Facet-dependent solar ammonia synthesis of BiOCl nanosheets via a proton-assisted electron transfer pathway
| Autor: | Hao Li, Jingu Shi, Kun Zhao, Lizhi Zhang, Jian Shang |
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| Rok vydání: | 2016 |
| Předmět: |
Proton
Chemistry chemistry.chemical_element 02 engineering and technology 010402 general chemistry 021001 nanoscience & nanotechnology Triple bond Photochemistry 01 natural sciences Oxygen 0104 chemical sciences Catalysis Ammonia production Electron transfer Adsorption General Materials Science Facet 0210 nano-technology |
| Zdroj: | Nanoscale. 8:1986-1993 |
| ISSN: | 2040-3372 2040-3364 |
| DOI: | 10.1039/c5nr07380d |
| Popis: | Under the pressure of a fossil fuels shortage and global climate change, solar ammonia synthesis and the need to develop N2 fixation under mild conditions is becoming more urgent need; however, their intrinsic mechanisms still remain unclear. Herein, we demonstrate that the kinetic inertia of N2 can be overcome using oxygen vacancies (OVs) of BiOCl as the catalytic centers to create lower energy molecular steps, which are amendable for the solar light driven N-N triple bond cleavage via a proton-assisted electron transfer pathway. Moreover, the distinct structures of OVs on different BiOCl facets strongly determine the N2 fixation pathways by influencing both the adsorption structure and the activation level of N2. The fixation of terminal end-on bound N2 on the OVs of BiOCl {001} facets follows an asymmetric distal mode by selectively generating NH3, while the reduction of side-on bridging N2 on the OVs of BiOCl {010} facets is more energetically favorable in a symmetric alternating mode to produce N2H4 as the main intermediate. |
| Databáze: | OpenAIRE |
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