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在由沸石咪唑酯骨架-8(ZIF-8)纳米晶体碳化的氮掺杂多孔碳修饰石墨毡电极上高产率的过氧化氢。

High yield of hydrogen peroxide on modified graphite felt electrode with nitrogen-doped porous carbon carbonized by zeolitic imidazolate framework-8 (ZIF-8) nanocrystals.

机构信息

School of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xi'an, 710021, China.

School of Environmental and Municipal Engineering, Lanzhou Jiaotong University, Lanzhou, 730070, China.

出版信息

Environ Pollut. 2019 Dec;255(Pt 2):113119. doi: 10.1016/j.envpol.2019.113119. Epub 2019 Aug 31.

Abstract

The aim of this work was to develop a new modified graphite felt (GF) as carbonaceous cathode for electro-Fenton (EF) application loaded with nitrogen-doped porous carbon (NPC) carbonized by zeolitic imidazolate framework-8 (ZIF-8) nanocrystals as carbon precursor. At initial pH 7, the highest generation rate of HO was 0.74 mg h cm by applying 12.5 mA cm by modified cathode, but in the same condition, the GF only had 0.067 mg h cm. The production efficiency increased 10 times. Additionally, phenol (50 mg L) could be largely removed by NPC modified cathode, the mineralization ratio and TOC reached 100% and 82.61% at 120 min of optimization condition, respectively. The NPC cathode kept its stability after 5 cycles. The materials were characterized by scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD) and linear sweep voltammetry (LSV). The results demonstrated that a homogenous NPC covered the carbon-based material GF. The existing graphitic-N and sp carbon of NPC promoted the electron transfer between carbon surface and oxygen molecules, as well as accelerated the oxygen reduction reaction (ORR) and the modified graphite felt had much higher electrocatalytic activity. In this work, several manufacturing parameters like the current, pH and load of NPC were optimized. The optimized design could improve the efficiency of new cathode with in situ electro-chemical production of HO and significantly offer a potential material for degradation of organic pollutants.

摘要

这项工作的目的是开发一种新的改性石墨毡(GF)作为碳质阴极,用于电芬顿(EF)应用,该阴极负载由沸石咪唑酯骨架-8(ZIF-8)纳米晶体碳化的氮掺杂多孔碳(NPC)作为碳前体。在初始 pH 为 7 的条件下,通过施加 12.5 mA cm 的电流,改性阴极的 HO 最高生成速率为 0.74 mg h cm,而在相同条件下,GF 仅为 0.067 mg h cm。生成效率提高了 10 倍。此外,NPC 改性阴极可以大量去除苯酚(50 mg L),在优化条件下 120 分钟时,矿化率和 TOC 分别达到 100%和 82.61%。NPC 阴极在 5 次循环后仍保持稳定。通过扫描电子显微镜(SEM)、X 射线光电子能谱(XPS)、X 射线衍射(XRD)和线性扫描伏安法(LSV)对材料进行了表征。结果表明,均匀的 NPC 覆盖了基于碳的材料 GF。NPC 中的存在的石墨-N 和 sp 碳促进了碳表面和氧分子之间的电子转移,以及加速了氧还原反应(ORR),并且改性石墨毡具有更高的电催化活性。在这项工作中,优化了电流、pH 值和 NPC 负载等几个制造参数。优化设计可以提高新阴极的效率,通过原位电化学产生 HO,并为降解有机污染物提供一种潜在的材料。

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