| 1. |
- Santangelo, James S., et al.
(författare)
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Global urban environmental change drives adaptation in white clover
- 2022
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Ingår i: Science. - : American Association for the Advancement of Science (AAAS). - 0036-8075 .- 1095-9203. ; 375
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Tidskriftsartikel (refereegranskat)abstract
- Urbanization transforms environments in ways that alter biological evolution. We examined whether urban environmental change drives parallel evolution by sampling 110,019 white clover plants from 6169 populations in 160 cities globally. Plants were assayed for a Mendelian antiherbivore defense that also affects tolerance to abiotic stressors. Urban-rural gradients were associated with the evolution of clines in defense in 47% of cities throughout the world. Variation in the strength of clines was explained by environmental changes in drought stress and vegetation cover that varied among cities. Sequencing 2074 genomes from 26 cities revealed that the evolution of urban-rural dines was best explained by adaptive evolution, but the degree of parallel adaptation varied among cities. Our results demonstrate that urbanization leads to adaptation at a global scale.
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| 2. |
- Abdellaoui, G., et al.
(författare)
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First observations of speed of light tracks by a fluorescence detector looking down on the atmosphere
- 2018
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Ingår i: Journal of Instrumentation. - : IOP PUBLISHING LTD. - 1748-0221. ; 13
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Tidskriftsartikel (refereegranskat)abstract
- EUSO-Balloon is a pathfinder mission for the Extreme Universe Space Observatory onboard the Japanese Experiment Module (JEM-EUSO). It was launched on the moonless night of the 25(th) of August 2014 from Timmins, Canada. The flight ended successfully after maintaining the target altitude of 38 km for five hours. One part of the mission was a 2.5 hour underflight using a helicopter equipped with three UV light sources (LED, xenon flasher and laser) to perform an inflight calibration and examine the detectors capability to measure tracks moving at the speed of light. We describe the helicopter laser system and details of the underflight as well as how the laser tracks were recorded and found in the data. These are the first recorded laser tracks measured from a fluorescence detector looking down on the atmosphere. Finally, we present a first reconstruction of the direction of the laser tracks relative to the detector.
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| 3. |
- Cavalca, Filippo, et al.
(författare)
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Nature and Distribution of Stable Subsurface Oxygen in Copper Electrodes During Electrochemical CO2 Reduction
- 2017
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Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 121:45, s. 25003-25009
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Tidskriftsartikel (refereegranskat)abstract
- Oxide-derived copper (OD-Cu) electrodes exhibit higher activity than pristine copper during the carbon dioxide reduction reaction (CO2RR) and higher selectivity toward ethylene. The presence of residual subsurface oxygen in OD-Cu has been proposed to be responsible for such improvements, although its stability under the reductive CO2RR conditions remains unclear. This work sheds light on the nature and stability of subsurface oxygen. Our spectroscopic results show that oxygen is primarily concentrated in an amorphous 1-2 nm thick layer within the Cu subsurface, confirming that subsurface oxygen is stable during CO2RR for up to 1 h at -1.15 V vs RHE. Besides, it is associated with a high density of defects in the OD-Cu structure. We propose that both low coordination of the amorphous OD-Cu surface and the presence of subsurface oxygen that withdraws charge from the copper sp- and d-bands might selectively enhance the binding energy of CO.
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| 4. |
- Diaz-Morales, Oscar, et al.
(författare)
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Catalytic effects of molybdate and chromate–molybdate films deposited on platinum for efficient hydrogen evolution
- 2023
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Ingår i: Journal of chemical technology and biotechnology (1986). - : Wiley. - 0268-2575 .- 1097-4660. ; 98:5, s. 1269-1278
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Tidskriftsartikel (refereegranskat)abstract
- BACKGROUND: Sodium chlorate (NaClO3) is extensively used in the paper industry, but its production uses strictly regulated highly toxic Na2Cr2O7 to reach high hydrogen evolution reaction (HER) Faradaic efficiencies. It is therefore important to find alternatives either to replace Na2Cr2O7 or reduce its concentration.RESULTS: The Na2Cr2O7 concentration can be significantly reduced by using Na2MoO4 as an electrolyte co-additive. Na2MoO4 in the millimolar range shifts the platinum cathode potential to less negative values due to an activating effect of cathodically deposited Mo species. It also acts as a stabilizer of the electrodeposited chromium hydroxide but has a minor effect on the HER Faradaic efficiency. X-ray photoelectron spectroscopy (XPS) results show cathodic deposition of molybdenum of different oxidation states, depending on deposition conditions. Once Na2Cr2O7 was present, molybdenum was not detected by XPS, as it is likely that only trace levels were deposited. Using electrochemical measurements and mass spectrometry we quantitatively monitored H2 and O2 production rates. The results indicate that 3 μmol L−1 Na2Cr2O7 (contrary to current industrial 10–30 mmol L−1) is sufficient to enhance the HER Faradaic efficiency on platinum by 15%, and by co-adding 10 mmol L−1 Na2MoO4 the cathode is activated while avoiding detrimental O2 generation from chemical and electrochemical reactions. Higher concentrations of Na2MoO4 led to increased oxygen production.CONCLUSION: Careful tuning of the molybdate concentration can enhance performance of the chlorate process using chromate in the micromolar range. These insights could be also exploited in the efficient hydrogen generation by photocatalytic water splitting and in the remediation of industrial wastewater.
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| 5. |
- Diaz-Morales, Oscar
(författare)
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Impurity as a virtue
- 2020
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Ingår i: NATURE ENERGY. - : NATURE PUBLISHING GROUP. - 2058-7546. ; 5:3, s. 193-194
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Tidskriftsartikel (övrigt vetenskapligt/konstnärligt)abstract
- Understanding the activity and stability of oxygen-evolving anodes is crucial for developing better water splitting electrolysers. Researchers now show the importance of interactions between iron and hydr(oxy)oxide hosts in dynamically-stable electrocatalysts that balance dissolution and deposition of iron present in the electrolyte.
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| 6. |
- Diaz-Morales, Oscar, et al.
(författare)
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Oxygen evolution reaction catalyzed by cost-effective metal oxides
- 2018
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Ingår i: Encyclopedia of Interfacial Chemistry: Surface Science and Electrochemistry. - : Elsevier. - 9780128098943 - 9780128097397 ; , s. 785-795
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Bokkapitel (övrigt vetenskapligt/konstnärligt)abstract
- Oxygen evolution anodes are extensively used in industrial processes like electroplating and electrowinning. These anodes also play a crucial role in enhancing the kinetics of the oxygen evolution reaction (OER), which is one of the major bottlenecks in the conversion and storage of clean and sustainable energy using electrolyzers. Therefore, the prediction, development and test of active, cost-effective, and stable OER materials is one of the central challenges of modern electrocatalysis and electrochemical engineering. In this framework, this article will discuss some of the computational tools that can be used to understand the activity of existing OER catalysts and also provide guidelines for the rational design of new OER materials. We will also present some of the most active catalysts for the OER in both acid and alkaline electrolytes. We will show the tremendous effect that the catalysts’ crystal structure and the electrolyte’s pH have on the catalytic activity. In this regard, theoretically and experimentally understanding the catalyst-electrolyte synergy at the interface is challenging, but it can allow one to carefully select the optimal operating conditions (e.g., catalyst’s crystal structure, cations, anions, pH) to design efficient electrolyzers.
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| 7. |
- Diaz, Oscar E., et al.
(författare)
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Perfluorooctanesulfonic acid modulates barrier function and systemic T-cell homeostasis during intestinal inflammation
- 2021
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Ingår i: DMM Disease Models and Mechanisms. - : The Company of Biologists. - 1754-8411 .- 1754-8403. ; 14:12, s. 1-11
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Tidskriftsartikel (refereegranskat)abstract
- The intestinal epithelium is continuously exposed to deleterious environmental factors that might cause aberrant immune responses leading to inflammatory disorders. However, what environmental factors might contribute to disease are poorly understood. Here, to overcome the lack of in vivo models suitable for screening of environmental factors, we used zebrafish reporters of intestinal inflammation. Using zebrafish, we interrogated the immunomodulatory effects of polyfluoroalkyl substances, which have been positively associated with ulcerative colitis incidence. Exposure to perfluorooctanesulfonic acid (PFOS) during 2,4,6-trinitro-benzene sulfonic acid (TNBS)-induced inflammation enhanced the expression of proinflammatory cytokines as well as neutrophil recruitment to the intestine of zebrafish larvae, which was validated in the TNBS-induced colitis mouse model. Moreover, PFOS exposure in mice undergoing colitis resulted in neutrophil-dependent increased intestinal permeability and enhanced PFOS translocation into the circulation. This was associated with a neutrophil-dependent expansion of systemic CD4+ T cells. Thus, our results indicate that PFOS worsens inflammation-induced intestinal damage with disruption of T-cell homeostasis beyond the gut and provides a novel in vivo toolbox to screen for pollutants affecting intestinal homeostasis.
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| 8. |
- Endrodi, Balazs, et al.
(författare)
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Selective electrochemical hydrogen evolution on cerium oxide protected catalyst surfaces
- 2020
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Ingår i: Electrochimica Acta. - : Elsevier BV. - 0013-4686 .- 1873-3859. ; 341
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Tidskriftsartikel (refereegranskat)abstract
- To date the only known solution to avoid the unwanted electrochemical reduction of hypochlorite and chlorate in industrial chlorate production, performed in undivided cells, is the addition of dichromate to the chlorate electrolyte. Because of the toxicity of this compound its use is restricted within the European Union to time limited authorization by REACH. Therefore, an alternative to sodium dichromate is essential to maintain, or even increase the process efficiency. The addition of cerium (III) salts to a hypochlorite solution increases the cathodic selectivity towards hydrogen evolution (HER), the preferred cathode process in industrial chlorate production. This is attributed to the deposition of a thin cerium oxide/hydroxide coating on the cathode, induced by the increased local alkalinity during electrolysis. Performing the electrodeposition of such protective coating ex situ, well-controlled coating thickness can be achieved. Optimizing the deposition conditions (time, current density), a coherent and stable coating is formed on the electrode surface. On this protected electrode surface the electrochemical reduction of hypochlorite is suppressed by ca. 90% compared to the bare Pt electrode, while the HER proceeds with high selectivity and unchanged kinetics. Interestingly, other electrochemical reactions (O-2 reduction, H2O2 reduction and oxidation) are also suppressed by the protective coating, suggesting that the deposited layer acts as an inorganic membrane on the electrode surface.
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| 9. |
- Gimpel, Thomas, et al.
(författare)
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Electrochemical Carbon Dioxide Reduction on Femtosecond Laser-Processed Copper Electrodes : Effect on the Liquid Products by Structuring and Doping
- 2021
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Ingår i: ACS Applied Energy Materials. - : American Chemical Society (ACS). - 2574-0962. ; 4:6, s. 5927-5934
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Tidskriftsartikel (refereegranskat)abstract
- A femtosecond laser process is presented increasing the surface area of copper electrocatalysts for an electrochemical CO2 reduction reaction (CO2RR). The laser treatment allows us to tune the surface morphology and the chemical composition of the copper electrocatalysts. This tunability is used to correlate the role of the surface area and catalyst dopants with the selectivity of the CO2RR. The liquid products of the CO2RR are monitored through ex situ nuclear magnetic resonance spectroscopy. The products’ distribution shows that the electrode surface area plays a key role in the electrochemical conversion of CO2 into multicarbon liquid products. We show that sulfur dopants boost the production of formate. Remarkably, by co-doping sulfur and fluoride, we show that the chalcogenide dopant counteracts the known boosting effect of fluoride to convert CO2 into multicarbon products. Oxygen doping in the range of 2–19 atom % does not significantly affect the distribution of liquid products from CO2 electroreduction. In a broad perspective, this work highlights the potential of the femtosecond laser process to fine-tune surfaces to produce photo- and electrocatalyst materials.
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| 10. |
- Görlin, Mikaela, et al.
(författare)
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Key activity descriptors of nickel-iron oxygen evolution electrocatalysts in the presence of alkali metal cations
- 2020
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Ingår i: Nature Communications. - : Springer Nature. - 2041-1723. ; 11:1
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Tidskriftsartikel (refereegranskat)abstract
- Efficient oxygen evolution reaction (OER) electrocatalysts are pivotal for sustainable fuel production, where the Ni-Fe oxyhydroxide (OOH) is among the most active catalysts for alkaline OER. Electrolyte alkali metal cations have been shown to modify the activity and reaction intermediates, however, the exact mechanism is at question due to unexplained deviations from the cation size trend. Our X-ray absorption spectroelectrochemical results show that bigger cations shift the Ni2+/(3+delta)+ redox peak and OER activity to lower potentials (however, with typical discrepancies), following the order CsOH>NaOH approximate to KOH>RbOH>LiOH. Here, we find that the OER activity follows the variations in electrolyte pH rather than a specific cation, which accounts for differences both in basicity of the alkali hydroxides and other contributing anomalies. Our density functional theory-derived reactivity descriptors confirm that cations impose negligible effect on the Lewis acidity of Ni, Fe, and O lattice sites, thus strengthening the conclusions of an indirect pH effect. It is commonly accepted that electrolyte alkali metal cations modify the catalytic activity for oxygen evolution reaction. Here the authors challenge this assumption, showing that the activity is actually affected by a change in the electrolyte pH rather than a specific alkali cation.
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| 11. |
- Han, Binghong, et al.
(författare)
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Iron-Based Perovskites for Catalyzing Oxygen Evolution Reaction
- 2018
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Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 122:15, s. 8445-8454
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Tidskriftsartikel (refereegranskat)abstract
- The slow kinetics of the oxygen evolution reaction (OER) is the main cause of energy loss in many low temperature energy storage techniques, such as metal air batteries and water splitting. A better understanding of both the OER mechanism and the degradation mechanism on different transition metal (TM) oxides is critical for the development of the, next generation of oxides as OER catalysts. In this paper, we systematically investigated the catalytic mechanism and lifetime of ABO(3-delta) perovskite catalysts for the OER, where A = Sr or Ca and B = Fe or Co. During the OER process, the Fe-based AFeO(3-delta) oxides with (delta approximate to 0.5 demonstrate no activation of lattice oxygen or pH dependence of the OER activity, which is different from the SrCoO25 with similar oxygen 2p-band position relative to the Fermi level. The difference was attributed to the larger changes in the electronic structure during the transition from the oxygen-deficient brownmillerite structure to the fully oxidized perovskite structure and the poor conductivity in Fe-based oxides, which hinders the uptake of oxygen from the electrolyte to the lattice under oxidative potentials. The low stability of Fe-based perovskites under OER conditions in a basic electrolyte also contributes to the different OER mechanism compared with the Co-based perovskites. This work reveals the influence of TM composition and electronic structure on the catalytic mechanism and operational stability of the perovskite OER catalysts.
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| 12. |
- Koroidov, Sergey, et al.
(författare)
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Chemisorbed oxygen or surface oxides steer the selectivity in Pd electrocatalytic propene oxidation observed by operando Pd L-edge X-ray absorption spectroscopy
- 2021
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Ingår i: Catalysis Science & Technology. - : Royal Society of Chemistry (RSC). - 2044-4753 .- 2044-4761. ; 11:10, s. 3347-3352
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Tidskriftsartikel (refereegranskat)abstract
- Controlled electrochemical oxidation of hydrocarbons to desired products is an attractive approach in catalysis. Here we study the electrochemical propene oxidation under operando conditions using Pd L-edge X-ray absorption spectroscopy (XAS) as a sensitive probe to elucidate surface processes occurring during catalysis. Together with ab initio multiple-scattering calculations, our XAS results enable assignment of characteristic changes of the Pd L-edge intensity and energy position in terms of a mechanistic understanding of the selective oxidation of propene. The results, supported by electrochemical density functional theory DFT simulations, show that in the potential range of 0.8–1.0 V vs. the reversible hydrogen electrode (RHE), selective oxidation of propene to acrolein and acrylic acid occurs on the metallic Pd surface. These reactions are proposed to proceed via the Langmuir–Hinshelwood mechanism. In contrast, for the potential range of 1.1–1.3 V vs. RHE, selective oxidation of propene to propylene glycol takes place on a Pd oxide surface.
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| 13. |
- Lindberg, Aleksandra, 1990-, et al.
(författare)
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Sources of Oxygen Produced in the Chlorate Process Utilizing Dimensionally Stable Anode (DSA) Electrodes Doped by Sn and Sb
- 2021
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Ingår i: Industrial & Engineering Chemistry Research. - : American Chemical Society (ACS). - 0888-5885 .- 1520-5045. ; 60:37, s. 13505-13514
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Tidskriftsartikel (refereegranskat)abstract
- Identifying the sources of oxygen in the chlorate process is challenging due to the complex set of chemical and electrochemical reactions involved. Here, two types of electrodes have been investigated-Ti0.7Ru0.3Ox, and electrodes with aimed composition Ti0.34Ru0.3Sn0.3Sb0.06Ox, both compared with platinum anodes. The cell oxygen off-gas was analyzed employing mass spectrometry together with ex situ UV-vis spectroscopy to quantify the kinetic rate constants. Noteworthy is that the respective rates of oxygen formation from anodic and chemical reactions in the presence of hypochlorite are of the same magnitude. The addition of Sn and Sb doubled the surface area of the electrodes and decreased oxygen production when electrodes were used for the first time. However, rate constants for total oxygen production with reused electrodes follow the trend: homogeneous hypochlorite decomposition < TiRu < TiRuSnSb to the highest value obtained by Pt. The same trend is noticed for rate constants concerning the hypochlorite decomposition.
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| 14. |
- Lindberg, Aleksandra, 1990-, et al.
(författare)
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Sources of oxygen produced in the chlorate process utilizing DSA electrodes doped by Sn and Sb
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Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- Identifying the sources of oxygen in the chlorate process is challenging due to the complex set of chemical and electrochemical reactions involved. Here, two types of electrodes have been investigated -Ti0.7Ru0.3Ox, and electrodes with aimed composition Ti0.34Ru0.3Sn0.3Sb0.06Ox, both compared with platinum anodes. The cell oxygen off-gas was analyzed employing mass spectrometry together with ex-situ UV-Vis spectroscopy to quantify the kinetic rate constants. Noteworthy is that the respective rates of oxygen formation from anodic and chemical reactions in the presence of hypochlorite are of the same magnitude. The addition of Sn and Sb doubled the surface area of the electrodes and decreased oxygen production when electrodes were used for the first time. However, rate constants for total oxygen production with reused electrodes, follow the trend: homogenous hypochlorite decomposition < TiRu < TiRuSnSb to the highest value obtained by Pt. The same trend is noticed for rate constants concerning the hypochlorite decomposition.
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| 15. |
- Liu, Chang, et al.
(författare)
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Stability and Effects of Subsurface Oxygen in Oxide-Derived Cu Catalyst for CO2 Reduction
- 2017
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Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 121:45, s. 25010-25017
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Tidskriftsartikel (refereegranskat)abstract
- Oxide-derived copper (OD-Cu) catalysts are promising candidates for the electrochemical CO2 reduction reaction (CO2RR) due to the enhanced selectivity toward ethylene over methane evolution, which has been linked to the presence of subsurface oxygen (O-sb). In this work, O-sb is investigated with theoretical methods. Although O-sb is unstable in slab models, it becomes stabilized within a manually reduced OD-Cu nanocube model which was calculated by self-consistent charge density functional tight binding (SCC-DFTB). The results obtained with SCC-DFTB for the full nanocube were confirmed with subcluster models extracted from the nanocube, calculated with both density functional theory (DFT) and SCC-DFTB. The. higher stability of O-sb in the nanocube is attributed to the disordered structure and greater flexibility. The adsorption strength of CO on Cu(100) is enhanced by O-sb withdrawing electron density from the Cu atom, resulting in reduction of the sigma-repulsion. Hence, the coverage of CO may be increased, facilitating its dimerization.
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| 16. |
- Parigi, Sara M., et al.
(författare)
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The spatial transcriptomic landscape of the healing mouse intestine following damage
- 2022
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Ingår i: Nature Communications. - : Springer Nature. - 2041-1723. ; 13:1
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Tidskriftsartikel (refereegranskat)abstract
- The colon is comprised of specialized cells that interact with each other to function, however, the molecular regionalization of the colon is incompletely understood. Here, the authors use spatial transcriptomics to generate a publicly available resource defining the transcriptomic regionalization of the colon during steady state and mucosal healing. The intestinal barrier is composed of a complex cell network defining highly compartmentalized and specialized structures. Here, we use spatial transcriptomics to define how the transcriptomic landscape is spatially organized in the steady state and healing murine colon. At steady state conditions, we demonstrate a previously unappreciated molecular regionalization of the colon, which dramatically changes during mucosal healing. Here, we identified spatially-organized transcriptional programs defining compartmentalized mucosal healing, and regions with dominant wired pathways. Furthermore, we showed that decreased p53 activation defined areas with increased presence of proliferating epithelial stem cells. Finally, we mapped transcriptomics modules associated with human diseases demonstrating the translational potential of our dataset. Overall, we provide a publicly available resource defining principles of transcriptomic regionalization of the colon during mucosal healing and a framework to develop and progress further hypotheses.
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| 17. |
- Stoerzinger, Kelsey A., et al.
(författare)
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Orientation-Dependent Oxygen Evolution on RuO2 without Lattice Exchange
- 2017
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Ingår i: ACS Energy Letters. - : American Chemical Society (ACS). - 2380-8195. ; 2:4, s. 876-881
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Tidskriftsartikel (refereegranskat)abstract
- RuO2 catalysts exhibit record activities toward the oxygen evolution reaction (OER), which is crucial to enable efficient and sustainable energy storage. Here we examine the RuO2 OER kinetics on rutile (110), (100), (101), and (111) orientations, finding (100) the most active. We assess the potential involvement of lattice oxygen in the OER mechanism with online electrochemical mass spectrometry, which showed no evidence of oxygen exchange on these oriented facets in acidic or basic electrolytes. Similar results were obtained for polyoriented RuO2 films and particles, in contrast to previous work, suggesting lattice oxygen is not exchanged in catalyzing OER on crystalline RuO2 surfaces. This hypothesis is supported by the correlation of activity with the number of active Ru-sites calculated by density functional theory, where more active facets bind oxygen more weakly. This new understanding of the active sites provides a design strategy to enhance the OER activity of RuO2 nanoparticles by facet engineering.
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