Efficient Hydrogenolysis of C–O Bond over Pd/P-TiO2: The Generation and Role of Brønsted Acid Site Triggered by Spillover Hydrogen

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2025-01-23 DOI:10.1021/acscatal.4c06939

Tingting Xiao, Jingrong Li, Jian Li, Qihang Gong, Peikai Luo, Xinluona Su, Haiyang Cheng, Chao Zhang, Fengyu Zhao

引用次数: 0

Abstract

The hydrogenolysis of cellulose-derived 5-hydroxymethylfurfural is essential for the production of fuels and chemicals from biomass. Herein, we fabricated a phosphorus-doped Pd/P-TiO₂ catalyst for the hydrodeoxygenation of 5-hydroxymethylfurfural to 2,5-dimethylfuran. A large number of defects and electron-deficient Ti⁴⁺ sites (_dTi⁴⁺) were formed by doping phosphorus into the TiO₂ support, which could promote hydrogen spillover and reactant adsorption. Moreover, the spilled active hydrogen induced the formation of P–O(H)-_dTi⁴⁺, which acted as a “Brønsted acidic site” to promote the activation of C–O bonds. Consequently, the Pd/P-TiO₂ catalyst exhibited superb activity for the hydrodeoxygenation of 5-hydroxymethylfurfural to 2,5-dimethylfuran at mild conditions of 150 °C under 1 MPa H₂.

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Pd/P-TiO2上C-O键的高效氢解：溢出氢触发Brønsted酸位的产生及其作用

纤维素衍生的5-羟甲基糠醛的氢解对于从生物质中生产燃料和化学品至关重要。本文制备了一种磷掺杂Pd/P-TiO2催化剂，用于5-羟甲基糠醛加氢脱氧为2,5-二甲基呋喃。在TiO2载体中掺杂磷，形成大量缺陷和缺电子Ti4+位点（dTi4+），促进氢溢出和反应物吸附。此外，溢出的活性氢诱导P-O (H)-dTi4+形成，P-O (H)-dTi4+作为“Brønsted酸性位点”促进C-O键的活化。结果表明，Pd/P-TiO2催化剂在150℃、1 MPa H2条件下，对5-羟甲基糠醛加氢脱氧为2,5-二甲基呋喃具有良好的催化活性。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.