Accelerating Semihydrogenation of Cinnamaldehyde by Water over a Au/α-MoC Catalyst

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2024-06-20 DOI:10.1021/acscatal.4c02448

Yuanhong Lu, Qiao Chen, Yunlong Zhang, Yan Wei, Xiaohui Hou, Rui Huang* and Dehui Deng*,

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Abstract

Replacing H₂ with H₂O as the hydrogen source for the water-involved selective hydrogenation of cinnamaldehyde to cinnamyl alcohol (WSHCC) is very attractive yet is underdeveloped by a much lower H₂O conversion rate than H₂. Here, we report the realization of a high-efficiency WSHCC process by a synergy of CO adsorption and H₂O dissociation over a Au/α-MoC_1–x boundary. It shows a specific molar rate of 60.86 mol mol_Au^–1 h^–1 to cinnamyl alcohol at 96 °C, which is nearly 12-fold that reported earlier, and maintains a high conversion of over 99% and a high selectivity of 77%. Mechanistic studies indicate that the Au/α-MoC_1–x boundary accommodates atomically dispersed Au^δ+ sites for adsorbing CO, vacating oxygen-covered α-MoC_1–x and thereby creating isolated Mo sites for the preferred adsorption and hydrogenation of C═O bonds over that of C═C bonds. This provides a catalyst design strategy for high-efficiency C═O hydrogenation by water.

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在 Au/α-MoC 催化剂上加速肉桂醛与水的半氢化反应

在肉桂醛到肉桂醇的水参与选择性加氢反应（WSHCC）中，用 H2O 替代 H2 作为氢源是非常有吸引力的，但由于 H2O 转化率远低于 H2 而未得到充分发展。在此，我们报告了在 Au/α-MoC1-x 边界上通过 CO 吸附和 H2O 解离的协同作用实现的高效 WSHCC 过程。在 96 °C时，它对肉桂醇的比摩尔速率为 60.86 mol molAu-1 h-1，是之前报道的近 12 倍，并保持了 99% 以上的高转化率和 77% 的高选择性。机理研究表明，Au/α-MoC1-x 边界容纳了原子分散的 Auδ+ 位点，用于吸附 CO，腾空了氧覆盖的 α-MoC1-x，从而产生了孤立的 Mo 位点，优先吸附 C═O 键而不是 C═C 键并使其氢化。这为水对 C═O 的高效氢化提供了催化剂设计策略。

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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.