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负载钌纳米粒子的胺功能化MIL-53(Al)作为氨硼烷水解脱氢的高效催化剂。

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

作者信息

Zhang Shuren, Zhou Liqun, Chen Menghuan

机构信息

Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Ministry of Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules, College of Chemistry and Chemical Engineering, Hubei University Wuhan 430062 PR China

出版信息

RSC Adv. 2018 Mar 29;8(22):12282-12291. doi: 10.1039/c8ra01507d. eCollection 2018 Mar 26.

DOI:10.1039/c8ra01507d
PMID:35539406
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9079245/
Abstract

Well-dispersed ruthenium nanoparticles (Ru NPs) are immobilized within the pores of amine-functionalized MIL-53 an impregnation-reduction method. The resulting Ru/MIL-53(Al)-NH 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 min (mol Ru) and an activation energy ( ) of 30.5 kJ mol. The amine groups present in the MIL-53(Al)-NH framework facilitate the formation and stabilization of ultra-small Ru NPs by preventing their aggregation. Additionally, the Ru/MIL-53(Al)-NH 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.

摘要

通过浸渍还原法将分散良好的钌纳米颗粒（Ru NPs）固定在胺功能化的MIL-53的孔内。相对于Ru/MIL-53(Al)催化剂，所得的Ru/MIL-53(Al)-NH催化剂在室温下对氨硼烷（AB）脱氢表现出优异的催化性能；其周转频率（TOF）为287 mol H min⁻¹（mol Ru）⁻¹，活化能（Ea）为30.5 kJ mol⁻¹。MIL-53(Al)-NH骨架中存在的胺基团通过防止超小Ru NPs聚集促进其形成和稳定。此外，Ru/MIL-53(Al)-NH催化剂表现出令人满意的耐久性和可重复使用性：在两次相应测试中，AB水解脱氢连续第五次循环后，分别保持了初始催化活性的72.4%和86.3%。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a45b/9079245/0f1d90db246e/c8ra01507d-f8.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a45b/9079245/c451d42c6bf5/c8ra01507d-f1.jpg
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