CeO2、TiO2和TiO2-CeO2载体对Ni2P催化苯甲醚加氢脱氧性能的影响,Energy & Fuels

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CeO2、TiO2和TiO2-CeO2载体对Ni2P催化苯甲醚加氢脱氧性能的影响
Energy & Fuels ( IF 5.2 ) Pub Date : 2023-06-02 , DOI: 10.1021/acs.energyfuels.2c04108
Pawnprapa Pitakjakpipop _{1,

2} , Chunshan Song _{1,

3}

Affiliation

这项工作使用合成的 CeO ₂、TiO ₂和 TiO ₂ -CeO _2载体和_商业载体（表示为 CeO ₂ -L 和 TiO ₂ -L) 以及块状 Ni ₂ P。表征表明 Ni ₂ P 纳米粒子很好地分散在合成的 CeO ₂上。Ni ₂ P/CeO _{2在合成载体上的那些 Ni}₂ P 以及常见材料如 SiO ₂中，以催化剂重量为基础表现出最高的活性、Al ₂ O ₃和活性炭。Ni ₂ P/TiO ₂ -CeO ₂（Ti/Ce 摩尔比为 0.98）根据周转频率（TOF，h ^{–1 ）提供优于 Ni}₂ P/CeO ₂的反应性，这表明 Ni 上有更多活性位点₂ P/TiO ₂ -CeO ₂比Ni ₂ P/CeO ₂。苯甲醚在催化剂上的TOF按以下顺序降低：Ni ₂ P/Ti _0.98 Ce _0.02 O ₂ > Ni ₂ P/TiO ₂ > Ni ₂P/CeO ₂ > 块状 Ni _{2 P。用于 Ni}₂ P的载体类型也影响产物分布，从而影响 HDO 途径。Ni ₂ P/CeO ₂有利于苯的选择性，这可能与Ni ₂ P/CeO _{2 Ni}^δ+位点的相对电子富集有关，促进苯甲醚脱甲氧基化后苯从催化剂表面脱附。Ni ₂ P/TiO ₂ -CeO ₂表现出明显更高的环己烷选择性，这可能是由于Ni ₂ P/TiO _2的Ni^δ+上的电子密度较低-CeO ₂和二元载体的酸性，促进苯深度加氢制环己烷。当Ni ₂ P/TiO ₂和Ni ₂ P/TiO ₂ -CeO ₂用于苯甲醚HDO时苯酚的存在可能与TiO ₂的酸度相关，这导致苯甲醚甲基化。在 TiO ₂中添加少量 CeO ₂并将其用作载体可协同改善 TOF 并抑制苯酚形成，同时提高环己烷选择性。Ni ₂ P/CeO ₂和Ni ₂ P/TiO ₂ -CeO ₂是苯甲醚 HDO 中有前途的催化剂，分别用于苯和环己烷的可调目标产物。

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Effects of CeO2, TiO2, and TiO2-CeO2 Supports on Catalytic Performance of Ni2P in Hydrodeoxygenation of Anisole

This work examined the effects of supports for nickel phosphide (Ni₂P) catalysts on anisole hydrodeoxygenation (HDO) using synthesized CeO₂, TiO₂, and TiO₂-CeO₂ supports and commercial supports (denoted as CeO₂-L and TiO₂-L) along with bulk Ni₂P. Characterization revealed that Ni₂P nanoparticles were well dispersed on the synthesized CeO₂. Ni₂P/CeO₂ exhibited the highest activity on a catalyst weight basis among those Ni₂P on synthesized supports as well as the common materials such as SiO₂, Al₂O₃, and activated carbon. Ni₂P/TiO₂-CeO₂ (at a Ti/Ce molar ratio of 0.98) afforded superior reactivity to Ni₂P/CeO₂ based on turnover frequency (TOF, h^–1), which points to more active sites on Ni₂P/TiO₂-CeO₂ than on Ni₂P/CeO₂. The TOF of anisole on catalysts decreased in the following order: Ni₂P/Ti_0.98Ce_0.02O₂ > Ni₂P/TiO₂ > Ni₂P/CeO₂ > bulk Ni₂P. The type of supports employed for Ni₂P also influenced the product distributions and thus HDO pathways. Ni₂P/CeO₂ favored benzene selectivity, and this may be related to the relative electron enrichment on the Ni^δ+ site of Ni₂P/CeO₂ that facilitated benzene desorption from the catalyst surface after demethoxylation of anisole. Ni₂P/TiO₂-CeO₂ exhibited significantly higher cyclohexane selectivity, which may be attributed to the lower electron density on Ni^δ+ of Ni₂P/TiO₂-CeO₂ and the acidity of binary support, promoting the deep hydrogenation of benzene to cyclohexane. The presence of phenol when Ni₂P/TiO₂ and Ni₂P/TiO₂-CeO₂ were employed in anisole HDO could be correlated with the acidity of TiO₂, which led to methylation of anisole. Adding a small amount of CeO₂ in TiO₂ and using it as support synergistically improved the TOF and suppressed phenol formation while increasing cyclohexane selectivity. Both Ni₂P/CeO₂ and Ni₂P/TiO₂-CeO₂ are promising catalysts in anisole HDO for the tunable target products of benzene and cyclohexane, respectively.

更新日期：2023-06-02

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