Efficient hot carrier injection in plasmonic semiconductor heterojunction for artificial photosynthesis of ammonia
We developed a plasmonic semiconductor p–n junction by in situ growing p-type Cu 3 BiS 3 in n-type Bi 2 S 3 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 p...
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| Published in | Nanotechnology Vol. 36; no. 18; pp. 185706 - 185717 |
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| Main Authors | , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
England
IOP Publishing
05.05.2025
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| Subjects | |
| Online Access | Get full text |
| ISSN | 0957-4484 1361-6528 1361-6528 |
| DOI | 10.1088/1361-6528/adc740 |
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| Abstract | We developed a plasmonic semiconductor p–n junction by in situ growing p-type Cu 3 BiS 3 in n-type Bi 2 S 3 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. In situ 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 3 BiS 3 to non-plasmonic Bi 2 S 3 , 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. |
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| AbstractList | We developed a plasmonic semiconductor p-n junction by
growing p-type Cu
BiS
in n-type Bi
S
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.
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
BiS
to non-plasmonic Bi
S
, 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. We developed a plasmonic semiconductor p–n junction by in situ growing p-type Cu 3 BiS 3 in n-type Bi 2 S 3 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. In situ 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 3 BiS 3 to non-plasmonic Bi 2 S 3 , 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. Plasmonic semiconductors are arising as potential photocatalysts for the artificial synthesis of green ammonia. However, plasmon excitation-generated hot carriers on a single nanoparticle are easily recombined, leading to low photoconversion efficiency, and energetic defects make plasmonic semiconductors subject to unexpected changes, limiting post-engineering. Here, we developed a plasmonic semiconductor p-n junction by in situ growing p-type Cu3BiS3 in n-type Bi2S3 nanorods by an ion exchange method. The formation of plasmonic semiconductor heterojunctions was verified through high-resolution transmission electron microscopy, Mott-Schottky tests, valence band spectroscopy, and X-ray diffraction (XRD). Additionally, the rapid transfer of hot carriers between the heterojunctions was investigated using transient absorption spectroscopy. The plasmonic p-n junction shows strong localized surface plasmon resonance absorption in the near-infrared range and delivers a 61 times 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 situ Fourier-transform infrared (FTIR) reveal that the plasmonic semiconductor heterojunction promotes the nitrogen chemisorption and activation. Using ultrafast transient absorption spectroscopy, we found that localized surface plasmon resonance (LSPR) induced hot carriers can be efficiently injected from plasmonic Cu3BiS3 to non-plasmonic Bi2S3, with sufficient energy to drive water oxidation. We further confirmed that photothermal effects have little 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.
.Plasmonic semiconductors are arising as potential photocatalysts for the artificial synthesis of green ammonia. However, plasmon excitation-generated hot carriers on a single nanoparticle are easily recombined, leading to low photoconversion efficiency, and energetic defects make plasmonic semiconductors subject to unexpected changes, limiting post-engineering. Here, we developed a plasmonic semiconductor p-n junction by in situ growing p-type Cu3BiS3 in n-type Bi2S3 nanorods by an ion exchange method. The formation of plasmonic semiconductor heterojunctions was verified through high-resolution transmission electron microscopy, Mott-Schottky tests, valence band spectroscopy, and X-ray diffraction (XRD). Additionally, the rapid transfer of hot carriers between the heterojunctions was investigated using transient absorption spectroscopy. The plasmonic p-n junction shows strong localized surface plasmon resonance absorption in the near-infrared range and delivers a 61 times 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 situ Fourier-transform infrared (FTIR) reveal that the plasmonic semiconductor heterojunction promotes the nitrogen chemisorption and activation. Using ultrafast transient absorption spectroscopy, we found that localized surface plasmon resonance (LSPR) induced hot carriers can be efficiently injected from plasmonic Cu3BiS3 to non-plasmonic Bi2S3, with sufficient energy to drive water oxidation. We further confirmed that photothermal effects have little 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.
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| Author | Li, Qiang Liu, Xinfeng Bai, Xiaoxia Wu, Keming Zhao, Zhenhuan Yue, Shuai |
| Author_xml | – sequence: 1 givenname: Keming surname: Wu fullname: Wu, Keming organization: National Center for Nanoscience and Technology CAS Key Laboratory of Standardization and Measurement for Nanotechnology, Beijing 100190, People’s Republic of China – sequence: 2 givenname: Qiang surname: Li fullname: Li, Qiang organization: Xidian Univerity School of Advanced Materials and Nanotechnology, Xi’an 710126, People’s Republic of China – sequence: 3 givenname: Shuai surname: Yue fullname: Yue, Shuai organization: National Center for Nanoscience and Technology CAS Key Laboratory of Standardization and Measurement for Nanotechnology, Beijing 100190, People’s Republic of China – sequence: 4 givenname: Xiaoxia orcidid: 0000-0003-1756-4868 surname: Bai fullname: Bai, Xiaoxia organization: Xidian Univerity School of Advanced Materials and Nanotechnology, Xi’an 710126, People’s Republic of China – sequence: 5 givenname: Xinfeng orcidid: 0000-0002-7662-7171 surname: Liu fullname: Liu, Xinfeng organization: National Center for Nanoscience and Technology CAS Key Laboratory of Standardization and Measurement for Nanotechnology, Beijing 100190, People’s Republic of China – sequence: 6 givenname: Zhenhuan orcidid: 0000-0001-5015-0064 surname: Zhao fullname: Zhao, Zhenhuan organization: Tufts University Department of Chemistry, Medford, MA 01255, United States of America |
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| Keywords | ammonia p–n junction plasmon photosynthesis semiconductor |
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| Snippet | We developed a plasmonic semiconductor p–n junction by in situ growing p-type Cu 3 BiS 3 in n-type Bi 2 S 3 nanorods by an ion exchange method. The formation... We developed a plasmonic semiconductor p-n junction by growing p-type Cu BiS in n-type Bi S nanorods by an ion exchange method. The formation of plasmonic... Plasmonic semiconductors are arising as potential photocatalysts for the artificial synthesis of green ammonia. However, plasmon excitation-generated hot... |
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| SubjectTerms | ammonia photosynthesis plasmon p–n junction semiconductor |
| Title | Efficient hot carrier injection in plasmonic semiconductor heterojunction for artificial photosynthesis of ammonia |
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