Broadband Plasmonic NbN Photocatalysts for Enhanced Hydrogen Generation from Ammonia Borane under Visible–Near-Infrared Illumination
Broadband Plasmonic NbN Photocatalysts for Enhanced Hydrogen Generation from Ammonia Borane under Visible–Near-Infrared Illumination
复制标题
宽带等离激元 NbN 光催化剂在可见光和近红外照明下增强硼烷氨的产氢能力
DOI：
10.1021/acs.jpclett.2c00876
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发表时间：
2022
影响因子：
5.7
通讯作者：
Wenlong Wang
中科院分区：
文献类型：
--
作者：
Xiaowei Zhang;Lisha Lu;Jianfang Wang;Lejuan Cai;Hao Ling;Xuedong Bai;Wenlong Wang
等离子体金属纳米结构的上级光捕获能力使其特别适合于与可再生燃料相关的光驱动化学转化中的应用。在这里，我们展示了使用氮化铌（NbN）纳米结构作为一种非贵重的等离子体光催化剂，用于氨硼烷（AB）的水解分解产生高效的H2。合成了具有分级花状纳米结构的多孔纳米结构NbN，以在可见光和近红外（NIR）区域实现强宽带等离子体吸收。当负载有最佳量（约2wt%）的纳米颗粒Ni作为催化中心时，等离子体NbN吸收剂在可见光和NIR照射下均显示出显著增强的AB分解放氢活性，反应速率分别为暗反应的4.6倍（>420 nm）和2.7倍（>780 nm）。进一步的动力学测量和机理研究表明，光催化活性源于等离子体激元热载流子的贡献。
The superior light-harvesting ability of plasmonic metallic nanostructures makes them uniquely suitable for applications in the light-driven chemical transformations relevant to renewable fuels. Here we demonstrate the use of niobium nitride (NbN) nanostructures as a nonprecious plasmonic photocatalyst for the highly efficient H2 generation from the hydrolytic decomposition of ammonia borane (AB). Porous nanostructured NbN with a hierarchical flower-like nanoarchitecture was synthesized to achieve strong broadband plasmonic absorption in the visible and near-infrared (NIR) regions. The plasmonic NbN absorbers, when loaded with an optimized amount (∼2 wt %) of nanoparticulate Ni as the catalytic centers, show notably enhanced activity toward AB decomposition for H2 evolution under both visible and NIR illumination, with the reaction rates being 4.6 (>420 nm) and 2.7 (>780 nm) times higher than that of the dark reaction. Further kinetic measurements and mechanistic investigations reveal that the photocatalytic activity originates from the plasmonic hot-carrier contributions.