Mild and Selective Hydrogenation of Nitrate to Ammonia in the Absence of Noble Metals
ACS Catalysis(2020)
摘要
Motivated by increased awareness about nitrate contamination of surface waters and its deleterious effects in human and animal health, we sought an alternative, non-noble metal catalyst for the chemical degradation of nitrate. First-row transition metal phosphides recently emerged as excellent alternatives for hydrogen evolution and hydrotreating reactions. We demonstrate that a key member of this family, Ni2P readily hydrogenates nitrate (NO3-) to ammonia (NH3) near ambient conditions with very high selectivity (96%). One of the few non-precious metal-based catalysts for this transformation, and among ca. 1% of catalysts with NH3 selectivity, Ni2P can be recycled multiple times with limited loss of activity. Both nitrite (NO2-) and nitric oxide (NO) interme-diates are also hydrogenated. Density functional theory (DFT) indicates that—in the absence of a catalyst—nitrite hydrogenation is the reaction bottleneck. A variety of adsorbates (H, O, N, NO) induce surface reconstruction with top-layer Ni-rich surf...
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关键词
nitrate removal,nitrate reduction,catalytic hydrogenation,Ni2P catalysts,non-precious metal,noble metal-free,high selectivity,ammonia
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