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通过物理封装SiO限制并与CeO进行化学金属-载体相互作用的Ni-Cu合金纳米颗粒用于甲烷干重整。

Ni-Cu Alloy Nanoparticles Confined by Physical Encapsulation with SiO and Chemical Metal-Support Interaction with CeO for Methane Dry Reforming.

作者信息

Shi Yu, Han Kaihang, Wang Fagen

机构信息

School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 202123, China.

Chinese Academy of Sciences Key Laboratory of Renewable Energy, Guangzhou 510640, China.

出版信息

Inorg Chem. 2022 Oct 3;61(39):15619-15628. doi: 10.1021/acs.inorgchem.2c02466. Epub 2022 Sep 21.

Abstract

Fabrication of sintering- and carbon-free Ni catalysts for methane dry reforming (MDR), which is attractive to upgrade greenhouse gases CH and CO, is challenging. In this work, we innovatively synthesized Ni-Cu alloy nanoparticles confined by physical encapsulation and chemical metal-support interaction (MSI); the synergism of alloy effect, size effect, MSI, and confinement effect in the catalysts gave high rates of CH and CO of 6.98 and 7.16 mmol/(gs), respectively, at 1023 K for 50 h. The rates were 2-3 times enhanced compared to those in the literature. XRD, TEM, H-TPR, and so forth revealed that the alloy effect, size effect, and MSI of Ni-Cu and CeO enhanced the MDR activity; MSI promoted the ceria surface lattice oxygen mobility and generated more oxygen vacancies, almost completely gasifying carbon deposits; chemical confinement from MSI and physical confinement from SiO nanospheres realized sintering-free alloys and CeO nanoparticles. The synergistic approach provides a universal strategy for sintering- and carbon-free Ni catalyst design for MDR reaction.

摘要

制备用于甲烷干重整(MDR)的无烧结和无碳镍催化剂具有挑战性,而甲烷干重整对于升级温室气体CH和CO具有吸引力。在这项工作中,我们创新性地合成了通过物理封装和化学金属-载体相互作用(MSI)限制的Ni-Cu合金纳米颗粒;催化剂中合金效应、尺寸效应、MSI和限制效应的协同作用在1023 K下50小时内分别给出了6.98和7.16 mmol/(gs)的高CH和CO速率。与文献中的速率相比,这些速率提高了2至3倍。XRD、TEM、H-TPR等表明,Ni-Cu和CeO的合金效应、尺寸效应和MSI提高了MDR活性;MSI促进了二氧化铈表面晶格氧迁移率并产生了更多氧空位,几乎完全气化了碳沉积物;MSI的化学限制和SiO纳米球的物理限制实现了无烧结合金和CeO纳米颗粒。这种协同方法为MDR反应的无烧结和无碳镍催化剂设计提供了一种通用策略。

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