Monday, 14 May 2018: 15:40
Room 614 (Washington State Convention Center)
With the industrial production of N-based fertilizers from the Haber-Bosch process in the early 20th century, increased crop production has been realized and it is estimated that half of the world’s population is supported by N-based fertilizers. Due to the high temperature, pressure, and feedstocks needed, the Haber-Bosch process consumes approximately 2% of the world energy production and is highly centralized which contributes additional energy and CO2 emissions to transport the ammonia to end users. Electrochemical production of ammonia offers a low temperature, low pressure alternative which can be scaled out and allows for on-site ammonia generation powered by renewable energy sources. With more discussions of carbon taxes for companies that produce CO2, a renewable distributed ammonia production network could become increasingly attractive. However, platinum group metal catalysts show low Faradaic efficiency and low specific ammonia production rates due to the facile hydrogen evolution reaction. In this work, we report the first experimental work of ENRR on metal nitrides. An MEA configuration is employed in the reactivity tests due to the low solubility of N2 in aqueous electrolytes, which poses challenges in product quantification and catalyst characterization. We established a rigorous and reliable procedure to quantify the amount of ammonia produced in ENRR on the catalyst containing N, and thus could be served as a N source. A combination of the Nessler method, UV-Vis spectroscopy, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and X-ray absorption spectroscopy (XAS) were employed. We show that the bulk remains unchanged and only a thin surface layer of the micro-size particles is participating in ENRR indicating the leaching of N from the catalyst does not contribute to the amount of ammonia detected in the Nessler method in any appreciable degree.