Role of oxygen species and active phase of CuCeZrOx prepared with bacterial cellulose for toluene catalytic oxidation

IF 6.4 3区 环境科学与生态学 Q2 ENERGY & FUELS
Chenhang Zhang , Chenchen Zhao , Running Kang , Qinglan Hao , Baojuan Dou , Feng Bin
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Abstract

The present study investigates the active phases and the role of oxygen species in the toluene oxidation process over CuCeZrOx catalysts prepared with bacterial cellulose (BC), and compares them with nitric acid pickling CuCeZrOx-BC(H) and CeZrOx-BC catalysts. The investigation is carried out using in-situ DRIFT, O2-TPD, H2-TPR, XRD, and TEM techniques. Our findings suggest that dispersed CuO species on the catalyst surface, Cu-Ce-Zr-O, and Ce-Zr-O solid solutions are active for toluene oxidation over CuCeZrOx-BC, with corresponding activities decreasing successively. The in-situ DRIFT results demonstrate that gaseous oxygen facilitates the chemisorption of toluene on active oxygen species, forming benzoyl oxide species and partially oxidizing the absorbed intermediates to benzyl alcohol at room temperature. Furthermore, lattice oxygen is experimentally found to be involved in the deep oxidation of toluene, and the lattice oxygen present in dispersed CuO species dominates the toluene oxidation process over CuCeZrOx-BC.

细菌纤维素制备CuCeZrOx在甲苯催化氧化中的作用及活性相
本研究研究了细菌纤维素(BC)制备的CuCeZrOx催化剂上的活性相及其氧在甲苯氧化过程中的作用,并将其与硝酸酸洗CuCeZrOx-BC(H)和CeZrOx-BC催化剂进行了比较。利用原位DRIFT、O2-TPD、H2-TPR、XRD和TEM技术进行了研究。我们的研究结果表明,分散在催化剂表面的CuO物种、Cu-Ce-Zr-O和Ce-Zr-O固溶体对CuCeZrOx-BC上的甲苯氧化具有活性,相应的活性依次降低。原位DRIFT结果表明,气态氧促进甲苯在活性氧物种上的化学吸附,形成苯甲酰氧化物物种,并在室温下将吸收的中间体部分氧化为苯甲醇。此外,实验发现晶格氧参与甲苯的深度氧化,并且存在于分散的CuO物种中的晶格氧在甲苯氧化过程中比CuCeZrOx BC占主导地位。
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来源期刊
Carbon Resources Conversion
Carbon Resources Conversion Materials Science-Materials Science (miscellaneous)
CiteScore
9.90
自引率
11.70%
发文量
36
审稿时长
10 weeks
期刊介绍: Carbon Resources Conversion (CRC) publishes fundamental studies and industrial developments regarding relevant technologies aiming for the clean, efficient, value-added, and low-carbon utilization of carbon-containing resources as fuel for energy and as feedstock for materials or chemicals from, for example, fossil fuels, biomass, syngas, CO2, hydrocarbons, and organic wastes via physical, thermal, chemical, biological, and other technical methods. CRC also publishes scientific and engineering studies on resource characterization and pretreatment, carbon material innovation and production, clean technologies related to carbon resource conversion and utilization, and various process-supporting technologies, including on-line or off-line measurement and monitoring, modeling, simulations focused on safe and efficient process operation and control, and process and equipment optimization.
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