氨
纳米颗粒
电化学
催化作用
电极
无机化学
材料科学
硝酸盐
铜
金属
亚硝酸盐
可逆氢电极
电催化剂
法拉第效率
化学
化学工程
纳米技术
工作电极
有机化学
冶金
物理化学
工程类
作者
Li Wang,Yue Cao,Hai Yan,Xinyan Wang,Senda Su,Wenming Ding,Zhenyu Liu,Xiaoman Li,Min Luo
出处
期刊:Dalton Transactions
[The Royal Society of Chemistry]
日期:2023-01-01
卷期号:52 (32): 11213-11221
被引量:5
摘要
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-2cat 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.
科研通智能强力驱动
Strongly Powered by AbleSci AI