Phase coexistence of multiple copper oxides on AgCu catalysts during ethylene epoxidation

Alloy catalysts under reaction conditions are complex entities. In oxidizing atmospheres, multiple phases can coexist on a catalyst s surface as a result of phase segregation and preferential oxidation. Such a scenario can result in unusual substoichiometric and metastable phases that could play important roles in catalytic processes. For instance, AgCu alloys known to exhibit enhanced epoxide selectivity in partial oxidation of ethylene form an oxide like surface structure under reaction conditions. Under these conditions, copper oxides are stable, while silver oxides are not. Consequently, copper segregates to the alloy s surface and forms an oxide overlayer. Little is known about the structure or function of such overlayers, and it is unknown whether they play an active role in the catalyst s enhanced selectivity. In order to develop a clearer picture of such catalysts, the current work utilizes several in situ spectroscopic and microscopic techniques to examine the copper oxide phases that form when AgCu is exposed to epoxidation conditions. It is found that several forms of oxidic Cu coexist simultaneously on the active catalyst s surface, namely, CuO, Cu2O, and some previously unreported form of oxidized Cu, referred to here as CuxOy. Online product analysis, performed during the in situ spectroscopic measurements, shows that increased epoxide selectivity is correlated with the presence of mixed copper oxidation states and the presence of the CuxOy species. These results support previous theoretical predictions that oxidic copper overlayers on silver play an active role in epoxidation. These results furthermore emphasize the need for in situ spectromicroscopic methods to understand the complexity of alloy catalyst

Do HCI and NLP Interact?

We examine the relationship between HCI and Natural Language Processing (NLP) by performing a bibliometric analysis and looking at the specific example of BioNLP. We identify opportunities for HCI to fertilise current NLP research and suggest that HCI will benefit from looking at advances in NLP more closely

Crossover from directed percolation to compact directed percolation

We study critical spreading in a surface-modified directed percolation model in which the left- and right-most sites have different occupation probabilities than in the bulk. As we vary the probability for growth at an edge, the critical exponents switch from the compact directed percolation class to ordinary directed percolation. We conclude that the nonuniversality observed in models with multiple absorbing configurations cannot be explained as a simple surface effect.Comment: 4 pages, Revtex, 5 figures postscrip

Nitrides as ammonia synthesis catalysts and as potential nitrogen transfer reagents

In this article, an overview of the application of selected metal nitrides as ammonia synthesis catalysts is presented. The potential development of some systems into nitrogen transfer reagents is also described

Effect of Solution Composition on the Energy Production by Capacitive Mixing in Membrane-Electrode Assembly

The final edited version of the paper can be found at: http://pubs.acs.org/articlesonrequest/AOR-c9UMxSzGY3eiU5SENNgT The complete citation is: Ahualli, S.; et al. Effect of Solution Composition on the Energy Production by Capacitive Mixing in Membrane-Electrode Assembly. Journal of Physical Chemistry, 118(29): 15590-15599 (2014). DOI:10.1021/jp504461mOpen access in the Journal on May 26, 2015In this work we consider the extent to which the presence of multi-valent ions in solution modifies the equilibrium and dynamics of the energy production in a capacitive cell built with ion-exchange membranes in contact with high surface area electrodes. The cell potential in open circuit (OCV) is controlled by the difference between both membrane potentials, simulated as constant volume charge regions. A theoretical model is elaborated for steady state OCV, first in the case of monovalent solutions, as a reference. This is compared to the results in multi-ionic systems, containing divalent cations in concentrations similar to those in real sea water. It is found that the OCV is reduced by about 25 % (as compared to the results in pure NaCl solutions) due to the presence of the divalent ions, even in low concentrations. Interestingly, this can be related to the “uphill” transport of such ions against their concentration gradients. On the contrary, their effect on the dynamics of the cell potential is negligible in the case of highly charged membranes. The comparison between model predictions and experimental results shows a very satisfactory agreement, and gives clues for the practical application of these recently introduced energy production methods.The research leading to these results received funding from the European Union 7th Framework Programme (FP7/2007-2013) under agreement No. 256868. Further financial support from Junta de Andalucia, Spain (PE2012-FQM 694) is also acknowledged. One of us, M.M.F., received financial support throughan FPU grant from the Universityof Granada