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Amine-functionalized MIL-53(Al) with embedded ruthenium nanoparticles as a highly efficient catalyst for the hydrolytic dehydrogenation of ammonia borane

机译:具有嵌入式钌纳米粒子的胺官能化MIL-53(Al)作为氨硼烷的水解脱氢的高效催化剂

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Well-dispersed ruthenium nanoparticles (Ru NPs) are immobilized within the pores of amine-functionalized MIL-53 via an in situ impregnation-reduction method. The resulting Ru/MIL-53(Al)-NH _(2) catalyst exhibits superior catalytic performance for the dehydrogenation of ammonia borane (AB) at ambient temperature relative to the Ru/MIL-53(Al) catalyst; it has a turnover frequency (TOF) of 287 mol H _(2) min ~(?1) (mol Ru) ~(?1) and an activation energy ( E _(a) ) of 30.5 kJ mol ~(?1) . The amine groups present in the MIL-53(Al)-NH _(2) framework facilitate the formation and stabilization of ultra-small Ru NPs by preventing their aggregation. Additionally, the Ru/MIL-53(Al)-NH _(2) catalyst exhibits satisfactory durability and reusability: 72.4% and 86.3% of the initial catalytic activity was maintained after the fifth successive cycle of the hydrolytic dehydrogenation of AB in the two respective tests.
机译:分散良好的钌纳米颗粒(Ru NPs)通过原位浸渍还原方法固定在胺官能化MIL-53的孔中。相对于Ru / MIL-53(Al)催化剂,所得的Ru / MIL-53(Al)-NH 2(2)催化剂在环境温度下对氨硼烷(AB)脱氢显示出优异的催化性能;它的周转频率(TOF)为287 mol H _(2)min〜(?1)(mol Ru)〜(?1)和活化能(E _(a))为30.5 kJ mol〜(?1 )。 MIL-53(Al)-NH_(2)骨架中存在的胺基团通过防止超小Ru NP聚集而促进其形成和稳定。此外,Ru / MIL-53(Al)-NH_(2)催化剂表现出令人满意的耐久性和可重复使用性:在两次AB水解连续第五次循环后,保持了72.4%和86.3%的初始催化活性。各自的测试。

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