Nanopatterning and nanoconfinement for deterministic control of the local homogeneous and heterogeneous chemical environment in electrocatalytic co2rr towards c3+ products
The electrocatalytic CO2 reduction reaction (CO2RR) holds the prospect to mitigate carbon emissions and at the same time convert CO2 into valuable chemicals, preferably from renewable energy sources. Depending on the number of electrons transferred, a variety of oxygenates and hydrocarbons can be obtained with already high selectivity demonstrated for C1 and C2 products. However, for the CO2RR to molecules with three or more carbon atoms (C3+) such as n-propanol, the fundamental knowledge and key-strategies to yield these economically attractive high-energy-density products are still lacking. In NANOconfine we propose a novel concept for CO2RR electrocatalysis, a so-called “inverse catalyst nanoconfined architecture”, that enables trapping and enhanced C-C coupling of crucial reaction intermediates by deterministic control of the local homogeneous and heterogeneous chemical environment. Specifically, we target for beyond-state-of-the-art Faradaic Efficiency >50% towards n-propanol as high-value liquid product. In order to design the optimal electrocatalyst architecture, a systematical approach is proposed to study the following effects on the CO2RR mechanism and product formation: (1) the near neighbor effect of co-catalysts in close proximity, (2) the confinement of reaction intermediates in regular arranged SiO2 mesopores (2-10nm) and (3) the confinement and surface chemistry of different mesoporous oxide 3D networks (MgO, ZnO, TiO2). From this understanding, we will build a demonstrator consisting of a nano-patterned co-catalysts (e.g. Cu and Ag) which interchange their reaction intermediates through a mesoporous oxide network so that they can undergo coupling to higher carbon products at neighboring electrocatalyst sites. NANOconfine will provide fundamental insights on the CO2RR reaction mechanism towards C3+ products in order to push forward the state-of-the-art of this emerging research topic.