Palladium-Nanoparticles Biohybrids in Applied Chemistry

Filice, Marco; Losada-Garcia, Noelia; Pérez-Rizquez, Carlos; Marciello, Marzia; Morales, María; Palomo, José M.

doi:10.3390/applnano2010001

Cited by 18 publications

(23 citation statements)

References 33 publications

(39 reference statements)

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“…Although there have been other publications related to plurizyme-like systems, ,− the approaches and the final obtained catalyst were different, resulting in several strategies to tackle a desired cascade process. One of them consisted in the self-assembly of histidine-tyrosine peptides to mimic catalytic microenvironments .…”

Section: Results and Discussionmentioning

confidence: 99%

Structural-Based Modeling in Protein Engineering. A Must Do

et al. 2021

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Biotechnological solutions will be a key aspect in our immediate future society, where optimized enzymatic processes through enzyme engineering might be an important solution for waste transformation, clean energy production, biodegradable materials, and green chemistry, for example. Here we advocate the importance of structural-based bioinformatics and molecular modeling tools in such developments. We summarize our recent experiences indicating a great prediction/success ratio, and we suggest that an early in silico phase should be performed in enzyme engineering studies. Moreover, we demonstrate the potential of a new technique combining Rosetta and PELE, which could provide a faster and more automated procedure, an essential aspect for a broader use.

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Section: Results and Discussionmentioning

confidence: 99%

Structural-Based Modeling in Protein Engineering. A Must Do

et al. 2021

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“…This result showed the relevance of using G@TLL instead of soluble TLL, where the hybrid prepared using the latter contained also high percentage of PdO species (data not shown). 39 ICP-OES experiment determined a Pd content of 2.2% (w/w).…”

Section: Preparation and Characterization Of G@enzyme-cunps Hybridsmentioning

confidence: 99%

“…[30][31][32][33] A recent technology developed by our group has allowed to synthesize nanobiohybrid systems at room temperature in aqueous media where stable, smallsized, monodispersed metallic nanoparticles are in situ synthesized induced by an enzyme scaffold. [34][35][36][37][38][39] In comparison with other methods where metal nanoparticles are directly support on the solid phase, in this strategy enzyme acts a key role in the in situ synthesis of the nanoparticles, controlling their growth (being able to produce nanoparticles with very small size) and morphology. 40 Moreover, the nanoparticles thus synthetized are homogeneously dispersed around protein structure avoiding aggregation problems where this biological matrix conferred an extreme high stability.…”

Section: Introductionmentioning

confidence: 99%

Enzyme-Graphene Nanometal biohybrid Architectures as Highly Efficient Multifunctional Catalysts for Cascade Reactions

Losada-Garcia

Urriolabeitia

Palomo

2022

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The development of new catalytic systems with different chemo- and biocatalytic functionalities for sustainable one-pot multistep transformations represents a big challenge in modern chemistry. Here, we have designed and synthesized novel enzyme-graphene nanometal hybrids of palladium and copper as multiactive heterogeneous catalysts. The in-situ formation of metallic nanoparticles of different size and species on enzymes (C. antartica lipase, CALB and and T. lanuginosus lipase), TLL) immobilized on multilayer graphene-anchored enzymes (G@CALB and G@TLL preparations) at room temperature and aqueous media allowed to create different kind of enzyme-metal nanoarchitectures, containing up to two enzymes and metallic nanoparticles of two different metals in the same compartment. The metallic nanoparticles were synthesized exclusively induced by the enzyme, homogeneously distributed on the enzymatic structure used as scaffold. The cooperative and synergistic participation of different chemo and biocatalytic components in the reduction process and especially in different cascade reactions was demonstrated. Domino cascade in aqueous media (enzymatic hydrolysis, metal reduction, and metal oxidation) was successfully performed from the different hybrid systems. The synthesis of glycoderivatives, transforming selectively peracetylated glucal to novel disaccharides, using G@CALB-Cu3(PO4)2NPs and G@CALB-Cu(0)NPs or α-peracetylated glucose to diacetyl-gluconic acid by G@TLL@CRL-Cu3(PO4)2NPs was successfully performed. Finally, the successful application in the dynamic kinetic resolution of racemic arylamine (>99% conversion and ee) in organic solvent catalyzed by G@CALB-Pd(0)NPs-Cu3(PO4)2NPs demonstrated the potential effect in synthetic chemistry, and the synergistic effect of catalysis between enzyme and metals. Furthermore, recycling studies demonstrated the high robustness of them.

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“…The advantages of using proteins as scaffold of metal nanoparticles are plenty. They stabilize the nanoparticles, can act as in situ reducing agent, produce monodisperse nanoparticles, control the shape and size of NPs and allow to synthetize them in water at room temperature in a more sustainable and "green" way (Benavente et al, 2018a(Benavente et al, , 2018b(Benavente et al, , 2020Cuenca et al, 2016;Filice et al, 2013Filice et al, , 2021Lopez-Tejedor et al, 2018aNaapuri et al, 2022;Palomo, 2019). On the other hand, the fact that the metal nanoparticles are attached to a bigger structure could led to a less activity compared to the free NPs, as different studies evidence (Bastos et al, 2020;Slavin et al, 2017).…”

Section: Introductionmentioning

confidence: 99%

“…In a first approach to evaluate the antimicrobial capacity of new bionanohybrids, the use of model reactions can be useful to get an idea of their behaviour before performing antimicrobial assays. In this way, model reactions based on oxidation of p-aminophenol and the reduction of p-nitrophenol, which have previously been studied in the laboratory, can be used for such purposes (Benavente et al, 2018b;Filice et al, 2021;Losada-Garcia et al, 2021;Palomo, 2019). It should be stressed that ROS mechanism, based on radicals generation, can be emulated through the Fenton oxidation reaction of paminophenol.…”

Section: Introductionmentioning

confidence: 99%

Design and synthesis of new nanobiomaterials with antimicrobial properties

Ortega-Nieto

Losada-Garcia

Pessela

et al. 2022

Preprint

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In this work, new nanostructured copper materials have been designed, synthetized and evaluated in order to produce a more efficient and sustainable copper bionanohybrid with catalytical and antimicrobial properties. Thus, conditions are sought where the most critical steps are reduced or minimized, such as the use of reducing agents or the cryogenization step. In addition, the new materials have been characterized through different techniques and their oxidative and reductive capacity has been evaluated, as well as their antimicrobial activity. We demonstrate that the addition of different quantities of reducing agent in the synthesis method generates copper bionanohybrids with different metallic species, nanoparticles sizes and morphologies (spherical, nanorod, nanowires structures) , and antimicrobial activity. The antimicrobial properties of the bionanohybrids were studied against two different strain of bacteria, Escherichia coli and Bacillus subtilis, through two different methods: by counting the CFU and via disk diffusion test, respectively. In both cases, Cu-PHOS-100%R, with the highest percentage of reducing agent, was the most efficient, achieving a MIC value against B. subtilis of 125 µg/mL and an E. coli percentage reduction of 95% in 4h. Notable results were also obtained with the bionanohybrids with lowest reduction percentages, such as Cu-PHOS-10%R, which showed a MIC of 250 µg/mL and a bacteria reduction of 82%.

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Palladium-Nanoparticles Biohybrids in Applied Chemistry

Cited by 18 publications

References 33 publications

Structural-Based Modeling in Protein Engineering. A Must Do

Structural-Based Modeling in Protein Engineering. A Must Do

Enzyme-Graphene Nanometal biohybrid Architectures as Highly Efficient Multifunctional Catalysts for Cascade Reactions

Design and synthesis of new nanobiomaterials with antimicrobial properties

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