Pnictogen‐Bonding Enzymes DOI Creative Commons
Giacomo Renno, Dongping Chen, Qingxia Zhang

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(45)

Published: July 5, 2024

Abstract The objective of this study was to create artificial enzymes that capitalize on pnictogen bonding, a σ‐hole interaction is essentially absent in biocatalysis. For purpose, stibine catalysts were equipped with biotin derivative and combined streptavidin mutants identify an efficient transfer hydrogenation catalyst for the reduction fluorogenic quinoline substrate. Increased catalytic activity from wild‐type best coincides depth σ hole Sb(V) center, emergence saturation kinetic behavior. Michaelis–Menten analysis reveals transition‐state recognition low micromolar range, more than three orders magnitude stronger millimolar substrate recognition. Carboxylates preferred by contribute hydrogen‐bonded ion pairing anion‐π interactions emerging pyridinium product. challenging stereoselectivity aqueous systems further emphasizes compatibility bonding higher order catalysis.

Language: Английский

Proline Analogues DOI
Vladimir Kubyshkin, Marina Rubini

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(13), P. 8130 - 8232

Published: June 28, 2024

Within the canonical repertoire of amino acid involved in protein biogenesis, proline plays a unique role as an presenting modified backbone rather than side-chain. Chemical structures that mimic but introduce changes into its specific molecular features are defined analogues. This review article summarizes existing chemical, physicochemical, and biochemical knowledge about this peculiar family structures. We group analogues from following compounds: substituted prolines, unsaturated fused structures, ring size homologues, heterocyclic, e.g., pseudoproline, bridged proline-resembling overview (1) occurrence nature their chemical synthesis, (2) physicochemical properties including conformation

Language: Английский

Citations

10

Pnictogen‐Bonding Enzymes DOI Creative Commons
Giacomo Renno, Dongping Chen, Qingxia Zhang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(45)

Published: July 5, 2024

Abstract The objective of this study was to create artificial enzymes that capitalize on pnictogen bonding, a σ‐hole interaction is essentially absent in biocatalysis. For purpose, stibine catalysts were equipped with biotin derivative and combined streptavidin mutants identify an efficient transfer hydrogenation catalyst for the reduction fluorogenic quinoline substrate. Increased catalytic activity from wild‐type best coincides depth σ hole Sb(V) center, emergence saturation kinetic behavior. Michaelis–Menten analysis reveals transition‐state recognition low micromolar range, more than three orders magnitude stronger millimolar substrate recognition. Carboxylates preferred by contribute hydrogen‐bonded ion pairing anion‐π interactions emerging pyridinium product. challenging stereoselectivity aqueous systems further emphasizes compatibility bonding higher order catalysis.

Language: Английский

Citations

4

Noncanonical Amino Acids: Bringing New-to-Nature Functionalities to Biocatalysis DOI Creative Commons
Bart Brouwer, Franco Della‐Felice, Jan Hendrik Illies

et al.

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(19), P. 10877 - 10923

Published: Sept. 27, 2024

Biocatalysis has become an important component of modern organic chemistry, presenting efficient and environmentally friendly approach to synthetic transformations. Advances in molecular biology, computational modeling, protein engineering have unlocked the full potential enzymes various industrial applications. However, inherent limitations natural building blocks sparked a revolutionary shift.

Language: Английский

Citations

4

Enzymatic Synthesis of Saturated Bioisosteres of Ortho‐Substituted Benzenes by Artificial Photoenzyme DOI Open Access
Yuting Bai, Yi-yun Sheng, Yi Fu

et al.

Chemistry - A European Journal, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 17, 2025

Saturated bioisosteres of ortho-substituted benzenes are significant interest due to their enhanced pharmacokinetic properties, such as improved metabolic stability and reduced toxicity, making them valuable in drug design development. However, efficient synthesis remains a challenge organic chemistry. Herein, we report the biocatalytic saturated using engineered artificial photoenzymes. The photoenzyme, incorporating genetically encoded unnatural amino acids with benzophenone photosensitizer residue, facilitate formation chiral moderate enantiomeric excess via energy transfer process. Our results demonstrate versatility photoenzymes mediating new-to-nature reactions that difficult achieve conventional chemical or enzymatic methods.

Language: Английский

Citations

0

Design and Evolution of an Artificial Friedel–Crafts Alkylation Enzyme Featuring an Organoboronic Acid Residue DOI

Shu‐Bin Mou,

Kai‐Yue Chen,

Thittaya Kunthic

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(39), P. 26676 - 26686

Published: Aug. 27, 2024

Creating artificial enzymes by the genetic incorporation of noncanonical amino acids with catalytic side chains would expand enzyme chemistries that have not been discovered in nature. Here, we report design an uses

Language: Английский

Citations

2

Pnictogen‐Bonding Enzymes DOI Creative Commons
Giacomo Renno, Dongping Chen, Qingxia Zhang

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(45)

Published: July 5, 2024

Abstract The objective of this study was to create artificial enzymes that capitalize on pnictogen bonding, a σ‐hole interaction is essentially absent in biocatalysis. For purpose, stibine catalysts were equipped with biotin derivative and combined streptavidin mutants identify an efficient transfer hydrogenation catalyst for the reduction fluorogenic quinoline substrate. Increased catalytic activity from wild‐type best coincides depth σ hole Sb(V) center, emergence saturation kinetic behavior. Michaelis–Menten analysis reveals transition‐state recognition low micromolar range, more than three orders magnitude stronger millimolar substrate recognition. Carboxylates preferred by contribute hydrogen‐bonded ion pairing anion‐π interactions emerging pyridinium product. challenging stereoselectivity aqueous systems further emphasizes compatibility bonding higher order catalysis.

Language: Английский

Citations

1