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采用具有分级孔的 LTA 沸石高效回收 Cu(II)及其在电化学脱硝中的资源利用:水污染物中废沸石的环保设计与再利用。

Efficient recovery of Cu(II) by LTA-zeolites with hierarchical pores and their resource utilization in electrochemical denitrification: Environmentally friendly design and reutilization of waste in water.

机构信息

Scholl of Environment, Tsinghua University, 30# Shuangqing Road, Hai Dian Distract, Beijing, 100086, China.

Scholl of Environment, Tsinghua University, 30# Shuangqing Road, Hai Dian Distract, Beijing, 100086, China.

出版信息

J Hazard Mater. 2020 Jul 15;394:122554. doi: 10.1016/j.jhazmat.2020.122554. Epub 2020 Mar 18.

Abstract

Water pollution seriously endangers human health and the environment. Here we prepared and tested mesoporous LTA zeolites for the adsorption of Cu(II) from aqueous media and the captured copper was further used for electrochemical nitrate reduction. The prepared hierarchically porous LTA exhibited a high capacity (341.5 mg g) for Cu(II) adsorption, following the pseudo-second-order kinetic and Freundlich adsorption isotherm models well. The Cu-LTA sample was characterised by various analytical methods, and Cu(I) species were identified as the active sites for nitrate electrochemical reduction. Based on the spectral characterization and reducibility, strong metal-support interaction was found between copper and LTA, which is beneficial to the dispersion of active sites and their contacts with nitrates. In total, 10.1 g-N-NO g-Cu was reduced over the Cu-LTA-modified cathode in a three-electrode system with high N selectivity (92.1 %). Compared to purely microporous zeolites, mesoporous LTA has a higher capacity for Cu(II) removal and nitrate reduction. The mesoporous structure allows easy access to the inner active sites with low diffusion resistance. The low Tafel slope and high current density confirm the high activity of the mesoporous Cu-LTA, making it a promising and efficient material for the removal and reuse of heavy metal ions.

摘要

水污染严重危害人类健康和环境。在这里,我们制备并测试了中孔 LTA 沸石用于从水介质中吸附 Cu(II),并进一步将捕获的铜用于电化学还原硝酸盐。所制备的分级多孔 LTA 对 Cu(II)吸附具有高容量(341.5mg/g),很好地遵循了伪二阶动力学和 Freundlich 吸附等温线模型。Cu-LTA 样品通过各种分析方法进行了表征,Cu(I)物种被鉴定为硝酸盐电化学还原的活性位。基于光谱表征和还原性,发现铜和 LTA 之间存在强烈的金属-载体相互作用,这有利于活性位的分散及其与硝酸盐的接触。在三电极系统中,Cu-LTA 修饰的阴极共还原了 10.1g-N-NO3--Cu,具有高 N 选择性(92.1%)。与纯微孔沸石相比,中孔 LTA 对 Cu(II)去除和硝酸盐还原具有更高的容量。介孔结构允许容易进入内部活性位,同时具有低扩散阻力。低塔菲尔斜率和高电流密度证实了介孔 Cu-LTA 的高活性,使其成为去除和再利用重金属离子的一种有前途且高效的材料。

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