Optical printing holds great potential to enable the use of the vast variety of colloidal nanoparticles (NPs) in nano- and microdevices and circuits. By means of optical forces, it enables the direct assembly of NPs, one by one, onto specific positions of solid surfaces with great flexibility of pattern design and no need of previous surface patterning. However, for unclear causes it was not possible to print identical NPs closer to each other than 300 nm. Here, we show that the repulsion restricting the optical printing of close by NPs arises from light absorption by the printed NPs and subsequent local heating. By optimizing heat dissipation, it is possible to reduce the minimum separation between NPs. Using a reduced graphene oxide layer on a sapphire substrate, we demonstrate for the first time the optical printing of Au-Au NP dimers. Modeling the experiments considering optical, thermophoretic, and thermo-osmotic forces we obtain a detailed understanding and a clear pathway for the optical printing fabrication of complex nano structures and circuits based on connected colloidal NPs.
The preferential CO oxidation (CO-PROX) reaction is paramount for the 22 purification of reformate H 2 -rich streams, where CuO/CeO 2 catalysts show promising 23 opportunities. This work sheds light on the lattice oxygen recovery mechanism on 24 CuO/CeO 2 catalysts during CO-PROX reaction, which is critical to guarantee both good 25 activity and selectivity, but that is yet to be well understood. Particularly, in situ Raman 26 spectroscopy reveals that oxygen vacancies in the ceria lattice do not form in significant 27 amounts until advanced reaction degrees, whereas pulse O 2 isotopic tests confirm the
Background: The mechanisms and pathways to impacts from public health research in the UK have not been widely studied. Through the lens of one funder (NIHR), our aims are to map the diversity of public health research, in terms of funding mechanisms, disciplinary contributions, and public health impacts, identify examples of impacts, and pathways to impact that existing reporting mechanisms may not otherwise have captured, and provide illustrations of how public health researchers perceive the generation of non-academic impact from their work. Methods: A total of 1386 projects were identified as 'public health research' by the NIHR and listed in the NIHR Public Health Overview database (2000)(2001)(2002)(2003)(2004)(2005)(2006)(2007)(2008)(2009)(2010)(2011)(2012)(2013)(2014)(2015)(2016). From these, a subset of 857 projects were matched as potentially having begun reporting impacts via an external data-gathering platform (Researchfish). Data on the 857 projects were analyzed quantitatively, and nine projects were selected to investigate further through semi-structured interviews with principal investigators. Two workshops took place to validate emerging and final findings and facilitate analysis.Results: In addition to the NIHR School for Public Health Research and the NIHR Public Health Research Programme, 89% of projects contained in the NIHR Public Health Overview portfolio as 'public health research' are funded via other NIHR research programmes, suggesting significant diversity in disciplines contributing to public health research and outcomes. The pathways to impact observed in our in-depth case studies include contributing to debates on what constitutes appropriate evidence for national policy change, acknowledging local 'unintended' impacts, building trusted relationships with stakeholders across health and non-health sectors and actors, collaborating with local authorities, and using non-academic dissemination channels. Conclusions: Public health as a discipline contributes substantially to impact beyond academia. To support the diversity of these impacts, we need to recognise localized smaller-scale impacts, and the difference in types of evidence required for community and local authority-based impacts. This will also require building capacity and resources to enable impact to take place from public health research. Finally, support is required for engagement with local authorities and working with non-health sectors that contribute to health outcomes.
Compositional changes taking place during the synthesis of alloyed CdSeZnS nanocrystals (NCs) allow shifting of the optical features to higher energy as the NCs grow. Under certain synthetic conditions, the effect of those changes on the surface/interface chemistry competes with and dominates over the conventional quantum confinement effect in growing NCs. These changes, identified by means of complementary advanced spectroscopic techniques such as XPS (X-ray photoelectron spectroscopy) and XAS (X-ray absorption spectroscopy), are understood in the frame of an ion migration and exchange mechanism taking place during the synthesis. Control over the synthetic routes during NC growth represents an alternative tool to tune the optical properties of colloidal quantum dots, broadening the versatility of the wet chemical methods.
In this work, photocatalytic reduction of methyl viologen is achieved using zinc tetra(4-N-methylpyridyl)porphine (ZnP) functionalized mesoporous titania thin films (MTTF). Also, ZnP sensitizing and photophysical properties are retained in the hybrid material.
Despite the increasing economic incentives and environmental advantages associated to their substitution, carbon-rich fossil fuels are expected to remain as the dominant worldwide source of energy through at least the next two decades and perhaps later. Therefore, both the control and reduction of CO2 emissions have become environmental issues of major concern and big challenges for the international scientific community. Among the proposed strategies to achieve these goals, conversion of CO2 by its reduction into high added value products, such as methane or syngas, has been widely agreed to be the most attractive from the environmental and economic points of view. In the present work, thermocatalytic reduction of CO2 with H2 was studied over a nanostructured ceria-supported nickel catalyst. Ceria nanocubes were employed as support, while the nickel phase was supported by means a surfactant-free controlled chemical precipitation method. The resulting nanocatalyst was characterized in terms of its physicochemical properties, with special attention paid to both surface basicity and reducibility. The nanocatalyst was studied during CO2 reduction by means of Near Ambient Pressure X-ray Photoelectron Spectroscopy (NAP-XPS). Two different catalytic behaviors were observed depending on the reaction temperature. At low temperature, with both Ce and Ni in an oxidized state, CH4 formation was observed, whereas at high temperature above 500 °C, the reverse water gas shift reaction became dominant, with CO and H2O being the main products. NAP-XPS was revealed as a powerful tool to study the behavior of this nanostructured catalyst under reaction conditions.
This study addresses the yet unresolved CO2 methanation mechanism on a Ru/CeO2 catalyst by means of near-ambient-pressure X-ray photoelectron spectroscopy (NAP–XPS) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) complemented with periodic density functional theory (DFT) calculations. NAP–XPS results show that the switch from H2 to CO2 + H2 mixture oxidizes both the Ru and CeO2 phases at low temperatures, which is explained by the CO2 adsorption modes assessed by means of DFT on each representative surface. CO2 adsorption on Ru is dissociative and moderately endergonic, leading to polybonded Ru-carbonyl groups whose hydrogenation is the rate-determining step in the overall process. Unlike on Ru metal, CO2 can be strongly adsorbed as carbonates on ceria surface oxygen sites or on the reduced ceria at oxygen vacancies as carboxylates (CO2 –δ), resulting in the reoxidation of ceria. Carboxylates can then evolve as CO, which is released either via direct splitting at relatively low temperatures or through stable formate species at higher temperatures. DRIFTS confirm the great stability of formates, whose depletion relates with CO2 conversion in the reaction cell, while carbonates remain on the surface up to higher temperatures. CO generation on ceria serves as an additional reservoir of Ru-carbonyls, cooperating to the overall CO2 methanation process. Altogether, this study highlights the noninnocent role of the ceria support in the performance of Ru/CeO2 toward CO2 methanation.
Supported Pd/CeO2 catalytic systems have been widely investigated in the low-temperature oxidation of CO (LTO CO) due to the unique oxygen storage capacity and redox properties of the ceria support, which highly influence the structural, chemical and electronic state of Pd species. Herein, operando near-ambient pressure XPS (NAP-XPS) technique has allowed the study of a conventional Pd/CeO2 catalyst surface during the CO oxidation reaction under experimental conditions closer to the actual catalytic reaction, unfeasible with other surface science techniques that demand UHV conditions. SEM, HRTEM and XRD analyses of the powder catalyst, prepared by conventional incipient wetness impregnation, reveal uniformly CeO2-loaded Pd NPs of less than 2 nm size, which generated an increase in oxygen vacancies with concomitant ceria reduction, as indicated by H2-TPR and Raman measurements. Adsorbed peroxide (O22−) species on the catalyst surface could also be detected by Raman spectra. Operando NAP-XPS results obtained at the ALBA Synchrotron Light Source revealed two kinds of Pd species under reaction conditions, namely PdOx and PdII ions in a PdxCe1−xO2−δ solution, the latter one appearing to be crucial for the CO oxidation. By means of a non-destructive depth profile analysis using variable synchrotron excitation energies, the location and the role of these palladium species in the CO oxidation reaction could be clarified: PdOx was found to prevail on the upper surface layers of the metallic Pd supported NPs under CO, while under reaction mixture it was rapidly depleted from the surface, leaving a greater amount in the subsurface layers (7% vs. 12%, respectively). On the contrary, the PdxCe1−xO2−δ phase, which was created at the Pd–CeO2 interface in contact with the gas environment, appeared to be predominant on the surface of the catalyst. Its presence was crucial for CO oxidation evolution, acting as a route through which active oxygen species could be transferred from ceria to Pd species for CO oxidation.
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