SolTIME · Solar Fuel Generation through Photoelectrochemical Reduction of CO2 Using Copper Porphyrins in Molecularly Designed Reaction Environments

Solar Fuel Generation through Photoelectrochemical Reduction of CO2 Using Copper Porphyrins in Molecularly Designed Reaction Environments

Solar technologies have become economically competitive because of investment in solar energy research, spurred in part by concerns over the detrimental environmental consequences associated with conventional energy sources. This has led to an electrical grid with an increasing share of solar electricity; and sometimes, even a surplus. To continue the trajectory towards climate-friendly energy sources, technologies must be developed that can profit from this inexpensive solar energy by storing it for times when the sun is not shining. One approach to solar fuel production is through the use of photovoltaics to drive electrochemical reactions, using semiconductors as light harvesting components for driving uphill solution-phase reactions to effectively store sunlight in chemical bonds. However, using photo-generated charges to synthesize fuels remains an outstanding challenge, due in part to the large energy requirements needed. Urgent measures are needed against climate change to limit global temperature rise. Nowadays, we are facing an energy transition where new technologies, together with societal changes, will be needed to shift from a fossil-based system of energy production and consumption to renewable energy sources like wind and solar. The share of renewable energy has considerably increased in the latest years, but these are intermittent energy sources, therefore storage solutions are also needed. Batteries development is an important asset, but additionally transformation of renewable energy to chemical energy in the form of fuels and other commodities is also needed, especially in sectors difficult to electrify. This research advances the field of solar fuels with an increased understanding of both structure-function relationships in solar-driven electrocatalysis. Managing ammonia oxidation to generate hydrogen fuel using molecular catalysts and sunlight to lower the required energy inputs is a significant advance compared to previous state-of-the-art constructs. Solar Fuels by Tuning Immobilized Molecular Catalytic Environments (SolTIME) has focused on the development of hybrid cathodes for ammonia oxidation using an integrated approach that houses molecular catalysts in distinct three-dimensional architectures in order to tune the reactivity and selectivity of the embedded catalyst, thus advancing fundamental knowledge of factors favoring performance in solar-driven electrochemical devices.

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