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    介孔碳限域Cu纳米颗粒用于电催化硝酸根脱除

    Cu nanoparticles confined by mesoporous carbon for electrocatalytic removal of nitrate

    • 摘要: 工业废水中硝酸盐的残留对生态环境造成了较大的负面影响,氮气绿色无毒,且无需二次处理,被认为是废水硝酸盐脱除的理想目标产物。电催化还原是一种可持续的废水硝酸盐脱除方法,目前为止仍然面临着动力学缓慢、目标产物选择性低和稳定性差等问题。Cu金属是硝酸盐还原常用的电催化剂之一,但在电极极化过程中,Cu原子易迁移和团聚生长,导致反应活性衰减,在工业应用中其耐久性往往较差,因此,对催化剂的电化学性能和稳定性提出了较高要求。通过分子介导的界面组装策略,合成了介孔碳原位限域Cu纳米颗粒的CNTs@mesoC@Cu催化剂,研究了其电催化硝酸根选择性还原的活性及反应机理。在3%浓度Cl-协同作用下,经24 h恒电位还原后,CNTs@MesoC@Cu催化剂可将模拟废水的总氮浓度C(NO3--N)从140 ppm降低至8.5 ppm,氮气选择性高于95%,符合污水综合排放标准;此外,经过120 h稳定性测试后,该催化剂对氮气的选择性仍保持在96%以上,证明其具有相当的循环稳定性。该催化剂在电催化硝酸根选择性还原中表现出良好的性能,导电碳纳米管@介孔碳基底束缚限制了表面的铜活性中心,使CNTs@mesoC@Cu能够保持稳定的电化学硝酸盐催化活性。这项研究为铜基电催化剂在大规模的工业应用方面提供了一种可行的解决方案。

       

      Abstract: The residue of nitrate in industrial wastewater has a great negative impact on the ecological environment. Nitrogen is green, non-toxic and does not need secondary treatment, so it is considered to be an ideal target product for nitrate removal of wastewater. Electrocatalytic reduction is a sustainable method for nitrate removal from wastewater, which is still faced with some problems, such as slow kinetics, low selectivity of target products and poor stability. Cu metal is one of the commonly used electrocatalysts for nitrate reduction, but in the process of electrode polarization, Cu atoms are easy to migrate and agglomerate, resulting in the decline of reaction activity, and its durability is often poor in industrial applications. Therefore, higher requirements are put forward for the electrochemical performance and stability of the catalyst. In this paper, mesoporous carbon in-situ limited Cu nanoparticles CNTs@mesoC@Cu catalysts were synthesized by molecular-mediated interfacial assembly strategy, and their electrocatalytic performance and reaction mechanism for selective reduction of nitrate were studied. Under the synergistic action of 3% concentration of Cl-, after potentiostatic reduction for 24 hours, the CNTs@MesoC@Cu catalyst can reduce the total nitrogen concentration C (NO3--N) of the simulated wastewater from 140ppm to 8.5ppm, and the nitrogen selectivity is higher than 95%, which meets the comprehensive sewage discharge standard. In addition, after 120 h stability test, the selectivity of the catalyst for nitrogen is still above 96%, which proves that it has considerable stability. The catalyst shows good performance in the selective reduction of nitrate. The binding of conductive carbon nanotubes @ mesoporous carbon substrate limits the copper active center on the surface, which enables CNTs@MesoC@Cu to maintain stable electrochemical nitrate catalytic activity. This study provides a feasible solution for the large-scale industrial application of copper-based electrocatalysts.

       

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