Gyanendra Kumar1, Maxime Cuypers1, Richard R Webby2, Thomas R Webb3,4, Stephen W White1. 1. Department of Structural Biology, Memphis, TN 38105, USA. 2. Department of Infectious Diseases, St. Jude Children's Research Hospital, Memphis, TN 38105, USA. 3. Wildflower Biopharma, Inc., 8650 Genesee Ave. STE 214, San Diego, CA 92122, USA. 4. Department of Chemistry and Biochemistry, University of California, Santa Cruz, Santa Cruz, CA 95064, USA.
Abstract
The endonuclease activity within the influenza virus cap-snatching process is a proven therapeutic target. The anti-influenza drug baloxavir is highly effective, but is associated with resistance mutations that threaten its clinical efficacy. The endonuclease resides within the N-terminal domain of the PA subunit (PAN) of the influenza RNA dependent RNA polymerase, and we report here complexes of PAN with RNA and DNA oligonucleotides to understand its specificity and the structural basis of baloxavir resistance mutations. The RNA and DNA oligonucleotides bind within the substrate binding groove of PAN in a similar fashion, explaining the ability of the enzyme to cleave both substrates. The individual nucleotides occupy adjacent conserved pockets that flank the two-metal active site. However, the 2' OH of the RNA ribose moieties engage in additional interactions that appear to optimize the binding and cleavage efficiency for the natural substrate. The major baloxavir resistance mutation at position 38 is at the core of the substrate binding site, but structural studies and modeling suggest that it maintains the necessary virus fitness via compensating interactions with RNA. These studies will facilitate the development of new influenza therapeutics that spatially match the substrate and are less likely to elicit resistance mutations.
The endonuclease activity within the pan class="Species">influenza virus cap-snatching process is a proven therapeutic target. The anti-pan class="Species">influenza drug pan class="Chemical">baloxavir is highly effective, but is associated with resistance mutations that threaten its clinical efficacy. The endonuclease resides within the N-terminal domain of the PA subunit (PAN) of the influenza RNA dependent RNA polymerase, and we report here complexes of PAN with RNA and DNA oligonucleotides to understand its specificity and the structural basis of baloxavir resistance mutations. The RNA and DNA oligonucleotides bind within the substrate binding groove of PAN in a similar fashion, explaining the ability of the enzyme to cleave both substrates. The individual nucleotides occupy adjacent conserved pockets that flank the two-metal active site. However, the 2' OH of the RNA ribose moieties engage in additional interactions that appear to optimize the binding and cleavage efficiency for the natural substrate. The major baloxavir resistance mutation at position 38 is at the core of the substrate binding site, but structural studies and modeling suggest that it maintains the necessary virus fitness via compensating interactions with RNA. These studies will facilitate the development of new influenza therapeutics that spatially match the substrate and are less likely to elicit resistance mutations.
Authors: Dominga Rogolino; Lieve Naesens; Jennifer Bartoli; Mauro Carcelli; Laura De Luca; Giorgio Pelosi; Ryjul W Stokes; Ria Van Berwaer; Serena Vittorio; Annelies Stevaert; Seth M Cohen Journal: Bioorg Chem Date: 2021-10-01 Impact factor: 5.275
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