催化作用
纳米反应器
氨生产
化学
电化学
氨
电解质
法拉第效率
无机化学
电极
有机化学
物理化学
作者
Xiujuan J. Dai,Lu Tian,Zhixue Liu,Weilin Xu,Yuping Liu,Yu Liu
出处
期刊:ACS Nano
[American Chemical Society]
日期:2022-11-04
卷期号:16 (11): 18398-18407
被引量:14
标识
DOI:10.1021/acsnano.2c06441
摘要
The high-efficiency transition metal-free electrocatalytic nitrate reduction reaction (NO3-RR) for ammonia synthesis has received more attention because of its green and environmentally friendly characteristics. Here, we report an efficient electrochemical NH3 synthesis directly from purely organic macrocyclic compounds α-, β-, and γ-cyclodextrins (CDs)-catalyzed transition metal-free electroreduction of nitrate under ambient conditions. In comparison with α-, and β-CDs, parent γ-CD presented uncommon catalytic performance with a relatively higher NH3 yield that can reach up to 2.28 mg h-1 cm-2 with a Faradaic efficiency (FE) of 63.2% at -0.9 V versus a reversible hydrogen electrode in alkaline medium, and the potassium ion-coordinated γ-CD complex can achieve a maximum NH3 production rate up to 4.66 mg h-1 cm-2 with an NH3 FE of 79.3%. Further comparison with permethyl-γ-CD, d-glucose, and poly(vinyl alcohol) for the NO3-RR indicated that the typical torus-shaped cyclic conformation and edge hydroxyl groups of parent CDs play important roles in the electrocatalytic process. The K+-mediated 3D γ-CD-K+ frameworks containing six CDs as nanoreactors greatly strengthen the enrichment effect of nitrate through hydrogen-bonding interaction and electrostatic interaction and promote the mass transfer, thus leading to the efficient NO3-RR in an alkaline electrolyte. This work provides a convenient, green, and economic method for high-performance NO3-RR, which has potential applications in the fields of environment, energy, and industry.
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