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基于多壁碳纳米管的复合材料作为水煤气变换和加氢甲酰化反应的催化剂载体

Multi-walled carbon nanotube-based composite materials as catalyst support for water-gas shift and hydroformylation reactions.

作者信息

Wolf Patrick, Logemann Morten, Schörner Markus, Keller Laura, Haumann Marco, Wessling Matthias

机构信息

Lehrstuhl für Chemische Reaktionstechnik (CRT), Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU) Egerlandstr. 3 91058 Erlangen Germany

Chemical Process Engineering, RWTH Aachen University Forckenbeckstr. 51 52074 Aachen Germany.

出版信息

RSC Adv. 2019 Sep 3;9(47):27732-27742. doi: 10.1039/c9ra04830h. eCollection 2019 Aug 29.

Abstract

In times of depleting fossil fuel reserves, optimizing industrial catalytic reactions has become increasingly important. One possibility for optimization is the use of homogenous catalysts, which are advantageous over heterogeneous catalysts because of mild reaction conditions as well as higher selectivity and activity. A new emerging technology, supported ionic liquid phase (SILP), was developed to permanently immobilize homogeneous catalyst complexes for continuous processes. However, these SILP catalysts are unable to form freestanding supports by themselves. This study presents a new method to introduce the SILP system into a support made from multi-walled carbon nanotubes (MWCNT). In a first step, SILP catalysts were prepared for hydroformylation as well as low-temperature water-gas shift (WGS) reactions. These catalysts were integrated into freestanding microtubes formed from MWCNTs, with silica (for hydroformylation) or alumina particles (for WGS) incorporated. In hydroformylation, the activity increased significantly by around 400% when the pure MWCNT material was used as SILP support. An opposite trend was observed for WGS, where pure alumina particles exhibited the highest activity. A significant advantage of the MWCNT composite materials is the possibility to coat them with separation layers, which allows their application in membrane reactors for more efficient processes.

摘要

在化石燃料储备日益枯竭的时代,优化工业催化反应变得越发重要。优化的一种可能性是使用均相催化剂,由于反应条件温和以及更高的选择性和活性,均相催化剂比非均相催化剂更具优势。一种新兴技术——负载离子液体相(SILP)被开发出来,用于将均相催化剂络合物永久固定以实现连续过程。然而,这些SILP催化剂自身无法形成独立的载体。本研究提出了一种将SILP体系引入由多壁碳纳米管(MWCNT)制成的载体中的新方法。第一步,制备用于氢甲酰化以及低温水煤气变换(WGS)反应的SILP催化剂。这些催化剂被整合到由MWCNT形成的独立微管中,并掺入了二氧化硅(用于氢甲酰化)或氧化铝颗粒(用于WGS)。在氢甲酰化反应中,当使用纯MWCNT材料作为SILP载体时活性显著提高约400%。对于WGS反应则观察到相反趋势,纯氧化铝颗粒表现出最高活性。MWCNT复合材料的一个显著优点是可以用分离层对其进行包覆,这使得它们能够应用于膜反应器以实现更高效的过程。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a37b/9070777/41b9b48ab615/c9ra04830h-f1.jpg

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