Uncoupling the size and support effects of Ni catalysIs for dry reforming of methane
Uncoupling the size and support effects of Ni catalysIs for dry reforming of methane
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DOI：
10.1016/j.apcatb.2016.10.069
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发表时间：
2017-04-01
影响因子：
22.1
通讯作者：
Lee, Hyunjoo
中科院分区：
文献类型：
--
作者：
Han, Joung Woo;Park, Jun Seong;Lee, Hyunjoo
甲烷干重整（DRM; CH 4 + CO2 2 H（2）+ 2CO）可以是利用温室气体生产有价值的合成气的好方法。镍基催化剂已被用于该反应;然而，镍的尺寸效应和载体效应是高度耦合的，因此不能单独观察。在这里，设计了一种独特的催化剂，其中Ni纳米颗粒尺寸和载体可以独立地变化。在800 ℃下测试了尺寸为2.6、5.2、9.0和17.3 nm的高度均匀的Ni纳米颗粒的DRM，而Ni尺寸没有显著变化，并且用5.2 nm的Ni纳米颗粒测试了各种金属氧化物（包括SiO2、Al（2）O3、MgO、ZrO 2、TiO 2）的覆盖层。分别评价了CH 4或CO2周转频率对Ni尺寸和载体的依赖性。2.6 nm的Ni纳米颗粒比17.3 nm的Ni纳米颗粒的甲烷周转频率高4.1倍。当用相同的5.2 nm Ni测试各种金属氧化物覆盖层时，Al 2 O3表现出比SiO2高4.3倍的甲烷周转频率。独立观察Ni纳米颗粒尺寸和载体的影响将为设计有效的甲烷干重整催化剂提供有价值的指导。(C)2016爱思唯尔B. V.保留所有权利。
The dry reforming of methane (DRM; CH4 + CO2 2H(2) + 2CO) can be a good way to utilize greenhouse gases for the production of valuable syn-gas. Ni-based catalysts have been used for this reaction; however, the Ni size effect and support effect were highly coupled and therefore could not be observed separately. Here, a unique catalyst in which the Ni nanoparticle size and support can be varied independently was devised. Highly uniform Ni nanoparticles with sizes of 2.6, 5.2, 9.0, and 17.3 nm were tested for DRM at 800 degrees C without a significant change in the Ni size, and overlayers of various metal oxides, including SiO2, Al(2)O3, MgO, ZrO2, TiO2, were tested with the 5.2 nm of Ni nanoparticles. The dependence of the CH4 or CO2 turnover frequency on the Ni size and support was evaluated separately. The 2.6 nm Ni nanoparticles showed 4.1 times higher methane turnover frequency than those with a size of 17.3 nm. When various metal oxide overlayers were tested with the same 5.2 nm Ni, Al2O3 exhibited 4.3 times higher methane turnover frequency than SiO2. The independent observation of the effects of the Ni nanoparticle size and support will provide valuable guidelines for designing effective methane dry reforming catalysts. (C) 2016 Elsevier B.V. All rights reserved.