Cavaye Hamish, E Ballas Christos, Kockelmann Winfried, Parker Stewart F, Collier Paul, York Andrew P E, Lennon David
ISIS Pulsed Neutron and Muon Source, STFC Rutherford Appleton Laboratory, Chilton, OX11 0QX, UK.
School of Chemistry, University of Glasgow, Joseph Black Building, Glasgow, G128QQ, UK.
Sci Rep. 2025 Mar 12;15(1):8579. doi: 10.1038/s41598-025-91179-6.
The combination of a heterogeneous catalyst operating within a defined reactor comes within the domain of reaction engineering, which takes cognisance of combined roles for both the catalyst and the reactor to define the overall operational system. One technique which is demonstrating much promise in investigating reaction engineering issues is neutron imaging. The technique is skewed towards monitoring hydrogen and hydrogenous species so, with hydrogen being ubiquitous in industrial organic chemistry and the penetrating power of the neutrons, neutron imaging can monitor hydrogen concentrations distributed throughout steel reactors whilst the reaction is taking place. In this way, neutron imaging can be used to assess the homogeneity of active catalyst beds and, additionally, determine how hydrogen is being partitioned throughout the catalyst bed as a function of time-on-stream. These are important parameters in the reaction engineering of catalytic systems involving transformations of hydrogen containing species. The article commences by reviewing the handful of existing neutron imaging studies in this field, then progresses to describe the application of the neutron imaging technique to investigate ethene hydrogenation over a 5 wt% Pd/C powder catalyst at 333 K and ambient pressure in a rectangular stainless-steel reactor. Modulations of the incident gas stream are seen to lead to spatially resolvable fronts moving across the bed and illustrate the diffusion of reagents from the reactor inlet across to the reactor exit. Thus, the investigation reveals spatially and temporally resolved elementary reactions that contribute to the hydrogenation process.
在特定反应器内运行的多相催化剂的组合属于反应工程领域,该领域认识到催化剂和反应器的综合作用以定义整个操作系统。在研究反应工程问题方面显示出很大前景的一种技术是中子成像。该技术倾向于监测氢和含氢物种,因此,由于氢在工业有机化学中无处不在且中子具有穿透能力,中子成像可以在反应进行期间监测分布在整个钢制反应器中的氢浓度。通过这种方式,中子成像可用于评估活性催化剂床层的均匀性,此外,还可确定氢如何作为运行时间的函数在整个催化剂床层中分配。这些是涉及含氢物种转化的催化系统反应工程中的重要参数。本文首先回顾了该领域现有的少数中子成像研究,然后进而描述了中子成像技术在矩形不锈钢反应器中于333 K和常压下研究5 wt% Pd/C粉末催化剂上乙烯加氢反应的应用。可以看到入射气流的调制导致在床层中移动的空间可分辨前沿,并说明了试剂从反应器入口扩散到反应器出口的情况。因此,该研究揭示了对加氢过程有贡献的空间和时间分辨的基元反应。