Study on Ammonia-induced Catalyst Poisoning in the Synthesis of Dimethyl Oxalate

*Hua-wei Liu  -  Gas Purification Division of Haiso Technology Co., Ltd, Hubei Industrial Gas Purification and utilization Key Laboratory, China
Sheng-tao Qian  -  Gas Purification Division of Haiso Technology Co., Ltd, Hubei Industrial Gas Purification and utilization Key Laboratory, China
Er-fei Xiao  -  Gas Purification Division of Haiso Technology Co., Ltd, Hubei Industrial Gas Purification and utilization Key Laboratory, China
Ying-jie Liu  -  Gas Purification Division of Haiso Technology Co., Ltd, Hubei Industrial Gas Purification and utilization Key Laboratory, China
Jun Lei  -  Gas Purification Division of Haiso Technology Co., Ltd, Hubei Industrial Gas Purification and utilization Key Laboratory, China
Xian-hou Wang  -  Gas Purification Division of Haiso Technology Co., Ltd, Hubei Industrial Gas Purification and utilization Key Laboratory, China
Yu-hua Kong  -  Gas Purification Division of Haiso Technology Co., Ltd, Hubei Industrial Gas Purification and utilization Key Laboratory, China
Received: 30 Nov 2020; Revised: 2 Jan 2021; Accepted: 6 Jan 2021; Published: 31 Mar 2021; Available online: 21 Jan 2021.
Open Access Copyright (c) 2021 by Authors, Published by BCREC Group
License URL: http://creativecommons.org/licenses/by-sa/4.0

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Abstract

On an industrial plant, we observed and examined the ammonia-poisoning catalyst for the synthesis of dimethyl oxalate (DMO). We investigated the catalytic activity in response to the amount of ammonia and revealed the mechanism of such poisoning by X-ray photoelectron spectroscopy (XPS) characterization. Our results show that only 0.002% ammonia in the feed gas can significantly deactivate the Pd-based catalyst. Two main reasons were proposed: one is that the competitive adsorption of ammonia on the active component Pd hinders the carbon    monoxide (CO) coupling reaction and the redox cycle between Pd0 and Pd2+; and the other is that the high-boiling nitrogen-containing amine compounds formed by reacting with ammonia have adsorbed on the catalyst, which hinders the progress of the catalytic reaction. The deactivation caused by the latter is irreversible. The catalytic activity can be completely restored by a low-temperature liquid-phase in-situ regeneration treatment. Copyright © 2021 by Authors, Published by BCREC Group. This is an open access article under the CC BY-SA License (https://creativecommons.org/licenses/by-sa/4.0).

 

Keywords: dimethyl oxalate; synthetic catalyst; ammonia poisoning; space-time yield; regeneration
Funding: Hubei Industrial Gas Purification and Utilization Key Laboratory

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