X-ray physico-chemical imaging during activation of cobalt-based Fischer-Tropsch synthesis catalysts.

X-ray physico-chemical imaging during activation of cobalt-based Fischer-Tropsch synthesis catalysts.
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DOI:
10.1098/rsta.2017.0057
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发表时间:
2018-01-13
期刊:
Philosophical transactions. Series A, Mathematical, physical, and engineering sciences
影响因子:
--
通讯作者:
Paterson J
Paterson J
中科院分区:
其他
文献类型:
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作者:
Beale AM;Jacques SDM;Di Michiel M;Mosselmans JFW;Price SWT;Senecal P;Vamvakeros A;Paterson J

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近年来,催化剂和其他功能材料在反应条件下的成像有了显著的进展。计算机断层扫描(CT)方法与X射线衍射(XRD)、X射线荧光(XRF)和X射线吸收近边光谱(XANES)等方法相结合,现在可以从偶然或设计不均匀的完整材料内部提取局部化学和物理状态信息。在这项工作中,对于用作费托合成(FTS)催化剂的含Co颗粒,我们跟踪在初始还原步骤(一个或多个)期间形成Co金属的相演变;首先,在小的长度尺度(约100微米)下工作。由于XRF-CT具有高的空间分辨率(微米空间分辨率),样本大小和密度的组合允许传输相对低能量的信号,从而能够记录“多模式”断层扫描,即同时进行XRF-CT、XANES-CT和XRD-CT。随后,我们表明高能XRD-CT可以用来揭示毫米级TiO 2三叶的晶粒尺寸的减少和均匀性的程度。在这两项研究中,CoO相被认为是持续存在或在特定的操作条件下发展,我们推测为什么会观察到这一点。这篇文章是讨论会议议题“为快速变化的世界提供可持续的催化解决方案”的一部分。
The imaging of catalysts and other functional materials under reaction conditions has advanced significantly in recent years. The combination of the computed tomography (CT) approach with methods such as X-ray diffraction (XRD), X-ray fluorescence (XRF) and X-ray absorption near-edge spectroscopy (XANES) now enables local chemical and physical state information to be extracted from within the interiors of intact materials which are, by accident or design, inhomogeneous. In this work, we follow the phase evolution during the initial reduction step(s) to form Co metal, for Co-containing particles employed as Fischer–Tropsch synthesis (FTS) catalysts; firstly, working at small length scales (approx. micrometre spatial resolution), a combination of sample size and density allows for transmission of comparatively low energy signals enabling the recording of ‘multimodal’ tomography, i.e. simultaneous XRF–CT, XANES–CT and XRD–CT. Subsequently, we show high-energy XRD–CT can be employed to reveal extent of reduction and uniformity of crystallite size on millimetre-sized TiO2 trilobes. In both studies, the CoO phase is seen to persist or else evolve under particular operating conditions and we speculate as to why this is observed. This article is part of a discussion meeting issue ‘Providing sustainable catalytic solutions for a rapidly changing world’.
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