Issue 5, 2013

Depleted uranium catalysts for chlorine production

Abstract

This study demonstrates depleted uranium as a remarkable heterogeneous catalyst for the oxidation of HCl to Cl2. This reaction comprises a sustainable approach to valorise byproduct HCl streams in the chemical industry. Bulk α-U3O8 showed an outstanding stability against chlorination, which is crucial for its durability in catalytic tests. UO2 and γ-UO3 transformed into α-U3O8 under reaction conditions. Uranium deposition on different carriers by dry impregnation concluded the superiority of zirconia as support. HAADF-STEM investigations revealed that the uranium oxide on the surface of this carrier is present in the form of a film-like nanostructure with a thickness ranging from a monolayer to 1 nm as well as atomic dispersion. The effect of variables (temperature, feed O2/HCl ratio, metal loading, and Cl2 co-feeding) on the performance of U3O8/ZrO2 has been studied. The HCl conversion over this catalyst increased with reaction time as a likely consequence of in situ re-dispersion of the original uranium phase into atomically dispersed UOx. As demonstrated by H2-TPR, the uranium in the generated UOx phase is more oxidised than in the original U3O8. Such a highly dispersed active phase is produced faster in the uncalcined sample. The extraordinary stable Cl2 production over U3O8/ZrO2 at 773 K for 100 h on stream indicates its potential for application in high-temperature HCl oxidation. Under these conditions, other known catalytic materials suffer from significant deactivation.

Graphical abstract: Depleted uranium catalysts for chlorine production

Supplementary files

Article information

Article type
Edge Article
Submitted
24 Nov 2012
Accepted
01 Feb 2013
First published
04 Feb 2013
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2013,4, 2209-2217

Depleted uranium catalysts for chlorine production

A. P. Amrute, F. Krumeich, C. Mondelli and J. Pérez-Ramírez, Chem. Sci., 2013, 4, 2209 DOI: 10.1039/C3SC22067B

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements