The conversion of carbon dioxide into value-added products is of great industrial and environmental interest. However, as carbon dioxide is relatively stable, the input energy required for this conversion is a significant limiting factor in the system's performance. By utilising energy from the sun, through a range of key routes, this limitation can be overcome. In this review, we present a comprehensive and critical overview of the potential routes to harvest the sun's energy, primarily through solar-thermal technologies and plasmonic resonance effects. Focusing on the localised heating approach, this review shortlists and compares viable catalysts for the photo-thermal catalytic conversion of carbon dioxide. Further, the pathways and potential products of different carbon dioxide conversion routes are outlined with the reverse water gas shift, methanation, and methanol synthesis being of key interest. Finally, the challenges in implementing such systems and the outlook to the future are detailed. Keywords: Carbon dioxide conversion, Photo-thermal, Plasmonic catalysis, Solar therma
Although photoexcitation has been employed to unlock the low-temperature equilibrium regimes of thermal catalysis, mechanism underlining potential interplay between electron excitations and surface chemical processes remains elusive. Here, we report an associative zinc oxide band-gap excitation and copper plasmonic excitation that can cooperatively promote methanol-production at the copper-zinc oxide interfacial perimeter of copper/zinc oxide/alumina (CZA) catalyst. Conversely, selective excitation of individual components only leads to the promotion of carbon monoxide production. Accompanied by the variation in surface copper oxidation state and local electronic structure of zinc, electrons originating from the zinc oxide excitation and copper plasmonic excitation serve to activate surface adsorbates, catalysing key elementary processes (namely formate conversion and hydrogen molecule activation), thus providing one explanation for the observed photothermal activity. These observations give valuable insights into the key elementary processes occurring on the surface of the CZA catalyst under light-heat dual activation.
To address an important challenge in the engineering of antioxidant nanoparticles, the present work devised a surface-to-bulk migration of oxygen vacancies in the oxygen radical-scavenging cerium-oxide nanoparticles. The study highlights the significance of surface oxygen vacancies in the intended cellular internalization and, subsequently, the radical scavenging activity of the nanoparticles inside the cells. The findings advise future development of therapeutic antioxidant nanomaterials to also include engineering of the particles for enhanced surface defects not only for the accessibility of their oxygen vacancies but also, equally important, rendering them bioavailable for cellular uptake.
31 August 2017 in ACS Applied Materials & Interfaces