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Synchronizing Deoxygenation and Hydrogenation to Effect Glycerol Hydrogenolysis over Pt/Nb2W15O50 at Low H2 Pressure
ACS Sustainable Chemistry & Engineering ( IF 8.4 ) Pub Date : 2024-04-10 , DOI: 10.1021/acssuschemeng.3c08096
Jinghu Chen 1, 2 , Hong Huang 1 , Hu Pan 1 , Yongyong Cao 1 , Lingchang Jiang 1 , Qineng Xia 1 , Xiangtong Meng 2 , Jieshan Qiu 2 , Han Zuilhof 3, 4 , Shaomin Liu 2
Affiliation  

The selective hydrogenolysis of glycerol to 1,3-propanediol (1,3-PDO) necessitates the precise tandem reactions of deoxygenation at a specific location and the ensuing hydrogenation steps. Herein, a solid solution-supported catalyst Pt/Nb2W15O50 was reported for the hydrogenolysis of glycerol to 1,3-PDO. We engineered the exceptional interaction between active Pt and oxygen vacancies to efficiently integrate the deoxygenation and hydrogenation steps in tandem. The strong interaction between active Pt and oxygen vacancies was established via hydrogen (H2) spillover and induced the generation of 1,3-PDO in situ. This synergistic effect confers Pt/Nb2W15O50 with high catalytic performance, combining a 75.6% conversion of glycerol and 66.5% selectivity to 1,3-PDO at a low H2 pressure of 1.0 MPa (noting that most catalysts require H2 pressures of ≥4 MPa). Moreover, the structure–performance relationship validated that there is a linear correlation between active Pt, oxygen vacancies, and 1,3-PDO yield. This study provides mechanistic insights into further catalyst developments for the valorization of other biomass-derived oxygenates.

中文翻译:

低氢气压力下同步脱氧和加氢在 Pt/Nb2W15O50 上进行甘油氢解

甘油选择性氢解为 1,3-丙二醇 (1,3-PDO) 需要在特定位置进行精确的脱氧串联反应以及随后的氢化步骤。在此,报道了固溶体负载的催化剂Pt/Nb 2 W 15 O 50用于甘油氢解成1,3-PDO。我们设计了活性铂和氧空位之间的特殊相互作用,以有效地串联脱氧和氢化步骤。通过氢(H 2 )溢出建立活性Pt和氧空位之间的强相互作用,并诱导原位生成1,3-PDO。这种协同效应赋予 Pt/Nb 2 W 15 O 50较高的催化性能,在 1.0 MPa 的低 H 2压力下,甘油转化率为 75.6%,1,3-PDO 选择性为 66.5% (注意大多数催化剂需要 H)2压力≥4 MPa)。此外,结构-性能关系验证了活性 Pt、氧空位和 1,3-PDO 产率之间存在线性相关性。这项研究为进一步开发催化剂以提高其他生物质衍生的含氧化合物的价值提供了机制见解。
更新日期:2024-04-10
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