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Thematische Bibliographien / Catalyse bioinspirée / Zeitschriftenartikel

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Zeitschriftenartikel zum Thema „Catalyse bioinspirée“

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Veröffentlicht am 23. November 2024

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1

Carrión, Erik N., Andrei Loas, Hemantbhai H. Patel, Marius Pelmuş, Karpagavalli Ramji und Sergiu M. Gorun. „Fluoroalkyl phthalocyanines: Bioinspired catalytic materials“. Journal of Porphyrins and Phthalocyanines 22, Nr. 05 (17.04.2018): 371–97. http://dx.doi.org/10.1142/s1088424618500189.

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The design of self oxidation-resistant catalytic materials based on organic molecules, although advantageous due to the ability to control their structures, is limited by the presence of labile C–H bonds. This mini review summarizes recent work aimed at first-row transition metal complexes of a new class of coordinating ligands, fluoroalkyl-substituted fluorophthalocyanines, R[Formula: see text]Pcs, ligands in which all, or the majority of their C–H bonds are replaced by a combination of fluoro- and perfluoroalkyl groups yielding porphyrin-bioinspired catalyst models. In the case of homogeneous systems, cobalt(II) complexes catalyze the aerobic oxidation of thiols to disulfides, a reaction of both biological significance and industrial importance. Zinc(II) complexes photo-generate excited state singlet oxygen, [Formula: see text]O[Formula: see text], resulting in both the incorporation of O[Formula: see text] in C–H bonds or, depending on the reaction parameters, oxidation of dyes, model pollutants. Catalyst heterogenization using oxidic and other supports yields stable, active hybrid materials. Functionalized R[Formula: see text]Pcs with acidic (–COOH) or basic (–NH[Formula: see text]R[Formula: see text], [Formula: see text] 2) groups exhibit scaffolds that afford both conjugation with biological vectors for theranostic applications as well as solid-supported materials with superior stability. Electrodes modified with hybrid R[Formula: see text]Pc-containing supports have also been used in photo-oxidations, replacing enzymes and H[Formula: see text]O[Formula: see text] associated reagents with a combination of light and air. An analytical device employed for the nano-level detection of environmentally deleterious antibiotics has been constructed.

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Chen, Jing, Yingchun Guo, Tengteng Kang, Xingchi Liu, Xiaomei Wang und Xu Zhang. „In Situ Growth of ZIF-8 Nanocrystals on the Pore Walls of 3D Ordered Macroporous TiO2 for a One-Pot Cascade Reaction“. Catalysts 11, Nr. 5 (21.04.2021): 533. http://dx.doi.org/10.3390/catal11050533.

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It is wise to mimic a bioinspired system to design a nanoreactor as a catalyst containing multiple components for a cascade reaction. Here, we report the uniform growth of well-dispersed nano-scale ZIF-8 crystals on the pore walls of 3DOM TiO2 via the TEA-assisted crystallization process. The UV-vis spectra indicate that the ZIF-8 photosensitizer can extend the visible-light absorption of 3DOM TiO2. The obtained nanoreactor can efficiently catalyze the one-pot aromatic alcohol oxidization and Knoevenagel condensation cascade reaction for larger molecules. This work offers an important strategy for preparing semiconductor–MOF multifunctional composites with a spatially separated compartmentation for the cascade reaction.

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3

Monkcom, Emily C., Pradip Ghosh, Emma Folkertsma, Hidde A. Negenman, Martin Lutz und Robertus J. M. Klein Gebbink. „Bioinspired Non-Heme Iron Complexes: The Evolution of Facial N, N, O Ligand Design“. CHIMIA International Journal for Chemistry 74, Nr. 6 (24.06.2020): 450–66. http://dx.doi.org/10.2533/chimia.2020.450.

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Iron-containing metalloenzymes that contain the 2-His-1-Carboxylate facial triad at their active site are well known for their ability to activate molecular oxygen and catalyse a broad range of oxidative transformations. Many of these reactions are synthetically challenging, and developing small molecular iron-based catalysts that can achieve similar reactivity and selectivity remains a long-standing goal in homogeneous catalysis. This review focuses on the development of bioinspired facial N,N,O ligands that model the 2-His-1-Carboxylate facial triad to a greater degree of structural accuracy than many of the polydentate N-donor ligands commonly used in this field. By developing robust, well-defined N,N,O facial ligands, an increased understanding could be gained of the factors governing enzymatic reactivity and selectivity.

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4

Nothling, Mitchell D., Zeyun Xiao, Nicholas S. Hill, Mitchell T. Blyth, Ayana Bhaskaran, Marc-Antoine Sani, Andrea Espinosa-Gomez et al. „A multifunctional surfactant catalyst inspired by hydrolases“. Science Advances 6, Nr. 14 (April 2020): eaaz0404. http://dx.doi.org/10.1126/sciadv.aaz0404.

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The remarkable power of enzymes to undertake catalysis frequently stems from their grouping of multiple, complementary chemical units within close proximity around the enzyme active site. Motivated by this, we report here a bioinspired surfactant catalyst that incorporates a variety of chemical functionalities common to hydrolytic enzymes. The textbook hydrolase active site, the catalytic triad, is modeled by positioning the three groups of the triad (-OH, -imidazole, and -CO2H) on a single, trifunctional surfactant molecule. To support this, we recreate the hydrogen bond donating arrangement of the oxyanion hole by imparting surfactant functionality to a guanidinium headgroup. Self-assembly of these amphiphiles in solution drives the collection of functional headgroups into close proximity around a hydrophobic nano-environment, affording hydrolysis of a model ester at rates that challenge α-chymotrypsin. Structural assessment via NMR and XRD, paired with MD simulation and QM calculation, reveals marked similarities of the co-micelle catalyst to native enzymes.

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Guo, Hao, Yu-Fei Ao, De-Xian Wang und Qi-Qiang Wang. „Bioinspired tetraamino-bisthiourea chiral macrocycles in catalyzing decarboxylative Mannich reactions“. Beilstein Journal of Organic Chemistry 18 (02.05.2022): 486–96. http://dx.doi.org/10.3762/bjoc.18.51.

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A series of tetraamino-bisthiourea chiral macrocycles containing two diarylthiourea and two chiral diamine units were synthesized by a fragment-coupling approach in high yields. Different chiral diamine units, including cyclohexanediamines and diphenylethanediamines were readily incorporated by both homo and hetero [1 + 1] macrocyclic condensation of bisamine and bisisothiocyanate fragments. With the easy synthesis, gram-scale of macrocycle products can be readily obtained. These chiral macrocycles were applied in catalyzing bioinspired decarboxylative Mannich reactions. Only 5 mol % of the optimal macrocycle catalyst efficiently catalyzed the decarboxylative addition of a broad scope of malonic acid half thioesters to isatin-derived ketimines with excellent yields and good enantioselectivity. The rigid macrocyclic framework and the cooperation between the thiourea and tertiary amine sites were found to be crucial for achieving efficient activation and stereocontrol. As shown in control experiments, catalysis with the acyclic analogues having the same structural motifs were non-selective.

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6

Gao, Bin, Tao Wang, Yang Li, Xiaoli Fan, Hao Gong, Cheng Jiang, Peng Li, Xianli Huang und Jianping He. „Promoting hole transfer for photoelectrochemical water oxidation through a manganese cluster catalyst bioinspired by natural photosystem II“. Chemical Communications 56, Nr. 30 (2020): 4244–47. http://dx.doi.org/10.1039/d0cc00955e.

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7

Deuss, Peter J., René den Heeten, Wouter Laan und Paul C. J. Kamer. „Bioinspired Catalyst Design and Artificial Metalloenzymes“. Chemistry - A European Journal 17, Nr. 17 (23.03.2011): 4680–98. http://dx.doi.org/10.1002/chem.201003646.

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8

Hunter, R. D., J. Davies, S. J. A. Hérou, A. Kulak und Z. Schnepp. „Milling as a route to porous graphitic carbons from biomass“. Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences 379, Nr. 2209 (13.09.2021): 20200336. http://dx.doi.org/10.1098/rsta.2020.0336.

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This paper reports a simple way to produce porous graphitic carbons from a wide range of lignocellulosic biomass sources, including nut shells, softwood sawdust, seed husks and bamboo. Biomass precursors are milled and sieved to produce fine powders and are then converted to porous graphitic carbons by iron-catalysed graphitization. Graphitizing the raw (unmilled) biomass creates carbons that are diverse in their porosity and adsorption properties. This is due to the inability of the iron catalyst precursor to penetrate the structure of dense biomass material. Milling enables much more efficient impregnation of the biomass and produces carbons with homogeneous properties. Lignocellulosic biomass (particularly waste biomass) is an attractive precursor to technologically important porous graphitic carbons as it is abundant and renewable. This simple method for preparing the biomass enables a wide range of biomass sources to be used to produce carbons with homogeneous properties. This article is part of the theme issue ‘Bio-derived and bioinspired sustainable advanced materials for emerging technologies (part 2)’.

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9

Sankar Agarwalla, Uday. „Bioinspired Non-heme Diiron Catalysts for Olefin Epoxidation with Hydrogen Peroxide in the Presence of Acetic Acid“. International Journal of Science and Research (IJSR) 11, Nr. 4 (05.04.2022): 1089–93. http://dx.doi.org/10.21275/sr22403000114.

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10

Phillips, Katherine R., Grant T. England, Steffi Sunny, Elijah Shirman, Tanya Shirman, Nicolas Vogel und Joanna Aizenberg. „A colloidoscope of colloid-based porous materials and their uses“. Chemical Society Reviews 45, Nr. 2 (2016): 281–322. http://dx.doi.org/10.1039/c5cs00533g.

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11

Mangiavacchi, Francesca, Letizia Crociani, Luca Sancineto, Francesca Marini und Claudio Santi. „Continuous Bioinspired Oxidation of Sulfides“. Molecules 25, Nr. 11 (11.06.2020): 2711. http://dx.doi.org/10.3390/molecules25112711.

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A simple, efficient, and selective oxidation under flow conditions of sulfides into their corresponding sulfoxides and sulfones is reported herein, using as a catalyst perselenic acid generated in situ by the oxidation of selenium (IV) oxide in a diluted aqueous solution of hydrogen peroxide as the final oxidant. The scope of the proposed methodology was investigated using aryl alkyl sulfides, aryl vinyl sulfides, and dialkyl sulfides as substrates, evidencing, in general, a good applicability. The scaled-up synthesis of (methylsulfonyl)benzene was also demonstrated, leading to its gram-scale preparation.

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12

Bhattacharya, Priyanka, Dan Du und Yuehe Lin. „Bioinspired nanoscale materials for biomedical and energy applications“. Journal of The Royal Society Interface 11, Nr. 95 (06.06.2014): 20131067. http://dx.doi.org/10.1098/rsif.2013.1067.

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The demand for green, affordable and environmentally sustainable materials has encouraged scientists in different fields to draw inspiration from nature in developing materials with unique properties such as miniaturization, hierarchical organization and adaptability. Together with the exceptional properties of nanomaterials, over the past century, the field of bioinspired nanomaterials has taken huge leaps. While on the one hand, the sophistication of hierarchical structures endows biological systems with multi-functionality, the synthetic control on the creation of nanomaterials enables the design of materials with specific functionalities. The aim of this review is to provide a comprehensive, up-to-date overview of the field of bioinspired nanomaterials, which we have broadly categorized into biotemplates and biomimics. We discuss the application of bioinspired nanomaterials as biotemplates in catalysis, nanomedicine, immunoassays and in energy, drawing attention to novel materials such as protein cages. Furthermore, the applications of bioinspired materials in tissue engineering and biomineralization are also discussed.

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13

Kung, Mayfair C., Mark V. Riofski, Michael N. Missaghi und Harold H. Kung. „Organosilicon platforms: bridging homogeneous, heterogeneous, and bioinspired catalysis“. Chem. Commun. 50, Nr. 25 (2014): 3262–76. http://dx.doi.org/10.1039/c3cc48766k.

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Organosilicon compounds form versatile structures such as cubic metallasiloxanes, cage-like silsesquioxanes, macromolecular nanocages, and flexible dendrimers and linear metallasiloxanes, and are useful as catalysts, ligands for metal complexes, and catalyst supports.

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14

Ren, Changxu, Peng Yang, Jiaonan Sun, Eric Y. Bi, Jinyu Gao, Jacob Palmer, Mengqiang Zhu, Yiying Wu und Jinyong Liu. „A Bioinspired Molybdenum Catalyst for Aqueous Perchlorate Reduction“. Journal of the American Chemical Society 143, Nr. 21 (18.05.2021): 7891–96. http://dx.doi.org/10.1021/jacs.1c00595.

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15

Deuss, Peter J., Rene den Heeten, Wouter Laan und Paul C. J. Kamer. „ChemInform Abstract: Bioinspired Catalyst Design and Artificial Metalloenzymes“. ChemInform 42, Nr. 31 (07.07.2011): no. http://dx.doi.org/10.1002/chin.201131266.

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16

Fogeron, Thibault, Jean-Philippe Porcher, Maria Gomez-Mingot, Tanya K. Todorova, Lise-Marie Chamoreau, Caroline Mellot-Draznieks, Yun Li und Marc Fontecave. „A cobalt complex with a bioinspired molybdopterin-like ligand: a catalyst for hydrogen evolution“. Dalton Transactions 45, Nr. 37 (2016): 14754–63. http://dx.doi.org/10.1039/c6dt01824f.

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A cobalt complex using a bioinspired ligand, that mimics the molybdopterin cofactor, displays very good activity for electrochemical proton reduction in terms of turnover frequency, faradic yields and stability.

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17

Zucca, Paolo, Gianmarco Cocco, Manuela Pintus, Antonio Rescigno und Enrico Sanjust. „Biomimetic Sulfide Oxidation by the Means of Immobilized Fe(III)-5,10,15,20-tetrakis(pentafluorophenyl)porphin under Mild Experimental Conditions“. Journal of Chemistry 2013 (2013): 1–7. http://dx.doi.org/10.1155/2013/651274.

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This paper describes the oxidation of inorganic sulfide to sulfate, minimizing the formation of elemental sulfur. The described catalytic reaction uses dilute hydrogen peroxide at nearly neutral pH values in the presence of a bioinspired, heterogenized, and commercial ferriporphin. A substantial increase of the percentage of sulfide converted to sulfate is obtained in comparison with the yields obtained when working with hydrogen peroxide alone. The biomimetic catalyst also proved to be a much more efficient catalyst than horseradish peroxidase. Accordingly, it could be suitable for large-scale applications. Further studies are in progress to drive sulfate yields up to nearly quantitative.

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18

He, Fei, Li Mi, Yanfei Shen, Xinghua Chen, Yiran Yang, Hao Mei, Songqin Liu, Toshiyuki Mori und Yuanjian Zhang. „Driving electrochemical oxygen reduction and hydrazine oxidation reaction by enzyme-inspired polymeric Cu(3,3′-diaminobenzidine) catalyst“. Journal of Materials Chemistry A 5, Nr. 33 (2017): 17413–20. http://dx.doi.org/10.1039/c7ta05183b.

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19

Farooq, Umera, Muhammad Fiaz, Hina Nawaz, Kashif Abdullah, Zahid Asghar Bajwa, Roman Azeem, Shumaila Ashraf und Muhammad Sharjeel. „Bioinspired Synthesis of Novel Different Nanoparticles and its Utility in Biodiesel and Animals Applications“. Haya: The Saudi Journal of Life Sciences 9, Nr. 10 (16.10.2024): 390–96. http://dx.doi.org/10.36348/sjls.2024.v09i10.003.

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Because of its ability to speed up the reaction, the catalyst is critical to its success. Most catalysts are either homogeneous or heterogeneous. It has been shown that utilizing a heterogeneous catalyst, which is easier to remove from the product after the reaction has been finished. Because of the large surface area of the Nano-catalyst results in high catalytic efficiency. To enhance the performance of catalysts a range of various types of support materials have been used. SO42--ZnO and So42-/TiO active acid catalyst was prepared and characterized. ZnO nanoparticles catalyst synthesized by precipitation of zinc nitrate for comparison with supported catalyst. Sulphated zinc oxide (SO42--ZnO) and sulphated titania (SO42-/TiO) catalysts were synthesized using impregnation methods, to test their efficacy in biodiesel production. Various waste oils from different wastes such as mutton or beef tallow, chicken fat, and methanol are preferred to use during the esterification of waste animal fat oils using solid acid catalysts to produce biodiesel. Biodiesel synthesis generates a substantial amount of glycerol as a byproduct. Effect of optimum parameters such as temperature 60 degree centigrade (°C) shown 90% yield, time 1 hour resulted in 85% yield, catalyst dose 2wt% resulted in 80% yield, stirring speed 250rpm resulted in 80% yield, methanol to oil ratio12:1 resulted as 85.5% yield for transesterification of waste fat oil. It is valuable that the supported acid catalysts showed more yield than simply synthesized ZnO nanocatalyst similarly sulphated zinc oxide showed more FAME yield than sulphated titania.

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Bour, James R., Ashley M. Wright, Xin He und Mircea Dincă. „Bioinspired chemistry at MOF secondary building units“. Chemical Science 11, Nr. 7 (2020): 1728–37. http://dx.doi.org/10.1039/c9sc06418d.

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21

Chaignon, Jérémy, Marie Gourgues, Lhoussain Khrouz, Nicolás Moliner, Laurent Bonneviot, Fabienne Fache, Isabel Castro und Belén Albela. „A bioinspired heterogeneous catalyst based on the model of the manganese-dependent dioxygenase for selective oxidation using dioxygen“. RSC Advances 7, Nr. 28 (2017): 17336–45. http://dx.doi.org/10.1039/c7ra00514h.

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22

Signorella, Sandra, und Christelle Hureau. „Bioinspired functional mimics of the manganese catalases“. Coordination Chemistry Reviews 256, Nr. 11-12 (Juni 2012): 1229–45. http://dx.doi.org/10.1016/j.ccr.2012.02.003.

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23

Tibbetts, Isobel, und George Kostakis. „Recent Bio-Advances in Metal-Organic Frameworks“. Molecules 25, Nr. 6 (12.03.2020): 1291. http://dx.doi.org/10.3390/molecules25061291.

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Metal-organic frameworks (MOFs) have found uses in adsorption, catalysis, gas storage and other industrial applications. Metal Biomolecule Frameworks (bioMOFs) represent an overlap between inorganic, material and medicinal sciences, utilising the porous frameworks for biologically relevant purposes. This review details advances in bioMOFs, looking at the synthesis, properties and applications of both bioinspired materials and MOFs used for bioapplications, such as drug delivery, imaging and catalysis, with a focus on examples from the last five years.

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Largeron, Martine. „Aerobic catalytic systems inspired by copper amine oxidases“. Pure and Applied Chemistry 92, Nr. 2 (25.02.2020): 233–42. http://dx.doi.org/10.1515/pac-2019-0107.

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AbstractThe goal of sustainable development has been accepted as a common policy in current society. In response to this challenge, the development of green processes which utilize environmentally benign oxidants, reduce chemical waste and handling costs, is highly desirable. Given the widespread importance of imines as pivotal synthetic intermediates and essential pharmacophores in numerous biologically active compounds, various catalytic methods allowing the aerobic oxidation of amines to imines have been developed. Recently, noticeable progress has arisen from the discovery of various quinone-based catalytic systems, inspired by copper amine oxidase enzymes (CuAOs), which are able to reproduce the selectivity of CuAOs for primary amines and even to expand the amine substrates scope. However, the need for synthesizing these catalysts prior use adversely affects the economics as well as the eco-friendly nature of the method. To surpass these drawbacks, the “second-order” biomimicry idea has been recently advanced to describe a system in which in situ modification of pre-catalyst components affords the active biomimetic catalyst. This minireview especially covers our recent contribution to the design of bioinspired quinone-based catalysts for the aerobic oxidation of amines to imines which has culminated in a dual bioinspired protocol as an example of “second-order” biomimicry.

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Ford, Courtney L., Yun Ji Park, Ellen M. Matson, Zachary Gordon und Alison R. Fout. „A bioinspired iron catalyst for nitrate and perchlorate reduction“. Science 354, Nr. 6313 (10.11.2016): 741–43. http://dx.doi.org/10.1126/science.aah6886.

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26

Mouchfiq, Ahmed, Tanya K. Todorova, Subal Dey, Marc Fontecave und Victor Mougel. „A bioinspired molybdenum–copper molecular catalyst for CO2 electroreduction“. Chemical Science 11, Nr. 21 (2020): 5503–10. http://dx.doi.org/10.1039/d0sc01045f.

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27

Simakova, Antonina, Matthew Mackenzie, Saadyah E. Averick, Sangwoo Park und Krzysztof Matyjaszewski. „Bioinspired Iron-Based Catalyst for Atom Transfer Radical Polymerization“. Angewandte Chemie 125, Nr. 46 (23.09.2013): 12370–73. http://dx.doi.org/10.1002/ange.201306337.

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28

Simakova, Antonina, Matthew Mackenzie, Saadyah E. Averick, Sangwoo Park und Krzysztof Matyjaszewski. „Bioinspired Iron-Based Catalyst for Atom Transfer Radical Polymerization“. Angewandte Chemie International Edition 52, Nr. 46 (23.09.2013): 12148–51. http://dx.doi.org/10.1002/anie.201306337.

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29

Li, Guangxun, Zhuo Tang, Hongxin Liu, Ying-wei Wang und Shiqi Zhang. „Bioinspired Catalysis: Self-Assembly of a Protein and DNA as a Catalyst for the Aldol Reaction in Aqueous Media“. Synlett 29, Nr. 05 (20.12.2017): 560–65. http://dx.doi.org/10.1055/s-0036-1591854.

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An interesting bioinspired catalyst formed from readily available DNA and a protein through electrostatic interaction in situ proved to be efficient in catalyzing aldol reactions under mild conditions in water. By using a self-assembling catalytic system formed from protamine and DNA, aldol adducts were obtained with high yields and moderate enantioselectivities. Preliminary experiments demonstrated that the chirality of the DNA could be effectively transferred to the reaction product through the bound molecules or proteins.

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Shteinman, Albert A. „Metallocavitins as Advanced Enzyme Mimics and Promising Chemical Catalysts“. Catalysts 13, Nr. 2 (15.02.2023): 415. http://dx.doi.org/10.3390/catal13020415.

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The supramolecular approach is becoming increasingly dominant in biomimetics and chemical catalysis due to the expansion of the enzyme active center idea, which now includes binding cavities (hydrophobic pockets), channels and canals for transporting substrates and products. For a long time, the mimetic strategy was mainly focused on the first coordination sphere of the metal ion. Understanding that a highly organized cavity-like enzymatic pocket plays a key role in the sophisticated functionality of enzymes and that the activity and selectivity of natural metalloenzymes are due to the effects of the second coordination sphere, created by the protein framework, opens up new perspectives in biomimetic chemistry and catalysis. There are two main goals of mimicking enzymatic catalysis: (1) scientific curiosity to gain insight into the mysterious nature of enzymes, and (2) practical tasks of mankind: to learn from nature and adopt from its many years of evolutionary experience. Understanding the chemistry within the enzyme nanocavity (confinement effect) requires the use of relatively simple model systems. The performance of the transition metal catalyst increases due to its retention in molecular nanocontainers (cavitins). Given the greater potential of chemical synthesis, it is hoped that these promising bioinspired catalysts will achieve catalytic efficiency and selectivity comparable to and even superior to the creations of nature. Now it is obvious that the cavity structure of molecular nanocontainers and the real possibility of modifying their cavities provide unlimited possibilities for simulating the active centers of metalloenzymes. This review will focus on how chemical reactivity is controlled in a well-defined cavitin nanospace. The author also intends to discuss advanced metal–cavitin catalysts related to the study of the main stages of artificial photosynthesis, including energy transfer and storage, water oxidation and proton reduction, as well as highlight the current challenges of activating small molecules, such as H2O, CO2, N2, O2, H2, and CH4.

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Wennemers, Helma. „Peptides – Molecular Allrounders“. CHIMIA International Journal for Chemistry 75, Nr. 6 (30.06.2021): 525–29. http://dx.doi.org/10.2533/chimia.2021.525.

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The enormous structural and functional diversity available through combining different amino acids into peptides offers numerous exciting opportunities. This article summarizes recent research highlights from my laboratory in the areas of asymmetric catalysis, supramolecular chemistry, and chemical biology. This scope includes the development of bioinspired peptide catalysts, synthetic collagen peptides, supramolecular porous assemblies, and cell-penetrating peptides.

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Cox, Nicholas, Dimitrios A. Pantazis, Frank Neese und Wolfgang Lubitz. „Artificial photosynthesis: understanding water splitting in nature“. Interface Focus 5, Nr. 3 (06.06.2015): 20150009. http://dx.doi.org/10.1098/rsfs.2015.0009.

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In the context of a global artificial photosynthesis (GAP) project, we review our current work on nature's water splitting catalyst. In a recent report (Cox et al . 2014 Science 345, 804–808 ( doi:10.1126/science.1254910 )), we showed that the catalyst—a Mn 4 O 5 Ca cofactor—converts into an ‘activated’ form immediately prior to the O–O bond formation step. This activated state, which represents an all Mn IV complex, is similar to the structure observed by X-ray crystallography but requires the coordination of an additional water molecule. Such a structure locates two oxygens, both derived from water, in close proximity, which probably come together to form the product O 2 molecule. We speculate that formation of the activated catalyst state requires inherent structural flexibility. These features represent new design criteria for the development of biomimetic and bioinspired model systems for water splitting catalysts using first-row transition metals with the aim of delivering globally deployable artificial photosynthesis technologies.

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Lin, Yuehe, und Dan (Annie) Du. „(Invited) New Bioinspired Nanomaterials for Biosensing and Cancer Theranostics“. ECS Meeting Abstracts MA2022-01, Nr. 53 (07.07.2022): 2202. http://dx.doi.org/10.1149/ma2022-01532202mtgabs.

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Nature is an excellent source of inspiration for the widespread application of science and technology. Researchers learn from biological principles and gradually develop from the earliest direct use of biological materials to the design and development of new biomimetic materials inspired by nature. Therefore, the innovation of bioinspired nanomaterials will enable tremendous advances in biology and biochemistry with biomimetic capabilities, such as biosensing, cell imaging, and drug delivery. In this presentation, I will discuss my group’s recent work on two bioinspired nanomaterials: nano-peptoids and single-atom nanozymes. The first type of bioinspired materials is a sequence-defined peptide-like materials that can mimic the structure and function of peptides and proteins. Compared with peptides and proteins, peptoids have a high degree of thermal and chemical stability, and are resistant to proteolytic degradation. In addition, due to the lack of intramolecular and intermolecular backbone hydrogen bond donors, it is possible to precisely control the peptoid and peptoid-substrate interactions, leading to bio-inspired synthesis of nanomaterials with a layered structure. As a peptide mimic, the peptoids has biocompatibility, non-toxicity and sequence-specific heteropolymers. Nano-peptoids can be synthesized with polar and hydrophobic monomers and have the following advantages: They can be easily processed into desired shapes (e.g. dendritic, sheets, tubes and vesicles), and the size range is 2-100 nm to enhance cell targeting and uptake. The application of nano-peptoids in cell imaging and cancer theranostics will be discussed. Another type of bioinspired nanomaterials with enzyme-like properties is single-atom nanoenzymes. As a biocatalyst, natural enzymes have the ability to accelerate various reaction rates with extremely high activity and selectivity under mild conditions. However, due to the temperature and pH-related denaturation of proteins and the possibility of contamination by bacteria or other reagents, the shelf life of natural enzymes is limited or uncertain, and their purification and production costs are high. Therefore, natural enzymes must narrow the range of conditions under which they can be used, limiting their further applications in biosensing and biomedicine. R Recent research has focused on the rational design of nanomaterials with inherent enzyme-like catalytic properties (for example, oxidase, peroxidase, catalase, superoxide dismutase, and so on) and exploration of their applications in various fields. Although much progress has been made, the development of nanozymes is still hampered by several challenges. Catalytic activity and substrate selectivity are the two most important issues that need to be resolved to allow the technology to reach full maturity. Therefore, rational design and tuning of nanomaterials is highly desirable for the development of novel enzyme-mimic nanomaterials with precise catalytic sites. We have developed various Fe-N-C based single atomic site catalysts which have similar structure with active site of peroxidase. These atomically-dispersed Fe-N-C materials have enzyme-like properties, therefore they are classified as single-atom nanozymes. Together with their abundantly exposed active sites and specific structures, these single atomic nanozymes have great potential for the enhancement of biocatalytic activity and selectivity in biosensing. Jiao, H. Yan, Y. Wu, W. Gu, C. Zhu, D. Du, Y. Lin. When Nanozymes Meet Single-Atom Catalysis. Angew. Chem. Int. Ed. 2020,132, 2585-2596 Zhu, S. Fu, Q. Shi, D. Du, Y. Lin. Single-Atom Electrocatalysts. Angew. Chem. Int. Ed. 2017, 56, 13944-13960. Cheng, J. Li, D. Liu, Y. Lin, D. Du. Single-Atom Nanozyme Based on Nanoengineered Fe-N-C Catalyst with Superior Peroxidase-Like Activity for Ultrasensitive Bioassays. Small, 2019, 1901485. Niu, Q. Shi, W. Zhu, D. Liu, H. Tian, S. Fu, N. Cheng, S. Li, J. N Smith, D. Du, Y. Lin. Unprecedented Peroxidase-mimicking Activity of Single-atom Nanozyme with Atomically Dispersed Fe-Nx Moieties Hosted by MOF Derived Porous Carbon. Biosensors & Bioelectronics, 2019, 142, 111495. Jiao, W. Xu, Y. Wu, H. Yan, W. Gu, D. Du, Y Lin, C. Zhu, Single-atom Catalysts Boost Signal Amplification for Biosensing. Chemical Society Reviews 2021, 50, 750-765 Luo, Y. Song, M. Wang, T. Jian, S. Ding, P. Mu, Z. Liao, Q. Shi, X. Cai, H. Jin, D. Du, W. Dong, C. Chen, Y. Lin. Bioinspired Peptoid Nanotubes for Targeted Tumor Cell Imaging and Chemo-Photodynamic Therapy. Small 2019, 1902485. Song, M. Wang, S. Akkineni, W. Yang, J.J. Hettige, H. Jin, Z. Liao, P. Mu, F. Yan, M. Baer, J. De Yoreo, D. Du, Y. Lin, C. Chen. Highly Bright and Photostable Two-Dimensional Nanomaterials Assembled from Sequence-Defined Peptoids. ACS Materials Letters 2021, 3, 420-427. Cai, M. Wang, P. Mu, T. Jian, D. Liu, S. Ding, Y. Luo, D. Du, Y. Song, C. Chen, Y. Lin. Sequence-Defined Nanotubes Assembled from IR780-Conjugated Peptoids for Chemophototherapy of Malignant Glioma. Research 2021, Article ID 9861384.

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Bagi, Nárcisz, József Kaizer und Gábor Speier. „Oxidation of thiols to disulfides by dioxygen catalyzed by a bioinspired organocatalyst“. RSC Advances 5, Nr. 57 (2015): 45983–86. http://dx.doi.org/10.1039/c5ra05529f.

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2,3-Dihydro-2,2,2-triphenylphenanthro[9,10-d]-1,3,2-λ⁵-oxazaphosphole serves as good catalyst for the oxidation of thiophenol, cysteine and glutathione to their disulfides by molecular oxygen.

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Brimblecombe, Robin, Annette Koo, G. Charles Dismukes, Gerhard F. Swiegers und Leone Spiccia. „Solar Driven Water Oxidation by a Bioinspired Manganese Molecular Catalyst“. Journal of the American Chemical Society 132, Nr. 9 (10.03.2010): 2892–94. http://dx.doi.org/10.1021/ja910055a.

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Gorun, Sergiu M. „Industrial applications of bioinspired catalysis: The anatomy of a catalyst“. Journal of Inorganic Biochemistry 59, Nr. 2-3 (August 1995): 615. http://dx.doi.org/10.1016/0162-0134(95)97706-v.

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Lee, Way-Zen, Tzu-Li Wang, Hao-Ching Chang, Yi-Ting Chen und Ting-Shen Kuo. „A Bioinspired ZnII/FeIII Heterobimetallic Catalyst for Thia-Michael Addition“. Organometallics 31, Nr. 11 (21.05.2012): 4106–9. http://dx.doi.org/10.1021/om300275a.

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Karlsson, Erik A., Bao-Lin Lee, Torbjörn Åkermark, Eric V. Johnston, Markus D. Kärkäs, Junliang Sun, Örjan Hansson, Jan-E. Bäckvall und Björn Åkermark. „Photosensitized Water Oxidation by Use of a Bioinspired Manganese Catalyst“. Angewandte Chemie International Edition 50, Nr. 49 (07.10.2011): 11715–18. http://dx.doi.org/10.1002/anie.201104355.

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Karlsson, Erik A., Bao-Lin Lee, Torbjörn Åkermark, Eric V. Johnston, Markus D. Kärkäs, Junliang Sun, Örjan Hansson, Jan-E. Bäckvall und Björn Åkermark. „Photosensitized Water Oxidation by Use of a Bioinspired Manganese Catalyst“. Angewandte Chemie 123, Nr. 49 (07.10.2011): 11919–22. http://dx.doi.org/10.1002/ange.201104355.

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Malini, S., Kalyan Raj, S. Madhumathy, Khalid Mohamed El-Hady, Saiful Islam und Mycal Dutta. „Bioinspired Advances in Nanomaterials for Sustainable Agriculture“. Journal of Nanomaterials 2022 (29.04.2022): 1–11. http://dx.doi.org/10.1155/2022/8926133.

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Rising demand for food production and an intensified usage of hazardous substances on the farmland are the driving force behind the emergence of green nanotechnology. Eco-friendly nanomaterials synthesised using plant sources and microorganisms are expected to catalyse a revolution in the agricultural sector by introducing nano-enabled smart sensors for metals along with organic toxins, supplying micronutrients; balancing the plant hormones, soil quality, and moisture content; stimulating plant growth; and minimising the usage of toxic chemicals by nanofertilizers and nanopesticides. As no single nanocompound has proved to be completely sustainable, this review discusses a wide variety of sustainable routes to implement nanomaterials to increase productivity, protect, and monitor crops through innovative nano-aided agricultural practices. Nevertheless, as the progress of research and commercialization in this area is still marginal, an understanding of complex dynamic behaviour, careful evaluation with targeted delivery of these compounds in the environment, and strong governmental regulatory norms are necessary to realize the effectiveness of green nanotechnology for sustainable agriculture. This article outlines some major advancements in recent years related to the implementation of eco-friendly nanomaterials in the agricultural sector. A systematic and comprehensive approach to adopting green nanotechnology would certainly promote a sustainable movement resulting in a beneficial economic and ecological impact.

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Lancaster, Louis, David P. Hickey, Matthew S. Sigman, Shelley D. Minteer und Ian Wheeldon. „Bioinspired design of a hybrid bifunctional enzymatic/organic electrocatalyst for site selective alcohol oxidation“. Chemical Communications 54, Nr. 5 (2018): 491–94. http://dx.doi.org/10.1039/c7cc08548f.

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Mauzeroll, Janine. „Bioinspired Nanomaterial Synthesis and Applications in Catalysis“. ECS Meeting Abstracts MA2022-01, Nr. 50 (07.07.2022): 2114. http://dx.doi.org/10.1149/ma2022-01502114mtgabs.

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We will discuss the use of a tobacco mosaic virus coat protein (TMVCP) as a versatile platform to synthesize a series of metallic nanomaterials and their applications in energy related electrocatalytic reactions. Taking advantage of the self-assembly properties of TMVCP under different solution conditions, nanoparticles can be embedded onto the disk protein surface or capped by protein subunits. We show that in addition to the eco-friendly synthesis merit, the as prepared materials are superior catalysts in electrocatalytic reactions. While the nanosized silver rings exhibit significant enhancement towards catalysing electrochemical carbon dioxide reduction reaction, the TMVCP-templated two platinum catalyst are promising candidates for methanol oxidation reaction. Besides electrocatalysis, potential applications of protein-metal hybrid systems in heterogeneous organic synthesis are also described. Gold and palladium nanoparticles capped by the bulky protein subunits are employed for two organic reactions and also showed remarkable kinetics.

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van Vliet, Liisa D., Pierre-Yves Colin und Florian Hollfelder. „Bioinspired genotype–phenotype linkages: mimicking cellular compartmentalization for the engineering of functional proteins“. Interface Focus 5, Nr. 4 (06.08.2015): 20150035. http://dx.doi.org/10.1098/rsfs.2015.0035.

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The idea of compartmentalization of genotype and phenotype in cells is key for enabling Darwinian evolution. This contribution describes bioinspired systems that use in vitro compartments—water-in-oil droplets and gel-shell beads—for the directed evolution of functional proteins. Technologies based on these principles promise to provide easier access to protein-based therapeutics, reagents for processes involving enzyme catalysis, parts for synthetic biology and materials with biological components.

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Brudvig, Gary W. „(Invited) Water Oxidation Catalysis with Atomically Defined Active Sites on Nanostructured Materials for Solar Energy Applications“. ECS Meeting Abstracts MA2023-01, Nr. 37 (28.08.2023): 2149. http://dx.doi.org/10.1149/ma2023-01372149mtgabs.

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Devising cost effective methods for efficiently capturing and storing solar energy is among the grand challenges of science (1). We are using insights from studies of natural photosynthetic systems (2) to develop bioinspired materials for photo-electrochemical water oxidation and solar fuel production by using molecular catalysts and dyes attached to mesoporous metal oxide photoanodes. Molecular catalysts are known for their high activity and tunability, but their solubility and limited stability often restrict their use in practical applications. We are developing anchoring chemistry to attach molecular water-oxidation catalysts to metal oxide surfaces (3), which not only greatly increases the stability of the molecular catalyst but also improves the catalytic performance of the oxide material. Our progress on the development and characterization of molecular iridium, copper and manganese water-oxidation catalysts (4-5), along with their application for photoelectrochemical water oxidation (6) and solar fuel production, will be discussed. Directing Matter and Energy: Five Challenges for Science and the Imagination, U.S. Department of Energy, Washington, DC, December 2007. D.J. Vinyard and G.W. Brudvig, Annu. Rev. Phys. Chem. (2017) 68, 101. J.L. Troiano, R.H. Crabtree and G.W. Brudvig, ACS Appl. Mater. Interfaces (2022) 14, 6582. S.W. Sheehan et al., Nature Comm. (2015) 6, 6469. K.J. Fisher et al., ACS Catalysis (2017) 7, 3384. Y. Zhao et al., Proc. Natl. Acad. Sci. U.S.A. (2018) 115, 2902.

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Jimeno, Ciril. „Amino Acylguanidines as Bioinspired Catalysts for the Asymmetric Aldol Reaction“. Molecules 26, Nr. 4 (05.02.2021): 826. http://dx.doi.org/10.3390/molecules26040826.

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The binding and stabilizing effect of arginine residues in certain aldolases served as inspiring source for the development of a family of amino acylguanidine organocatalysts. Screening and optimization led to identify the threonine derivative as the most suitable catalyst for the asymmetric aldol addition of hydroxyacetone, affording the syn diastereomer in high ee. In contrast, the proline derivative yielded the anti diasteromer. MMFF models suggest the presence of an extensive hydrogen bonding network between the acylguanidinium group and the reaction intermediates.

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Hisaeda, Yoshio, Keishiro Tahara, Hisashi Shimakoshi und Takahiro Masuko. „Bioinspired catalytic reactions with vitamin B12 derivative and photosensitizers“. Pure and Applied Chemistry 85, Nr. 7 (10.04.2013): 1415–26. http://dx.doi.org/10.1351/pac-con-12-10-05.

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As part of a study directed toward design of good catalytic systems based upon a hydrophobic vitamin B12, heptamethyl cobyrinate perchlorate, we describe the preparation of various nanomaterials using the vitamin B12 derivative and photosensitizers. Examples include vitamin B12-hyperbranched polymers (HBPs), human serum albumin (HSA) containing vitamin B12 derivatives, a vitamin B12-titanium dioxide hybrid catalyst, a vitamin B12-Ru complex combined system, and a vitamin B12-rose bengal combined system. These bioinspired materials have the potential as catalytic systems for the degradation of organic halide pollutants and for molecular transformations via radical intermediates during irradiation by UV or visible light, and offer a variety of applications that are of great interest in terms of green chemistry.

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Ji, Chunqing, Shanshan Liu, Kongzhao Su, El-Sayed M. El-Sayed, Heyuan Liu, Wenjing Wang, Fenglei Qiu, Xiyou Li und Daqiang Yuan. „Pyrogallol[4]arene Coordination Nanocapsule Micelle as Bioinspired Water Reduction Catalyst“. ACS Materials Letters 3, Nr. 9 (11.08.2021): 1315–20. http://dx.doi.org/10.1021/acsmaterialslett.1c00362.

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Kühn, Ulrike, Sabine Warzeska, Hans Pritzkow und Roland Krämer. „A Bioinspired Dicopper(II) Catalyst for the Transesterification of Dimethyl Phosphate“. Journal of the American Chemical Society 123, Nr. 33 (August 2001): 8125–26. http://dx.doi.org/10.1021/ja015562c.

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Lifschitz, Alejo M., Ryan M. Young, Jose Mendez-Arroyo, C. Michael McGuirk, Michael R. Wasielewski und Chad A. Mirkin. „Cooperative Electronic and Structural Regulation in a Bioinspired Allosteric Photoredox Catalyst“. Inorganic Chemistry 55, Nr. 17 (10.05.2016): 8301–8. http://dx.doi.org/10.1021/acs.inorgchem.6b00095.

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Bortoli, Marco, Francesco Zaccaria, Marco Dalla Tiezza, Matteo Bruschi, Célia Fonseca Guerra, F. Matthias Bickelhaupt und Laura Orian. „Oxidation of organic diselenides and ditellurides by H2O2for bioinspired catalyst design“. Physical Chemistry Chemical Physics 20, Nr. 32 (2018): 20874–85. http://dx.doi.org/10.1039/c8cp02748j.

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The reactivity of differently substituted diselenides and ditellurides toward H₂O₂, an ancient but still currently debated issue, was investigatedin silicoto assess the role the chalcogen and the groups directly bound to it have on the reaction energetics.

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