| 1. |
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- 2019
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Tidskriftsartikel (refereegranskat)
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| 2. |
- Bousquet, Jean, et al.
(författare)
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Allergic Rhinitis and its Impact on Asthma (ARIA) Phase 4 (2018) : Change management in allergic rhinitis and asthma multimorbidity using mobile technology
- 2019
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Ingår i: Journal of Allergy and Clinical Immunology. - : Elsevier. - 0091-6749 .- 1097-6825. ; 143:3, s. 864-879
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Tidskriftsartikel (refereegranskat)abstract
- Allergic Rhinitis and its Impact on Asthma (ARIA) has evolved from a guideline by using the best approach to integrated care pathways using mobile technology in patients with allergic rhinitis (AR) and asthma multimorbidity. The proposed next phase of ARIA is change management, with the aim of providing an active and healthy life to patients with rhinitis and to those with asthma multimorbidity across the lifecycle irrespective of their sex or socioeconomic status to reduce health and social inequities incurred by the disease. ARIA has followed the 8-step model of Kotter to assess and implement the effect of rhinitis on asthma multimorbidity and to propose multimorbid guidelines. A second change management strategy is proposed by ARIA Phase 4 to increase self-medication and shared decision making in rhinitis and asthma multimorbidity. An innovation of ARIA has been the development and validation of information technology evidence-based tools (Mobile Airways Sentinel Network [MASK]) that can inform patient decisions on the basis of a self-care plan proposed by the health care professional.
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| 3. |
- Escott-Price, Valentina, et al.
(författare)
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Gene-Wide Analysis Detects Two New Susceptibility Genes for Alzheimer's Disease
- 2014
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Ingår i: PLOS ONE. - : Public Library of Science (PLoS). - 1932-6203. ; 9:6, s. e94661-
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Tidskriftsartikel (refereegranskat)abstract
- Background: Alzheimer's disease is a common debilitating dementia with known heritability, for which 20 late onset susceptibility loci have been identified, but more remain to be discovered. This study sought to identify new susceptibility genes, using an alternative gene-wide analytical approach which tests for patterns of association within genes, in the powerful genome-wide association dataset of the International Genomics of Alzheimer's Project Consortium, comprising over 7 m genotypes from 25,580 Alzheimer's cases and 48,466 controls. Principal Findings: In addition to earlier reported genes, we detected genome-wide significant loci on chromosomes 8 (TP53INP1, p = 1.4x10(-6)) and 14 (IGHV1-67 p = 7.9x10(-8)) which indexed novel susceptibility loci. Significance: The additional genes identified in this study, have an array of functions previously implicated in Alzheimer's disease, including aspects of energy metabolism, protein degradation and the immune system and add further weight to these pathways as potential therapeutic targets in Alzheimer's disease.
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| 4. |
- Jones, Lesley, et al.
(författare)
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Convergent genetic and expression data implicate immunity in Alzheimer's disease
- 2015
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Ingår i: Alzheimer's & Dementia. - : Wiley. - 1552-5260 .- 1552-5279. ; 11:6, s. 658-671
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Tidskriftsartikel (refereegranskat)abstract
- Background: Late-onset Alzheimer's disease (AD) is heritable with 20 genes showing genome-wide association in the International Genomics of Alzheimer's Project (IGAP). To identify the biology underlying the disease, we extended these genetic data in a pathway analysis. Methods: The ALIGATOR and GSEA algorithms were used in the IGAP data to identify associated functional pathways and correlated gene expression networks in human brain. Results: ALIGATOR identified an excess of curated biological pathways showing enrichment of association. Enriched areas of biology included the immune response (P = 3.27 X 10(-12) after multiple testing correction for pathways), regulation of endocytosis (P = 1.31 X 10(-11)), cholesterol transport (P = 2.96 X 10(-9)), and proteasome-ubiquitin activity (P = 1.34 X 10(-6)). Correlated gene expression analysis identified four significant network modules, all related to the immune response (corrected P = .002-.05). Conclusions: The immime response, regulation of endocytosis, cholesterol transport, and protein ubiquitination represent prime targets for AD therapeutics.
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| 5. |
- Nene, Vishvanath, et al.
(författare)
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Genome sequence of Aedes aegypti, a major arbovirus vector.
- 2007
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Ingår i: Science (New York, N.Y.). - : American Association for the Advancement of Science (AAAS). - 1095-9203 .- 0036-8075. ; 316:5832, s. 1718-23
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Tidskriftsartikel (refereegranskat)abstract
- We present a draft sequence of the genome of Aedes aegypti, the primary vector for yellow fever and dengue fever, which at approximately 1376 million base pairs is about 5 times the size of the genome of the malaria vector Anopheles gambiae. Nearly 50% of the Ae. aegypti genome consists of transposable elements. These contribute to a factor of approximately 4 to 6 increase in average gene length and in sizes of intergenic regions relative to An. gambiae and Drosophila melanogaster. Nonetheless, chromosomal synteny is generally maintained among all three insects, although conservation of orthologous gene order is higher (by a factor of approximately 2) between the mosquito species than between either of them and the fruit fly. An increase in genes encoding odorant binding, cytochrome P450, and cuticle domains relative to An. gambiae suggests that members of these protein families underpin some of the biological differences between the two mosquito species.
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| 6. |
- Fresard, Laure, et al.
(författare)
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Identification of rare-disease genes using blood transcriptome sequencing and large control cohorts
- 2019
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Ingår i: Nature Medicine. - : NATURE PUBLISHING GROUP. - 1078-8956 .- 1546-170X. ; 25:6, s. 911-919
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Tidskriftsartikel (refereegranskat)abstract
- It is estimated that 350 million individuals worldwide suffer from rare diseases, which are predominantly caused by mutation in a single gene(1). The current molecular diagnostic rate is estimated at 50%, with whole-exome sequencing (WES) among the most successful approaches(2-5). For patients in whom WES is uninformative, RNA sequencing (RNA-seq) has shown diagnostic utility in specific tissues and diseases(6-8). This includes muscle biopsies from patients with undiagnosed rare muscle disorders(6,9), and cultured fibroblasts from patients with mitochondrial disorders(7). However, for many individuals, biopsies are not performed for clinical care, and tissues are difficult to access. We sought to assess the utility of RNA-seq from blood as a diagnostic tool for rare diseases of different pathophysiologies. We generated whole-blood RNA-seq from 94 individuals with undiagnosed rare diseases spanning 16 diverse disease categories. We developed a robust approach to compare data from these individuals with large sets of RNA-seq data for controls (n = 1,594 unrelated controls and n = 49 family members) and demonstrated the impacts of expression, splicing, gene and variant filtering strategies on disease gene identification. Across our cohort, we observed that RNA-seq yields a 7.5% diagnostic rate, and an additional 16.7% with improved candidate gene resolution.
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| 7. |
- Verho, Oscar, et al.
(författare)
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Application and mechanistic studies of a water-oxidation catalyst in alcohol oxidation by employing oxygen-transfer reagents
- 2012
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Ingår i: Chemistry - A European Journal. - : Wiley. - 0947-6539 .- 1521-3765. ; 18:52, s. 16947-16954
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Tidskriftsartikel (refereegranskat)abstract
- By using a dimeric ruthenium complex in combination with tert-butyl hydrogen peroxide (TBHP) as stoichiometric oxidant, a mild and efficient protocol for the oxidation of secondary benzylic alcohols was obtained, thereby giving the corresponding ketones in high yields within 4 h. However, in the oxidation of aliphatic alcohols, the TBHP protocol suffered from low conversions owing to a competing Ru-catalyzed disproportionation of the oxidant. Gratifyingly, by switching to Oxone (2 KHSO5⋅KHSO4⋅K2SO4 triple salt) as stoichiometric oxidant, a more efficient and robust system was obtained that allowed for the oxidation of a wide range of aliphatic and benzylic secondary alcohols, giving the corresponding ketones in excellent yields. The mechanism for these reactions is believed to involve a high-valent RuV–oxo species. We provide support for such an intermediate by means of mechanistic studies.
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| 8. |
- Abdel-Magied, Ahmed F., et al.
(författare)
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Chemical and Photochemical Water Oxidation Mediated by an Efficient Single-Site Ruthenium Catalyst
- 2016
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Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 9:24, s. 3448-3456
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Tidskriftsartikel (refereegranskat)abstract
- Water oxidation is a fundamental step in artificial photosynthesis for solar fuels production. In this study, we report a single-site Ru-based water oxidation catalyst, housing a dicarboxylate-benzimidazole ligand, that mediates both chemical and light-driven oxidation of water efficiently under neutral conditions. The importance of the incorporation of the negatively charged ligand framework is manifested in the low redox potentials of the developed complex, which allows water oxidation to be driven by the mild one-electron oxidant [Ru(bpy)(3)](3+) (bpy = 2,2'-bipyridine). Furthermore, combined experimental and DFT studies provide insight into the mechanistic details of the catalytic cycle.
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| 9. |
- Abdel-Magied, Ahmed F., et al.
(författare)
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Substituent Effects in Molecular Ruthenium Water Oxidation Catalysts Based on Amide Ligands
- 2017
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Ingår i: ChemCatChem. - : Wiley. - 1867-3880 .- 1867-3899. ; 9:9, s. 1583-1587
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Tidskriftsartikel (refereegranskat)abstract
- The production of clean and sustainable energy is considered as one of the most urgent issues for our society. Mastering the oxidation of water to dioxygen is essential for the production of solar fuels. A study of the influence of the substituents on the catalytic activity of a series of mononuclear Ru complexes (2a-e) based on a tetradentate ligand framework is presented. At neutral pH, using [Ru(bpy)(3)](PF6)(3) (bpy=2,2'-bipyridine) as the terminal oxidant, a good correlation between the turnover frequency (TOF) and the Hammett sigma(meta) parameters was obtained. Additionally, a general pathway for the deactivation of Ru-based catalysts 2a-e during the catalytic oxidation of water through poisoning by carbon monoxide was demonstrated. These results highlight the importance of ligand design for fine-tuning the catalytic activity of water oxidation catalysts.
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| 10. |
- Das, Biswanath, et al.
(författare)
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Water oxidation catalyzed by molecular di- and nonanuclear Fe complexes: importance of a proper ligand framework
- 2016
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Ingår i: Dalton Transactions. - : ROYAL SOC CHEMISTRY. - 1477-9226 .- 1477-9234. ; 45:34, s. 13289-13293
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Tidskriftsartikel (refereegranskat)abstract
- The synthesis of two molecular iron complexes, a dinuclear iron(III,III) complex and a nonanuclear iron complex, based on the di-nucleating ligand 2,2-(2-hydroxy-5-methyl-1,3-phenylene)bis(1H-benzo[d]imidazole-4-carboxylic acid) is described. The two iron complexes were found to drive the oxidation of water by the one-electron oxidant [Ru(bpy)(3)](3+).
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| 11. |
- Deiana, Luca, et al.
(författare)
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Combined Heterogeneous Metal/Chiral Amine : Multiple Relay Catalysis for Versatile Eco-Friendly Synthesis
- 2014
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Ingår i: Angewandte Chemie International Edition. - : Wiley. - 1433-7851 .- 1521-3773. ; 53:13, s. 3447-3451
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Tidskriftsartikel (refereegranskat)abstract
- Herein is described a versatile and broad synergistic strategy for expansion of chemical space and the synthesis of valuable molecules (e.g. carbocycles and heterocycles), with up to three quaternary stereocenters, in a highly enantioselective fashion from simple alcohols (31examples, 95:5 to >99.5:0.5 e.r.) using integrated heterogeneous metal/chiral amine multiple relay catalysis and air/O-2 as the terminal oxidant. A novel highly 1,4-selective heterogeneous metal/amine co-catalyzed hydrogenation of enals was also added to the relay catalysis sequences.
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| 12. |
- Deiana, Luca, 1982-, et al.
(författare)
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Enantioselective Heterogeneous Synergistic Catalysis for Asymmetric Cascade Transformations
- 2014
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Ingår i: Advanced Synthesis and Catalysis. - : Wiley. - 1615-4150 .- 1615-4169. ; 356:11-12, s. 2485-2492
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Tidskriftsartikel (refereegranskat)abstract
- A modular design for a novel heterogeneous synergistic catalytic system, which simultaneously activates the electrophile and nucleophile by the combined activation modes of a separate metal and non-metal catalyst, for asymmetric cascade transformations on a solid surface is disclosed. This modular catalysis strategy generates carbocycles (up to 97.5: 2.5 er) as well as spirocyclic oxindoles (97.5: 2.5 to > 99: 0.5 er), containing all-carbon quaternary centers, in a highly enantioselective fashion via a one-pot dynamic relay process.
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| 13. |
- Deiana, Luca, 1982-, et al.
(författare)
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Highly Enantioselective Cascade Transformations by Merging Heterogeneous Transition Metal Catalysis with Asymmetric Aminocatalysis
- 2012
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Ingår i: Scientific Reports. - : Springer Science and Business Media LLC. - 2045-2322. ; 2, s. 851-
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Tidskriftsartikel (refereegranskat)abstract
- The concept of combining heterogeneous transition metal and amine catalysis for enantioselective cascade reactions has not yet been realized. This is of great advantage since it would allow for the recycling of expensive and non-environmentally friendly transition metals. We disclose that the use of a heterogeneous Pd-catalyst in combination with a simple chiral amine co-catalyst allows for highly enantioselective cascade transformations. The preparative power of this process has been demonstrated in the context of asymmetric cascade Michael/carbocyclization transformations that delivers cyclopentenes bearing an all carbon quaternary stereocenters in high yields with up to 30: 1 dr and 99% ee. Moreover, a variety of highly enantioselective cascade hetero-Michael/carbocyclizations were developed for the one-pot synthesis of valuable dihydrofurans and pyrrolidines (up to 98% ee) by using bench-stable heterogeneous Pd and chiral amines as co-catalysts.
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| 14. |
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| 15. |
- Gustafson, Karl P. J., et al.
(författare)
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Water oxidation mediated by ruthenium oxide nanoparticles supported on siliceous mesocellular foam
- 2017
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Ingår i: Catalysis Science & Technology. - : Royal Society of Chemistry. - 2044-4753 .- 2044-4761. ; 7:1, s. 293-299
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Tidskriftsartikel (refereegranskat)abstract
- Artificial photosynthesis is an attractive strategy for converting solar energy into fuel. In this context, development of catalysts for oxidation of water to molecular oxygen remains a critical bottleneck. Herein, we describe the preparation of a well-defined nanostructured RuO2 catalyst, which is able to carry out the oxidation of water both chemically and photochemically. The developed heterogeneous RuO2 nanocatalyst was found to be highly active, exceeding the performance of most known heterogeneous water oxidation catalysts when driven by chemical or photogenerated oxidants.
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| 16. |
- Görbe, Tamás, et al.
(författare)
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Design of a Pd(0)-CalB CLEA Biohybrid Catalyst and Its Application in a One-Pot Cascade Reaction
- 2017
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Ingår i: ACS Catalysis. - : American Chemical Society (ACS). - 2155-5435. ; 7:3, s. 1601-1605
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Tidskriftsartikel (refereegranskat)abstract
- Herein, a design of a biohybrid catalyst is described, consisting of Pd nanoparticles and a cross-linked network of aggregated lipase B enzyme of Candida antarctica (CalB CLEA) functioning as an active support for the Pd nanoparticles. Both entities of the hybrid catalyst showed good catalytic activity. The applicability was demonstrated in a one-pot reaction, where the Pd-catalyzed cycloisomerization of 4-pentynoic acid afforded a lactone that serves as an acyl donor in a subsequent selective enzymatic kinetic resolution of a set of sec-alcohols. The catalyst proved to be robust and could be recycled five times without a significant loss of activity.
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| 17. |
- Ibrahem, Ismail, et al.
(författare)
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Copper Nanoparticles on Controlled Pore Glass and TEMPO for the Aerobic Oxidation of Alcohols
- 2018
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Ingår i: ChemNanoMat. - : Wiley. - 2199-692X. ; 4:1, s. 71-75
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Tidskriftsartikel (refereegranskat)abstract
- Herein, we report on the facile synthesis of a heterogeneous copper nanocatalyst and its combination with 2,2,6,6-tetramethyl-1-piperidinyloxy (TEMPO) for the aerobic oxidation of alcohols to their corresponding carbonyl compounds. This low cost copper nanocatalyst was found to exhibit excellent recyclability, making it a highly attractive catalytic system from an economical and environmental point of view. Extensive characterization of the catalyst by a number of techniques revealed that it was comprised of well-dispersed Cu(I/II) nanoparticles with an average size of around 6nm.
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| 18. |
- Iqbal, M. Naeem, et al.
(författare)
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Mesoporous Ruthenium Oxide : A Heterogeneous Catalyst for Water Oxidation
- 2017
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Ingår i: ACS Sustainable Chemistry and Engineering. - : American Chemical Society (ACS). - 2168-0485. ; 5:11, s. 9651-9656
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Tidskriftsartikel (refereegranskat)abstract
- Herein we report the synthesis of mesoporous ruthenium oxide (MP-RuO2) using a template-based approach. The catalytic efficiency of the prepared MP-RuO2 was compared to commercially available ruthenium oxide nanoparticles (C-RuO2) as heterogeneous catalysts for water oxidation. The results demonstrated superior performance of MP-RuO2 for oxygen evolution compared to the C-RuO2 with respect to recyclability, amount of generated oxygen, and stability over several catalytic runs.
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| 19. |
- Johnston, Eric V., et al.
(författare)
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Efficient aerobic ruthenium-catalyzed oxidation of secondary alcohols by the use of a hybrid electron transfer catalyst
- 2010
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Ingår i: European Journal of Organic Chemistry. - : Wiley. - 1434-193X .- 1099-0690. ; :10, s. 1971-1976
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Tidskriftsartikel (refereegranskat)abstract
- Biomimetic aerobic oxidation of secondary alcohols has been performed using hybrid catalyst 1 and Shvo's catalyst 2. This combination allows mild reaction conditions and low catalytic loading, due to the efficiency of intramolecular electron transfer. By this method a wide range of different alcohols have been converted into their corresponding ketones. Oxidation of benzylic as well as aliphatic, electron-rich, electron-deficient and sterically hindered alcohols could be oxidized in excellent yield and selectivity. Oxidation of (S)-1-phenyl-ethanol showed that no racemization occurred during the course of the reaction, indicating that the hydride 2b adds to the quinone much faster than it re-adds to the ketone product. The kinetic deuterium isotope effect of the oxidation was determined by the use of 1-phenylethanol (3a) and 1-deuterio-1-phenylethanol (3a-d1) in parallel and competitive manner, which gave the same isotope effect within experimental error (k(H)/k(D) approximate to 2.8). This indicates that there is no strong coordination of the substrate to the catalyst.
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| 20. |
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| 21. |
- Johnston, Eric V., et al.
(författare)
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Efficient synthesis of hybrid (hydroquinone-Schiff base)cobalt oxidation catalysts
- 2009
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Ingår i: European Journal of Organic Chemistry. - : Wiley. - 1434-193X .- 1099-0690. ; :23, s. 3973-3976
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Tidskriftsartikel (refereegranskat)abstract
- Hybrid catalysts A and B have recently been found to efficiently transfer electrons from a metal catalyst to molecular oxygen in biomimetic oxidations. In the present work hybrid catalysts A and B were synthesized in high yield from inexpensive starting materials. The key step is an efficient Suzuki cross-coupling, which allows the use of unprotected aldehyde 5. The new synthesis of the title hybrid catalysts is easy to carry out and can be scaled up.
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| 22. |
- Johnston, Eric V, et al.
(författare)
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Enantioselective synthesis of (R)-bufuralol via dynamic kinetic resolution in the key step
- 2010
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Ingår i: Journal of Organic Chemistry. - : American Chemical Society. - 0022-3263 .- 1520-6904. ; 75:13, s. 4596-4599
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Tidskriftsartikel (refereegranskat)abstract
- An enantioselective synthesis of (R)-bufuralol via a ruthenium- and enzyme-catalyzed dynamic kinetic resolution (DKR) has been achieved. The synthesis starts from readily available 2-ethylphenol and provides (R)-bufuralol in high ee and a good overall yield of 31%.
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| 23. |
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| 24. |
- Johnston, Eric V, et al.
(författare)
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Novel dinuclear Ru-complex for water oxidation
- 2010
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Ingår i: Abstracts of Papers, 240th ACS National Meeting, Boston, MA, United States, August 22-26, 2010 (2010). - : American Chemical Society.
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Konferensbidrag (övrigt vetenskapligt/konstnärligt)
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| 25. |
- Johnston, Eric V., et al.
(författare)
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Oxidation of carbonyl compounds
- 2010. - 2
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Ingår i: Modern Oxidation Methods. - Weinheim : Wiley-VCH Verlag GmbH & Co. KGaA. - 9783527323203 ; , s. 353-369
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Bokkapitel (övrigt vetenskapligt/konstnärligt)
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| 26. |
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| 27. |
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| 28. |
- Kärkäs, Markus D., et al.
(författare)
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Artificial Photosynthesis : Photosynthesis: From Nanosecond Electron Transfer to Catalytic Water Oxidation
- 2014
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Ingår i: Accounts of Chemical Research. - : American Chemical Society (ACS). - 0001-4842 .- 1520-4898. ; 47:1, s. 100-111
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Forskningsöversikt (refereegranskat)abstract
- Human society faces a fundamental challenge as energy consumption is projected to increase due to population and economic growth as fossil fuel resources decrease. Therefore the transition to alternative and sustainable energy sources is of the Utmost importance. The conversion of solar energy into chemical energy, by splitting H2O to generate molecular O-2 and H-2, could contribute to solving the global energy problem. Developing such a system will require the combination of several complicated processes, such as light-harvesting, charge separation, electron transfer, H2O oxidation, and reduction of the generated protons. The primary processes of charge separation and catalysis, which occur in the natural photosynthetic machinery, provide us with an excellent blueprint for the design of such systems. This Account describes our efforts to construct supramolecular assemblies capable of carrying out photoinduced electron transfer and to develop artificial water oxidation catalysts (WOCs). Early work in our group focused on linking a ruthenium chromophore to a manganese-based oxidation catalyst. When we incorporated a tyrosine unit into these supramolecular assemblies, we could observe fast intramolecular electron transfer from the manganese centers, via the tyrosine moiety, to the photooxidized ruthenium center, which clearly resembles the processes occurring in the natural system. Although we demonstrated multi-electron transfer in our artificial systems, the bottleneck proved to be the stability of the WOCs. Researchers have developed a number of WOCs, but the majority can only catalyze H2O oxidation in the presence of strong oxidants such as Ce-IV, which is difficult to generate photochemically. By contrast, illumination of ruthenium(II) photosensitizers in the presence of a sacrificial acceptor generates [Ru(bpy)(3)](3+)-type oxidants. Their oxidation potentials are significantly lower than that of Ce-IV, but our group recently showed that incorporating negatively charged groups into the ligand backbone could decrease the oxidation potential of the catalysts and, at the same time, decrease the potential for H2O oxidation. This permitted us to develop both ruthenium- and manganese-based WOCs that can operate under neutral conditions, driven by the mild oxidant [Ru(bpy)(3)](3+). Many hurdles to the development of viable systems for the production of solar fuels remain. However, the combination of important features from the natural photosynthetic machinery and novel artificial components adds insights into the complicated catalytic processes that are involved in splitting H2O.
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| 29. |
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| 30. |
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| 31. |
- Kärkäs, Markus D., 1984-, et al.
(författare)
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Light-Induced Water Oxidation by a Ru complex Containing a Bio-Inspired Ligand
- 2011
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Ingår i: Chemistry - A European Journal. - : Wiley. - 0947-6539 .- 1521-3765. ; 17:28, s. 7953-7959
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Tidskriftsartikel (refereegranskat)abstract
- The new Ru complex 8 containing the bio-inspired ligand 7 was successfully synthesized and characterized. Complex 8 efficiently catalyzes water oxidation using Ce(IV) and Ru(III) as chemical oxidants. More importantly, this complex has a sufficiently low overpotential to utilize ruthenium polypyridyl-type complexes as photosensitizers.
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| 32. |
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| 33. |
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| 34. |
- Lee, Bao-Lin, 1976-, et al.
(författare)
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Synthesis and characterization of oligonuclear Ru, Co, and Cu oxidation catalysts
- 2010
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Ingår i: European Journal of Inorganic Chemistry. - : Wiley. - 1434-1948 .- 1099-1948 .- 1099-0682. ; :34, s. 5462-5470
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Tidskriftsartikel (refereegranskat)abstract
- In this work, we report the preparation and crystal structures of three new oligonuclear complexes, Ru-2(bbpmp)(mu-OAc)(3) (4), [Co-2(bbpmp)(mu-OAc)(mu-OMe)](PF6) (5), [Cu-4(Hbbpmp)(2)(mu-OAc)(H2O)(2)](OAc)(PF6)(2) (6) {H(3)bbpmp = 2,6-bis[(2-hydroxybenzyl)-(2-pyridylmethyl)aminomethyl]-4-methylphenol (3)}. The structures of the complexes were determined by single-crystal X-ray diffraction. The oxidation states of ruthenium, cobalt and copper in the complexes are +3, +3 and +2, respectively. In 4 and 5, Ru-III and Co-III are coordinated to four oxygen and two nitrogen atoms in an octahedral geometry, while in 6, Cu-II adopts both octahedral (CuN2O4) and square-pyramidal (CuN2O3) geometry. The potential of the three complexes as oxidation catalysts has been investigated.
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| 35. |
- Nagendiran, Anuja, et al.
(författare)
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Cycloisomerization of Acetylenic Acids to gamma-Alkylidene Lactones using a Palladium(II) Catalyst Supported on Amino-Functionalized Siliceous Mesocellular Foam
- 2014
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Ingår i: Journal of Organic Chemistry. - : American Chemical Society (ACS). - 0022-3263 .- 1520-6904. ; 79:3, s. 1399-1405
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Tidskriftsartikel (refereegranskat)abstract
- Cycloisomerization of various gamma-acetylenic acids to their corresponding gamma-alkylidene lactones by the use of a heterogeneous Pd(II) catalyst supported on amino-functionalized siliceous mesocellular foam is described. Substrates containing terminal as well as internal alkynes were cyclized in high to excellent yields within 2-24 h under mild reaction conditions. The protocol exhibited high regio- and stereoselectivity, favoring the exo-dig product with high Z selectivity. Moreover, the catalyst displayed excellent stability under the employed reaction conditions, as demonstrated by its good recyclability and low leaching.
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| 36. |
- Olsen, Peter, et al.
(författare)
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Cyclic allylic carbonates as a renewable platform for protecting chemistry in water
- 2018
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Ingår i: Green Chemistry. - : Royal Society of Chemistry (RSC). - 1463-9262 .- 1463-9270. ; 20:14, s. 3186-3190
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Tidskriftsartikel (refereegranskat)abstract
- The present work explores different cyclic allylic carbonates as a potential class of allylcarbamate precursors. The 5-membered carbonate formed a carbamate with very good thermal and pH stability, which could be cleanly deprotected in aqueous solution, in just 30 min with 2 mol% Pd(OAc)(2) as catalyst. The polar nature of the installed motif made it possible to deprotect highly unpolar substrates in water as solvent.
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| 37. |
- Olsen, Peter, et al.
(författare)
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Synthesis of highly functional carbamates through ring-opening of cyclic carbonates with unprotected α-amino acids in water
- 2018
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Ingår i: Green Chemistry. - : Royal Society of Chemistry (RSC). - 1463-9262 .- 1463-9270. ; 20:2, s. 469-475
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Tidskriftsartikel (refereegranskat)abstract
- The present work shows that it is possible to ring-open cyclic carbonates with unprotected amino acids in water. Fine tuning of the reaction parameters made it possible to suppress the degree of hydrolysis in relation to aminolysis. This enabled the synthesis of functionally dense carbamates containing alkenes, carboxylic acids, alcohols and thiols after short reaction times at room temperature. When Glycine was used as the nucleophile in the ring-opening with four different five membered cyclic carbonates, containing a plethora of functional groups, the corresponding carbamates could be obtained in excellent yields (>90%) without the need for any further purification. Furthermore, the orthogonality of the transformation was explored through ring-opening of divinylenecarbonate with unprotected amino acids equipped with nucleophilic side chains, such as serine and cysteine. In these cases the reaction selectively produced the desired carbamate, in 70 and 50% yield respectively. The synthetic design provides an inexpensive and scalable protocol towards highly functionalized building blocks that are envisioned to find applications in both the small and macromolecular arena.
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| 38. |
- Persson, Andreas K. Å., 1983-, et al.
(författare)
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Copper-catalyzed N-allenylation of allylic sulfonamides
- 2009
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Ingår i: Organic Letters. - : American Chemical Society (ACS). - 1523-7060 .- 1523-7052. ; 11:17, s. 3814-3817
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Tidskriftsartikel (refereegranskat)abstract
- Allylic allenic amides have been synthesized via a copper-catalyzed cross-coupling between allylic sulfonamides and bromoallenes in moderate to good yields. Copper(I) thiophene-2-carboxylate (CuTC) was used a source of copper with DMEDA as the ligand. The allenylated products obtained are potential substrates for palladium-catalyzed carbocyclizations.
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| 39. |
- Rinde, Mia, et al.
(författare)
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Mesoporous silica with precisely controlled pores reduces food efficiency and suppresses weight gain in mice
- 2020
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Ingår i: Nanomedicine. - : Future Medicine Ltd. - 1743-5889 .- 1748-6963. ; 15:2, s. 131-144
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Tidskriftsartikel (refereegranskat)abstract
- Aim: Obesity is a risk factor for cardiovascular disease and diabetes. We aimed to elucidate the effects of distinct mesoporous silica particles (MSPs) supplemented in food on metabolic parameters in obesity. Materials & methods: MSPs with precisely controlled pore size were synthesized, characterized and compared with a control in a C57Bl/6 mouse diet-induced obesity model, studying weight, adiposity, metabolic regulation and food efficiency. Results: The most effective MSPs reduced adipose tissue formation to 6.5 +/- 0.5 g compared with 9.4 +/- 1.2 g, leptin levels nearly halved from 32.8 +/- 7.4 to 16.9 +/- 1.9 ng/ml and a 33% reduction of food efficiency. Control MSP showed no effects. Conclusion: Results demonstrate potential of distinct MSPs to improve metabolic risk factors. Further studies investigating mechanism of action and confirming human safety are needed.
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| 40. |
- Shatskiy, Andrey, et al.
(författare)
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Catalyst-solvent interactions in a dinuclear Ru-based water oxidation catalyst
- 2016
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Ingår i: Dalton Transactions. - : Royal Society of Chemistry (RSC). - 1477-9226 .- 1477-9234. ; 45:47, s. 19024-19033
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Tidskriftsartikel (refereegranskat)abstract
- Photocatalytic water oxidation represents a key process in conversion of solar energy into fuels and can be facilitated by the use of molecular transition metal-based catalysts. A novel straightforward approach for covalent linking of the catalytic units to other moieties is demonstrated by preparation of a dinuclear complex containing two [Ru(pdc)(pic)(3)]-derived units (pdc = 2,6-pyridinedicarboxylate, pic = 4-picoline). The activity of this complex towards chemical and photochemical oxidation of water was evaluated and a detailed insight is given into the interactions between the catalyst and acetonitrile, a common co-solvent employed to increase solubility of water oxidation catalysts. The solvent-induced transformations were studied by electrochemical and spectroscopic techniques and the relevant quantitative parameters were extracted.
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| 41. |
- Verho, Oscar, et al.
(författare)
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Mesoporous silica nanoparticles applied as a support for Pd and Au nanocatalysts in cycloisomerization reactions
- 2014
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Ingår i: APL Materials. - : AIP Publishing. - 2166-532X. ; 2:11, s. 113316-
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Tidskriftsartikel (refereegranskat)abstract
- Ultra-small mesoporous silica nanoparticles (MSNs) have been synthesized at room temperature with particle sizes ranging from 28 to 45 nm. These MSNs have been employed as heterogeneous supports for palladium and gold nanocatalysts. The colloidal nature of the MSNs is highly useful for catalytic applications as it allows for better mass transfer properties and a more uniform distribution of the nanocatalysts in solution. The two nanocatalysts were evaluated in the cycloisomerization of alkynoic acids and demonstrated to produce the corresponding alkylidene lactones in good to excellent yields under mild conditions. In addition to their high activity, the catalysts exhibit low degree of metal leaching and straight-forward recycling, which highlight the practical utility of MSNs as supports for nanocatalysts. (C) 2014 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License.
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| 42. |
- Verho, Oscar, et al.
(författare)
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Nanopalladium on Amino-Functionalized Mesocellular Foam : An Efficient Catalyst for Suzuki Reactions and Transfer Hydrogenations
- 2013
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Ingår i: ChemCatChem. - : Wiley. - 1867-3880 .- 1867-3899. ; 5:2, s. 612-618
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Tidskriftsartikel (refereegranskat)abstract
- The applications of a heterogeneous Pd0-AmP-MCF nanoparticle catalyst in Suzuki cross-coupling reactions and transfer hydrogenations of alkenes are described. The catalyst was highly efficient for both transformations, resulting in 1)coupling of a wide range of aryl halides with various boronic acids in high yields and 2)chemoselective reduction of a variety of alkenes with the use of 1-methyl-1,4-cyclohexadiene as hydrogen donor. Moreover, the catalyst can be recycled several times without any significant decrease in activity or leaching of metal into solution, making the protocol economical and environmentally friendly. In the case of the Suzuki cross-coupling, a 15-fold increase in reaction rate was observed if the reaction was performed under microwave irradiation compared to conventional heating in an oil bath.
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| 43. |
- Verho, Oscar, et al.
(författare)
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Nanopalladium on Amino-Functionalized Mesocellular Foam as an Efficient and Recyclable Catalyst for the Selective Transfer Hydrogenation of Nitroarenes to Anilines
- 2014
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Ingår i: ChemCatChem. - : Wiley-VCH Verlagsgesellschaft. - 1867-3880 .- 1867-3899. ; 6:1, s. 205-211
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Tidskriftsartikel (refereegranskat)abstract
- Herein, we report on the use of nanopalladium on amino-functionalized siliceous mesocellular foam as an efficient heterogeneous catalyst for the transfer hydrogenation of nitroarenes to anilines. In all cases, the protocol proved to be highly selective and favored the formation of the desired aniline as the single product in high yields with short reaction times if naturally occurring and renewable -terpinene was employed as the hydrogen donor. Furthermore, the catalyst displayed excellent recyclability over five cycles and negligible leaching of metal into solution, which makes it an eco-friendly and economic catalyst to perform this transformation. The scalability of the protocol was demonstrated with the reduction of 4-nitroanisole on a 2g scale, in which p-anisidine was isolated in 98% yield.
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| 44. |
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| 45. |
- Verho, Oscar, et al.
(författare)
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Well-Defined Palladium Nanoparticles Supported on Siliceous Mesocellular Foam as Heterogeneous Catalysts for the Oxidation of Water
- 2015
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Ingår i: Chemistry - A European Journal. - : Wiley. - 0947-6539 .- 1521-3765. ; 21:15, s. 5909-5915
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Tidskriftsartikel (refereegranskat)abstract
- Herein, we describe the use of Pd nanoparticles immobilized on an amino-functionalized siliceous mesocellular foam for the catalytic oxidation of H2O. The Pd nanocatalyst proved to be capable of mediating the four-electron oxidation of H2O to O-2, both chemically and photochemically. The Pd nanocatalyst is easy to prepare and shows high chemical stability, low leaching, and recyclability. Together with its promising catalytic activity, these features make the Pd nanocatalyst of potential interest for future sustainable solar-fuel production.
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| 46. |
- Waara, Erik R., et al.
(författare)
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Entrapping Digestive Enzymes with Engineered Mesoporous Silica Particles Reduces Metabolic Risk Factors in Humans
- 2020
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Ingår i: Advanced Healthcare Materials. - : Wiley. - 2192-2640 .- 2192-2659. ; 9:11
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Tidskriftsartikel (refereegranskat)abstract
- Engineered mesoporous silica particles (MSP) are thermally and chemically stable porous materials composed of pure silica and have attracted attention for their potential biomedical applications. Oral intake of engineered MSP is shown to reduce body weight and adipose tissue in mice. Here, clinical data from a first-in-humans study in ten healthy individuals with obesity are reported, demonstrating a reduction in glycated hemoglobin (HbA1c) and low-density lipoprotein cholesterol, which are well-established metabolic and cardiovascular risk factors. In vitro investigations demonstrate sequestration of pancreatic alpha-amylase and lipase in an MSP pore-size dependent manner. Subsequent ex vivo experiments in conditions mimicking intestinal conditions and in vivo experiments in mice show a decrease in enzyme activity upon exposure to the engineered MSP, presumably by the same mechanism. Therefore, it is suggested that tailored MSP act by lowering the digestive enzyme availability in the small intestine, resulting in decreased digestion of macronutrient and leading to reduced caloric uptake. This novel MSP based mechanism-of-action, combined with its excellent safety in man, makes it a promising future agent for prevention and treatment of metabolic diseases.
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