computational Science, Frederick National Laboratory for Cancer Research, Frederick, MD, USA.

Tomoyuki Numata (T)

Department of Bioscience and Biotechnology, Graduate School of Bioresource and Bioenvironmental Sciences, Kyushu University, Fukuoka, Japan.

John S Schneekloth (JS)

Chemical Biology Laboratory, Center for Cancer Research, National Cancer Institute, Frederick, MD, USA. schneeklothjs@mail.nih.gov.

Articles similaires

alpha-Synuclein Humans Animals Mice Lewy Body Disease
Adenosine Triphosphate Adenosine Diphosphate Mitochondrial ADP, ATP Translocases Binding Sites Mitochondria

Conservation of the cooling agent binding pocket within the TRPM subfamily.

Kate Huffer, Matthew C S Denley, Elisabeth V Oskoui et al.
1.00
TRPM Cation Channels Animals Binding Sites Mice Pyrimidinones
Receptor, Cannabinoid, CB1 Ligands Molecular Dynamics Simulation Protein Binding Thermodynamics

Classifications MeSH