Cu2O/CF电极的制备及其电还原硝酸盐

郭峰; 谢陈鑫; 韩恩山; 张程蕾; 赵慧; 滕厚开

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中国环境科学 ›› 2023, Vol. 43 ›› Issue (12) : 6341-6351.

水污染与控制

Cu₂O/CF电极的制备及其电还原硝酸盐

郭峰^1,2, 谢陈鑫², 韩恩山¹, 张程蕾², 赵慧², 滕厚开²

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Electrocatalytic reduction of nitrate to dinitrogen by Cu₂O/CF electrode

GUO Feng^1,2, XIE Chen-xin², HAN En-shan¹, ZHANG Cheng-lei², ZHAO Hui², TENG Hou-kai²

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摘要

对比了原位生长法和电沉积法在泡沫铜(CF)上制备的s-Cu₂O/CF和e-Cu₂O/CF电极应用于电化学还原NO₃^-的性能.在0.05mol/L Cl^-和100mg/L NO₃^--N的初始条件下,s-Cu₂O/CF电极对NO₃^-的去除率为92.1%,N₂选择性为81.1%.循环伏安法(CV)和线性扫描伏安法(LSV)表明,电化学还原NO₃^-是通过NO₃^-和源自CF的Cu⁰之间的电子转移实现的.原位生长的Cu₂O作为双功能催化剂、电子中介或桥梁,不仅可以促进NO₃^-还原还可以产生还原性氢(H*),进一步促进NO₂^-向NH₄⁺和N₂转化.同时,经过8次循环实验,s-Cu₂O/CF仍保持其电催化活性.最后,为了评估s-Cu₂O/CF阴极的实际应用潜力,采用Ir-Ru/Ti阳极预氧化、s-Cu₂O/CF阴极后还原两阶段处理策略,对实际废水化学需氧量(COD)和总氮(TN)的去除率达到了93.6%和75.2%.

Abstract

During the whole electrolysis process, the electrocatalytic activity of cathode materials is affected by the multi-electron kinetic reaction. Presently, copper-based materials have received much attention as one of the most significant electrochemical nitrate reduction reaction (NITRR) electrocatalysts. However, there are still no reports of effective solutions to the problems of activity limitation and selectivity. In this work, we compared the NITRR performance of s-Cu₂O/CF and e-Cu₂O/CF catalysts prepared on copper foam (CF) by in situ growth and electrodeposition, respectively. An extremely high NO₃^- removal rate of 92.1% and N₂selectivity of 81.1% were attained by the s-Cu₂O/CF catalyst in the electrolyte containing 0.05mol/L Cl^- and 100mg/L NO₃^--N. Cyclic voltammetry and linear sweep voltammetry showed that the NITRR process was achieved by electron transfer between nitrate (NO₃^-) and Cu⁰derived from CF. In situ grown s-Cu₂O/CF, as a bifunctional catalyst for electronic media or bridge, promotes not only NO₃^- reduction but also the production of reduced hydrogen (H*), which further enhances the conversion of NO₂^- to NH₄⁺ or N₂. After eight cycles of experiments, s-Cu₂O/CF still maintained excellent electrocatalytic activity, which further demonstrates its great application potential in the NITRR. Furthermore, a two-step treatment strategy of Ir-Ru/Ti anodic pre-oxidation and s-Cu₂O/CF cathodic post-reduction was adopted to remove 93.6% of chemical oxygen demand (COD) and 75.2% of total nitrogen (TN) from the actual wastewater.

导出引用

郭峰, 谢陈鑫, 韩恩山, 张程蕾, 赵慧, 滕厚开. Cu₂O/CF电极的制备及其电还原硝酸盐[J]. 中国环境科学. 2023, 43(12): 6341-6351

GUO Feng, XIE Chen-xin, HAN En-shan, ZHANG Cheng-lei, ZHAO Hui, TENG Hou-kai. Electrocatalytic reduction of nitrate to dinitrogen by Cu₂O/CF electrode[J]. China Environmental Science. 2023, 43(12): 6341-6351

中图分类号： X730.1

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