Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
Publication date: 16th December 2024
The chemical industry uses the energy-intense Haber-Bosch process for the thermocatalytic nitrogen reduction reaction (NRR) to form NH3 from N2 and H2, while nitrate and nitric acid are industrially produced by catalytic oxidation of NH3 (Ostwald process). Researchers worldwide are exploring low-energy electrochemical or photo-electrochemical NRR and nitrogen oxidation reaction (NOR). The project aims at developing an integrated reactor which combines both NRR and NOR using sustainably sourced electricity and sunlight as energy input. This could pave the way to small-scale chemical plants for decentralized production of ammonium nitrate as fertilizer or feedstock for local industries. This project uses a molecule-to-reactor holistic concept in designing the flow reaction system, which combines expertise from the Streb group and the Ziegenbalg group.
In the first funding period, the project proposed to develop noble-metal-free single atom catalysts (SACs, 1 metal reaction center) and single-site catalysts (SSCs 2 metal reaction centers) anchored to molecular metal oxides (polyoxometalates, POMs). Variation of the SAC/SSC metal sites will allow control of NRR/NOR performance, while POM-anchoring will provide a stable, well-defined all-oxo coordination environment. Deposition of these molecular precursors on high-porosity and highly conductive electrodes is achieved by wet-chemical, microwave or hydrothermal POM-conversion to solid-state oxides to facilitate stable mechanical and electrical linkage between catalyst and electrode.
During the first funding period, we have got some preliminary results regarding the synthesis of bimetallic alloys (CuNi and CuRu) for electrocatalytic nitrate/nitrite to ammonia conversion. The CuNi alloy obtained nitrate-to-ammonia Faradaic efficiencies (FE) of up to 83% and NH3 yield rates up to 860 μg h-1cm-2 at -0.38 V vs. RHE; while the CuRu alloy (with ultra-low Ru loading of 0.48 wt.%) obtained nitrate-to-ammonia FE of 88.4 % at -0.6 V vs RHE and a yield rate of 62.5 mg h-1 cm-2 at -1.0 V vs. RHE. In addition, we have synthesized a new bimetallic CuNi functionalized polyoxometalate/copper foam composite electrode, which show high activity toward nitrate to ammonia conversion (nitrate-to-ammonia FE of 95 % and a yield rate of 88.4 mg h-1 cm-2 at -1.0 V vs. RHE). This bimetallic CuNi functionalized polyoxometalate/copper foam composite electrode is also currently being studied for electrocatalytic NRR.
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