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通过氧化石墨烯提高 HKUST-1 的催化性能用于苯酚氧化。

Enhancing the catalytic behaviour of HKUST-1 by graphene oxide for phenol oxidation.

机构信息

School of Chemistry and Chemical Engineering, Southeast University, Nanjing, People's Republic of China.

出版信息

Environ Technol. 2021 Feb;42(5):694-704. doi: 10.1080/09593330.2019.1643410. Epub 2019 Jul 17.

Abstract

The composites of graphite oxide (GrO) and the HKUST-1 framework were synthesized by the typical solvothermal method and applied as heterogeneous catalysts for catalytic wet peroxide oxidation (CWPO) of phenol. XRD, FT-IR, Raman and SEM were conducted to characterize the samples. For catalytic oxidation of 150 mL 100 mg L phenol, the dose of 30 mg (0.2 g L) catalysts and 0.46 mL HO were kept constant. The GrO-3/HKUST-1 (3% content of GrO) showed higher catalytic activity than the HKUST-1 framework and other GrO/HKUST-1 composites with 99% phenol conversion and 86% COD removal efficiency were obtained at 50°C after 30 min and 8 h. The effect of temperature (40-80°C) and pH (4-9) on catalytic oxidation of phenol by GrO-3/HKUST-1 was investigated. The results showed that the degradation of phenol was obtained with optimum efficiency at 60°C with complete phenol conversion and 93% COD reduction. Furthermore, the acid and alkali resistance abilities were enhanced to a certain degree by the integration of GrO compared with the parent framework HKUST-1. Three successive runs were conducted in the natural pH (6.8) of 150 mL 100 mg L phenol solution which indicated that the synthesized GrO-3/HKUST-1 composite had satisfactory reusability due to the prevention of carbon deposit and negligible Cu leaching (8 ppm). The GrO/HKUST-1 composite could be a kind of promising heterogeneous catalysts for catalytic degradation of organic compounds. Similar to other catalysts, the catalytic oxidation of phenol also relies on the formation of hydroxyl radicals.

摘要

氧化石墨(GrO)和 HKUST-1 骨架的复合材料通过典型的溶剂热法合成,并作为非均相催化剂应用于苯酚的催化湿式过氧化物氧化(CWPO)。通过 XRD、FT-IR、Raman 和 SEM 对样品进行了表征。在 150 mL 100 mg L 苯酚的催化氧化中,保持 30 mg(0.2 g L)催化剂和 0.46 mL HO 的剂量不变。GrO-3/HKUST-1(GrO 含量为 3%)表现出比 HKUST-1 骨架更高的催化活性,在 50°C 下 30 min 后,99%的苯酚转化率和 86%的 COD 去除效率可得到 8 h。研究了温度(40-80°C)和 pH(4-9)对 GrO-3/HKUST-1 催化氧化苯酚的影响。结果表明,在 60°C 下,苯酚的降解达到最佳效率,苯酚完全转化,COD 降低 93%。此外,与母体骨架 HKUST-1 相比,GrO 的整合在一定程度上提高了酸碱抗性能力。在 150 mL 100 mg L 苯酚溶液的自然 pH(6.8)下进行了三次连续运行,表明合成的 GrO-3/HKUST-1 复合材料由于防止积碳和铜浸出(8 ppm),具有令人满意的可重复使用性。GrO/HKUST-1 复合材料可能是一种有前途的用于催化降解有机化合物的非均相催化剂。与其他催化剂一样,苯酚的催化氧化也依赖于羟基自由基的形成。

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