期刊
ADVANCED MATERIALS
卷 34, 期 36, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202204306
关键词
Cu electrocatalysts; enrichment effect; NO; (3); (-) electroreduction; porous carbon frameworks
类别
资金
- National Natural Science Foundation of China [92061111, U1932146, U19A2015]
- National Science Fund for Distinguished Young Scholars [21925204]
- National Key Research and Development Program of China [2021YFA1500500, 2019YFA0405600]
- China Postdoctoral Program for Innovative Talents [BX20200324]
- Provincial Key Research and Development Program of Anhui [202004a05020074]
- CAS project for young scientists in basic research [YSBR-022]
- K. C. Wong Education [GJTD-2020-15]
- DNL Cooperation Fund, CAS [DNL202003]
- Fundamental Research Funds for the Central Universities
A Cu-based catalyst, Cu@C, is developed for the electroreduction of nitrate at ultralow concentrations, achieving high Faradaic efficiency and NH3 yield rate. The mechanism involves concentration of NO3- enabled by the porous carbon framework, facilitating efficient electroreduction into NH3.
The electroreduction of nitrate (NO3-) pollutants to ammonia (NH3) offers an alternative approach for both wastewater treatment and NH3 synthesis. Numerous electrocatalysts have been reported for the electroreduction of NO3- to NH3, but most of them demonstrate poor performance at ultralow NO3- concentrations. In this study, a Cu-based catalyst for electroreduction of NO3- at ultralow concentrations is developed by encapsulating Cu nanoparticles in a porous carbon framework (Cu@C). At -0.3 V vs reversible hydrogen electrode (RHE), Cu@C achieves Faradaic efficiency for NH3 of 72.0% with 1 x 10(-3) m NO3-, which is 3.6 times higher than that of Cu nanoparticles. Notably, at -0.9 V vs RHE, the yield rate of NH3 for Cu@C is 469.5 mu g h(-1) cm(-2), which is the highest value reported for electrocatalysts with 1 x 10(-3) m NO3-. An investigation of the mechanism reveals that NO3- can be concentrated owing to the enrichment effect of the porous carbon framework in Cu@C, thereby facilitating the mass transfer of NO3- for efficient electroreduction into NH3 at ultralow concentrations.
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