期刊
DALTON TRANSACTIONS
卷 52, 期 32, 页码 11213-11221出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d3dt01412f
关键词
-
By electroreducing Cu metal-organic framework (Cu-MOF) precursors, a polyhedral-supported Cu nanoparticle binder-free monolithic electrode (Cu-BTC-Cu) is synthesized, which displays high ammonia yield and faradaic efficiency, inhibits the release of nitrite, and exhibits favorable stability.
Electrocatalytic nitrate reduction to ammonia, which removes nitrates from aquatic ecosystems, is a potential alternative to the classical Haber-Bosch process. Nevertheless, the selectivity of ammonia is often affected by the toxic by-product nitrite. Here, the polyhedral-supported Cu nanoparticle binder-free monolithic electrode (Cu-BTC-Cu) is synthesized by the in situ electroreduction of Cu metal-organic framework (Cu-MOF) precursors. The Cu-BTC-Cu displays a high ammonia yield of 4.00 mg h(-1) cm(cat)(-2) and a faradaic efficiency of 83.8% in 0.05 M K2SO4 (pH = 7), greatly outperforming the rod-supported (Cu-BTEC-Cu) and unsupported (Cu-BDC-Cu) Cu nanoparticle monolithic electrodes. Impressively, the Cu-BTC-Cu can inhibit significantly the release of by-product NO2- and present favourable stability after 10 consecutive cycles. These preeminent properties can be attributed to the polyhedral structure, which enables better dispersion of Cu nanoparticles and brings more active sites. Moreover, the reaction mechanism of Cu-BTC-Cu is analysed by electrochemical in situ characterization and several key intermediates are captured. This work provides new insights into the modification of the electrocatalytic nitrate reduction activity of Cu-based catalysts and ideas for the design of high-efficiency electrodes.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据