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负载于金属有机骨架的非贵金属纳米粒子作为可见光照射下促进氨硼烷产氢的高效、稳定催化剂。

Non-Noble-Metal Nanoparticle Supported on Metal-Organic Framework as an Efficient and Durable Catalyst for Promoting H2 Production from Ammonia Borane under Visible Light Irradiation.

机构信息

Graduate School of Engineering, Osaka University , Suita, Osaka 565-0871, Japan.

Unit of Elements Strategy Initiative for Catalysts & Batteries, Kyoto University , Kyoto 606-8501, Japan.

出版信息

ACS Appl Mater Interfaces. 2016 Aug 24;8(33):21278-84. doi: 10.1021/acsami.6b04169. Epub 2016 Aug 10.

Abstract

In this work, we propose a straightforward method to enhance the catalytic activity of AB dehydrogenation by using non-noble-metal nanoparticle supported on chromium-based metal-organic framework (MIL-101). It was demonstrated to be effective for hydrogen generation from ammonia borane under assistance of visible light irradiation as a noble-metal-free catalyst. The catalytic activity of metal nanoparticles supported on MIL-101 under visible light irradiation is remarkably higher than that without light irradiation. The TOFs of Cu/MIL-101, Co/MIL-101, and Ni/MIL-101 are 1693, 1571, and 3238 h(-1), respectively. The enhanced activity of catalysts can be primarily attributed to the cooperative promoting effects from both non-noble-metal nanoparticles and photoactive metal-organic framework in activating the ammonia borane molecule and strong ability in the photocatalytic production of hydroxyl radicals, superoxide anions, and electron-rich non-noble-metal nanoparticle. This work sheds light on the exploration of active non-noble metals supported on photoactive porous materials for achieving high catalytic activity of various redox reactions under visible light irradiation.

摘要

在这项工作中,我们提出了一种通过使用负载在基于铬的金属有机骨架(MIL-101)上的非贵金属纳米粒子来增强 AB 脱氢催化活性的简单方法。结果表明,在可见光照射下,作为无贵金属催化剂,它可有效地从氨硼烷中产生氢气。负载在 MIL-101 上的金属纳米粒子在可见光照射下的催化活性明显高于无光照时的催化活性。Cu/MIL-101、Co/MIL-101 和 Ni/MIL-101 的 TOFs 分别为 1693、1571 和 3238 h(-1)。催化剂活性的增强主要归因于非贵金属纳米粒子和光活性金属有机骨架在激活氨硼烷分子方面的协同促进作用,以及在光催化生成羟基自由基、超氧阴离子和富电子非贵金属纳米粒子方面的强能力。这项工作为探索在可见光照射下实现各种氧化还原反应的高催化活性的负载在光活性多孔材料上的活性非贵金属提供了思路。

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