The electrocatalytic reduction of CO2 is studied on a series of electrodes (based on Cu, Co, Fe and Pt metal nanoparticles deposited on carbon nanotubes or carbon black and then placed at the interface between a Nafion membrane and a gas-diffusion-layer electrode) on two types of cells: one operating in the presence of a liquid bulk electrolyte and the other in the absence of the electrolyte (electrolyte-less conditions). The results evidence how the latter conditions allow productivity of about one order of magnitude higher and how to change the type of products formed. Under electrolyte-less conditions, the formation of >C2 products such as acetone and isopropanol is observed, but not in liquid-phase cell operations on the same electrodes. The relative order of productivity in CO2 electrocatalytic reduction in the series of electrodes investigated is also different between the two types of cells. The implications of these results in terms of possible differences in the reaction mechanism are commented on, as well as in terms of the design of photoelectrocatalytic (PEC) solar cells.
A meso-p-nitroaniline-calix[4]pyrrole derivative trans-coordinated to a Pt(II) center was synthesized and its structure solved by X-ray analysis. Adenosine monophosphate (AMP) was used as a model compound to evaluate the potential for the assisted delivery of the metal to the DNA nucleobases via the phosphate anion-binding properties of the calix[4]pyrrole unit. An NMR investigation of the kinetics of AMP complexation in the absence of an H-bonding competing solvent (dry CD(3)CN) was consistent with this hypothesis, but we could not detect the interaction of the calix[4]pyrrole with phosphate in the presence of water. However, in vitro tests of the new trans-calixpyrrole-Pt(II) complex on different cancer cell lines indicate a cytotoxic activity that is unquestionably derived from the coexistence of both the trans-Pt(II) fragment and the calix[4]pyrrole unit.
The prospects, needs
and limits in current approaches in catalysis
to accelerate the transition to
e
-chemistry, where
this term indicates a fossil fuel-free chemical production, are discussed.
It is suggested that
e
-chemistry is a necessary element
of the transformation to meet the targets of net zero emissions by
year 2050 and that this conversion from the current petrochemistry
is feasible. However, the acceleration of the development of catalytic
technologies based on the use of renewable energy sources (indicated
as reactive catalysis) is necessary, evidencing that these are part
of a system of changes and thus should be assessed from this perspective.
However, it is perceived that the current studies in the area are
not properly addressing the needs to develop the catalytic technologies
required for
e
-chemistry, presenting a series of
relevant aspects and directions in which research should be focused
to develop the framework system transformation necessary to implement
e
-chemistry.
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