用于直接合成过氧化氢的新型设计钯镍异质纳米催化剂

Tan-Thanh Huynh, Thi Tran Anh Tuan, M. Nugraha
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摘要

过氧化氢(H2O2)是一种广泛使用的环保型氧化剂,在纸浆和纸张漂白、电子半导体制造、化学品和洗涤剂合成以及废水处理等应用中,水是氧化作用的唯一副产品。直接合成法是满足市场需求的环保型 H2O2 生产方法的首选。由于双金属钯镍纳米催化剂的催化活性和材料体系的结构特点,本研究选择了双金属钯镍纳米催化剂。首先,基于介孔碳模板,在 750∘C 下进行氢辅助热处理后,开发了有序结构的双金属 PdNi 纳米催化剂。X 射线吸收光谱(XAS)和高分辨率过渡电子显微镜(HR-TEM)证实了无序结构转变为合金化程度较高的有序金属间结构钯镍合金。然后,为了改善氧氧化反应,TiO2-C 作为一种有序支撑结构材料,利用双电子通路选择性促进了金属与支撑物之间的强相互作用。XAS 和 X 射线光电子能谱 (XPS) 技术更清楚地证明了金属与支撑物之间的相互作用,电子从 TiO2-C 支撑物中的缺陷转移到有序合金钯镍纳米催化剂上,从而使 H2O2 在环境条件下的生产率和选择性创下新高。本研究的结果将有助于设计出具有有序结构的新型异质纳米催化剂。杂化载体和活性位点之间的电子传递可以阐明催化行为,并促进过氧化氢直接合成过程中的进一步研究。关键词:过氧化氢;直接合成;异相纳米催化剂 PdNi;TiO2-C
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New Design PdNi Heterogeneous Nanocatalysts for the Direct Synthesis of Hydrogen Peroxide
Hydrogen peroxide (H2O2) is a widely used chemical as an eco-friendly oxidizing agent, with water being the only byproduct of oxidation in applications like bleaching pulp and paper, making electronic semiconductors, chemical and detergent synthesis, and wastewater treatment. The direct synthesis approach is preferred to provide the environmentally friendly production of H2O2 for market requirements. Bimetallic PdNi nanocatalysts were chosen for this study because of their catalytic activity and the structural characteristics of the material system. First, for the development of order-structured bimetallic PdNi nanocatalysts based on mesoporous carbon template after hydrogen-assisted heat treatment at 750∘C. The transformation of the disordered structure into ordered intermetallically structured PdNi alloys with higher alloying extents was confirmed by X-ray absorption spectroscopy (XAS) and high-resolution transition electron microscopy (HR-TEM). Then, to improve the oxygen oxidation reaction, two-electron pathway selectivity was used by TiO2-C as a support-ordered structure material to facilitate strong metal-support interactions. XAS and X-ray photoelectron spectra (XPS) techniques show more clear evidence of metal-support interactions with electron transfer from defects in the TiO2-C support to the ordered alloyed PdNi nanocatalysts, resulting in record productivity and selectivity of H2O2 production at ambient conditions. The results demonstrated in this study will enlighten a reliable design of new heterogeneous nanocatalysts with ordered structure. Electron transfer between hybrid support and active sites can clarify the catalytic behavior and prompt further research during the direct synthesis of hydrogen peroxide. Keywords: hydrogen peroxide, direct synthesis, heterogeneous nanocatalysts PdNi, TiO2-C
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