Efficient hot carrier injection in plasmonic semiconductor heterojunction for artificial photosynthesis of ammonia.

IF 2.9 4区 材料科学 Q3 MATERIALS SCIENCE, MULTIDISCIPLINARY
Keming Wu, Qiang Li, Shuai Yue, Xiaoxia Bai, Xinfeng Liu, Zhenhuan Zhao
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Abstract

We developed a plasmonic semiconductor p-n junction byin situgrowing p-type Cu3BiS3in n-type Bi2S3nanorods by an ion exchange method. The formation of plasmonic semiconductor heterojunctions was verified through high-resolution transmission electron microscopy, Mott-Schottky tests, x-ray photoelectron spectroscopy-based valence band spectra, and powder x-ray diffraction. Additionally, the rapid transfer of hot carriers between the heterojunctions was investigated using ultrafast transient absorption spectroscopy (TAS). The plasmonic p-n junction shows strong localized surface plasmon resonance (LSPR) absorption in the near-infrared (IR) range and delivers a 61-fold enhancement of the ammonia production rate under full spectrum irradiation in pure water. It can achieve an apparent quantum efficiency of 0.45% at 400 nm and 0.16% at 1000 nm.In situFourier-transform IR reveals that the plasmonic semiconductor heterojunction promotes the nitrogen chemisorption and activation. Based on TAS measurements, we found that LSPR induced hot carriers can be efficiently injected from plasmonic Cu3BiS3to non-plasmonic Bi2S3, with sufficient energy to drive water oxidation reaction. We further confirmed that photothermal effects have negligible contribution to the photocatalytic performance in the water-particle suspension system. The present study shows a potential strategy utilizing plasmonic semiconductors made of earth-abundant elements for green ammonia synthesis.

等离子体半导体异质结高效热载流子注入用于氨的人工光合作用。
等离子体半导体是人工合成绿氨的潜在光催化剂。然而,在单个纳米颗粒上,等离子激元激发产生的热载流子容易重组,导致光转换效率低,并且能量缺陷使等离子体半导体容易发生意想不到的变化,限制了后期工程。本文采用离子交换法在n型Bi2S3纳米棒中原位生长p型Cu3BiS3,制备了等离子体半导体p-n结。通过高分辨率透射电子显微镜、Mott-Schottky测试、价带光谱和x射线衍射(XRD)验证了等离子体半导体异质结的形成。此外,利用瞬态吸收光谱研究了热载流子在异质结之间的快速转移。等离子体p-n结在近红外范围内表现出强烈的局部表面等离子体共振吸收,在纯水全光谱照射下,氨的产率提高了61倍。400 nm和1000 nm的表观量子效率分别为0.45%和0.16%。原位傅里叶红外(FTIR)研究表明,等离子体半导体异质结促进了氮的化学吸附和活化。利用超快瞬态吸收光谱技术,我们发现局部表面等离子体共振(LSPR)诱导的热载流子可以有效地从等离子体Cu3BiS3注入到非等离子体Bi2S3中,并具有足够的能量驱动水氧化。进一步证实了光热效应对水颗粒悬浮体系光催化性能的影响不大。目前的研究表明,利用地球上丰富的元素制成的等离子体半导体进行绿色氨合成是一种潜在的策略。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Nanotechnology
Nanotechnology 工程技术-材料科学:综合
CiteScore
7.10
自引率
5.70%
发文量
820
审稿时长
2.5 months
期刊介绍: The journal aims to publish papers at the forefront of nanoscale science and technology and especially those of an interdisciplinary nature. Here, nanotechnology is taken to include the ability to individually address, control, and modify structures, materials and devices with nanometre precision, and the synthesis of such structures into systems of micro- and macroscopic dimensions such as MEMS based devices. It encompasses the understanding of the fundamental physics, chemistry, biology and technology of nanometre-scale objects and how such objects can be used in the areas of computation, sensors, nanostructured materials and nano-biotechnology.
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