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在泡沫镍上碳封装的 Cu-Fe 电活性纳米催化剂对硝酸盐的电催化还原。

Electrocatalytic reduction of nitrate by carbon encapsulated Cu-Fe electroactive nanocatalysts on Ni foam.

机构信息

College of Environmental Science and Engineering, Hunan University, Changsha, 410082, PR China; Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha, 410082, PR China.

Hunan Ecological and Environmental Monitoring Center, Changsha, 410027, PR China.

出版信息

J Colloid Interface Sci. 2023 Mar 15;634:440-449. doi: 10.1016/j.jcis.2022.12.006. Epub 2022 Dec 9.

Abstract

Electrocatalytic denitrification is an attractive and effective method for complete elimination of nitrate (NO). However, its application is limited by the activity and stability of the electrocatalyst. In this work, a novel bimetallic electrode was synthesized, in which N-doped graphitized carbon sealed with Cu and Fe nanoparticles and immobilized them on nickel foam (CuFe NPs@NC/NF) without any chemical binder. The immobilized Cu-Fe nanoparticles not only facilitated the adsorption of the reactant but also enhanced the electron transfer between the cathode and NO, thus promoting the electrochemical reduction of NO. Therefore, the as-prepared electrode exhibited enhanced electrocatalytic activity for NO reduction. The composite electrode with the Cu/Fe molar ratio of 1:2 achieved the highest NO removal (79.4 %) and the lowest energy consumption (0.0023 kW h mg). Furthermore, the composite electrode had a robust NO removal capacity under various conditions. Benefitting from the electrochlorination on the anode, this electrochemical system achieved nitrogen (N) selectivity of 94.0 %. Moreover, CuFe NPs@NC/NF exhibited good stability after 15 cycles, which should be attributed to the graphitized carbon layer. This study confirmed that CuFe NPs@NC/NF electrode is a promising and inexpensive electrode with long-term stability for electrocatalytic denitrification.

摘要

电催化反硝化是一种很有吸引力和有效性的完全消除硝酸盐(NO)的方法。然而,其应用受到电催化剂的活性和稳定性的限制。在这项工作中,合成了一种新型的双金属电极,其中氮掺杂石墨化碳封装的铜和铁纳米颗粒,并将其固定在泡沫镍上(CuFe NPs@NC/NF),而无需任何化学粘合剂。固定化的 Cu-Fe 纳米颗粒不仅促进了反应物的吸附,而且增强了阴极和 NO 之间的电子转移,从而促进了 NO 的电化学还原。因此,所制备的电极对 NO 还原表现出增强的电催化活性。Cu/Fe 摩尔比为 1:2 的复合电极实现了最高的 NO 去除率(79.4%)和最低的能耗(0.0023kW·h·mg)。此外,在各种条件下,复合电极都具有很强的 NO 去除能力。得益于阳极上的电化学氯化作用,该电化学系统实现了 94.0%的氮气(N)选择性。此外,CuFe NPs@NC/NF 经过 15 次循环后表现出良好的稳定性,这应归因于石墨化碳层。这项研究证实,CuFe NPs@NC/NF 电极是一种很有前途和廉价的电极,具有长期稳定的电催化反硝化性能。

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