Single-nanoparticle-thick three-phase plasmonic catalysis for efficient nitrogen photofixation without sacrificial agents
Plasmonic catalysis promises efficient green ammonia production from nitrogen gas, water, and (sun)light. However, existing designs are limited by poor catalytic performance and reliance on organic sacrificial agents. Here, we achieve efficient ammonia photosynthesis at ambient conditions without sa...
| Main Authors: | , , , , , , |
|---|---|
| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2024
|
| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/180220 |
| _version_ | 1811682153752166400 |
|---|---|
| author | Boong, Siew Kheng Chong, Carice Zhang, Jiajia Raja Mogan, Tharishinny Ni, Yimeng Li, Haitao Lee, Hiang Kwee |
| author2 | School of Chemistry, Chemical Engineering and Biotechnology |
| author_facet | School of Chemistry, Chemical Engineering and Biotechnology Boong, Siew Kheng Chong, Carice Zhang, Jiajia Raja Mogan, Tharishinny Ni, Yimeng Li, Haitao Lee, Hiang Kwee |
| author_sort | Boong, Siew Kheng |
| collection | NTU |
| description | Plasmonic catalysis promises efficient green ammonia production from nitrogen gas, water, and (sun)light. However, existing designs are limited by poor catalytic performance and reliance on organic sacrificial agents. Here, we achieve efficient ammonia photosynthesis at ambient conditions without sacrificial agent by introducing a single-particle-thick plasmonic superlattice at a three-phase catalytic interface. By organizing Ag-square superlattice on a hydrogel to create an electromagnetically hot solid-liquid-gas tri-interface, our three-phase plasmonic catalyst achieves a superior ammonia formation rate of 101 µmol h−1 g−1, surpassing conventional two-phase configuration by ∼33-fold. More importantly, our unique design attains up to ∼26-fold and ∼2500-fold enhancements in ammonia formation rate and apparent quantum yield, respectively. Mechanistic investigations uncover the importance of three-phase plasmonic interface to efficiently concentrate light and enrich immiscible gas-liquid reactants at point-of-catalysis, thereby boosting nitrogen photofixation. Our work offers valuable insights for designing multifunctional plasmonic ensembles towards sustainable chemical manufacturing and a carbon-free hydrogen economy. |
| first_indexed | 2024-10-01T03:52:19Z |
| format | Journal Article |
| id | ntu-10356/180220 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T03:52:19Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1802202024-09-27T15:31:38Z Single-nanoparticle-thick three-phase plasmonic catalysis for efficient nitrogen photofixation without sacrificial agents Boong, Siew Kheng Chong, Carice Zhang, Jiajia Raja Mogan, Tharishinny Ni, Yimeng Li, Haitao Lee, Hiang Kwee School of Chemistry, Chemical Engineering and Biotechnology Institute of Materials Research and Engineering, A*STAR Chemistry Three-phase interface Plasmon catalysis Plasmonic catalysis promises efficient green ammonia production from nitrogen gas, water, and (sun)light. However, existing designs are limited by poor catalytic performance and reliance on organic sacrificial agents. Here, we achieve efficient ammonia photosynthesis at ambient conditions without sacrificial agent by introducing a single-particle-thick plasmonic superlattice at a three-phase catalytic interface. By organizing Ag-square superlattice on a hydrogel to create an electromagnetically hot solid-liquid-gas tri-interface, our three-phase plasmonic catalyst achieves a superior ammonia formation rate of 101 µmol h−1 g−1, surpassing conventional two-phase configuration by ∼33-fold. More importantly, our unique design attains up to ∼26-fold and ∼2500-fold enhancements in ammonia formation rate and apparent quantum yield, respectively. Mechanistic investigations uncover the importance of three-phase plasmonic interface to efficiently concentrate light and enrich immiscible gas-liquid reactants at point-of-catalysis, thereby boosting nitrogen photofixation. Our work offers valuable insights for designing multifunctional plasmonic ensembles towards sustainable chemical manufacturing and a carbon-free hydrogen economy. Agency for Science, Technology and Research (A*STAR) Ministry of Education (MOE) Nanyang Technological University Submitted/Accepted version H.K.L. thanks the funding supports from the Singapore Ministry of Education (AcRF Tier 1 RS13/20 and RG4/21), A*STAR Singapore (MTC IRG M23M6c0098, AME YIRG A2084c0158), the National University of Singapore Center of Hydrogen Innovation (CHI-P2022-05), and the Nanyang Technological University start-up grants. 2024-09-25T01:25:27Z 2024-09-25T01:25:27Z 2024 Journal Article Boong, S. K., Chong, C., Zhang, J., Raja Mogan, T., Ni, Y., Li, H. & Lee, H. K. (2024). Single-nanoparticle-thick three-phase plasmonic catalysis for efficient nitrogen photofixation without sacrificial agents. Nano Energy, 128(Part B), 109922-. https://dx.doi.org/10.1016/j.nanoen.2024.109922 2211-2855 https://hdl.handle.net/10356/180220 10.1016/j.nanoen.2024.109922 2-s2.0-85197311692 Part B 128 109922 en RS13/20 RG4/21 MTC IRG M23M6c0098 AME YIRG A2084c0158 CHI-P2022-05 NTU-SUG Nano Energy © 2024 Elsevier Ltd. All rights reserved. This article may be downloaded for personal use only. Any other use requires prior permission of the copyright holder. The Version of Record is available online at http://doi.org/10.1016/j.nanoen.2024.109922. application/pdf |
| spellingShingle | Chemistry Three-phase interface Plasmon catalysis Boong, Siew Kheng Chong, Carice Zhang, Jiajia Raja Mogan, Tharishinny Ni, Yimeng Li, Haitao Lee, Hiang Kwee Single-nanoparticle-thick three-phase plasmonic catalysis for efficient nitrogen photofixation without sacrificial agents |
| title | Single-nanoparticle-thick three-phase plasmonic catalysis for efficient nitrogen photofixation without sacrificial agents |
| title_full | Single-nanoparticle-thick three-phase plasmonic catalysis for efficient nitrogen photofixation without sacrificial agents |
| title_fullStr | Single-nanoparticle-thick three-phase plasmonic catalysis for efficient nitrogen photofixation without sacrificial agents |
| title_full_unstemmed | Single-nanoparticle-thick three-phase plasmonic catalysis for efficient nitrogen photofixation without sacrificial agents |
| title_short | Single-nanoparticle-thick three-phase plasmonic catalysis for efficient nitrogen photofixation without sacrificial agents |
| title_sort | single nanoparticle thick three phase plasmonic catalysis for efficient nitrogen photofixation without sacrificial agents |
| topic | Chemistry Three-phase interface Plasmon catalysis |
| url | https://hdl.handle.net/10356/180220 |
| work_keys_str_mv | AT boongsiewkheng singlenanoparticlethickthreephaseplasmoniccatalysisforefficientnitrogenphotofixationwithoutsacrificialagents AT chongcarice singlenanoparticlethickthreephaseplasmoniccatalysisforefficientnitrogenphotofixationwithoutsacrificialagents AT zhangjiajia singlenanoparticlethickthreephaseplasmoniccatalysisforefficientnitrogenphotofixationwithoutsacrificialagents AT rajamogantharishinny singlenanoparticlethickthreephaseplasmoniccatalysisforefficientnitrogenphotofixationwithoutsacrificialagents AT niyimeng singlenanoparticlethickthreephaseplasmoniccatalysisforefficientnitrogenphotofixationwithoutsacrificialagents AT lihaitao singlenanoparticlethickthreephaseplasmoniccatalysisforefficientnitrogenphotofixationwithoutsacrificialagents AT leehiangkwee singlenanoparticlethickthreephaseplasmoniccatalysisforefficientnitrogenphotofixationwithoutsacrificialagents |