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Precise Design and Construction of 3D Nanoflowers Hollow Spherical NiO@MnMOx (M = Co, Cu, and Fe) Catalysts for Efficiently Catalytic Elimination of 1,2-Dichlorobenzene
Industrial & Engineering Chemistry Research ( IF 4.2 ) Pub Date : 2021-09-22 , DOI: 10.1021/acs.iecr.1c02530
Weitong Ling 1, 2 , Haijun Zhao 1 , Fei Zha 2 , Zhicheng Tang 1
Affiliation  

In this work, a series of three-dimensional (3D) Ni-based catalysts with hollow spherical shell and nanoflowers structures were successfully synthesized by hydrothermal and interfacial reaction methods, including Ni/C–Ar@MnCo NPs, NiO@MnCo NPs, NiO@MnCu NPs, and NiO@MnFe NPs. The Ni-based catalysts exhibited outstanding catalytic performance for the catalytic oxidation removal of 1,2-dichlorobenzene (o-DCB). What was interesting was that the NiO@MnCoOx catalyst derived from a NiO@MnCo NPs precursor exhibited a best catalytic performance with the temperature corresponding to 90% conversion (T90) at 375 °C for the catalytic oxidation of (o-DCB). Through Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), H2-temperature programmed reduction (H2-TPR), and temperature-programmed desorption of NH3/O2(NH3/O2-TPD) characterizations, it is found that NiO@MnCoOx catalyst possessed large specific surface area, more surface Ni2+, Mn4+, and Co3+ species, rich reactive oxygen species, strong redox ability, and a large number of strong acid sites, which jointly promoted the conversion of o-DCB at lower temperatures. Furthermore, a possible catalytic mechanism relating to Langmuir–Hinshelwood (L–H) models was proposed based on the active oxygen source on account of XPS, O2-TPD, and in situ DRIFTS measurements on catalytic performance. This strategy provides a new idea for the design of Ni-based composite catalysts and is of high importance for the design and synthesis of hollow nanoflowers.

中文翻译:

3D 纳米花空心球形 NiO@MnMOx(M = Co、Cu 和 Fe)催化剂的精确设计和构建,用于有效催化消除 1,2-二氯苯

在这项工作中,通过水热和界面反应方法成功合成了一系列具有空心球壳和纳米花结构的三维(3D)镍基催化剂,包括 Ni/C-Ar@MnCo NPs、NiO@MnCo NPs、NiO @MnCu NPs 和 NiO@MnFe NPs。Ni基催化剂在催化氧化去除1,2-二氯苯( o - DCB)方面表现出优异的催化性能。什么是有趣的是,氧化镍@ MnCoO X催化剂从的NiO @碳酸锰的NP衍生前体显示与对应于90%的转化率(温度的最佳催化性能Ť 90)在375℃下的催化氧化(Ô-DCB)。通过Brunauer-Emmett-Teller (BET)、X射线衍射(XRD)、X射线光电子能谱(XPS)、H 2 -程序升温还原(H 2 -TPR )和NH 3 /O的程序升温解吸2 (NH 3 /O 2 -TPD) 表征发现,NiO@MnCoO x催化剂具有较大的比表面积,更多的表面 Ni 2+、Mn 4+和 Co 3+物种,丰富的活性氧物种,强氧化还原能力,以及大量的强酸位点,共同促进了o-DCB 在较低温度下。此外,由于 XPS、O 2 -TPD 和对催化性能的原位 DRIFTS 测量,基于活性氧源提出了与 Langmuir-Hinshelwood (L-H) 模型相关的可能催化机制。该策略为镍基复合催化剂的设计提供了新思路,对中空纳米花的设计和合成具有重要意义。
更新日期:2021-10-06
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