期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 301, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120829
关键词
Nitrate reduction; Electrochemical reduction; Bimetallic sites; Relay catalytic effect; Water treatment
资金
- National Natural Science Foundation of China (NSFC) [21876128, 22076140, 21971197, 51772217, U1932119]
- National Key Basic Research Program of China [2017YFA0403402]
- Shanghai Rising-Star Program [20QA1409500]
- Shanghai Large Scientific Facilities Center
Selective electrocatalytic conversion of NO3- to N-2 using metal-organic framework-derived electrocatalyst was achieved with high efficiency, meeting drinking water standards. The study elucidated reaction intermediates and mechanistic pathways, highlighting the crucial role of neighboring Fe-Ni catalytic sites in enhancing and selectively catalyzing the reaction.
Selective electrocatalytic conversion of NO3- to N-2 is an environmental-friendly strategy to close the anthropogenic nitrogen-based cycle. This work reported a metal-organic framework-derived electrocatalyst with earthabundant bimetallic sites, showing quantitative (similar to 97.9% conversion) and selective (similar to 99.3%) nitrate-to-N-2 transformation. More importantly, both post-catalysis concentrations of NO3- and NO2- meet the drinking water limit requirements, set by World Health Organization. The reaction intermediates and mechanistic pathways in electrocatalytic reduction of NO3- to N-2 are elucidated by a variety of in-situ experimental studies and DFT calculations. The enhanced and selective electrocatalytic performances are ascribed to the relay catalytic effects of the neighboring Fe-Ni catalytic sites residing in the porous carbon electrocatalysts, which are structurally determined by X-ray absorption spectroscopy (XAS) as well as calculated structural model, with Fe sites decreasing the reaction barrier for NO3- conversion and Ni centers facilitating the adsorption and activation of reaction intermediates (NO2-, NO* and N2O*).
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