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

Effect of Titania Polymorphs on the Structure and Catalytic Performance of the Pt–WOx/TiO2 Catalyst in Glycerol Hydrogenolysis to 1,3-Propanediol
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二氧化钛多晶型物对Pt-WOx/TiO2催化剂甘油氢解制1,3-丙二醇结构及催化性能的影响

DOI:
10.1021/acssuschemeng.2c02205
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发表时间:
2022-07
期刊:
ACS Sustainable Chemistry & Engineering
影响因子:
--
通讯作者:
Baoning Zong
Baoning Zong
中科院分区:
其他
文献类型:
--
作者:
Yang Zeng;Lan Jiang;Xiaoxin Zhang;Songhai Xie;Yan Pei;Gongbing Zhou;Weiming Hua;Minghua Qiao;Zhen-Hua Li;Baoning Zong

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生物质衍生甘油催化氢解制1,3-丙二醇(1,3- pdo)是可持续生产增值化学品的重要工艺。然而,对于载体的多晶型对该反应的影响还缺乏了解。本文制备了金红石型TiO2(r-TiO2)和锐钛矿型TiO2(a-TiO2)多晶型负载的Pt-WOx /TiO2催化剂,研究了TiO2的晶相对结构性质和甘油氢解催化性能的影响。研究发现,tio2晶型对Pt纳米颗粒(NPs)的大小和woxs的分散和位置有深远的影响,这源于pto2与tio2晶型之间的晶体结构差异以及woxs与不同tio2晶型之间相互作用的差异。在甘油氢解中,Pt-WOx /r- tio2催化剂的1,3- pdo选择性为51.2%,甘油转化为液体产物的选择性为74.5%,1,3- pdo的收率为38.1%。相比之下,Pt-WOx /a- tio2催化剂表现出较差的甘油转化率和1,3- pdo选择性,在相同的反应条件下仅产生1.0%的1,3- pdo。Pt - WOx/r-TiO2催化剂的优异催化性能归功于r-TiO2多晶型,它比a- tio2多晶型更容易从Pt NPs向反应中间体的氢溢出,这一点得到了比物理混合Pt/r-TiO2+ WOx/r-TiO2催化剂更高的1,3- pdo产率44.8%的证实。这项工作证明了tio2载体的多晶型在设计有效的pt - woxs基甘油氢解制1,3- pdo催化剂中的关键作用。
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–WOx/TiO2catalysts supported on rutile TiO2(r-TiO2) and anatase TiO2(a-TiO2) polymorphs were prepared to investigate the crystal phase effect of TiO2on the structural property and catalytic performance in glycerol hydrogenolysis. The TiO2polymorph was identified to impose profound effects on the size of the Pt nanoparticles (NPs) and the dispersion and location of the WOxspecies, which originated from the discrepancies in the crystal structures between the PtO2and the TiO2polymorphs and the discrepancies in the interactions of WOxwith different TiO2polymorphs. In glycerol hydrogenolysis, the Pt–WOx/r-TiO2catalyst 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–WOx/a-TiO2catalyst 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–WOx/r-TiO2catalyst is attributed to the r-TiO2polymorph that facilitates a faster hydrogen spillover than the a-TiO2polymorph from the Pt NPs to the reaction intermediate on the WOxspecies, which is substantiated by an even higher 1,3-PDO yield of 44.8% over the physically mixed Pt/r-TiO2+ WOx/r-TiO2catalyst. This work demonstrates the critical role of the polymorph of the TiO2support in the design of efficacious Pt–WOx-based catalysts for glycerol hydrogenolysis to 1,3-PDO.
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