Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 304, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2021.121001
Keywords
Room temperature; Two-dimensional assembly; Diminutive cobalt oxides; N2 photofixation; N-15 isotope
Funding
- Australian Research Council, Australia [DP190100295, LE190100014]
- Australian National University Futures Scheme, Australia [Q4601024]
- National Key Research and Development Program of China [2018YFA0305800]
- National Natural Science Foundation of China [11834014]
- Fundamental Research Funds for the Central Universities
- China Scholarship Council [CSC202104910079]
- Australian Center for Advanced Photovoltaics, Australia
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In this study, a room-temperature strategy was developed to achieve efficient nitrogen photofixation by assembling two-dimensional CoO-Co3O4 composite materials on reduced graphene oxide. The study revealed that the photoreaction-induced cation oxidation could be reversely triggered by photo-reactivating Co3O4, thereby maintaining excellent catalytic activity.
Ammonia is an indispensable chemical to the ecosystem and human beings. Storing solar energy in N-H bonds in NH3 is a promising sustainable alternative to the energy-consuming Haber Bosch process. However, nitrogen photofixation with this strategy still suffers from several unsolved issues, such as high-energy consumption with carbon footprint, short lifetime of photocatalysts, and nitrogen contamination in redox reactions. In this study, a room-temperature strategy is developed to two-dimensionally assemble the diminutive CoO-Co3O4 mixed-oxide composites on reduced graphene oxide. They proffer great surface area and deep-red-light absorbing defect states, which enable them to exhibit over 14 times higher photoactivity than template-free single components. The unveiled photoreaction-induced cation oxidation is reversely triggerable by photo-reactivating Co3O4 back to active CoO, with well-maintained photoactivity after six-cycles. All these room-temperature processes, from catalyst synthesis, nitrogen photofixation, to catalyst reactivation, offer facile way towards upscaling and hold great promise for practical zero-emission N-2 photofixation.
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