Novel Core-Shell (ε-MnO2/CeO2)@CeO2 Composite Catalyst with a Synergistic Effect for Efficient Formaldehyde Oxidation.,ACS Applied Materials & Interfaces

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Novel Core-Shell (ε-MnO2/CeO2)@CeO2 Composite Catalyst with a Synergistic Effect for Efficient Formaldehyde Oxidation.
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2020-08-11 , DOI: 10.1021/acsami.0c09263
Shuai Zhang ₁ , Haozhe Wang ₂ , Huayan Si _{2,

3} , Xiaoqian Jia _{1,

3} , Ziyan Wang ₁ , Qiang Li _{1,

3} , Jing Kong ₂ , Jianbin Zhang _{1,

2,

3}

Affiliation

A novel core–shell (ε-MnO₂/CeO₂)@CeO₂ composite catalyst with a synergistic effect was prepared by hydrothermal reaction and thermal decomposition and its application to high-efficiency oxidation removal of formaldehyde (HCHO) was systemically investigated. The (MnCO₃/CeO₂)@CeO₂ precursor was prepared first by the one-pot hydrothermal reaction of Mn²⁺ and Ce³⁺ solutions with a CO₂-storage material (CO₂SM) without any external templates or surfactants required. The thermal decomposition of the precursor afforded the core–shell (ε-MnO₂/CeO₂)@CeO₂ composite catalyst with excellent catalytic performance. HCHO in the feed gas (180 ppm HCHO, 21% O₂, N₂ balanced) at a gas hourly space velocity of 100 L/(g_cat h) is 100% converted over the catalyst at 80 °C. The conversion rate remains above 95% in 72 h and above 73.8% in 140 h, suggesting the strong stability of the catalyst at high gas flow rates and relatively low temperatures. The synergistic mechanism of the catalyst was explored by X-ray diffraction, Raman, Brunauer–Emmett–Teller, transmission electron microscopy, and X-ray photoelectron spectroscopy. The number of defects in the catalyst and the strength of the Mn–O bond in ε-MnO₂ can be tuned by adjusting the synthesis conditions. More oxygen vacancies on the surface of CeO₂ can make the synergistic effect of the catalyst stronger, which significantly improves the lattice oxygen (O_latt) activity on the surface of ε-MnO₂. Our work has provided new insights into the preparation of the desired composite catalysts with excellent performances.

中文翻译：

具有协同作用的新型核-壳（ε-MnO2/ CeO2）@ CeO2复合催化剂，可有效甲醛氧化。

一种新颖的芯-壳（ε-的MnO ₂ /的CeO ₂）@CeO ₂具有协同作用的复合催化剂是由水热反应和热分解中的应用，以高效率氧化除去的甲醛（HCHO）的制备进行了系统研究。（MnCO ₃ / CeO ₂）@CeO ₂前驱体是通过Mn ²⁺和Ce ³⁺溶液与CO ₂储存材料（CO ₂ SM）的一锅法水热反应制备的，不需要任何外部模板或表面活性剂。得到核-壳前体的热分解（ε-的MnO ₂ /的CeO ₂）@CeO ₂复合催化剂，具有优异的催化性能。进料气中的HCHO（180 ppm HCHO，21％O ₂，N ₂平衡）在80 L的催化剂气速下通过100 L /（g _cat h）的气时空速转化。转化率在72小时内保持在95％以上，在140小时内保持在73.8％以上，这表明催化剂在高气体流速和相对较低的温度下具有很强的稳定性。通过X射线衍射，拉曼光谱，Brunauer–Emmett–Teller，透射电子显微镜和X射线光电子能谱探索了催化剂的协同机理。在催化剂的缺陷和数量在MnO的键的强度ε-的MnO ₂可以通过调节合成条件来调节。的CeO的表面上更氧空位₂可以使催化剂更强，这显著改善晶格氧（O的协同效应_LATT）活性ε-的MnO的表面上₂。我们的工作为制备具有优异性能的所需复合催化剂提供了新见识。

更新日期：2020-09-10

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