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Heterogeneous thermal catalytic processes are vital for industrial production of fuels, fertilizers, and other chemicals necessary for sustaining human life. However, these processes are highly energy-intensive, requiring a vast consumption of fossil fuels. An emerging class of heterogeneous catalysts that are thermally driven but also exhibit a photochemically enhanced rate can potentially reduce process energy intensity by partially substituting conventional heat (where fossil fuels are needed) with solar energy. Such catalyst systems have yet to be practically utilized. Here, we demonstrate a compact electrically heated photo- and thermal annular reactor module to reduce CO2 to CO, via the reverse water gas shift reaction. A first-principles-based design approach was taken in developing a SiO2 on an Al photo- and thermal catalyst system for the model photo- and thermal indium oxide hydroxide (In2O3–x(OH)y) catalysts. A 5-fold light enhancement in the CO production rate and over 70 h of stable CO production were achieved. This represents the highest light enhancement effect reported for this model photocatalyst to date. The reactor presented herein allows continuous operation and a significant reduction of 31% in heater power consumption when provided with an additional 2 suns of irradiation, demonstrating the strong photo- and thermal-harvesting performances of the catalyst system developed in this work.
Urea, an agricultural fertilizer, nourishes humanity. The century‐old Bosch–Meiser process provides the world's urea. It is multi‐step, consumes enormous amounts of non‐renewable energy, and has a large CO2 footprint. Thus, developing an eco‐friendly synthesis for urea is a priority. Herein we report a single‐step Pd/LTA‐3A catalyzed synthesis of urea from CO2 and NH3 under ambient conditions powered solely by solar energy. Pd nanoparticles serve the dual function of catalyzing the dissociation of NH3 and providing the photothermal driving force for urea formation, while the absorption capacity of LTA‐3A removes by‐product H2O to shift the equilibrium towards urea production. The solar urea conversion rate from NH3 and CO2 is 87 μmol g−1 h−1. This advance represents a first step towards the use of solar energy in urea production. It provides insights into green fertilizer production, and inspires the vision of sustainable, modular plants for distributed production of urea on farms.
