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Near‐Infrared‐Plasmonic Energy Upconversion in a Nonmetallic Heterostructure for Efficient H2 Evolution from Ammonia Borane

机译:非金属异质结构中的近红外激光能量上转换可有效地从氨硼烷中释放出氢气

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摘要

Plasmonic metal nanostructures have been widely used to enhance the upconversion efficiency of the near‐infrared (NIR) photons into the visible region via the localized surface plasmon resonance (LSPR) effect. However, the direct utilization of low‐cost nonmetallic semiconductors to both concentrate and transfer the NIR‐plasmonic energy in the upconversion system remains a significant challenge. Here, a fascinating process of NIR‐plasmonic energy upconversion in Yb3+/Er3+‐doped NaYF4 nanoparticles (NaYF4:Yb‐Er NPs)/W18O49 nanowires (NWs) heterostructures, which can selectively enhance the upconversion luminescence by two orders of magnitude, is demonstrated. Combined with theoretical calculations, it is proposed that the NIR‐excited LSPR of W18O49 NWs is the primary reason for the enhanced upconversion luminescence of NaYF4:Yb‐Er NPs. Meanwhile, this plasmon‐enhanced upconversion luminescence can be partly absorbed by the W18O49 NWs to re‐excite its higher energy LSPR, thus leading to the selective enhancement of upconversion luminescence for the NaYF4:Yb‐Er/W18O49 heterostructures. More importantly, based on this process of plasmonic energy transfer, an NIR‐driven catalyst of NaYF4:Yb‐Er NPs@W18O49 NWs quasi‐core/shell heterostructure, which exhibits a ≈35‐fold increase in the catalytic H2 evolution from ammonia borane (BH3NH3) is designed and synthesized. This work provides insight on the development of nonmetallic plasmon‐sensitized optical materials that can potentially be applied in photocatalysis, optoelectronic, and photovoltaic devices.
机译:等离子体金属纳米结构已被广泛用于通过局部表面等离子体激元共振(LSPR)效应来提高近红外(NIR)光子进入可见区域的上转换效率。然而,在上转换系统中直接利用低成本的非金属半导体来集中和转移近红外等离子体能仍然是一个巨大的挑战。在此,掺入Yb 3 + / Er 3 + 的NaYF4纳米粒子(NaYF4:Yb-Er NPs)/ W18O49纳米线(NWs)的NIR等离子体能量上转换的迷人过程展示了可以选择性地将上转换发光增强两个数量级的异质结构。结合理论计算,提出W18O49 NW的近红外激发LSPR是NaYF4:Yb-Er NP增强上转换发光的主要原因。同时,W18O49 NW可以部分吸收这种等离激元增强的上转换发光,以激发其更高能量的LSPR,从而选择性地增强NaYF4:Yb-Er / W18O49异质结构的上转换发光。更重要的是,基于该等离子能量转移过程,由NIR驱动的NaYF4:Yb-Er NPs @ W18O49 NWs准核/壳杂化结构的催化剂在氨硼烷催化的H2放出过程中表现出约35倍的增加(BH 3 NH 3 )被设计并合成。这项工作为非金属等离子体激元敏感的光学材料的发展提供了见识,这些材料可潜在地应用于光催化,光电和光伏设备。

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