Highly Efficient Electrochemical Nitrate Reduction to Ammonia in Strong Acid Conditions with Fe M-Trinuclear-Cluster Metal-Organic Frameworks.

Angew Chem Int Ed Engl

Key Laboratory of Mesoscopic Chemistry, State Key Laboratory of Coordination Chemistry, State Key Laboratory of Analytical Chemistry for Life Sciences, School of Chemistry and Chemical Engineering, Nanjing University, No.168, Xianlin Road, Nanjing, 210023, China.

Published: July 2023

AI Article Synopsis

  • - Nitrate-containing industrial wastewater threatens global food security and public health, and traditional methods of treatment face challenges due to acidic conditions found in these wastes.
  • - Electrocatalytic nitrate reduction shows a more sustainable solution, converting nitrates into valuable ammonia (NH) with high efficiency and stability, particularly under acidic conditions.
  • - The study introduces innovative Fe M trinuclear cluster metal-organic frameworks (MOFs) that effectively reduce nitrates in acidic environments, achieving significant ammonia yield, selectivity, and producing ammonium sulfate directly for use as fertilizer, enhancing wastewater treatment processes.

Article Abstract

Nitrate-containing industrial wastewater poses a serious threat to the global food security and public health safety. As compared to the traditional microbial denitrification, electrocatalytic nitrate reduction shows better sustainability with ultrahigh energy efficiency and the production of high-value ammonia (NH ). However, nitrate-containing wastewater from most industrial processes, such as mining, metallurgy, and petrochemical engineering, is generally acidic, which contradicts the typical neutral/alkaline working conditions for both denitrifying bacteria and the state-of-the-art inorganic electrocatalysts, leading to the demand for pre-neutralization and the problematic hydrogen evaluation reaction (HER) competition and catalyst dissolution. Here, we report a series of Fe M (M=Fe, Co, Ni, Zn) trinuclear cluster metal-organic frameworks (MOFs) that enable the highly efficient electrocatalytic nitrate reduction to ammonium under strong acidic conditions with excellent stability. In pH=1 electrolyte, the Fe Co-MOF demonstrates the NH yield rate of 20653.5 μg h  mg with 90.55 % NH -Faradaic efficiency (FE), 98.5 % NH -selectivity and up to 75 hr of electrocatalytic stability. Additionally, successful nitrate reduction in high-acidic conditions directly produce the ammonium sulfate as nitrogen fertilizer, avoiding the subsequent aqueous ammonia extraction and preventing the ammonia spillage loss. This series of cluster-based MOF structures provide new insights into the design principles of high-performance nitrate reduction catalysts under environmentally-relevant wastewater conditions.

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Source
http://dx.doi.org/10.1002/anie.202305246DOI Listing

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