PulseUS · Pulsed Potential-Mediated Tandem Electrolysis of CO2 and Nitrate for Efficient Urea Synthesis

Sustainable solutions for global warming and groundwater pollution depend on reducing fossil fuel use and controlling wastewater discharges. Electrochemical urea production from CO2 and NO3- offers a promising approach to closing carbon and nitrogen cycles. However, traditional methods are energy-intensive and produce significant CO2 emissions, while current electrochemical processes face issues with selectivity, rate, and durability. Symmetrical pulsed potential electrolysis addresses key issues of continuous potential application, but optimal performance remains elusive due to the lack of effective strategies for controlling the evolving electrode microenvironment, which governs reaction kinetics and product distribution. This approach further reduces effective reduction time by half, limiting urea yield. I hereby propose developing dual-atom catalysts (DACs) by integrating CO2- (e.g., Cu) and NO3-- (e.g., Mo) selective sites on a suitable support, alongside a novel electrolysis method called Asymmetric Low-Frequency Pulsed Potential Electrolysis (ALFPE). These DACs will enable efficient C-N coupling, while ALFPE will precisely control the catalyst’s microenvironment to enhance activity, selectivity, and stability for urea production. The underlying mechanisms will be studied using in situ spectroscopy (FTIR, Raman) and DFT simulations, examining the effects of ALFPE parameters, electrolyte composition, and reactor design. Supported by LTU’s advanced research ecosystem, the project will foster interdisciplinary collaboration and utilize the Experimental Physics lab. I commit to the broad dissemination/communication of PulseUS outcomes, engaging audiences from secondary school students to researchers.