Pd(OH)2/CeO2在六苄基六氮杂异伍兹烷和四乙酰基二苄基六氮杂异伍兹烷催化氢解脱苄反应中的应用

doi:10.12382/bgxb.2021.0126

摘要/Abstract

摘要： Pd(OH)₂催化剂对六硝基六氮杂异伍兹烷（CL-20）的制备具有关键作用。选择CeO₂为催化剂载体，用沉积-沉淀法制备8种Pd(OH)₂/CeO₂催化剂，考察制备温度、浸渍时间、碱源、沉淀pH及载体结构对Pd(OH)₂/CeO₂催化氢解脱苄反应活性的影响。结果表明：Pd(OH)₂/CeO₂可同时作为六苄基六氮杂异伍兹烷（HBIW）和四乙酰基二苄基六氮杂异伍兹烷（TADBIW）氢解脱苄反应的催化剂，并表现出优异的催化活性，产物收率分别可达91%和95%；将其用于HBIW氢解脱苄反应，在金属Pd用量为底物HBIW质量的0.10%时，TADBIW的产率最高可达91%；将其用于TADBIW氢解脱苄反应，Pd用量为底物TADBIW质量的0.28%时，产率可达87%；所用研究方法使用少量Pd催化剂高效地催化HBIW和TADBIW的氢解脱苄反应，为低成本制备CL-20拓宽了道路。

关键词: Pd催化剂, 载体, 氢解脱苄, 六苄基六氮杂异伍兹烷, 四乙酰基二苄基六氮杂异伍兹烷

Abstract: Palladium hydroxide catalysts play a key role in the preparation of hexanitrohexaazais- owurtzitane (CL-20).Eight kinds of Pd(OH)₂/CeO₂ catalysts，for which two kinds of CeO₂ are used as catalyst support，were prepared by deposition-precipitation method. The effects of the preparation temperature，immersion time，the kinds of alkali，pH and the structure of support on the catalytic performance of Pd(OH)₂/CeO₂ are investigated.Pd(OH)₂/CeO₂ catalysts exhibit excellent catalytic activity in the hydrogenolytic debenzylation reaction of both hexabenzylhexaazaisowurtzitane (HPIW) and tetraacetyl-dibenzyl-hexaazaisowurtzitane(TADBIW)，and the yields of products can reach 91% and 95%，respectively.When the amount of Pd used in catalyst is 0.10% (wt/wt) of HBIW substrate，the yield of TADBIW reachs 91%.When the amount of Pd is 0.28%（wt/wt）of TADBIW substrate，the yield of the product is as high as 87%.In this research，a small amount of Pd catalyst is used to efficiently catalyze the hydrogenolytic debenzylation reaction of HBIW and TADBIW，which broadens the way for low-cost preparation of CL-20.

Key words: palladiumcatalyst, catalystsupport, hydrogenolyticdebenzylation, hexabenzylhexaa-zaisowurtzitane, tetraacetyl-dibenzyl-hexaazaisowurtzitane

中图分类号:

O643.3
TJ55

鲍伶香, 严致远, 宋建伟, 卫改霞, 孙成辉, 庞思平. Pd(OH)₂/CeO₂在六苄基六氮杂异伍兹烷和四乙酰基二苄基六氮杂异伍兹烷催化氢解脱苄反应中的应用[J]. 兵工学报, 2022, 43(3): 524-532.

BAO Lingxiang, YAN Zhiyuan, SONG Jianwei, WEI Gaixia, SUN Chenghui, PANG Siping. Pd(OH)₂/CeO₂ Catalyst for Hydrogenolytic Debenzylation Reaction of Hexabenzylhexaazaisowurtzitane and Tetraacetyl-dibenzyl-hexaazaisowurtzitane[J]. Acta Armamentarii, 2022, 43(3): 524-532.

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Pd(OH)₂/CeO₂在六苄基六氮杂异伍兹烷和四乙酰基二苄基六氮杂异伍兹烷催化氢解脱苄反应中的应用

Pd(OH)₂/CeO₂ Catalyst for Hydrogenolytic Debenzylation Reaction of Hexabenzylhexaazaisowurtzitane and Tetraacetyl-dibenzyl-hexaazaisowurtzitane

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