具有优化 CeO2 载体形态的 Ni/CeO2 纳米催化剂用于 CH4 氧化,ACS Applied Nano Materials

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具有优化 CeO2 载体形态的 Ni/CeO2 纳米催化剂用于 CH4 氧化
ACS Applied Nano Materials ( IF 5.3 ) Pub Date : 2023-03-07 , DOI: 10.1021/acsanm.2c05496
Junjie Chen ₁ , Hien N. Pham ₂ , Tala Mon ₁ , Todd J. Toops ₃ , Abhaya K. Datye ₂ , Zhenglong Li ₄ , Eleni A. Kyriakidou ₁

Affiliation

CH ₄在非贵金属Ni/CeO ₂催化剂上的催化氧化引起了广泛关注。_{控制CeO 2}载体的形态可以在不改变催化剂组成的情况下提高CH _{4氧化活性。}在此，评估了一系列具有不同 CeO 2 载体形态（纳米颗粒 (P)、棒状 (R)、立方体 (C)）的 2 wt% Ni/CeO 2纳米催化剂_和_合成程序（沉淀、溶胶-凝胶 (SG)）因为它们的 CH ₄氧化性能。_{CeO 2}载体和相应的Ni负载催化剂的氧化还原性能通过H ₂表征-程序升温还原和储氧能力 (OSC) 测量。建立了CeO ₂载体和 Ni/CeO _{2催化剂的 CeO}₂形态、表面积、氧化还原性质和 CH ₄氧化活性之间的关系。研究结果表明，与 CeO ₂ -P 和 CeO ₂ -C 载体相比，CeO ₂ -R 具有更多的表面氧空位以及改进的 OSC 和 CH _{4氧化活性。}对于含 Ni 的催化剂观察到相同的 CH _{4氧化活性模式（Ni/CeO}₂ -R > Ni/CeO ₂ -P > Ni/CeO ₂-C）。与CeO ₂ -R相比，通过使用溶胶-凝胶合成法（CeO _{2 -SG）增加CeO}₂表面积提高了CeO ₂ -SG和Ni/CeO ₂ -SG的表面氧空位量和CH ₄氧化性能和Ni/CeO ₂ -R，分别。_{最后，与传统的 Pd/Al 2} O ₃相比，所有研究的 Ni/CeO ₂纳米催化剂都显示出改进的水热稳定性。

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Ni/CeO2 Nanocatalysts with Optimized CeO2 Support Morphologies for CH4 Oxidation

Catalytic oxidation of CH₄ over nonprecious Ni/CeO₂ catalysts has attracted wide attention. Controlling the morphology of a CeO₂ support can enhance the CH₄ oxidation activity without changing the catalyst composition. Herein, a series of 2 wt % Ni/CeO₂ nanocatalysts with different CeO₂ support morphologies (nanoparticles (P), rods (R), cubes (C)) and synthetic procedures (precipitation, sol-gel (SG)) were evaluated for their CH₄ oxidation performance. The redox properties of CeO₂ supports and corresponding Ni loaded catalysts were characterized by H₂-temperature-programmed reduction and oxygen storage capacity (OSC) measurements. The relationship among the CeO₂ morphologies, surface areas, redox properties, and CH₄ oxidation activity for both CeO₂ supports and Ni/CeO₂ catalysts was established. The findings suggest that CeO₂-R has a greater amount of surface oxygen vacancies as well as an improved OSC and CH₄ oxidation activity compared to CeO₂-P and CeO₂-C supports. The same CH₄ oxidation activity pattern was observed for the Ni containing catalysts (Ni/CeO₂-R > Ni/CeO₂-P > Ni/CeO₂-C). Increasing the CeO₂ surface area by using a sol-gel synthesis method (CeO₂-SG) improved the amount of surface oxygen vacancies and CH₄ oxidation performance of CeO₂-SG and Ni/CeO₂-SG compared to CeO₂-R and Ni/CeO₂-R, respectively. Finally, all studied Ni/CeO₂ nanocatalysts showed improved hydrothermal stability compared to conventional Pd/Al₂O₃.

更新日期：2023-03-07

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