氨
化学
铜
无机化学
氢
离解(化学)
硝酸盐
氟
氨生产
电极
环境化学
有机化学
物理化学
作者
Weixing Zhang,Yancai Yao,Ziyue Chen,Shengxi Zhao,Fang Guo,Lizhi Zhang
标识
DOI:10.1021/acs.est.4c00151
摘要
Electrocatalytic nitrate reduction to ammonia (NITRR) offers an attractive solution for alleviating environmental concerns, yet in neutral media, it is challenging as a result of the reliance on the atomic hydrogen (H*) supply by breaking the stubborn HO–H bond (∼492 kJ/mol) of H2O. Herein, we demonstrate that fluorine modification on a Cu electrode (F-NFs/CF) favors the formation of an O–H···F hydrogen bond at the Cu–H2O interface, remarkably stretching the O–H bond of H2O from 0.98 to 1.01 Å and lowering the energy barrier of water dissociation into H* from 0.64 to 0.35 eV at neutral pH. As a benefit from these advantages, F-NFs/CF could rapidly reduce NO3– to NH3 with a rate constant of 0.055 min–1 and a NH3 selectivity of ∼100%, far higher than those (0.004 min–1 and 9.2%) of the Cu counterpart. More importantly, we constructed a flow-through coupled device consisting of a NITRR electrolyzer and a NH3 recovery unit, realizing 98.1% of total nitrogen removal with 99.3% of NH3 recovery and reducing the denitrification cost to $5.1/kg of N. This study offers an effective strategy to manipulate the generation of H* from water dissociation for efficient NO3–-to-NH3 conversion and sheds light on the importance of surface modification on a Cu electrode toward electrochemical reactions.
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