Enhancing CO2 electrolysis through synergistic control of non-stoichiometry and doping to tune cathode surface structures

K.X. acknowledges Natural Science Foundation of China (91545123) and Natural Science Foundation of Fujian Province (2016J01275) for funding this work. C.L. acknowledges support by the Strategic Priority Research Program of the Chinese Academy of Sciences, Grant No. XDB20000000 and Hundred Talents Program of the Chinese Academy of Sciences. J.T.S.I. acknowledges funding from EPSRC Platform Grant EP/K015540/1 and Royal Society Wolfson Merit Award WRMA 2012/R2.Sustainable future energy scenarios require significant efficiency improvements in both electricity generation and storage. High-temperature solid oxide cells, and in particular carbon dioxide electrolysers, afford chemical storage of available electricity that can both stabilize and extend the utilization of renewables. Here we present a double doping strategy to facilitate CO2 reduction at perovskite titanate cathode surfaces, promoting adsorption/activation by making use of redox active dopants such as Mn linked to oxygen vacancies and dopants such as Ni that afford metal nanoparticle exsolution. Combined experimental characterization and first-principle calculations reveal that the adsorbed and activated CO2 adopts an intermediate chemical state between a carbon dioxide molecule and a carbonate ion. The dual doping strategy provides optimal performance with no degradation being observed after 100 h of high-temperature operation and 10 redox cycles, suggesting a reliable cathode material for CO2 electrolysis.Publisher PDFPeer reviewe

Enhancing CO₂ electrolysis through synergistic control of non-stoichiometry and doping to tune cathode surface structures

Sustainable future energy scenarios require significant efficiency improvements in both electricity generation and storage. High-temperature solid oxide cells, and in particular carbon dioxide electrolysers, afford chemical storage of available electricity that can both stabilize and extend the utilization of renewables. Here we present a double doping strategy to facilitate CO2 reduction at perovskite titanate cathode surfaces, promoting adsorption/activation by making use of redox active dopants such as Mn linked to oxygen vacancies and dopants such as Ni that afford metal nanoparticle exsolution. Combined experimental characterization and first-principle calculations reveal that the adsorbed and activated CO2 adopts an intermediate chemical state between a carbon dioxide molecule and a carbonate ion. The dual doping strategy provides optimal performance with no degradation being observed after 100 h of high-temperature operation and 10 redox cycles, suggesting a reliable cathode material for CO2 electrolysis

Luminescent Composite Carbon/SiO2 Structures: Synthesis and Applications

Luminescent carbon nanostructures (CNSs) have attracted great interest from the scientific community due to their photoluminescent properties, structural features, low toxicity, and a great variety of possible applications. Unfortunately, a few problems hinder their further development. These include the difficulties of separating a mixture of nanostructures after synthesis and the dependence of their properties on the environment and the aggregate state. The application of a silica matrix to obtain luminescent composite particles minimizes these problems and improves optical properties, reduces photoluminescence quenching, and leads to wider applications. We describe two methods for the formation of silica composites containing CNSs: inclusion of CNSs into silica particles and their grafting onto the silica surface. Moreover, we present approaches to the synthesis of multifunctional particles. They combine the unique properties of silica and fluorescent CNSs, as well as magnetic, photosensitizing, and luminescent properties via the combination of functional nanoparticles such as iron oxide nanoparticles, titanium dioxide nanoparticles, quantum dots (QDs), and gold nanoclusters (AuNCs). Lastly, we discuss the advantages and challenges of these structures and their applications. The novelty of this review involves the detailed description of the approaches for the silica application as a matrix for the CNSs. This will support researchers in solving fundamental and applied problems of this type of carbon-based nanoobjects