Tuning the Electron Localization of Gold Enables the Control of Nitrogen-to-Ammonia Fixation
The (photo)electrochemical N2 reduction reaction (NRR) provides a favorable avenue for the production of NH3 using renewable energy in mild operating conditions. Understanding and building an efficient catalyst with high NH3 selectivity represents an area of intense interest for the early stages of...
| Main Authors: | , , , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
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WILEY-V C H VERLAG GMBH
2019
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| Online Access: | http://purl.org/au-research/grants/arc/LE140100150 http://hdl.handle.net/20.500.11937/90892 |
| _version_ | 1848765453134987264 |
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| author | Zheng, Jianyun Lyu, Y. Qiao, M. Veder, Jean P Marco, Roland D. Bradley, J. Wang, R. Li, Y. Huang, A. Jiang, San Ping Wang, S. |
| author_facet | Zheng, Jianyun Lyu, Y. Qiao, M. Veder, Jean P Marco, Roland D. Bradley, J. Wang, R. Li, Y. Huang, A. Jiang, San Ping Wang, S. |
| author_sort | Zheng, Jianyun |
| building | Curtin Institutional Repository |
| collection | Online Access |
| description | The (photo)electrochemical N2 reduction reaction (NRR) provides a favorable avenue for the production of NH3 using renewable energy in mild operating conditions. Understanding and building an efficient catalyst with high NH3 selectivity represents an area of intense interest for the early stages of development for NRR. Herein, we introduce a CoOx layer to tune the local electronic structure of Au nanoparticles with positive valence sites for boosting conversion of N2 to NH3. The catalysts, possessing high average oxidation states (ca. 40 %), achieve a high NH3 yield rate of 15.1 μg cm−2 h−1 and a good faradic efficiency of 19 % at −0.5 V versus reversible hydrogen electrode. Experimental results and simulations reveal that the ability to tune the oxidation state of Au enables the control of N2 adsorption and the concomitant energy barrier of NRR. Altering the Au oxidation state provides a unique strategy for control of NRR in the production of valuable NH3. |
| first_indexed | 2025-11-14T11:35:29Z |
| format | Journal Article |
| id | curtin-20.500.11937-90892 |
| institution | Curtin University Malaysia |
| institution_category | Local University |
| language | English |
| last_indexed | 2025-11-14T11:35:29Z |
| publishDate | 2019 |
| publisher | WILEY-V C H VERLAG GMBH |
| recordtype | eprints |
| repository_type | Digital Repository |
| spelling | curtin-20.500.11937-908922023-05-04T05:47:32Z Tuning the Electron Localization of Gold Enables the Control of Nitrogen-to-Ammonia Fixation Zheng, Jianyun Lyu, Y. Qiao, M. Veder, Jean P Marco, Roland D. Bradley, J. Wang, R. Li, Y. Huang, A. Jiang, San Ping Wang, S. Science & Technology Physical Sciences Chemistry, Multidisciplinary Chemistry electrocatalysis gold nanoparticles nitrogen reduction reaction photoelectrochemistry REDUCTION REACTION electrocatalysis gold nanoparticles nitrogen reduction reaction photoelectrochemistry The (photo)electrochemical N2 reduction reaction (NRR) provides a favorable avenue for the production of NH3 using renewable energy in mild operating conditions. Understanding and building an efficient catalyst with high NH3 selectivity represents an area of intense interest for the early stages of development for NRR. Herein, we introduce a CoOx layer to tune the local electronic structure of Au nanoparticles with positive valence sites for boosting conversion of N2 to NH3. The catalysts, possessing high average oxidation states (ca. 40 %), achieve a high NH3 yield rate of 15.1 μg cm−2 h−1 and a good faradic efficiency of 19 % at −0.5 V versus reversible hydrogen electrode. Experimental results and simulations reveal that the ability to tune the oxidation state of Au enables the control of N2 adsorption and the concomitant energy barrier of NRR. Altering the Au oxidation state provides a unique strategy for control of NRR in the production of valuable NH3. 2019 Journal Article http://hdl.handle.net/20.500.11937/90892 10.1002/anie.201909477 English http://purl.org/au-research/grants/arc/LE140100150 http://purl.org/au-research/grants/arc/DP180100568 http://purl.org/au-research/grants/arc/DP180100731 WILEY-V C H VERLAG GMBH fulltext |
| spellingShingle | Science & Technology Physical Sciences Chemistry, Multidisciplinary Chemistry electrocatalysis gold nanoparticles nitrogen reduction reaction photoelectrochemistry REDUCTION REACTION electrocatalysis gold nanoparticles nitrogen reduction reaction photoelectrochemistry Zheng, Jianyun Lyu, Y. Qiao, M. Veder, Jean P Marco, Roland D. Bradley, J. Wang, R. Li, Y. Huang, A. Jiang, San Ping Wang, S. Tuning the Electron Localization of Gold Enables the Control of Nitrogen-to-Ammonia Fixation |
| title | Tuning the Electron Localization of Gold Enables the Control of Nitrogen-to-Ammonia Fixation |
| title_full | Tuning the Electron Localization of Gold Enables the Control of Nitrogen-to-Ammonia Fixation |
| title_fullStr | Tuning the Electron Localization of Gold Enables the Control of Nitrogen-to-Ammonia Fixation |
| title_full_unstemmed | Tuning the Electron Localization of Gold Enables the Control of Nitrogen-to-Ammonia Fixation |
| title_short | Tuning the Electron Localization of Gold Enables the Control of Nitrogen-to-Ammonia Fixation |
| title_sort | tuning the electron localization of gold enables the control of nitrogen-to-ammonia fixation |
| topic | Science & Technology Physical Sciences Chemistry, Multidisciplinary Chemistry electrocatalysis gold nanoparticles nitrogen reduction reaction photoelectrochemistry REDUCTION REACTION electrocatalysis gold nanoparticles nitrogen reduction reaction photoelectrochemistry |
| url | http://purl.org/au-research/grants/arc/LE140100150 http://purl.org/au-research/grants/arc/LE140100150 http://purl.org/au-research/grants/arc/LE140100150 http://hdl.handle.net/20.500.11937/90892 |