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首页> 外文期刊>Catalysis science & technology >Synergistic effect between gold nanoparticles and Fe-doped gamma-MnO(2)toward enhanced aerobic selective oxidation of ethanol
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Synergistic effect between gold nanoparticles and Fe-doped gamma-MnO(2)toward enhanced aerobic selective oxidation of ethanol

机译：金纳米粒子之间的协同效应对增强有氧Fe-doped gamma-MnO (2)乙醇的选择性氧化

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摘要

Developing synergistic catalysts between gold nanoparticles (AuNPs) and supports is crucial to enhance the catalytic efficiency of supported AuNP catalysts for the aerobic selective oxidation of ethanol to acetaldehyde (AC). In this study, for the first time, AuNPs supported on metal-doped gamma-MnO2(Au/M-gamma-MnO2, M = Mg, Ca, Al, La, Fe, Co, Ni, Cu, Zn) catalysts with high gold dispersion were prepared by the colloidal deposition method and used in gas-phase ethanol oxidation to achieve up to 85% AC yield at 200 degrees C. It was found that the Au/M-gamma-MnO(2)catalysts show obviously higher reducibility and activity than the M-gamma-MnO(2)supports, and catalyst prereduction can further improve the catalytic activity. The strongest gold-support synergy was observed in the optimal Au/Fe-gamma-MnO(2)catalyst with a moderate Fe-doping amount, which can achieve the highest space-time-yield (similar to 3.2 g g(cat)(-1)h(-1)) and outperform the previously reported supported AuNP catalysts at 200 degrees C. Kinetic isotope effect studies clearly suggest that the alpha-C-H cleavage is more rate-limiting than the O-H cleavage in ethanol oxidation and the surface adsorbed oxygen species on MnO(2)is involved in the initial ethanol activation. By comparing the XPS spectra of the fresh and spent Au/Fe-gamma-MnO(2)catalysts, a novel Au-Mn-Fe synergy was proposed to account for its superior catalytic activity. The Mn(2+)and Fe(2+)defect-enriched catalyst interface is thought to facilitate the activation of O(2)and ethanol at lower temperature.
机译：发展协同催化剂之间的黄金纳米颗粒(AuNPs)和支持是至关重要的提高催化效率的支持AuNP有氧选择性的催化剂乙醇氧化乙醛(AC)。这项研究中,首次AuNPs支持在metal-doped gamma-MnO2 (Au / M-gamma-MnO2 M =Mg, Ca、Al La Fe、Co、Ni、Cu、Zn) catalysts高金分散准备的胶体沉积方法和用于气相乙醇氧化达到85% AC收益率在200度c,这是发现非盟/ M-gamma-MnO(2)催化剂显示明显更高比的还原性和活动M-gamma-MnO(2)支持,预还原催化剂可以进一步提高催化活性。最强的金牌支持协同中观察到最优盟/ Fe-gamma-MnO(2)的催化剂温和Fe-doping量,从而实现最高space-time-yield(类似于3.2 gh g(猫)(1)(1))和比以前报告支持AuNP催化剂在200度c .动力学同位素效应研究清楚地显示alpha-C-H乳沟是更多的病原比乙醇氧化和地裂表面吸附氧物种MnO (2)参与最初的乙醇激活。比较新鲜的XPS谱和花非盟/ Fe-gamma-MnO(2)催化剂,小说Au-Mn-Fe协同提出了占其优越的催化活性。铁(2 +)defect-enriched接口是催化剂认为促进O(2)和的激活乙醇在较低的温度。

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