A surficial in situ growth strategy to fabricate monolithic catalysts of mesoporous Co-Cu bimetallic oxides supported on Ni foam for ethyl acetate efficiently oxidation

IF 6.3 2区 材料科学 Q2 CHEMISTRY, PHYSICAL
Yanfei Jian, Xinyu Wang, Mudi Ma, Rui Yang, Qiyuan Liu, Lianghui Xia, Lu Li, Chi He
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Abstract

A series of monolithic Cu-doped Co3O4 supported on Ni foam (NF) catalysts with mesoporous structure were successfully prepared by in situ hydrothermal synthesis, where the oxygen species and textural properties were regulated by varying the Cu/Co ratio of bimetallic mixed oxides supported on Ni foam. The role of oxygen species in catalytic oxidation of ethyl acetate (EA) was also elucidated. As a result, the monolithic catalyst with Co/Cu molar ratio of 1/2, labeled as CoCu2Ox-NF, exhibited the highest conversion rate for EA oxidation (T99 = 230 °C, GHSV = 3000 h−1). The results of characterization show that its robust catalytic performance could be attributed to superior reducibility, sufficient Co3+ species and high mobility of active oxygen. In addition, the larger surface area and pore volume were also beneficial to catalytic performance due to increased gas diffusion. The characterization results of fresh and used catalysts and the study of reaction mechanism showed that lattice oxygen species played an important role in EA oxidation process which accelerated the EA activation and deep oxidation of carboxylate species over CoCu2Ox-NF. As expected, the CoCu2Ox-NF catalyst also presented good stability over EA oxidation in the presence of toluene as well as o-xylene. Hence, CoCu2Ox-NF possessed satisfactory universality and long-term durability, which is a promising catalyst for industrial application.

Abstract Image

泡沫镍负载介孔Co-Cu双金属氧化物整体式高效氧化乙酸乙酯催化剂的表面原位生长策略
采用原位水热合成方法成功制备了一系列介孔结构的单片Cu掺杂Co3O4泡沫镍催化剂,通过改变泡沫镍负载的双金属混合氧化物的Cu/Co比来调节其氧的种类和结构性能。探讨了氧在催化氧化乙酸乙酯(EA)中的作用。结果表明,Co/Cu摩尔比为1/2的整体催化剂,标记为cocu2o - nf,具有最高的EA氧化转化率(T99 = 230 °C, GHSV = 3000 h−1)。表征结果表明,其强劲的催化性能可归因于优异的还原性、充足的Co3+种类和高的活性氧迁移率。此外,更大的表面积和孔隙体积也有利于气体扩散,从而提高催化性能。新鲜催化剂和二手催化剂的表征结果和反应机理研究表明,晶格氧在EA氧化过程中起重要作用,加速了cocu2o - nf上羧酸盐的EA活化和深度氧化。正如预期的那样,cocu2o - nf催化剂在甲苯和邻二甲苯的存在下也表现出良好的EA氧化稳定性。因此,cocu2o - nf具有良好的通用性和长期耐久性,是一种具有工业应用前景的催化剂。
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来源期刊
Applied Surface Science
Applied Surface Science 工程技术-材料科学:膜
CiteScore
12.50
自引率
7.50%
发文量
3393
审稿时长
67 days
期刊介绍: Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.
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