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使用纳米颗粒改性聚砜中空纤维作为气液接触器进行甲酸的湿式空气氧化。

Wet air oxidation of formic acid using nanoparticle-modified polysulfone hollow fibers as gas-liquid contactors.

机构信息

Department of Chemistry, Michigan State University, East Lansing, Michigan 48824, USA.

出版信息

ACS Appl Mater Interfaces. 2012 Mar;4(3):1440-8. doi: 10.1021/am201693e. Epub 2012 Feb 22.

Abstract

Catalytic wet air oxidation (CWAO) using membrane contactors is attractive for remediation of aqueous pollutants, but previous studies of even simple reactions such as formic acid oxidation required multiple passes through tubular ceramic membrane contactors to achieve high conversion. This work aims to increase single-pass CWAO conversions by using polysulfone (PS) hollow fibers as contactors to reduce diffusion distances in the fiber lumen. Alternating adsorption of polycations and citrate-stabilized platinum colloids in fiber walls provides catalytically active PS hollow fibers. Using a single PS fiber, 50% oxidation of a 50 mM formic acid feed solution results from a single pass through the fiber lumen (15 cm length) with a solution residence time of 40 s. Increasing the number of PS fibers to five while maintaining the same volumetric flow rate leads to over 90% oxidation, suggesting that further scale up in the number of fibers will facilitate high single pass conversions at increased flow rates. The high conversion compared to prior studies with ceramic fibers stems from shorter diffusion distances in the fiber lumen. However, the activity of the Pt catalyst is 20-fold lower than in previous ceramic fibers. Focusing the Pt deposition near the fiber lumen and limiting pore wetting to this region might increase the activity of the catalyst.

摘要

膜接触器催化湿式氧化(CWAO)在处理水污染物方面具有吸引力,但即使对于甲酸氧化等简单反应的先前研究也需要通过多个管状陶瓷膜接触器来实现高转化率。这项工作旨在通过使用聚砜(PS)中空纤维作为接触器来减少纤维内腔中的扩散距离,从而提高单通过 CWAO 转化率。纤维壁中交替吸附多阳离子和柠檬酸稳定的铂胶体提供了催化活性的 PS 中空纤维。使用单个 PS 纤维,在纤维内腔(15 厘米长)中通过一次通过,溶液停留时间为 40 秒,就可以使 50mM 甲酸进料溶液的氧化率达到 50%。在保持相同体积流速的情况下,将 PS 纤维的数量增加到五个,会导致超过 90%的氧化,这表明进一步增加纤维数量将在增加流速的情况下促进高单通过转化率。与使用陶瓷纤维的先前研究相比,高转化率源自纤维内腔中较短的扩散距离。然而,Pt 催化剂的活性比以前的陶瓷纤维低 20 倍。将 Pt 沉积集中在纤维内腔附近并将孔润湿限制在该区域内,可能会提高催化剂的活性。

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