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Au@Nb@HxK1-xNbO3 nanopeapods with near-infrared active plasmonic hot-electron injection for water splitting

机译:Au @ Nb @ HxK1-xNbO3纳米豆荚与近红外活性等离子体热电子注入水分解

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摘要

Full-spectrum utilization of diffusive solar energy by a photocatalyst for environmental remediation and fuel generation has long been pursued. In contrast to tremendous efforts in the UV-to-VIS light regime of the solar spectrum, the NIR and IR areas have been barely addressed although they represent about 50% of the solar flux. Here we put forward a biomimetic photocatalyst blueprint that emulates the growth pattern of a natural plant—a peapod—to address this issue. This design is exemplified via unidirectionally seeding core-shell Au@Nb nanoparticles in the cavity of semiconducting HxK1−xNbO3 nanoscrolls. The biomimicry of this nanopeapod (NPP) configuration promotes near-field plasmon–plasmon coupling between bimetallic Au@Nb nanoantennas (the peas), endowing the UV-active HxK1−xNbO3 semiconductor (the pods) with strong VIS and NIR light harvesting abilities. Moreover, the characteristic 3D metal-semiconductor junction of the Au@Nb@HxK1−xNbO3 NPPs favors the transfer of plasmonic hot carriers to trigger dye photodegradation and water photoelectrolysis as proofs-of-concept. Such broadband solar spectral response renders the Au@Nb@HxK1−xNbO3 NPPs highly promising for widespread photoactive devices.
机译:长期以来,人们一直在追求光催化剂对光谱扩散光的利用,以进行环境修复和产生燃料。与在太阳光谱的紫外-可见光领域所做的巨大努力相比,尽管近红外和红外区域约占太阳通量的50%,但几乎没有得到解决。在这里,我们提出了仿生光催化剂的蓝图,该蓝图模仿了天然植物(豌豆)的生长模式,以解决此问题。通过在半导体HxK1-xNbO3纳米卷的腔体中单向接种核-壳Au @ Nb纳米粒子来举例说明此设计。这种纳米豆脚(NPP)的仿生结构促进了双金属Au @ Nb纳米天线(豌豆)之间的近场等离激元-等离激元耦合,使具有紫外线活性的HxK1-xNbO3半导体(豆荚)具有强大的VIS和NIR光收集能力。此外,作为概念证明,Au @ Nb @ HxK1-xNbO3 NPP的特征性3D金属-半导体结有利于等离子体热载流子的转移,以触发染料光降解和水光电解。这样的宽带太阳光谱响应使得Au @ Nb @ HxK1-xNbO3 NPP对于广泛的光敏器件非常有前途。

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