Browsing by Author "Heck, Kimberly"
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Item Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst(Springer Nature, 2021) Wu, Zhen-Yu; Karamad, Mohammadreza; Yong, Xue; Huang, Qizheng; Cullen, David A.; Zhu, Peng; Xia, Chuan; Xiao, Qunfeng; Shakouri, Mohsen; Chen, Feng-Yang; Kim, Jung Yoon (Timothy); Xia, Yang; Heck, Kimberly; Hu, Yongfeng; Wong, Michael S.; Li, Qilin; Gates, Ian; Siahrostami, Samira; Wang, HaotianElectrochemically converting nitrate, a widespread water pollutant, back to valuable ammonia is a green and delocalized route for ammonia synthesis, and can be an appealing and supplementary alternative to the Haber-Bosch process. However, as there are other nitrate reduction pathways present, selectively guiding the reaction pathway towards ammonia is currently challenged by the lack of efficient catalysts. Here we report a selective and active nitrate reduction to ammonia on Fe single atom catalyst, with a maximal ammonia Faradaic efficiency of ~ 75% and a yield rate of up to ~ 20,000 μg h−1 mgcat.−1 (0.46 mmol h−1 cm−2). Our Fe single atom catalyst can effectively prevent the N-N coupling step required for N2 due to the lack of neighboring metal sites, promoting ammonia product selectivity. Density functional theory calculations reveal the reaction mechanisms and the potential limiting steps for nitrate reduction on atomically dispersed Fe sites.Item Niobium Oxide Photocatalytically Oxidizes Ammonia in Water at Ambient Conditions(SciELO, 2024) Elias, Welman; Clark, Chelsea; Heck, Kimberly; Arredondo, Jacob; Wang, Bo; Toro, Andras; Kürtib, László; Wong, Michael; Nanosystems Engineering Research Center for Nanotechnology-Enabled Water TreatmentAmmonia contamination in water is a significant environmental issue since it is toxic and leads to eutrophication. Photocatalysis has been investigated as a strategy for ammonia degradation but can potentially form toxic nitrite (NO2–) and nitrate (NO3–) byproducts. This work reports on the ability of niobium oxide (Nb2O5) to photocatalytically oxidize aqueous-phase ammonia (NH3). Whereas as-synthesized Nb2O5 showed little catalytic activity (< 1% NH3 conversion after 6 h of UV-C irradiation, at room temperature and atmospheric pressure, and under O2 headspace), Nb2O5 treated in basic solution (OH-Nb2O5) was able to photocatalytically degrade NH3 at ca. 9% conversion after six hours, with ca. 70% selectivity to the desired N2, with a first-order rate constant of ca. 12 times higher than the as synthesize catalyst (1.6 × 10–3 min–1 vs. 2.0 × 10–2 min–1). Raman spectroscopic analysis indicated the presence of terminal Nb=O species after base treatment of Nb2O5, implicating them as catalytically active sites. These results underscore how a simple structural modification can significantly affect photocatalytic activity for aqueous ammonia oxidation.