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用于选择性CO加氢制轻质烯烃的静电纺丝Fe-Al-O纳米带

Electrospun Fe-Al-O Nanobelts for Selective CO Hydrogenation to Light Olefins.

作者信息

Elishav Oren, Shener Yuval, Beilin Vadim, Landau Miron V, Herskowitz Moti, Shter Gennady E, Grader Gideon S

机构信息

The Nancy and Stephen Grand Technion Energy Program, Technion-Israel Institute of Technology, Haifa 3200003, Israel.

The Wolfson Department of Chemical Engineering, Technion-Israel Institute of Technology, Haifa 3200003, Israel.

出版信息

ACS Appl Mater Interfaces. 2020 Jun 3;12(22):24855-24867. doi: 10.1021/acsami.0c05765. Epub 2020 May 20.

Abstract

Ceramic nanobelt catalysts consisting of Fe-Al-O spinel modified with potassium were synthesized for CO hydrogenation into hydrocarbons. Nanobelts and hollow nanofibers were produced utilizing the internal heat released by oxidation of the organic component within the fibers. This extremely fast and short heating facilitated crystallization of the desired phase, while maintaining small grains and a large surface area. We investigated the effects of mat thickness, composition, and heating rate on the final morphology. A general transformation mechanism for electrospun nanofibers that correlates for the first time the mat's thickness and the rate of oxidation during thermal treatment was proposed. The catalytic performance of carburized ceramic K/Fe-Al-O nanobelts was compared to the K/Fe-Al-O spinel powder. The electrospun catalyst showed a superior carbon dioxide conversion of 48% and a selectivity of 52% to light C-C olefins, while the powder catalyst produced mainly C hydrocarbons. Characterization of steady state catalytic materials by energy-dispersive X-ray spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, high-resolution transmission electron microscopy, and N-adsorption methods revealed that high olefin selectivity of the electrospun materials is related to a high extent of reduction of surface iron atoms because of more efficient interaction with the potassium promoter.

摘要

合成了由钾改性的Fe-Al-O尖晶石组成的陶瓷纳米带催化剂,用于将CO加氢转化为烃类。利用纤维内有机成分氧化释放的内部热量制备了纳米带和中空纳米纤维。这种极快且短暂的加热促进了所需相的结晶,同时保持了小晶粒和大表面积。我们研究了毡层厚度、组成和加热速率对最终形态的影响。提出了一种电纺纳米纤维的一般转变机制,首次将毡层厚度与热处理过程中的氧化速率联系起来。将渗碳陶瓷K/Fe-Al-O纳米带的催化性能与K/Fe-Al-O尖晶石粉末进行了比较。电纺催化剂表现出优异的二氧化碳转化率48%和对轻质C-C烯烃的选择性52%,而粉末催化剂主要生成C烃。通过能量色散X射线光谱、X射线衍射、X射线光电子能谱、高分辨率透射电子显微镜和N吸附方法对稳态催化材料进行表征,结果表明,电纺材料的高烯烃选择性与表面铁原子的高度还原有关,这是由于与钾促进剂的相互作用更有效。

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