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作 者:刘松麟 杨庆峰[1] 邱辉强 孙宇雯 刘阳桥[3] LIU Songlin;YANG Qingfeng;QIU Huiqiang;Sun Yuwen;LIU Yangqiao(Green Chemical Engineering Technology Research and Development Center,Shanghai Advanced Research Institute,Chinese Academy of Sciences,Shanghai 201210,China;University of Chinese Academy of Sciences,Beijing 100049,China;Shanghai Institute of Ceramics,Chinese Academy of Science,Shanghai 200050,China)
机构地区:[1]中国科学院上海高等研究院绿色化学工程技术研究与发展中心,上海201210 [2]中国科学院大学,北京100049 [3]中国科学院上海硅酸盐研究所,上海200050
出 处:《水处理技术》2025年第2期99-104,109,共7页Technology of Water Treatment
基 金:国家自然科学基金项目(51878647,61574148)。
摘 要:过量硝酸盐(NO_(3)^(-))在废水中的排放已成为一个显著的环境问题。针对这一问题,利用电化学方法去除废水中的硝酸盐氮(NO_(3)^(-)-N)显得尤为重要。本研究通过水热合成,利用原位生长的金属有机框架(MOF)合成路径,在Fe_(2)O_(3)基材上负载CuO,成功研发了一种新型电极。这种电极在提升NO_(3)^(-)-N的电催化还原性能方面表现出色。实验表明,在电流密度为10 mA/cm^(2)的条件下,经过两小时反应,当NO_(3)^(-)-N初始浓度为50 mg/L时,其去除率可达96.72%;当NO_(3)^(-)-N浓度提高至100 mg/L时,去除率依然高达94.15%。即使在电流密度降至5 mA/cm2(NO_(3)^(-)-N初始浓度为50mg/L)的条件下,去除率也能达到85.85%。这些结果表明,该电极材料在不同条件下均展现出良好的硝酸盐氮去除效果。当氯离子(Cl^(-))浓度为750 mg/L时,总氮(TN)的去除率可达94%。通过叔丁醇(TBA)自由基清除实验,我们发现该材料去除硝酸盐氮的机制是通过电子的直接转移。在进行10次循环实验后,NO_(3)^(-)-N的去除率略有提升至98.78%,同时Cu和Fe的浸出量分别为4.3μg/L和4.65μg/L,表明该材料具有优良的稳定性和极低的金属浸出量。因此,该材料在实际废水处理应用中具有巨大的潜力。Excessive nitrate(NO_(3)^(-))wastewater discharge is a significant environmental challenge,necessitating exploration of electrochemical methods for NO_(3)^(-)-N removal.This study introduces a novel electrode fabricated using a hydrothermal method.The process involved synthesizing Metal-Organic Frameworks(MOFs)in situ on an Fe_(2)O_(3)base and incorporating CuO,significantly boosting the electrocatalytic reduction efficiency for NO_(3)^(-)-N.At a current density of 10 mA/cm^(2),the electrode achieved a 96.72%NO_(3)^(-)-N removal rate within two hours with an initial concentration of 50 mg/L.At a higher concentration of 100 mg/L,this rate was marginally lower at 94.15%.Remarkably,the removal efficiency remained high at 85.85%even at a reduced current density of 5 mA/cm2 and an initial NO_(3)^(-)-N concentration of 50 mg/L.These results demonstrate consistent effectiveness of the electrode across varying conditions.Furthermore,the total nitrogen(TN)removal rate reached 94%with a chloride ion(Cl^(-))concentration of 750 mg/L.Experiments using tert-butyl alcohol(TBA)-based free radical scavenging indicate that direct electron transfer is the primary mechanism for NO_(3)^(-)-N reduction.The removal efficiency slightly increased to 98.78%after 10 cycles.Meanwhile,the leaching amounts of Cu and Fe were 4.3μg/L and 4.65μg/L,respectively,underscoring the material's stability and reinforcing its potential in practical wastewater treatment applications.
关 键 词:钛基纳米电极 硝酸盐 电催化 金属有机框架(MOF)
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