Effects of CeO<sub>2</sub>, TiO<sub>2</sub>, and TiO<sub>2</sub>‑CeO<sub>2</sub> Supports on Catalytic Performance\nof Ni<sub>2</sub>P in Hydrodeoxygenation of Anisole
Pawnprapa Pitakjakpipop (16016158)Chunshan Song (1293936)
Abstract
This work examined the effects of\nsupports for nickel phosphide\n(Ni<sub>2</sub>P) catalysts on anisole hydrodeoxygenation (HDO) using\nsynthesized CeO<sub>2</sub>, TiO<sub>2</sub>, and TiO<sub>2</sub>-CeO<sub>2</sub> supports and commercial supports (denoted as CeO<sub>2</sub>-L and TiO<sub>2</sub>-L) along with bulk Ni<sub>2</sub>P. Characterization\nrevealed that Ni<sub>2</sub>P nanoparticles were well dispersed on\nthe synthesized CeO<sub>2</sub>. Ni<sub>2</sub>P/CeO<sub>2</sub> exhibited\nthe highest activity on a catalyst weight basis among those Ni<sub>2</sub>P on synthesized supports as well as the common materials\nsuch as SiO<sub>2</sub>, Al<sub>2</sub>O<sub>3</sub>, and activated\ncarbon. Ni<sub>2</sub>P/TiO<sub>2</sub>-CeO<sub>2</sub> (at a Ti/Ce\nmolar ratio of 0.98) afforded superior reactivity to Ni<sub>2</sub>P/CeO<sub>2</sub> based on turnover frequency (TOF, h<sup>–1</sup>), which points to more active sites on Ni<sub>2</sub>P/TiO<sub>2</sub>-CeO<sub>2</sub> than on Ni<sub>2</sub>P/CeO<sub>2</sub>. The TOF\nof anisole on catalysts decreased in the following order: Ni<sub>2</sub>P/Ti<sub>0.98</sub>Ce<sub>0.02</sub>O<sub>2</sub> > Ni<sub>2</sub>P/TiO<sub>2</sub> > Ni<sub>2</sub>P/CeO<sub>2</sub> > bulk\nNi<sub>2</sub>P. The type of supports employed for Ni<sub>2</sub>P\nalso\ninfluenced the product distributions and thus HDO pathways. Ni<sub>2</sub>P/CeO<sub>2</sub> favored benzene selectivity, and this may\nbe related to the relative electron enrichment on the Ni<sup>δ+</sup> site of Ni<sub>2</sub>P/CeO<sub>2</sub> that facilitated benzene\ndesorption from the catalyst surface after demethoxylation of anisole.\nNi<sub>2</sub>P/TiO<sub>2</sub>-CeO<sub>2</sub> exhibited significantly\nhigher cyclohexane selectivity, which may be attributed to the lower\nelectron density on Ni<sup>δ+</sup> of Ni<sub>2</sub>P/TiO<sub>2</sub>-CeO<sub>2</sub> and the acidity of binary support, promoting\nthe deep hydrogenation of benzene to cyclohexane. The presence of\nphenol when Ni<sub>2</sub>P/TiO<sub>2</sub> and Ni<sub>2</sub>P/TiO<sub>2</sub>-CeO<sub>2</sub> were employed in anisole HDO could be correlated\nwith the acidity of TiO<sub>2</sub>, which led to methylation of anisole.\nAdding a small amount of CeO<sub>2</sub> in TiO<sub>2</sub> and using\nit as support synergistically improved the TOF and suppressed phenol\nformation while increasing cyclohexane selectivity. Both Ni<sub>2</sub>P/CeO<sub>2</sub> and Ni<sub>2</sub>P/TiO<sub>2</sub>-CeO<sub>2</sub> are promising catalysts in anisole HDO for the tunable target products\nof benzene and cyclohexane, respectively.
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