A Bioinspired Molybdenum Catalyst for Aqueous Perchlorate Reduction
Perchlorate (ClO4 –) is a pervasive, harmful, and inert anion on both Earth and Mars. Current technologies for ClO4 – reduction entail either harsh conditions or multicomponent enzymatic processes. Herein, we report a heterogeneous ( L )Mo–Pd/C catalyst directly prepared from Na2MoO4, a bidentate n...
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Veröffentlicht in: | Journal of the American Chemical Society 2021-06, Vol.143 (21), p.7891-7896 |
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Format: | Artikel |
Sprache: | eng |
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Zusammenfassung: | Perchlorate (ClO4 –) is a pervasive, harmful, and inert anion on both Earth and Mars. Current technologies for ClO4 – reduction entail either harsh conditions or multicomponent enzymatic processes. Herein, we report a heterogeneous ( L )Mo–Pd/C catalyst directly prepared from Na2MoO4, a bidentate nitrogen ligand ( L ), and Pd/C to reduce aqueous ClO4 – into Cl– with 1 atm of H2 at room temperature. A suite of instrument characterizations and probing reactions suggest that the MoVI precursor and L at the optimal 1:1 ratio are transformed in situ into oligomeric MoIV active sites at the carbon–water interface. For each Mo site, the initial turnover frequency (TOF0) for oxygen atom transfer from ClO x – substrates reached 165 h–1. The turnover number (TON) reached 3840 after a single batch reduction of 100 mM ClO4 –. This study provides a water-compatible, efficient, and robust catalyst to degrade and utilize ClO4 – for water purification and space exploration. |
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ISSN: | 0002-7863 1520-5126 |
DOI: | 10.1021/jacs.1c00595 |