Better Together: Photoredox/Copper Dual Catalysis in Atom Transfer Radical Polymerization DOI Creative Commons
Julian Sobieski, Adam Gorczyński, Arman Moini Jazani

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 29, 2024

Abstract Photomediated Atom Transfer Radical Polymerization (photoATRP) is an activator regeneration method, which allows for the controlled synthesis of well‐defined polymers via light irradiation. Traditional photoATRP often limited by need high‐energy ultraviolet or violet light. These could negatively affect control and selectivity polymerization, promote side reactions, may not be applicable to biologically relevant systems. This drawback can circumvented introduction catalytic amount photocatalysts, absorb visible and/or NIR and, therefore, controlled, regenerative ATRP performed with dual‐catalytic cycle. Herein, a critical summary recent developments in field dual‐catalysis concerning Cu‐catalyzed provided. Contributions involved species are examined mechanistically, followed challenges future directions towards next generation advanced functional macromolecular materials.

Language: Английский

Microtiter Plate Immobilization Screening for Prototyping Heterogeneous Enzyme Cascades DOI
Idania L. López, Mercedes Sánchez‐Costa, Alejandro H. Orrego

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(35)

Published: July 22, 2024

Abstract Immobilization is a key enabling technology in applied biocatalysis that facilitates the separation, recovery, and reuse of heterogeneous biocatalysts. However, finding consensus immobilization protocol for several enzymes forming multi‐enzyme system extremely difficult relies on combinatorial trial‐and‐error approach. Herein, we describe which 17 different carriers functionalized with reactive groups are tested 96‐well microtiter plate to screen up 21 protocols 18 enzymes. This screening includes an activity stability assay select optimal chemistry achieve most active stable The information retrieved from can be rationalized using Python‐based application CapiPy. Finally, through scoring results, find assemble immobilized four‐enzyme transform vinyl acetate into ( S )‐3‐hydroxybutyric acid. methodology opens path speed prototyping pathways chemical manufacturing.

Language: Английский

Citations

4
Enhancing lipase enzymatic performance with dynamic covalent dextran-based hydrogels DOI
Meng Sun, Jie Gao, Yingying Zhao

et al.

International Journal of Biological Macromolecules, Journal Year: 2025, Volume and Issue: unknown, P. 141254 - 141254

Published: Feb. 1, 2025

Language: Английский

Citations

0
High-Throughput Screening Identifies Anionic Polymer Supports that Improve Enzyme Activity at Low pH and High Temperature DOI
Evan A. Bisirri, Joel L. Kaar, Daniel K. Schwartz

et al.

Langmuir, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 20, 2025

Elevated temperatures and nonoptimal pH can destabilize enzyme structure or change the protonation state of catalytic residues resulting in attenuated performance. Enzyme immobilization on polymer supports enables fine-tuning highly varied vicinal chemistries to improve performance by promoting correctly folded adjusting local microenvironment more favorable conditions. Herein, we sought investigate how multicomponent random copolymer brushes composed monomers with anionic, cationic, neutral (zwitterionic, mixed-charge), aromatic properties stabilize covalently tethered lipase A fromBacillus subtilis at low high temperature. Polymer brush compositions were screened using a high-throughput approach involving combinatorial synthesis situ characterization immobilized function. Although cationic provided modest improvement over soluble maximum activity thermal stability pH, substantial enhancements observed for anionic zwitterionic supports, increases temperature optima as great 40 °C (from 80 °C) an increase than 300%. These observations counter expectations regarding role surface charge attributed instead preservation due stabilizing electrostatic interactions between negatively charged moieties net positively A. Our findings suggest that stabilization polymers may offset unfavorable changes certain situations, while other situations these effects be synergistic.

Language: Английский

Citations

0
Nanourchin‐like Uricase‐Poly(L‐proline) Conjugate with Retained Enzymatic Activity, Mitigated Immunogenicity, and Sustained Efficacy Upon Repeated Administrations DOI Open Access

Ruichi Zhao,

Yangming Zhang,

Banlai Ruan

et al.

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: March 5, 2025

The poor half-life and strong immunogenicity of proteins such as uricase (UOx), a therapeutic enzyme for chronic refractory gout hyperuricemia, are pressing clinical challenges. Although conjugation poly(ethylene glycol) (PEGylation) UOx can improve the pharmacokinetics, preexisting or induced anti-PEG antibodies, which lead to accelerate blood clearance (ABC) reduced response rate, have been major hurdle. Herein, we report facile "grafting-from" preparation nanourchin-like uricase-poly(L-proline) conjugate, namely UOx-PLP, with high grafting-density, enhanced thermal, lyophilization, freeze-thaw, proteolytic stability. Through transient preblocking strategy in synthesis, UOx-PLP overcomes activity loss retains ~82 % activity. In Sprague-Dawley rats, stimulates minimum complement activation anti-UOx antibodies. Unlike PEG-UOx gave significantly after repetitive administrations, shows no sign ABC effect. Moreover, remain almost unchanged when cross-administrated rats previously received titers Finally, efficacy five straight administrations knock-out hyperuricemia mice model, whereas experiences sharp upon same treatment. Overall, simple outstanding nonclinical results highlight enormous potential future translation.

Language: Английский

Citations

0
Nanourchin‐like Uricase‐Poly(L‐proline) Conjugate with Retained Enzymatic Activity, Mitigated Immunogenicity, and Sustained Efficacy Upon Repeated Administrations DOI Open Access

Ruichi Zhao,

Yangming Zhang,

Banlai Ruan

et al.

Angewandte Chemie, Journal Year: 2025, Volume and Issue: unknown

Published: March 5, 2025

Abstract The poor half‐life and strong immunogenicity of proteins such as uricase (UOx), a therapeutic enzyme for chronic refractory gout hyperuricemia, are pressing clinical challenges. Although conjugation poly(ethylene glycol) (PEGylation) UOx can improve the pharmacokinetics, preexisting or induced anti‐PEG antibodies, which lead to accelerate blood clearance (ABC) reduced response rate, have been major hurdle. Herein, we report facile “grafting‐from” preparation nanourchin‐like uricase‐poly( L ‐proline) conjugate, namely UOx‐PLP, with high grafting‐density, enhanced thermal, lyophilization, freeze‐thaw, proteolytic stability. Through transient preblocking strategy in synthesis, UOx‐PLP overcomes activity loss retains ~82 % activity. In Sprague‐Dawley rats, stimulates minimum complement activation anti‐UOx antibodies. Unlike PEG‐UOx gave significantly after repetitive administrations, shows no sign ABC effect. Moreover, remain almost unchanged when cross‐administrated rats previously received titers Finally, efficacy five straight administrations knock‐out hyperuricemia mice model, whereas experiences sharp upon same treatment. Overall, simple outstanding nonclinical results highlight enormous potential future translation.

Language: Английский

Citations

0
Tailoring polymer architectures to drive molecular sieving in protein-polymer hybrids DOI Creative Commons
Kriti Kapil, Hironobu Murata, Lucca Trachsel

et al.

Sustainable Chemistry and Pharmacy, Journal Year: 2025, Volume and Issue: 45, P. 101988 - 101988

Published: March 14, 2025

Language: Английский

Citations

0
Construction of site-specific immobilized lipase in bio-inspired “rigid and flexible” composite PVIm/ZIF-8 for long-cycle biodiesel synthesis from waste cooking oil DOI
Qian Wang,

Xinyuan Zheng,

Meiling Ge

et al.

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 162208 - 162208

Published: April 1, 2025

Language: Английский

Citations

0
Better Together: Photoredox/Copper Dual Catalysis in Atom Transfer Radical Polymerization DOI Creative Commons
Julian Sobieski, Adam Gorczyński, Arman Moini Jazani

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 29, 2024

Abstract Photomediated Atom Transfer Radical Polymerization (photoATRP) is an activator regeneration method, which allows for the controlled synthesis of well‐defined polymers via light irradiation. Traditional photoATRP often limited by need high‐energy ultraviolet or violet light. These could negatively affect control and selectivity polymerization, promote side reactions, may not be applicable to biologically relevant systems. This drawback can circumvented introduction catalytic amount photocatalysts, absorb visible and/or NIR and, therefore, controlled, regenerative ATRP performed with dual‐catalytic cycle. Herein, a critical summary recent developments in field dual‐catalysis concerning Cu‐catalyzed provided. Contributions involved species are examined mechanistically, followed challenges future directions towards next generation advanced functional macromolecular materials.

Language: Английский

Citations

1
Microtiter Plate Immobilization Screening for Prototyping Heterogeneous Enzyme Cascades DOI
Idania L. López, Mercedes Sánchez‐Costa, Alejandro H. Orrego

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(35)

Published: July 22, 2024

Abstract Immobilization is a key enabling technology in applied biocatalysis that facilitates the separation, recovery, and reuse of heterogeneous biocatalysts. However, finding consensus immobilization protocol for several enzymes forming multi‐enzyme system extremely difficult relies on combinatorial trial‐and‐error approach. Herein, we describe which 17 different carriers functionalized with reactive groups are tested 96‐well microtiter plate to screen up 21 protocols 18 enzymes. This screening includes an activity stability assay select optimal chemistry achieve most active stable The information retrieved from can be rationalized using Python‐based application CapiPy. Finally, through scoring results, find assemble immobilized four‐enzyme transform vinyl acetate into ( S )‐3‐hydroxybutyric acid. methodology opens path speed prototyping pathways chemical manufacturing.

Language: Английский

Citations

0
Better Together: Photoredox/Copper Dual Catalysis in Atom Transfer Radical Polymerization DOI Creative Commons
Julian Sobieski, Adam Gorczyński, Arman Moini Jazani

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 29, 2024

Abstract Photomediated Atom Transfer Radical Polymerization (photoATRP) is an activator regeneration method, which allows for the controlled synthesis of well‐defined polymers via light irradiation. Traditional photoATRP often limited by need high‐energy ultraviolet or violet light. These could negatively affect control and selectivity polymerization, promote side reactions, may not be applicable to biologically relevant systems. This drawback can circumvented introduction catalytic amount photocatalysts, absorb visible and/or NIR and, therefore, controlled, regenerative ATRP performed with dual‐catalytic cycle. Herein, a critical summary recent developments in field dual‐catalysis concerning Cu‐catalyzed provided. Contributions involved species are examined mechanistically, followed challenges future directions towards next generation advanced functional macromolecular materials.

Language: Английский

Citations

0