二氧化钛多晶型对 Pt-WOx/TiO2 催化剂甘油氢解制 1,3-丙二醇的结构和催化性能的影响,ACS Sustainable Chemistry & Engineering

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二氧化钛多晶型对 Pt-WOx/TiO2 催化剂甘油氢解制 1,3-丙二醇的结构和催化性能的影响
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2022-07-13 , DOI: 10.1021/acssuschemeng.2c02205
Yang Zeng ₁ , Lan Jiang ₁ , Xiaoxin Zhang ₂ , Songhai Xie ₁ , Yan Pei ₁ , Gongbing Zhou ₃ , Weiming Hua ₁ , Minghua Qiao ₁ , Zhen-Hua Li ₁ , Baoning Zong ₂

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生物质衍生甘油催化氢解为 1,3-丙二醇 (1,3-PDO) 是可持续生产增值化学品的重要过程。然而，对载体多晶型物对该反应的影响缺乏了解。在此，制备了两种负载在金红石型 TiO ₂ (r-TiO ₂ ) 和锐钛矿型 TiO ₂ (a-TiO ₂ ) 多晶型上的Pt-WO _x /TiO _{2催化剂，研究了 TiO}₂的晶相对结构性能和催化性能的影响。甘油氢解的性能。_二氧化钛多晶型物被确定对 Pt 纳米粒子 (NP) 的尺寸和 WO _x物种的分散和位置产生深远的影响，这源于 PtO ₂和 TiO ₂多晶型物之间晶体结构的差异以及在WO _x与不同TiO ₂多晶型物的相互作用。在甘油氢解中，Pt-WO _x /r-TiO ₂催化剂的 1,3-PDO 选择性为 51.2%，甘油转化为液体产物的率为 74.5%，1,3-PDO 的产率为 38.1%。相比之下，Pt-WO _x /a-TiO ₂催化剂显示出较差的甘油转化率和 1,3-PDO 选择性，在相同反应条件下仅产生 1.0% 的 1,3-PDO。_{Pt-WO x} /r-TiO ₂催化剂的优异催化性能归因于 r-TiO _{2多晶型物，与 a-TiO}₂多晶型物相比，r-TiO 2多晶型物有利于氢从 Pt NPs 更快地溢出到 WO _x上的反应中间体与物理混合的 Pt/r-TiO ₂ + WO _x /r-TiO ₂催化剂相比，1,3-PDO 的产率更高（44.8%）证实了这一点。这项工作证明了 TiO _{2多晶型物的关键作用}支持设计用于甘油氢解为 1,3-PDO 的有效 Pt-WO _x基催化剂。

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Effect of Titania Polymorphs on the Structure and Catalytic Performance of the Pt–WOx/TiO2 Catalyst in Glycerol Hydrogenolysis to 1,3-Propanediol

Catalytic hydrogenolysis of biomass-derived glycerol to 1,3-propanediol (1,3-PDO) represents an important process for the sustainable production of value-added chemicals. However, there is a dearth of understanding of the effect of the polymorph of the support on this reaction. Herein, two Pt–WO_x/TiO₂ catalysts supported on rutile TiO₂ (r-TiO₂) and anatase TiO₂ (a-TiO₂) polymorphs were prepared to investigate the crystal phase effect of TiO₂ on the structural property and catalytic performance in glycerol hydrogenolysis. The TiO₂ polymorph was identified to impose profound effects on the size of the Pt nanoparticles (NPs) and the dispersion and location of the WO_x species, which originated from the discrepancies in the crystal structures between the PtO₂ and the TiO₂ polymorphs and the discrepancies in the interactions of WO_x with different TiO₂ polymorphs. In glycerol hydrogenolysis, the Pt–WO_x/r-TiO₂ catalyst gave a 1,3-PDO selectivity of 51.2% at a glycerol conversion to liquid products of 74.5%, yielding 38.1% of 1,3-PDO. In contrast, the Pt–WO_x/a-TiO₂ catalyst showed much inferior glycerol conversion and 1,3-PDO selectivity, yielding only 1.0% of 1,3-PDO under identical reaction conditions. The superior catalytic performance of the Pt–WO_x/r-TiO₂ catalyst is attributed to the r-TiO₂ polymorph that facilitates a faster hydrogen spillover than the a-TiO₂ polymorph from the Pt NPs to the reaction intermediate on the WO_x species, which is substantiated by an even higher 1,3-PDO yield of 44.8% over the physically mixed Pt/r-TiO₂ + WO_x/r-TiO₂ catalyst. This work demonstrates the critical role of the polymorph of the TiO₂ support in the design of efficacious Pt–WO_x-based catalysts for glycerol hydrogenolysis to 1,3-PDO.

更新日期：2022-07-13

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