{"title":"Efficient hot carrier injection in plasmonic semiconductor heterojunction for artificial photosynthesis of ammonia.","authors":"Keming Wu, Qiang Li, Shuai Yue, Xiaoxia Bai, Xinfeng Liu, Zhenhuan Zhao","doi":"10.1088/1361-6528/adc740","DOIUrl":null,"url":null,"abstract":"<p><p>We developed a plasmonic semiconductor p-n junction by<i>in situ</i>growing p-type Cu<sub>3</sub>BiS<sub>3</sub>in n-type Bi<sub>2</sub>S<sub>3</sub>nanorods 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.<i>In situ</i>Fourier-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 Cu<sub>3</sub>BiS<sub>3</sub>to non-plasmonic Bi<sub>2</sub>S<sub>3</sub>, 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.</p>","PeriodicalId":19035,"journal":{"name":"Nanotechnology","volume":" ","pages":""},"PeriodicalIF":2.9000,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nanotechnology","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1088/1361-6528/adc740","RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
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.
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.