Unraveling the Dependence of Critical Active Sites of WOx on Rh/WOx Catalysts in Tetrahydrofurfuryl Alcohol Hydrogenolysis,ACS Sustainable Chemistry & Engineering

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Unraveling the Dependence of Critical Active Sites of WOx on Rh/WOx Catalysts in Tetrahydrofurfuryl Alcohol Hydrogenolysis
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2023-08-16 , DOI: 10.1021/acssuschemeng.3c01461
Man Yang ₁ , Yuxiang Jiao ₁ , Jianglin Duan ₂ , Keying Wu ₁ , Hailiang Song ₁ , Shaodong Sun ₁ , Yujing Ren ₂

Affiliation

Taking the background of the ambiguous role of oxophilic metal oxide in metal-acid bifunctional catalysts for the important field of tetrahydrofurfuryl alcohol (THFA) hydrogenolysis, a linear relationship between the W═O/W–OH content in sub-nano-Rh-supported WO_x and 1,5-pentanediol (1,5-PeD) yields from THFA hydrogenolysis has been established. It reveals that the higher reduction temperature promotes the surface Rh/W ratio. Thus, hydrogen spillover is facilitated, leading to more surface W═O structures and thereby more in-situ-reduced W–OH generation. W–OH structures work as the active sites to provide in situ Brønsted acid, resulting in enhanced selective activation for secondary C–O bonds of THFA. This discovery reveals the unique role of the surface structure on oxophilic metal oxide in chemoselective hydrogenolysis of the secondary C–O bond in polyols.

中文翻译：

揭示四氢糠醇氢解中 WOx 关键活性位点对 Rh/WOx 催化剂的依赖性

以亲氧金属氧化物在四氢糠醇（THFA）氢解这一重要领域的金属酸双功能催化剂中的模糊作用为背景，亚纳米Rh负载的W=O/W-OH含量之间存在线性关系WOx _{_}已经确定了 THFA 氢解的 1,5-戊二醇 (1,5-PeD) 产率。结果表明，较高的还原温度可提高表面 Rh/W 比值。因此，促进了氢溢出，导致更多的表面W=O结构，从而更多地原位减少了W-OH的生成。W-OH结构作为活性位点提供原位布朗斯台德酸，从而增强THFA二级C-O键的选择性活化。这一发现揭示了亲氧金属氧化物的表面结构在多元醇中仲C-O键的化学选择性氢解中的独特作用。

更新日期：2023-08-16

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