Synergistic tuning of the phase structure of alumina and ceria-zirconia in supported palladium catalysts for enhanced methane combustion

Synergistic tuning of the phase structure of alumina and ceria-zirconia in supported palladium catalysts for enhanced methane combustion
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协同调节负载钯催化剂中氧化铝和氧化铈-氧化锆的相结构以增强甲烷燃烧

DOI:
10.1016/j.ijhydene.2021.07.151
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发表时间:
2021-08
影响因子:
7.2
通讯作者:
Ying Zheng
Ying Zheng
中科院分区:
工程技术2区
文献类型:
--
作者:
Jia Lin;Yelin Chen;Jiangli Huang;Guohui Cai;Yihong Xiao;Yingying Zhan;Ying Zheng

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CeO 2-ZrO 2-Al 2 O3复合氧化物负载钯催化剂(Pd/CZA)是一种很有前途的催化氧化反应催化剂。然而,甲烷在Pd基催化剂上的有效和稳定的氧化仍然是一个长期的挑战。在此,我们提出了一个简单的策略,以提高催化性能的Pd/CZA通过精心调整载体的相结构。在较高温度(1200、1300 °C)下焙烧载体,可诱导Al_2O_3的相转变(由γ-相转变为α-相)和CeO_2-ZrO_2固溶体(CZ)的形成。α-Al_2O_3与PdO之间的弱相互作用使催化剂的还原性能得到改善。同时,结晶良好的CZ相具有较高的氧迁移率,有利于Pd再氧化为PdO,产生大量的表面活性Pd 2+物种。再加上α-Al 2 O3的疏水性,1300 °C焙烧的CZA载体制备的催化剂表现出优异的低温活性和惊人的稳定性,并大大提高了对甲烷燃烧的耐水性。
CeO2–ZrO2–Al2O3composite oxides supported palladium catalysts (Pd/CZA) are promising candidates for catalytic oxidation reactions. However, the efficient and stable oxidation of methane over Pd-based catalysts remains a longstanding challenge. Herein, we present a facile strategy to boost the catalytic performance of Pd/CZA through elaborately tuning the phase structure of supports. Calcining supports at relatively high temperatures (1200, 1300 °C) induced the phase transition of alumina (from γ-to α-) and the development of CeO2–ZrO2solid solution (CZ). The weak interaction between α-Al2O3and PdO resulted in an improved reducibility of catalysts. Meanwhile, the higher oxygen mobility originated from well-crystallized CZ phase contributed to the reoxidation of Pd to PdO, giving rise to abundant surface active Pd2+species. Coupled with the hydrophobicity of α-Al2O3, the catalyst prepared with CZA supports calcined at 1300 °C demonstrated an excellent low-temperature activity, astounding stability and greatly enhanced water resistance towards methane combustion.
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