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从废弃的锂离子锰酸盐电池中用锰基多氧化物去除含氧挥发性有机化合物的促进作用:用 Fe、Bi 和 Ce 掺杂剂进行改性。

Promotional removal of oxygenated VOC over manganese-based multi oxides from spent lithium-ions manganate batteries: Modification with Fe, Bi and Ce dopants.

机构信息

School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dong Chuan Road, Shanghai 200240, PR China.

School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dong Chuan Road, Shanghai 200240, PR China; Shanghai Institute of Pollution Control and Ecology Security, Shanghai 200092, PR China.

出版信息

Sci Total Environ. 2020 Oct 20;740:139951. doi: 10.1016/j.scitotenv.2020.139951. Epub 2020 Jun 11.

Abstract

In this work, cathode materials of spent lithium-ions manganate batteries are recovered as the precursor of manganese-based oxides catalysts and furthermore, different amount of Fe, Bi, Ce are introduced to modify their properties. A series of MnOx(MS)-X Fe, MnOx(MS)-X Bi and MnOx(MS)-X Ce samples with crystal phase of MnO are synthesized using combustion method and then the catalytic behavior and physicochemical properties of prepared catalysts are investigated. Compared to binary MnOx-5% Fe, MnOx-15% Bi and MnOx-10% Ce samples, multi MnOx(MS)-5% Fe, MnOx(MS)-15 Bi and MnOx(MS)-10% Ce catalysts display enhanced catalytic performance significantly in the removal of oxygenated VOC, which could be attributed to larger specific surface area, higher concentration of surface active oxygen species and Mn ions and better reducibility at low temperature. In-situ DRIFTS results imply that main oxygen-containing functional groups such as carbonyl (-C=O), carboxyl (-COO), hydroxyl (-OH) can be observed during VOC oxidation and by comparison, it can be found that gas-phase O plays a crucial role in facilitating the further oxidation of by-products into CO. In addition, TD/GC-MS results point out that the main by-products are formaldehyde; 2-propanol, 1-methoxy-; ethanol, 2-methoxy-, acetate; 2-ethoxyethyl acetate; acetic acid during VOC oxidation.

摘要

在这项工作中,回收废旧锂离子锰酸盐电池的阴极材料作为锰基氧化物催化剂的前体,进一步引入不同量的 Fe、Bi、Ce 来修饰其性质。采用燃烧法合成了一系列具有 MnO 晶相的 MnOx(MS)-XFe、MnOx(MS)-XBi 和 MnOx(MS)-XCe 样品,研究了制备催化剂的催化性能和物理化学性质。与二元 MnOx-5%Fe、MnOx-15%Bi 和 MnOx-10%Ce 样品相比,多相 MnOx(MS)-5%Fe、MnOx(MS)-15%Bi 和 MnOx(MS)-10%Ce 催化剂在去除含氧挥发性有机化合物方面表现出显著增强的催化性能,这归因于更大的比表面积、更高浓度的表面活性氧物种和 Mn 离子以及更好的低温还原性。原位 DRIFTS 结果表明,在 VOC 氧化过程中可以观察到主要的含氧官能团,如羰基(-C=O)、羧基(-COO)、羟基(-OH),相比之下,可以发现气相 O 在促进副产物进一步氧化成 CO 方面起着至关重要的作用。此外,TD/GC-MS 结果指出,在 VOC 氧化过程中主要的副产物是甲醛;2-丙醇,1-甲氧基-;乙醇,2-甲氧基-,醋酸盐;2-乙氧基乙基醋酸盐;醋酸。

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