Atomically Dispersed Palladium to Enhance the Propyne Semihydrogenation over CeO2 Catalysts,Industrial & Engineering Chemistry Research

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Atomically Dispersed Palladium to Enhance the Propyne Semihydrogenation over CeO2 Catalysts
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2023-09-27 , DOI: 10.1021/acs.iecr.3c02392
Qiang Yuwen ₁ , Kelin Yan ₁ , Xiaohu Ge ₁ , Gang Qian ₁ , Jing Zhang ₁ , Yueqiang Cao _{1,

2} , Xinggui Zhou ₁ , Xuezhi Duan ₁

Affiliation

Metal oxides such as ceria (CeO₂) have been emerging as promising catalysts for selective hydrogenation, but the intrinsic activity is still limited due to the unfavorable activation of hydrogen under mild conditions. Herein, we report anchoring atomically dispersed Pd atoms onto as-synthesized CeO₂ nanorods (r-CeO₂) to decorate the oxide catalyst toward enhanced propyne semihydrogenation. Detailed characterizations, including aberration-corrected scanning transmission electron microscopy with atomic resolution, X-ray photoelectron spectroscopy (XPS), and diffuse reflectance infrared Fourier transform spectroscopy of CO adsorption, reveal the successful anchoring of atomically dispersed Pd on CeO₂ nanorods via a facile loading process. The catalytic tests show that the as-synthesized Pd_0.1/r-CeO₂ catalysts exhibit significantly increased hydrogenation activity as compared to the undecorated r-CeO₂, and the selectivity to target propylene is achieved to 95.3% at full conversion of propyne at around 95 °C on the Pd_0.1/CeO₂ catalyst. XPS, electron paramagnetic resonance, and temperature-programmed reduction tests unravel that the atomically dispersed Pd species remarkably promote the formation of oxygen vacancies on the surface of r-CeO₂, which is beneficial for H₂ activation and subsequently propyne semihydrogenation.

中文翻译：

原子分散钯在 CeO2 催化剂上增强丙炔半加氢反应

_{二氧化铈（CeO 2} ）等金属氧化物已成为选择性加氢的有前途的催化剂，但由于在温和条件下氢的不利活化，其内在活性仍然受到限制。在此，我们报告将原子分散的Pd原子锚定到合成的CeO ₂纳米棒(r-CeO ₂ )上以装饰氧化物催化剂以增强丙炔半氢化。详细的表征，包括具有原子分辨率的像差校正扫描透射电子显微镜、X射线光电子能谱 (XPS) 和 CO 吸附的漫反射红外傅立叶变换光谱，揭示了通过简单的方法将原子分散的 Pd 成功锚定在 CeO ₂纳米棒上。加载过程。_{催化测试表明，与未修饰的r-CeO 2}相比，所合成的Pd _0.1 /r-CeO ₂催化剂表现出显着提高的加氢活性，并且在丙炔完全转化的温度下，目标丙烯的选择性达到95.3％。在Pd _0.1 /CeO ₂催化剂上95℃ 。_{XPS、电子顺磁共振和程序升温还原测试表明，原子分散的Pd物质显着促进r-CeO 2}表面氧空位的形成，这有利于H 2活化_和随后的丙炔半氢化。

更新日期：2023-09-27

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