Catalytic oxidation of toluene promoted by Mn-Ce solid solutions with multiple active sites and high oxygen mobility

IF 4.7 2区 化学 Q2 CHEMISTRY, PHYSICAL
Zedong Chen , Jiabin Zhou , Xianjie Liu , Dan Liu , Quanjun Xiang
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引用次数: 0

Abstract

In this study, the active site density and lattice oxygen mobility on the surface of (MnCe)Ox solid solution catalysts were synchronously optimized by controlling the ratio and sequence of the addition of tetrapropylammonium hydroxide and dextran. This led to the exceptional performance of co-modified Mn-Ce solid solution catalysts in efficiently degrading toluene. The best catalytic performance of toluene oxidation was achieved after applying 0.1 mol/L tetrapropylammonium hydroxide followed by 2 % dextran modified (MnCe)Ox (0.1T-2 % D-MC). The toluene conversion rate reached 90 % at 211 °C. As observed by scanning electron microscopy (SEM) and Raman spectroscopy (Raman), tetrapropylammonium hydroxide tends to interact with CeO2, thus generating oxygen vacancies. Meanwhile, the porous structure on the catalyst surface was induced to form, the specific surface area was increased, the active component grain size was reduced, and the active site density was increased. Oxygen temperature programmed desorption (O2-TPD) and X-ray photoelectron spectroscopy (XPS) results showed that dextran interacted with MnOx to produce lattice defects, and complexed with metal ions, thus the rate of cycling of lattice oxygen species was increased. The Mn-CeO2 (111)-Ov-OH model exhibits excellent adsorption capacity for toluene and oxygen molecules (-0.9025 eV, −5.9739 eV). A new approach to utilize organic substances and auxiliary agents with targeting properties as modifiers is proposed in this paper. The limitations of MnCe binary catalysts in practical applications were successfully broken through. A new idea and method for solving related scientific problems are provided by the research results.
具有多活性位点和高氧迁移率的锰铈固溶体对甲苯的催化氧化作用
本研究通过控制四丙基氢氧化铵和葡聚糖的加入比例和顺序,同步优化了(MnCe)Ox固溶体催化剂表面的活性位点密度和晶格氧迁移率。这使得共改性锰铈固溶体催化剂在高效降解甲苯方面表现优异。以0.1 mol/L四丙基氢氧化铵为催化剂,再以2 %葡聚糖修饰(MnCe)Ox (0.1 t -2 % D-MC)为催化剂,甲苯氧化反应效果最佳。在211℃时,甲苯的转化率达到90 %。通过扫描电镜(SEM)和拉曼光谱(Raman)观察到,四丙基氢氧化铵倾向于与CeO2相互作用,从而产生氧空位。同时,诱导催化剂表面形成多孔结构,增加了比表面积,减小了活性组分粒度,增加了活性位点密度。氧温程序解吸(O2-TPD)和x射线光电子能谱(XPS)结果表明,右旋糖酐与MnOx相互作用产生晶格缺陷,并与金属离子络合,从而提高了晶格氧的循环速率。Mn-CeO2 (111)-Ov-OH模型对甲苯和氧分子具有良好的吸附能力(-0.9025 eV, - 5.9739 eV)。提出了一种利用具有靶向性的有机物质和助剂作为改性剂的新方法。成功突破了MnCe二元催化剂在实际应用中的局限性。研究成果为解决相关科学问题提供了新的思路和方法。
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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
期刊介绍: Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.
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