journal article·2023-12Open access

Atroposelective synthesis of eight-membered lactam-bridged N-arylindoles via stepwise cut-and-sew strategy

Ling-Fei Tao, Fen Huang, Xin Zhao, Linghui Qian, Jia-Yu Liao

Cell Reports Physical Science· Volume 4· Issue 12

Abstract

The development of efficient processes for the preparation of structurally diverse axially chiral biaryls has been an important goal in synthetic organic chemistry and asymmetric catalysis. However, in sharp contrast to the well-established open-chain biaryls, the catalytic enantioselective construction of medium-sized bridged biaryls remains underdeveloped. In particular, no enantioselective synthesis of such frameworks possessing a configurationally stable stereogenic C-N axis with step- or pot-economy has been disclosed. Herein, we report a practical synthesis of atropisomeric eight-membered lactam-bridged N-arylindoles through a conceptually intriguing stepwise cut-and-sew strategy. The key to success lies in the development of a silver-catalyzed atroposelective ring-opening/cyclization cascade reaction of N-arylindole lactams with isocyanoacetates to establish C-N axial chirality. This method features operational simplicity, good functional group tolerance, high efficiency, as well as good to high enantiocontrol. It is also noteworthy that these scaffolds exhibit large Stokes shifts, demonstrating their potential applications as fluorescent dyes.
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Research context

OpenAlex topics: Axial and Atropisomeric Chirality Synthesis · Molecular spectroscopy and chirality · Alkaloids: synthesis and pharmacology

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (71)

Show source-provided references
1. The Challenge of Atropisomerism in Drug Discovery10.1002/anie.200901719 ↗
2. Assessing Atropisomer Axial Chirality in Drug Discovery and Development10.1021/jm200584g ↗
3. A twist of nature - the significance of atropisomers in biological systems10.1039/C4NP00121D ↗
4. Recent progress toward developing axial chirality bioactive compounds10.1016/j.ejmech.2022.114700 ↗
5. BINAP: An Efficient Chiral Element for Asymmetric Catalysis10.1021/ar00178a005 ↗
6. Binaphthol-derived phosphoric acid as a versatile catalyst for enantioselective carbon-carbon bond forming reactions10.1039/b807577h ↗
7. Enantioselective Fluorescent Recognition of Free Amino Acids: Challenges and Opportunities10.1002/anie.202003969 ↗
8. Atroposelective Synthesis of Axially Chiral Biaryl Compounds10.1002/anie.200462661 ↗
9. Recent advances and new concepts for the synthesis of axially stereoenriched biaryls10.1039/C5CS00012B ↗
10. Nonbiaryl and Heterobiaryl Atropisomers: Molecular Templates with Promise for Atropselective Chemical Transformations10.1021/acs.chemrev.5b00136 ↗
11. Stereoselective arene formation10.1039/C7CS00875A ↗
12. Atroposelective transformation of axially chiral (hetero)biaryls. From desymmetrization to modern resolution strategies10.1039/D0CS00870B ↗
13. Recent Advances in Catalytic Asymmetric Construction of Atropisomers10.1021/acs.chemrev.0c01306 ↗
14. Carbene-Catalyzed Asymmetric Construction of Atropisomers10.1002/anie.202108630 ↗
15. Synthesis of Atropisomers by Transition-Metal-Catalyzed Asymmetric C-H Functionalization Reactions10.1021/jacs.1c07635 ↗
16. Natural Bridged Biaryls with Axial Chirality and Antimitotic Properties10.1016/S1572-5995(03)80011-X ↗
17. Catalytic asymmetric synthesis of medium-sized bridged biaryls10.1039/D2CC04000J ↗
18. Steganacin and Steganangin, Novel Antileukemic Lignan Lactones from Steganotaenia araliacea10.1021/ja00785a054 ↗
19. New isocoumarins and alkaloid from Chinese insect medicine, Eupolyphaga sinensis Walker10.1016/j.fitote.2012.06.005 ↗
20. Rhazinilam Mimics the Cellular Effects of Taxol by Different Mechanisms of Action10.1002/cm.970280405 ↗
21. The Lactone Concept: An Efficient Pathway to Axially Chiral Natural Products and Useful Reagents10.1055/s-1999-3435 ↗
22. Stereoselective Total Synthesis of Axially Chiral Natural Products via Biaryl Lactones10.1021/ar000106z ↗
23. First Atropo-Enantioselective Ring Opening of Achiral Biaryls Containing Lactone Bridges with Chiral Hydride-Transfer Reagents Derived from Borane10.1002/anie.199207611 ↗
24. Catalytic atropo-Enantioselective Reduction of Biaryl Lactones to Axially Chiral Biaryl Compounds10.1021/ol800802c ↗
25. Dynamic Kinetic Resolution of Biaryl Lactones via a Chiral Bifunctional Amine Thiourea-Catalyzed Highly Atropo-enantioselective Transesterification10.1021/jacs.6b03609 ↗
26. Design and Synthesis of Chiral oxa-Spirocyclic Ligands for Ir-Catalyzed Direct Asymmetric Reduction of Bringmann’s Lactones with Molecular H210.1021/jacs.8b03642 ↗
27. Catalytic Dynamic Kinetic Resolutions in Tandem to Construct Two-Axis Terphenyl Atropisomers10.1021/jacs.0c08057 ↗
28. Catalytic Atroposelective Dynamic Kinetic Resolution of Biaryl Lactones with Activated Isocyanides10.1021/acs.orglett.1c01632 ↗
29. Transition Metal-Catalyzed Biaryl Atropisomer Synthesis via a Torsional Strain Promoted Ring-Opening Reaction10.1021/acs.accounts.2c00175 ↗
30. Recent Progress in Cyclic Aryliodonium Chemistry: Syntheses and Applications10.1021/acs.chemrev.2c00591 ↗
31. Palladium-Catalyzed Heck and Carbonylation Reactions of a Dinaphthaleneiodonium Salt Forming Functionalized 2-Iodo-1,1’-binaphthyls10.1002/adsc.200404202 ↗
32. Enhanced Reactivity by Torsional Strain of Cyclic Diaryliodonium in Cu-Catalyzed Enantioselective Ring-Opening Reaction10.1016/j.chempr.2018.01.017 ↗
33. Atroposelective Three-Component Coupling of Cyclic Diaryliodoniums and Sodium Cyanate Enabled by the Dual-Role of Phenol
34. Nickel-Catalyzed Asymmetric Grignard Cross-Coupling of Dinaphthothiophene Giving Axially Chiral 1,1’-Binaphthyls10.1021/ja0282588 ↗
35. Enantioselective Carbon-Carbon Bond Cleavage for Biaryl Atropisomers Synthesis10.1016/j.chempr.2019.04.008 ↗
36. Catalytic asymmetric C-Si bond activation via torsional strain-promoted Rh-catalyzed aryl-Narasaka acylation10.1038/s41467-020-18273-3 ↗
37. Organocatalytic asymmetric N-sulfonyl amide C-N bond activation to access axially chiral biaryl amino acids10.1038/s41467-020-14799-8 ↗
38. Cooperative catalysis-enabled C-N bond cleavage of biaryl lactams with activated isocyanides10.1039/D2CC01625G ↗
39. Nickel-Catalyzed Enantioselective Arylative Activation of Aromatic C-O Bond10.1021/jacs.1c09797 ↗
40. Torsional strain inversed chemoselectivity in a Pd-catalyzed atroposelective carbonylation reaction of dibenzothiophenium10.1039/D2SC00341D ↗
41. Torsional Strain-Independent Catalytic Enantioselective Synthesis of Biaryl Atropisomers10.1002/anie.202211303 ↗
42. Palladium-Catalyzed Stereoselective Cleavage of C-P Bond: Enantioselective Construction of Atropisomers Containing a P-Stereogenic Center10.1002/anie.202211710 ↗
43. Organocatalytic dynamic kinetic resolution of N-arylindole lactams: atroposelective construction of axially chiral amino acids bearing a C-N chiral axis10.1007/s11426-021-1209-2 ↗
44. Dirhodium(II)/Phosphine Catalyst with Chiral Environment at Bridging Site and Its Application in Enantioselective Atropisomer Synthesis10.1021/acscentsci.2c01207 ↗
45. Catalytically atroposelective ring-opening of configurationally labile compounds to access axially chiral biaryls10.1039/D2QO00946C ↗
46. Axially Chiral Dibenzazepinones by a Palladium(0)-Catalyzed Atropo-enantioselective C-H Arylation10.1002/anie.201806527 ↗
47. Organocatalytic Enantioselective Construction of Chiral Azepine Skeleton Bearing Multiple-Stereogenic Elements10.1002/anie.202108040 ↗
48. Asymmetric synthesis of dibenzo[b,d]azepines by Cu-catalyzed reductive or borylative cyclization10.1039/D1SC04980A ↗
49. Atroposelective Access to 1,3-Oxazepine-Containing Bridged Biaryls via Carbene-Catalyzed Desymmetrization of Imines
50. Diastereo- and Atroposelective Synthesis of Bridged Biaryls Bearing an Eight-Membered Lactone through an Organocatalytic Cascade10.1021/jacs.9b08510 ↗
51. Counterion-Mediated Enantioconvergent Synthesis of Axially Chiral Medium Rings10.1021/jacs.2c05485 ↗
52. Atroposelective Construction of Nine-Membered Carbonate-Bridged Biaryls10.1002/anie.202206501 ↗
53. Ring Closure Reactions of Bifunctional Chain Molecules10.1021/ar00064a001 ↗
54. Metal-Mediated Synthesis of Medium-Sized Rings10.1021/cr990407q ↗
55. Construction of Medium-Sized Rings by Gold Catalysis10.1021/acs.chemrev.0c00793 ↗
56. Recent advances for the catalytic asymmetric construction of medium-sized rings
57. Diastereo- and Enantioselective Silver-Catalyzed [3+3] Cycloaddition and Kinetic Resolution of Azomethine Imines with Activated Isocyanides10.1002/anie.202202679 ↗
58. Simultaneous Construction of C-N Axial and Central Chirality via Silver-Catalyzed Desymmetrizative [3+2] Cycloaddition of Prochiral N-Aryl Maleimides with Activated Isocyanides10.1021/acs.orglett.2c01761 ↗
59. Diastereo- and enantioselective synthesis of biaryl aldehydes bearing both axial and central chirality10.1039/D3CC00708A ↗
60. Isocyanoacetate Derivatives: Synthesis, Reactivity, and Application10.1021/cr900411f ↗
61. To each his own: isonitriles for all flavors. Functionalized isocyanides as valuable tools in organic synthesis10.1039/C6CS00444J ↗
62. Catalytic Enantioselective Isocyanide-Based Reactions: Beyond Passerini and Ugi Multicomponent Reactions10.1002/chem.202003224 ↗
63. A New Family of Cinchona-Derived Amino Phosphine Precatalysts: Application to the Highly Enantio- and Diastereoselective Silver-Catalyzed Isocyanoacetate Aldol Reaction10.1021/ja110534g ↗
64. Highly Diastereo- and Enantioselective Silver-Catalyzed Double [3+2] Cyclization of α-Imino Esters with Isocyanoacetate10.1002/anie.201402788 ↗
65. Catalytic Asymmetric Construction of Axially Chiral Indole-Based Frameworks: An Emerging Area10.1002/chem.202001397 ↗
66. Chiral Pd-Catalyzed Enantioselective Syntheses of Various N-C Axially Chiral Compounds and Their Synthetic Applications10.1021/acs.accounts.0c00767 ↗
67. Asymmetric Synthesis of Axially Chiral C-N Atropisomers
68. Atropisomers beyond the C-C axial chirality: Advances in catalytic asymmetric synthesis10.1016/j.chempr.2022.04.011 ↗
69. Organocatalytic Atroposelective Synthesis of Indole Derivatives Bearing Axial Chirality: Strategies and Applications10.1021/acs.accounts.2c00465 ↗
70. Bayesian methods for the conformational classification of eight-membered rings10.1107/S0108768105023931 ↗
71. Enantioenrichment by Crystallization10.1021/op700239a ↗