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Excellent stability of Pd/mpg-C3N4 in catalytic hydrodebenzylation of 2,4,6,8,10,12-Hexabenzyl-2,4,6,8,10,12- hexaazaisowurtzitane (HBIW)
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2021-08-08 , DOI: 10.1016/j.apcata.2021.118310
Wei Liu 1 , Shengfu Li 1 , Chongchong She 1 , Yeye Yang 2 , Shusen Chen 1 , Shaohua Jin 1 , Kun Chen 1
Affiliation  

The low stability and poisoning of the palladium-based catalysts in the debenzylation of HBIW elevated the cost of the hydrogenolysis, and thus restricted the application of 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane (HNIW). To address this problem, Pd/mpg-C3N4 was prepared by depositing palladium nanoparticles on mesoporous graphite carbon nitride (mpg-C3N4), and used for the catalytic hydrogenolysis in the conversion of HBIW to TADBIW under the atmospheric pressure. After optimizing the reaction condition and the usage amount, the highest yield of 81.7 % was obtained at 45℃ after reaction for 8 h when the ratio of palladium to HBIW was 1%. A yield of 74 % was obtained when the ratio of palladium to HBIW was 0.4 %. More importantly, Pd/mpg-C3N4 can be recycled unprecedently for three times in the conversion of HBIW to TADBIW while preserving the reasonable activity. Such results should benefit for promoting the application of HNIW and also the design of the heterogeneous catalysts for hydrodebenzylation.



中文翻译:

Pd/mpg-C3N4 在 2,4,6,8,10,12-Hexabenzyl-2,4,6,8,10,12-hexaazaisowurtzitane (HBIW) 的催化加氢脱苄中具有出色的稳定性

钯基催化剂在HBIW脱苄过程中稳定性低和中毒,提高了氢解成本,从而限制了2,4,6,8,10,12-六硝基-2,4,6,8的应用,10,12-六氮杂异武兹烷 (HNIW)。为了解决这个问题,Pd/mpg-C 3 N 4通过在介孔石墨碳氮化物(mpg-C 3 N 4),并用于在常压下将 HBIW 转化为 TADBIW 的催化氢解。优化反应条件和用量后,当钯与HBIW的比例为1%时,在45℃反应8h后产率最高,为81.7%。当钯与 HBIW 的比率为 0.4% 时,获得了 74% 的产率。更重要的是,Pd/mpg-C 3 N 4在HBIW向TADBIW的转化过程中可以前所未有地循环3次,同时保持合理的活性。这些结果应该有利于促进 HNIW 的应用以及用于加氢脱苄的多相催化剂的设计。

更新日期:2021-08-19
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