Identification and Directed Development of Non‐Organic Catalysts with Apparent Pan‐Enzymatic Mimicry into Nanozymes for Efficient Prodrug Conversion

Walther, Raoul; Winther, Anna K.; Fruergaard, Anne Sofie; Akker, Wouter van den; Sørensen, Lise; Nielsen, Signe Maria; Olesen, Morten T. Jarlstad; Dai, Yitao; Jeppesen, Henrik S.; Lamagni, Paolo; Savateev, Aleksandr; Pedersen, Søren Lykke; Riber, Camilla Frich; Vigier‐Carrière, Cécile; Lock, Nina; Singh, Mandeep; Bansal, Vipul; Meyer, Rikke Louise; Zelikin, Alexander N.

doi:10.1002/anie.201812668

Cited by 65 publications

(48 citation statements)

References 25 publications

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“…We have previously reported on the structural instability of trenH-SnS-1 upon dispersion in water (Hvid et al, 2017). The crystalline structure of the thiostannate transforms to an amorphous phase in aqueous solution within 1 h. Similar structural instability has been observed for the compound AEPz-SnS-1 [AEPz = 1-(2-aminoethyl)piperazine; Walther et al, 2019], which is structurally closely related to trenH-SnS-1. However, the chemical nature of the amorphous products has not previously been studied, and the phase transition is poorly understood.…”

Section: àsupporting

confidence: 58%

“…the c axis, is strikingly similar in the two compounds, as it is 19.2195 (5) and 19.0860 (8) Å for AEPz-SnS-1 and trenH-SnS-1, respectively, according to Le Bails refinements of the pristine compound PXRD data ( Fig. S1) (Filsø et al, 2017;Walther et al, 2019). Solid-state NMR has furthermore confirmed the incorporation of AEPz into the structure (Fig.…”

Section: àmentioning

confidence: 61%

“…Synthesis of AEPz-SnS-1. AEPz-SnS-1 was recently reported (Walther et al, 2019). Herein, we synthesized the compound using a slightly modified two-step solvothermal protocol to minimize SnO 2 impurities.…”

Section: Synthesismentioning

confidence: 99%

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Structural changes during water-mediated amorphization of semiconducting two-dimensional thiostannates

Hvid

Jeppesen

Miola

et al. 2019

Int Union Crystallogr J

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Owing to their combined open-framework structures and semiconducting properties, two-dimensional thiostannates show great potential for catalytic and sensing applications. One such class of crystalline materials consists of porous polymeric [Sn3S7 2−] n sheets with molecular cations embedded in-between. The compounds are denoted R-SnS-1, where R is the cation. Dependent on the cation, some R-SnS-1 thiostannates transition into amorphous phases upon dispersion in water. Knowledge about the fundamental chemical properties of the thiostannates, including their water stability and the nature of the amorphous products, has not yet been established. This paper presents a time-resolved study of the transition from the crystalline to the amorphous phase of two violet-light absorbing thiostannates, i.e. AEPz-SnS-1 [AEPz = 1-(2-aminoethyl)piperazine] and trenH-SnS-1 [tren = tris(2-aminoethyl)amine]. X-ray total scattering data and pair distribution function analysis reveal no change in the local intralayer coordination during the amorphization. However, a rapid decrease in the crystalline domain sizes upon suspension in water is demonstrated. Although scanning electron microscopy shows no significant decrease of the micrometre-sized particles, transmission electron microscopy reveals the formation of small particles (∼200–400 nm) in addition to the larger particles. The amorphization is associated with disorder of the thiostannate nanosheet stacking. For example, an average decrease in the interlayer distance (from 19.0 to 15.6 Å) is connected to the substantial loss of the organic components as shown by elemental analysis and X-ray photoelectron spectroscopy. Despite the structural changes, the light absorption properties of the amorphisized R-SnS-1 compounds remain intact, which is encouraging for future water-based applications of such materials.

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Section: àsupporting

confidence: 58%

Section: àmentioning

confidence: 61%

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Structural changes during water-mediated amorphization of semiconducting two-dimensional thiostannates

Hvid

Jeppesen

Miola

et al. 2019

Int Union Crystallogr J

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“…[ 4a,5 ] In our own recent work, we identified an unexpected activity of nanozymes in conversion of glucuronide prodrugs into the corresponding therapeutics. [ 6 ] The importance of our findings was that glucuronides are privileged prodrugs in medicinal chemistry [ 7 ] and the discovery of glucuronidase‐like activity of nanozymes offered opportunities to achieve localized drug synthesis using biocompatible, natural metabolites and drug precursors. [ 6 ] From a different perspective, our finding was significant in uncovering a novel mode of nanozyme‐based mimicry, namely glycosidase mimicry.…”

Section: Introductionmentioning

confidence: 99%

“…[ 6 ] The importance of our findings was that glucuronides are privileged prodrugs in medicinal chemistry [ 7 ] and the discovery of glucuronidase‐like activity of nanozymes offered opportunities to achieve localized drug synthesis using biocompatible, natural metabolites and drug precursors. [ 6 ] From a different perspective, our finding was significant in uncovering a novel mode of nanozyme‐based mimicry, namely glycosidase mimicry. Nevertheless, one fundamentally important question has not been considered: do nanozymes exhibit mimicry of glucuronidase by mechanism?…”

Section: Introductionmentioning

confidence: 99%

Nanozymes and Glucuronides: Glucuronidase, Esterase, and/or Transferase Activity

Walther

Akker

Fruergaard

et al. 2020

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Nanozymes are fundamentally interesting catalysts that are investigated as alternatives to fragile protein‐enzymes for applications in biotechnology, for prodrug activation, and use in biomedicine, as well as the catalysts that contributed to the Origin of Life. However, until now, nanozymes mostly have been documented to exhibit activity as red/ox catalysts, whereas examples of activity outside this broad class of reactions are very few. Herein, activity of nanozymes on glucuronide prodrugs is investigated, specifically focusing on the mechanism of prodrug conversion reactions. The main finding of this work is that nanozymes exhibit glucuronide‐like activity, but also catalyze prodrug conversion via esterase‐like mechanism and facilitate group transfer reactions.

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Application of Drug Delivery System Based on Nanozyme Cascade Technology in Chronic Wound

Wang,

Li,

Liu

et al. 2024

Adv Healthcare Materials

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Chronic wounds are characterized by long‐term inflammation, including diabetic ulcers, traumatic ulcers, etc., which provide an optimal environment for bacterial proliferation. At present, antibiotics are the main clinical treatment method for chronic wound infections. However, the overuse of antibiotics may accelerate the emergence of drug‐resistant bacteria, which poses a significant threat to human health. Therefore, there is an urgent need to develop new therapeutic strategies for bacterial infections. Nanozyme‐based antimicrobial therapy (NABT) is an emerging antimicrobial strategy with broad‐spectrum activity and low drug resistance compared to traditional antibiotics. NABT has shown great potential as an emerging antimicrobial strategy by catalyzing the generation of reactive oxygen species (ROS) with its enzyme‐like catalytic properties, producing a powerful bactericidal effect without developing drug resistance. Nanozyme‐based cascade antimicrobial technology offers a new approach to infection control, effectively improving antimicrobial efficacy by activating cascades against bacterial cell membranes and intracellular DNA while minimizing potential side effects. However, it is worth noting that this technology is still in the early stages of research. This article comprehensively reviews wound classification, current methods for the treatment of wound infection, different types of nanozymes, the application of nanozyme cascade reaction technology in antimicrobial therapy, and future challenges and prospects.

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Identification and Directed Development of Non‐Organic Catalysts with Apparent Pan‐Enzymatic Mimicry into Nanozymes for Efficient Prodrug Conversion

Abstract: Identification and directed development of non-organic catalysts with apparent pan-enzymatic mimicry into nanozymes for efficient prodrug conversion

Cited by 65 publications

References 25 publications

Structural changes during water-mediated amorphization of semiconducting two-dimensional thiostannates

Structural changes during water-mediated amorphization of semiconducting two-dimensional thiostannates

Nanozymes and Glucuronides: Glucuronidase, Esterase, and/or Transferase Activity

Application of Drug Delivery System Based on Nanozyme Cascade Technology in Chronic Wound

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