期刊
CATALYSIS SCIENCE & TECHNOLOGY
卷 12, 期 10, 页码 3281-3288出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2cy00289b
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资金
- Topsector Energy by the Ministry of Economic Affairs and Climate Policy, The Netherlands
Inefficient fertilizer use in agriculture causes nitrate runoff, which can be mitigated by electrochemical conversion to ammonia, especially with the introduction of inert gas flow to increase mass transport and partial current density.
Inefficient fertilizer use in agriculture causes nitrate runoff, polluting rivers and streams. This pollution can be mitigated by partially converting nitrate into ammonia - rebalancing the composition to ammonium nitrate, and allowing recycling of fertilizer. Here, we present efficient electrochemical conversion of nitrate (50 mM) to ammonia in acidic electrolyte using tubular porous Ti electrodes. A high faradaic efficiency (FE) of 58% and partial current density to ammonia of -33 mA cm(-2) at -1 V vs. RHE were achieved in the absence of inert gas purge. Additionally, we reveal that hydroxylamine is formed, as well as NO and N2O by spontaneous decomposition of nitrite, as has been determined by EC-MS analysis. The effective increase in local mass transport by introducing a flow of inert gas exiting the wall of the hollow fiber electrode results in an unprecedently high partial current density to ammonia of similar to-75 mA cm(-2), while maintaining a faradaic efficiency to ammonia of up to 45%. This concept facilitates nitrate conversion at high FE even at low concentrations, and holds promise for development to practical scale if electrochemical potential and exiting gas flow rate are well controlled.
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