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CLC number: O643.3

On-line Access: 2021-02-05

Received: 2020-03-16

Revision Accepted: 2020-09-04

Crosschecked: 2021-01-12

Cited: 0

Clicked: 1813

Citations:  Bibtex RefMan EndNote GB/T7714

 ORCID:

Yao Yang

https://orcid.org/0000-0003-3611-2859

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Journal of Zhejiang University SCIENCE A 2021 Vol.22 No.2 P.94-105

http://doi.org/10.1631/jzus.A2000100


Catalytic effects of V2O5 on oxidative pyrolysis of spent cation exchange resin


Author(s):  Qi Song, Jian-hua Shen, Yong Yang, Yao Yang, Bin-bo Jiang, Zu-wei Liao

Affiliation(s):  Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, Zhejiang University, Hangzhou 310027, China; more

Corresponding email(s):   yao_yang@zju.edu.cn

Key Words:  Waste disposal, Cation exchange resin, V2O5, Catalysis, Oxidative pyrolysis


Qi Song, Jian-hua Shen, Yong Yang, Yao Yang, Bin-bo Jiang, Zu-wei Liao. Catalytic effects of V2O5 on oxidative pyrolysis of spent cation exchange resin[J]. Journal of Zhejiang University Science A, 2021, 22(2): 94-105.

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author="Qi Song, Jian-hua Shen, Yong Yang, Yao Yang, Bin-bo Jiang, Zu-wei Liao",
journal="Journal of Zhejiang University Science A",
volume="22",
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pages="94-105",
year="2021",
publisher="Zhejiang University Press & Springer",
doi="10.1631/jzus.A2000100"
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%0 Journal Article
%T Catalytic effects of V2O5 on oxidative pyrolysis of spent cation exchange resin
%A Qi Song
%A Jian-hua Shen
%A Yong Yang
%A Yao Yang
%A Bin-bo Jiang
%A Zu-wei Liao
%J Journal of Zhejiang University SCIENCE A
%V 22
%N 2
%P 94-105
%@ 1673-565X
%D 2021
%I Zhejiang University Press & Springer
%DOI 10.1631/jzus.A2000100

TY - JOUR
T1 - Catalytic effects of V2O5 on oxidative pyrolysis of spent cation exchange resin
A1 - Qi Song
A1 - Jian-hua Shen
A1 - Yong Yang
A1 - Yao Yang
A1 - Bin-bo Jiang
A1 - Zu-wei Liao
J0 - Journal of Zhejiang University Science A
VL - 22
IS - 2
SP - 94
EP - 105
%@ 1673-565X
Y1 - 2021
PB - Zhejiang University Press & Springer
ER -
DOI - 10.1631/jzus.A2000100


Abstract: 
Pyrolysis is a cost-effective and safe method for the disposal of radioactive spent resins. In this work, the catalytic effects of v2O5 on the pyrolysis of cation exchange resin are investigated for the first time. The results show that it is a better catalyst than others so far studied and achieves a lowering of final pyrolysis temperature and residual rate simultaneously when aided by physical blending. The maximum reductions of the final pyrolysis temperature and the residual rate are 173 °C and 11.9% (in weight), respectively. Under the action of v2O5, low-temperature (445 °C) removal of partial sulfonic acid groups occurs and the pyrolysis of the resin copolymer matrix is promoted. This is demonstrated by the analysis of pyrolysis residues at different temperatures by X-ray photoelectron spectroscopy (XPS) and element analysis. The catalytic activity of v2O5 is determined by effects both at acid sites and oxidation-reduction centers via H2-TPR (temperature programmed reduction), O2-TPD (temperature programmed desorption), CO2-TPD, and NH3-TPD. The catalytic effect of oxidation-reduction centers in v2O5 is achieved by close contact with the sulfur bond through chemisorption under the effect of acid sites. v2O5 is also believed to be the reason for the removal of partial sulfonic acid groups at lower temperatures (445 °C). v2O5 is an effective catalyst for spent resin pyrolysis and can be further applied in industry.

V2O5对废阳离子交换树脂氧化裂解的催化作用

目的:核工业会产生大量的放射性废树脂,由于无法再生,需要对其进行安全减容处理.氧化裂解是一种经济、有效且安全的处理方法,但目前所使用的催化剂仅能降低裂解的温度,难以同时减少残渣量以达到进一步减容的目的.本文旨在探讨V2O5对废树脂氧化裂解的催化作用,期望在降低裂解温度的同时能减少裂解残渣量,并探究其催化机理.
创新点:1. 通过添加V2O5为催化剂,在降低废树脂裂解温度的同时,首次降低了裂解残渣量;2. V2O5的催化效果通过其酸性中心和氧化还原中心协同作用实现;3. V2O5有助于磺酸基团的低温脱除.
方法:1. 通过热重分析,发现V2O5对废树脂氧化裂解反应具有较好的催化作用(图1);2. 通过X射线光电子能谱分析和元素分析,考察V2O5在反应过程中的作用效果及其与其他催化剂的区别(图3和4);3. 通过对不同的催化剂进行H2-TPR、O2-TPD、CO2-TPD和NH3-TPD表征,探究V2O5的催化机理(图5~8).
结论:1. V2O5对废树脂的氧化裂解具有一定的促进作用,能同时降低裂解温度和裂解残渣量;2. V2O5能促进硫键的分解与转化,并能在低温下促进磺酸基团的脱除;3. V2O5的催化效果是通过其酸性中心和氧化还原中心协同作用实现的;在酸性中心吸附硫键的作用下,氧化还原中心破坏硫键结构.

关键词:废物处理;阳离子交换树脂;V2O5;催化;氧化裂解

Darkslateblue:Affiliate; Royal Blue:Author; Turquoise:Article

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