Covalent Organic Framework Bifunctional Catalyst for Glucose Oxidation Reaction Coupled Nitrate to Ammonia Electrolysis
Akansha Chaturvedi, Safa Gaber, Sukhjot Kaur, Kayaramkodath Chandran Ranjeesh, Tharamani C. Nagaiah, Dinesh Shetty
Abstract
High Resolution Image Download MS PowerPoint Slide Ammonia is a crucial feedstock for the chemical industry, a carbon-free energy source, and a safe source for hydrogen storage. The electrochemical nitrate reduction reaction (NO 3 RR) is one promising strategy for greener ammonia synthesis due to high water solubility and low N═O bond dissociation energy of NO 3 – . More importantly, polluted water is a source of NO 3 – . Herein, we rationally designed a bifunctional covalent organic framework catalyst (Ru-Tta-Dfp) having a triazine- and pyridine-rich backbone with inherent Ru-nanocluster sites to control both NO 3 – and H + diffusion and interactions to achieve selective conversion of NO 3 – to ammonia monitored by operando Raman spectroscopy (93.93% faradaic efficiency and yield rate of 1.16 mg h –1 cm –2 at −0.4 V vs RHE). Moreover, we have developed a strategy for the first time to couple the anodic glucose oxidation reaction (GOR) to facilitate the cathodic NO 3 RR with reduced energy consumption and to achieve value-added products at both electrodes. Notably, NO 3 RR-GOR full cell studies generate a ∼2.5 times higher NH 3 yield rate than that of NO 3 RR-OER.