1.福州大学石油化工学院,福建 福州350108
2.中国石油大学(北京)化学工程与环境学院,北京 102249
阴义轩(1993—),女,硕士研究生,893584980@qq.com
袁珮(1983—),女,博士,教授,yuanpei@fzu.edu.cn
收稿:2019-02-11,
修回:2019-04-11,
网络首发:2026-07-24,
纸质出版:2019-07-05
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阴义轩, 成婷婷, 鲍晓军, 袁珮. 丁腈橡胶非均相加氢催化剂失活原因及再生性能研究[J]. 化工学报, 2019, 70(7): 2528-2539
YIN Yixuan, CHENG Tingting, BAO Xiaojun, YUAN Pei. Deactivation and regeneration of heterogeneous catalysts for hydrogenation of nitrile butadiene rubber[J]. CIESC Journal, 2019, 70(7): 2528-2539
阴义轩, 成婷婷, 鲍晓军, 袁珮. 丁腈橡胶非均相加氢催化剂失活原因及再生性能研究[J]. 化工学报, 2019, 70(7): 2528-2539 DOI: 10.11949/0438-1157.20190113.
YIN Yixuan, CHENG Tingting, BAO Xiaojun, YUAN Pei. Deactivation and regeneration of heterogeneous catalysts for hydrogenation of nitrile butadiene rubber[J]. CIESC Journal, 2019, 70(7): 2528-2539 DOI: 10.11949/0438-1157.20190113.
对丁腈橡胶非均相催化加氢制备高附加值氢化丁腈橡胶过程中催化剂失活的原因进行了探究,发现造成催化剂活性下降的原因并不是贵金属纳米颗粒的流失、团聚或中毒,而是催化剂表面的活性位被聚合物覆盖而无法与反应物接触,因此将覆盖在活性位上的聚合物进行脱除才是催化剂再生和重复利用的关键。根据相似相容原理选择单溶剂或者混合溶剂对反应后催化剂进行处理,结果表明经过乙酸乙酯、丁酮、
N
N
-二甲基甲酰胺以及
N
-甲基吡咯烷酮这四种有机溶剂处理后,其催化加氢活性可以恢复至新鲜催化剂活性的90%;当用混合溶剂处理后,其催化活性可以提高至新鲜催化剂活性的95%,且循环利用4次其催化活性仍能保持不变。
The reason for the deactivation of catalysts in the process of preparing high value-added hydrogenated nitrile rubber by heterogeneous catalytic hydrogenation of nitrile rubber was investigated. It was found that the cause of the decrease in catalyst activity was not the loss
agglomeration or poisoning of noble metal nanoparticles. The reactants could not contact with the active sites
which was the real reason for the reduced activity. Therefore
the effective removal of the polymers from the active sites was the key to catalyst regeneration and reuse. Secondly
based on the similarity-intermiscibility theory
the recycled catalyst was treated with a single or a mixed solvent to elute the polymers and recover its activity. The results showed that the catalyst activity could be restored to 90% of the fresh catalyst activity by washing with ethyl acetate
butanone
N
N
-dimethylfirmamide or
N
-methylpyrrolidone. When treated with a mixed solvent
its catalyst activity co
uld be increased to 95% of the fresh catalyst activity
and could remain steady after recycling 4 times. SEM and TG characterization results showed that after the organic solvent regeneration
Pd active sites on the surface of the catalyst were exposed
thus its hydrogenation activity was remarkably improved.
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