Preparation of a Gangue-Based X-type Zeolite Molecular Sieve as a Multiphase Fenton Catalyst and Its Catalytic Performance,ACS Omega

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Preparation of a Gangue-Based X-type Zeolite Molecular Sieve as a Multiphase Fenton Catalyst and Its Catalytic Performance
ACS Omega ( IF 3.7 ) Pub Date : 2021-07-02 , DOI: 10.1021/acsomega.1c02469
MiaoSen Zhang ₁ , XiaoLi Wang ₁

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In this study, a series of X-type zeolite molecular sieve catalysts, modified with copper (Cu-X), were prepared by an alkali fusion–hydrothermal synthesis using coal gangue from Inner Mongolia. These catalysts were used in the degradation of the methylene blue dye by a Fenton-like reaction. Characterization results showed that Cu is considered to be present in the surface structure of the zeolite in the form of doped Cu ions and metal oxide. It is believed that Cu²⁺ is the main active site involved in the Fenton reaction. The X-ray photoelectron spectroscopy (XPS) spectra indicated that Cu²⁺ and Cu⁺ coexist in the catalysts and participate together in the Fenton reaction. The degradation of methylene blue by the Cu-X catalysts was investigated to determine the optimal catalytic conditions in terms of six aspects: catalyst dosage, initial solution concentration, initial pH of the solution, H₂O₂ dosage, copper loading, and reaction temperature. The experimental results showed that CX-1.0 had excellent activity and stability for the degradation and decolorization of the methylene blue dye, which could completely degrade the dye within 90 min, and the total organic carbon removal rate reached as high as 97.8%. Electron spin resonance (ESR) and radical capture experiments showed that ^•OH played a dominant role in the Fenton-like reaction. Combined with XPS, ESR, and catalytic tests, the redox cycle of Cu⁺/Cu²⁺ was found to be accelerating the generation of reactive radicals in the Fenton system.

中文翻译：

煤矸石基X型沸石分子筛多相Fenton催化剂的制备及其催化性能

本研究以内蒙古煤矸石为原料，通过碱熔-水热合成法制备了一系列铜（Cu-X）改性的X型沸石分子筛催化剂。这些催化剂用于通过类芬顿反应降解亚甲基蓝染料。表征结果表明，Cu被认为以掺杂Cu离子和金属氧化物的形式存在于沸石的表面结构中。据信Cu ²⁺是参与芬顿反应的主要活性位点。 X射线光电子能谱(XPS)谱表明Cu ²⁺和Cu ⁺共存于催化剂中并共同参与Fenton反应。研究了Cu-X催化剂降解亚甲基蓝的情况，从催化剂用量、初始溶液浓度、溶液初始pH、H ₂ O ₂用量、铜负载量、反应温度六个方面确定了最佳催化条件。。实验结果表明，CX-1.0对亚甲基蓝染料的降解脱色具有优异的活性和稳定性，可在90 min内完全降解染料，总有机碳去除率高达97.8%。电子自旋共振（ESR）和自由基捕获实验表明^· OH 在类芬顿反应中起主导作用。结合XPS、ESR和催化测试，发现Cu ⁺ /Cu ²⁺的氧化还原循环加速了Fenton体系中反应自由基的产生。

更新日期：2021-07-20

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