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Now showing 1 - 4 of 4
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    Cobalt-based nanoparticles prepared from MOF-carbon templates as efficient hydrogenation catalysts
    (Cambridge : RSC, 2018) Murugesan, Kathiravan; Senthamarai, Thirusangumurugan; Sohail, Manzar; Alshammari, Ahmad S.; Pohl, Marga-Martina; Beller, Matthias; Jagadeesh, Rajenahally V.
    The development of efficient and selective nanostructured catalysts for industrially relevant hydrogenation reactions continues to be an actual goal of chemical research. In particular, the hydrogenation of nitriles and nitroarenes is of importance for the production of primary amines, which constitute essential feedstocks and key intermediates for advanced chemicals, life science molecules and materials. Herein, we report the preparation of graphene shell encapsulated Co3O4- and Co-nanoparticles supported on carbon by the template synthesis of cobalt-terephthalic acid MOF on carbon and subsequent pyrolysis. The resulting nanoparticles create stable and reusable catalysts for selective hydrogenation of functionalized and structurally diverse aromatic, heterocyclic and aliphatic nitriles, and as well as nitro compounds to primary amines (>65 examples). The synthetic and practical utility of this novel non-noble metal-based hydrogenation protocol is demonstrated by upscaling several reactions to multigram-scale and recycling of the catalyst.
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    Ultra-small cobalt nanoparticles from molecularly-defined Co-salen complexes for catalytic synthesis of amines
    (Cambridge : RSC, 2020) Senthamarai, Thirusangumurugan; Chandrashekhar, Vishwas G.; Gawande, Manoj B.; Kalevaru, Narayana V.; Zbořil, Radek; Kamer, Paul C.J.; Jagadeesh, Rajenahally V.; Beller, Matthias
    We report the synthesis of in situ generated cobalt nanoparticles from molecularly defined complexes as efficient and selective catalysts for reductive amination reactions. In the presence of ammonia and hydrogen, cobalt-salen complexes such as cobalt(ii)-N,N′-bis(salicylidene)-1,2-phenylenediamine produce ultra-small (2-4 nm) cobalt-nanoparticles embedded in a carbon-nitrogen framework. The resulting materials constitute stable, reusable and magnetically separable catalysts, which enable the synthesis of linear and branched benzylic, heterocyclic and aliphatic primary amines from carbonyl compounds and ammonia. The isolated nanoparticles also represent excellent catalysts for the synthesis of primary, secondary as well as tertiary amines including biologically relevant N-methyl amines. This journal is © The Royal Society of Chemistry.
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    Structure of Ni(OH)2 intermediates determines the efficiency of NiO-based photocathodes – a case study using novel mesoporous NiO nanostars
    (Cambridge : RSC, 2019) Wahyuono, Ruri Agung; Dellith, Andrea; Schmidt, Christa; Dellith, Jan; Ignaszak, Anna; Seyring, Martin; Rettenmayr, Markus; Fize, Jennifer; Artero, Vincent; Chavarot-Kerlidou, Murielle; Dietzek, Benjamin
    We report the wet chemical synthesis of mesoporous NiO nanostars (NS) as photocathode material for dye-sensitized solar cells (DSSCs). The growth mechanism of NiO NS as a new morphology of NiO is assessed by TEM and spectroscopic investigations. The NiO NS are obtained upon annealing of preformed β-Ni(OH)2 into pristine NiO with low defect concentrations and favorable electronic configuration for dye sensitization. The NiO NS consist of fibers self-assembled from nanoparticles yielding a specific surface area of 44.9 m2 g-1. They possess a band gap of 3.83 eV and can be sensitized by molecular photosensitizers bearing a range of anchoring groups, e.g. carboxylic acid, phosphonic acid, and pyridine. The performance of NiO NS-based photocathodes in photoelectrochemical application is compared to that of other NiO morphologies, i.e. nanoparticles and nanoflakes, under identical conditions. Sensitization of NiO NS with the benchmark organic dye P1 leads to p-DSSCs with a high photocurrent up to 3.91 mA cm-2 whilst the photoelectrochemical activity of the NiO NS photocathode in aqueous medium in the presence of an irreversible electron acceptor is reflected by generation of a photocurrent up to 23 μA cm-2 © 2019 The Royal Society of Chemistry.
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    Mechanistic insight into the non-hydrolytic sol–gel process of tellurite glass films to attain a high transmission
    (Cambridge : RSC, 2020) Pan, Xuanzhao; Zhao, Jiangbo; Qian, Gujie; Zhang, Xiaozhou; Ruan, Yinlan; Abell, Andrew; Ebendorff-Heidepriem, Heike
    The development of amorphous films with a wide transmission window and high refractive index is of growing significance due to the strong demand of integrating functional nanoparticles for the next-generation hybrid optoelectronic films. High-index TeO2-based glass films made via the sol-gel process are particularly suitable as their low temperature preparation process promises high compatibility with a large variety of nanoparticles and substrates that suffer from low thermal stability. However, due to the lack of in-depth understanding of the mechanisms of the formation of undesired metallic-Te (highly absorbing species) in the films, the preparation of high-transmission TeO2-based sol-gel films has been severely hampered. Here, by gaining insight into the mechanistic chemistry of metallic-Te formation at different stages during the non-hydrolytic sol-gel process, we identify the chemical route to prevent the generation of metallic-Te in a TeO2-based film. The as-prepared TeO2-based film exhibits a high transmission that is close to the theoretical limit. This opens up a new avenue for advancing the performance of hybrid optoelectronic films via incorporating a large variety of unique nanoparticles. © 2020 The Royal Society of Chemistry.