Multivalent Ce-MOFs as biomimetic laccase nanozyme for environmental remediation

Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 450, P. 138220 - 138220

Published: July 21, 2022

Language: Английский

---

Engineering carbon assimilation in plants

Journal of Integrative Plant Biology, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 9, 2025

Abstract Carbon assimilation is a crucial part of the photosynthetic process, wherein inorganic carbon, typically in form CO 2 , converted into organic compounds by living organisms, including plants, algae, and subset bacteria. Although several carbon fixation pathways have been elucidated, Calvin–Benson–Bassham (CBB) cycle remains fundamental to metabolism, playing pivotal role biosynthesis starch sucrose cyanobacteria. However, Ribulose‐1,5‐bisphosphate carboxylase/oxygenase (RuBisCO), key carboxylase enzyme CBB cycle, exhibits low kinetic efficiency, substrate specificity, high temperature sensitivity, all which potential limit flux through this pathway. Consequently, RuBisCO needs be present at very concentrations, one factors contributing its status as most prevalent protein on Earth. Numerous attempts made optimize catalytic efficiency thereby promote plant growth. Furthermore, limitations process highlight benefits engineering or discovering more efficient mechanisms, either improving itself introducing alternative pathways. Here, we review advances artificial engineering, integration synthetic biology, genetic metabolic pathway optimization, intelligence order create plants capable performing photosynthesis. We additionally provide perspective current challenges solutions alongside personal opinion promising future directions emerging field.

Language: Английский

---

Synthetic prodrug design enables biocatalytic activation in mice to elicit tumor growth suppression

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Jan. 10, 2022

Considering the intrinsic toxicities of transition metals, their incorporation into drug therapies must operate at minimal amounts while ensuring adequate catalytic activity within complex biological systems. As a way to address this issue, study investigates design synthetic prodrugs that are not only tuned be harmless, but can robustly transformed in vivo reach therapeutically relevant levels. To accomplish this, retrosynthetic prodrug highlights potential naphthylcombretastatin-based prodrugs, which form highly active cytostatic agents via sequential ring-closing metathesis and aromatization. Structural adjustments will also done improve aspects related reactivity, bioactivity, hydrolytic stability. The developed therapy is found possess excellent anticancer activities cell-based assays. Furthermore, activation by intravenously administered glycosylated artificial metalloenzymes induce significant reduction implanted tumor growth mice.

Language: Английский

---

Target‐Specific Bioorthogonal Reactions for Precise Biomedical Applications

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(49)

Published: Aug. 7, 2023

Abstract Bioorthogonal chemistry is a promising toolbox for dissecting biological processes in the native environment. Recently, bioorthogonal reactions have attracted considerable attention medical field treating diseases, since this approach may lead to improved drug efficacy and reduced side effects via situ synthesis. For precise biomedical applications, it prerequisite that should occur right locations on appropriate therapeutic targets. In minireview, we highlight design development of targeted treatment. First, compile recent strategies achieving target‐specific reactions. Further, emphasize their application treatment different Finally, perspective provided challenges future directions emerging safe, efficient, translatable disease

Language: Английский

---

A De Novo Metalloenzyme for Cerium Photoredox Catalysis

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(38), P. 25976 - 25985

Published: Aug. 8, 2024

Cerium photoredox catalysis has emerged as a powerful strategy to activate molecules under mild conditions. Radical intermediates are formed using visible light and simple complexes of the earth-abundant lanthanide. Here, we report an artificial photoenzyme enabling this chemistry inside protein. We utilize de novo designed protein scaffold that tightly binds lanthanide ions in its central cavity. Upon visible-light irradiation, cerium-dependent enzyme catalyzes radical C-C bond cleavage 1,2-diols aqueous solution. Protein engineering led variants with improved photostability metal binding behavior. The cleaves range aromatic aliphatic substrates, including lignin surrogates. Surface display on

Language: Английский

---

A Polyoxometalate‐Based Pathologically Activated Assay for Efficient Bioorthogonal Catalytic Selective Therapy

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(32)

Published: June 9, 2023

Since polyoxometalates (POMs) can undergo reversible multi-electron redox transformations, they have been used to modulate the electronic environment of metal nanoparticles for catalysis. Besides, POMs possess unique structures and acid-responsive self-assembly ability. These properties inspired us tackle drawbacks copper-catalyzed azide-alkyne cycloaddition (CuAAC) reaction in biomedical applications, such as low catalytic efficiency unsatisfactory disease selectivity. Herein, we construct molybdenum (Mo)-based POM nanoclusters doped with Cu (Cu-POM NCs) a highly efficient bioorthogonal catalyst, which is responsive pathologicallyacid H2 S selective antibiofilm therapy. Leveraging merits POMs, Cu-POM NCs exhibit biofilm-responsive behavior, CuAAC-mediated situ synthesis antibacterial molecules, NIR-II photothermal effect selectively triggered by pathogens. The consumption bacterial at pathological site extremely decreases number persisterbacteria, conducive inhibition tolerance elimination biofilms. Unlocked sites endowed property, constructed POM-based platform provides new insights into design catalysts

Language: Английский

---

Artificial metalloenzyme assembly in cellular compartments for enhanced catalysis

Nature Chemical Biology, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 8, 2025

Language: Английский

---

Progress, Challenges, and Opportunities with Artificial Metalloenzymes in Biosynthesis

Biochemistry, Journal Year: 2022, Volume and Issue: 62(2), P. 221 - 228

Published: Feb. 23, 2022

In this Perspective, we present progress, outstanding challenges, and opportunities for the incorporation of artificial metalloenzymes (ArMs) into biosynthetic pathways. We first explain discoveries within field ArMs that led to potential inclusion these enzymes in biosynthesis. then describe specific barriers our laboratory, collaboration with laboratories Keasling Mukhopadhyay, addressed establish a pathway containing an ArM. This biosynthesis produced unnatural cyclopropyl terpenoid by combining heterologous production terpene modification its terminal alkene ArM built from cytochrome P450. Finally, remaining challenges related application synthetic biology.

Language: Английский

---

Organometallic catalysis in aqueous and biological environments: harnessing the power of metal carbenes

Chemical Science, Journal Year: 2022, Volume and Issue: 13(22), P. 6478 - 6495

Published: Jan. 1, 2022

Metal-catalyzed carbene transformations can be implemented in aqueous mixtures, and even under the stringent conditions of living cells, provided substrates catalysts are properly tuned to present a good balance between stability reactivity.

Language: Английский

---

Whole-cell-catalyzed hydrogenation/deuteration of aryl halides with a genetically repurposed photodehalogenase

Chem, Journal Year: 2023, Volume and Issue: 9(7), P. 1897 - 1909

Published: April 6, 2023

Language: Английский

---