Tunable Methacrylamides for Covalent Ligand Directed Release Chemistry.


Journal

Journal of the American Chemical Society
ISSN: 1520-5126
Titre abrégé: J Am Chem Soc
Pays: United States
ID NLM: 7503056

Informations de publication

Date de publication:
07 04 2021
Historique:
pubmed: 26 3 2021
medline: 26 3 2021
entrez: 25 3 2021
Statut: ppublish

Résumé

Targeted covalent inhibitors are an important class of drugs and chemical probes. However, relatively few electrophiles meet the criteria for successful covalent inhibitor design. Here we describe α-substituted methacrylamides as a new class of electrophiles suitable for targeted covalent inhibitors. While typically α-substitutions inactivate acrylamides, we show that hetero α-substituted methacrylamides have higher thiol reactivity and undergo a conjugated addition-elimination reaction ultimately releasing the substituent. Their reactivity toward thiols is tunable and correlates with the p

Identifiants

pubmed: 33761747
doi: 10.1021/jacs.0c10644
pmc: PMC8041284
doi:

Types de publication

Journal Article Research Support, Non-U.S. Gov't

Langues

eng

Sous-ensembles de citation

IM

Pagination

4979-4992

Références

ACS Chem Biol. 2018 Jul 20;13(7):1810-1823
pubmed: 29924581
Eur J Med Chem. 2017 Oct 20;139:542-563
pubmed: 28837920
Chem Rev. 2010 May 12;110(5):2620-40
pubmed: 20000749
Curr Protoc Cytom. 2008 Apr;Chapter 12:Unit 12.12
pubmed: 18770644
Nat Rev Drug Discov. 2018 Aug;17(8):559-587
pubmed: 29700501
J Anal Methods Chem. 2018 Dec 13;2018:1986468
pubmed: 30647984
Cell. 2017 Jan 26;168(3):527-541.e29
pubmed: 28111073
J Am Chem Soc. 2011 Aug 10;133(31):12009-20
pubmed: 21732629
J Am Chem Soc. 2018 Mar 21;140(11):4004-4017
pubmed: 29473744
Cell. 2020 Aug 20;182(4):1009-1026.e29
pubmed: 32730809
Molecules. 2020 Feb 17;25(4):
pubmed: 32079289
Drug Discov Today. 2018 Mar;23(3):727-735
pubmed: 29337202
Cell Chem Biol. 2020 Mar 19;27(3):334-349.e11
pubmed: 31991094
Angew Chem Int Ed Engl. 2015 Nov 16;54(47):14099-102
pubmed: 26426864
Angew Chem Int Ed Engl. 2019 Dec 19;58(52):18823-18829
pubmed: 31584233
J Am Chem Soc. 2020 Jun 10;142(23):10358-10372
pubmed: 32412754
AAPS J. 2014 Sep;16(5):899-913
pubmed: 25004822
J Am Chem Soc. 2016 Dec 14;138(49):15841-15844
pubmed: 27960302
Angew Chem Int Ed Engl. 2016 Oct 17;55(43):13408-13421
pubmed: 27539547
Proc Natl Acad Sci U S A. 2010 Jul 20;107(29):13075-80
pubmed: 20615965
Nat Chem Biol. 2015 Jul;11(7):525-31
pubmed: 26006010
Nat Rev Drug Discov. 2011 Apr;10(4):307-17
pubmed: 21455239
J Am Chem Soc. 2019 Feb 20;141(7):2782-2799
pubmed: 30592612
Nature. 2016 Jun 15;534(7608):570-4
pubmed: 27309814
ACS Cent Sci. 2019 Jun 26;5(6):949-959
pubmed: 31263754
Angew Chem Int Ed Engl. 2020 Aug 17;59(34):14326-14330
pubmed: 32472602
Science. 2009 Dec 18;326(5960):1690-4
pubmed: 19965381
Bioorg Med Chem. 2019 May 15;27(10):2066-2074
pubmed: 30975501
J Med Chem. 2014 Dec 11;57(23):10072-9
pubmed: 25375838
Angew Chem Int Ed Engl. 2019 Feb 4;58(6):1739-1743
pubmed: 30561862
J Am Chem Soc. 2012 Mar 7;134(9):3961-4
pubmed: 22352855
Cell. 2017 Oct 19;171(3):696-709.e23
pubmed: 28965760
Chem Soc Rev. 2018 Jan 2;47(1):12-27
pubmed: 29099127
J Am Chem Soc. 2020 Oct 28;142(43):18522-18531
pubmed: 33047956
Chem Pharm Bull (Tokyo). 2000 Feb;48(2):298-300
pubmed: 10705526
Chem Biol. 2013 Feb 21;20(2):146-59
pubmed: 23438744
J Am Chem Soc. 2017 Oct 11;139(40):14181-14191
pubmed: 28915034
J Am Chem Soc. 2014 Sep 10;136(36):12624-30
pubmed: 25153195
J Hematol Oncol. 2016 Mar 09;9:21
pubmed: 26957112
Contrast Media Mol Imaging. 2018 Oct 22;2018:8541915
pubmed: 30425608
Anal Chem. 2019 Nov 5;91(21):13639-13646
pubmed: 31560193
SLAS Discov. 2017 Jan;22(1):3-20
pubmed: 27703080
Angew Chem Int Ed Engl. 2020 Feb 10;59(7):2829-2836
pubmed: 31782878
J Med Chem. 2017 Feb 9;60(3):839-885
pubmed: 27996267
Acc Chem Res. 2019 Oct 15;52(10):2806-2817
pubmed: 31483607
J Chem Inf Model. 2018 Feb 26;58(2):464-471
pubmed: 29320178
Curr Top Microbiol Immunol. 2019;420:375-417
pubmed: 30105421
J Am Chem Soc. 2016 Oct 12;138(40):13438-13446
pubmed: 27652602
J Pharm Anal. 2020 Oct;10(5):426-433
pubmed: 33133726
Spectrochim Acta A Mol Biomol Spectrosc. 2018 Oct 5;203:77-84
pubmed: 29860171
Nat Chem Biol. 2005 Sep;1(4):203-9
pubmed: 16408036
J Med Chem. 2020 Oct 22;63(20):11602-11614
pubmed: 32965113
J Am Chem Soc. 2020 Jul 8;142(27):11734-11742
pubmed: 32369353
Chem Sci. 2019 Feb 13;10(12):3573-3585
pubmed: 30996949
J Med Chem. 2001 Aug 16;44(17):2719-34
pubmed: 11495584
Nat Chem Biol. 2014 Sep;10(9):760-767
pubmed: 25038787
Nat Commun. 2018 May 14;9(1):1870
pubmed: 29760386
Angew Chem Int Ed Engl. 2015 Aug 24;54(35):10313-6
pubmed: 26110718
Medchemcomm. 2017 Dec 11;9(2):244-253
pubmed: 30108918
J Med Chem. 2019 Jun 27;62(12):5673-5724
pubmed: 30565923
Nat Chem Biol. 2012 Apr 01;8(5):471-6
pubmed: 22466421
J Am Chem Soc. 2019 Feb 27;141(8):3507-3514
pubmed: 30689386
Nature. 2010 Dec 9;468(7325):790-5
pubmed: 21085121
Curr Opin Chem Biol. 2015 Feb;24:18-26
pubmed: 25461720
Chem Soc Rev. 2020 May 7;49(9):2617-2687
pubmed: 32227030

Auteurs

Rambabu N Reddi (RN)

Department of Organic Chemistry, The Weizmann Institute of Science, Rehovot, 7610001, Israel.

Efrat Resnick (E)

Department of Organic Chemistry, The Weizmann Institute of Science, Rehovot, 7610001, Israel.

Adi Rogel (A)

Department of Organic Chemistry, The Weizmann Institute of Science, Rehovot, 7610001, Israel.

Boddu Venkateswara Rao (BV)

Department of Organic Chemistry, The Weizmann Institute of Science, Rehovot, 7610001, Israel.

Ronen Gabizon (R)

Department of Organic Chemistry, The Weizmann Institute of Science, Rehovot, 7610001, Israel.

Kim Goldenberg (K)

Department of Organic Chemistry, The Weizmann Institute of Science, Rehovot, 7610001, Israel.
Department of Immunology, The Weizmann Institute of Science, Rehovot, 7610001, Israel.

Neta Gurwicz (N)

Department of Immunology, The Weizmann Institute of Science, Rehovot, 7610001, Israel.

Daniel Zaidman (D)

Department of Organic Chemistry, The Weizmann Institute of Science, Rehovot, 7610001, Israel.

Alexander Plotnikov (A)

Wohl Institute for Drug Discovery of the Nancy and Stephen Grand Israel National Center for Personalized Medicine, The Weizmann Institute of Science, Rehovot, 7610001, Israel.

Haim Barr (H)

Wohl Institute for Drug Discovery of the Nancy and Stephen Grand Israel National Center for Personalized Medicine, The Weizmann Institute of Science, Rehovot, 7610001, Israel.

Ziv Shulman (Z)

Department of Immunology, The Weizmann Institute of Science, Rehovot, 7610001, Israel.

Nir London (N)

Department of Organic Chemistry, The Weizmann Institute of Science, Rehovot, 7610001, Israel.

Classifications MeSH