d-缺电子Ru单原子催化剂提高木质素衍生物的碳利用率以生产绿色环己醇和甲醇

IF 13.1 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-05-05 DOI:10.1021/acscatal.5c01124

Shunlin Li, Zhenzhen Li, Linlin Duan, Guohua Yao, Xiaolong Wang, Yang Yang, Ying Wan

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引用次数: 0

摘要

将生物质直接转化为没有副产品的生物燃料是一个巨大的挑战。为了解决这一问题，我们在有序介孔钛/碳复合材料（OMTC）上合成了一种d电子缺陷钌单原子催化剂。该催化剂在温和条件下（1 MPa H2，水为溶剂），愈创木酚完全转化为环己醇和甲醇，且具有完全选择性。结构和光谱分析表明，Ru原子分散在OMTC载体中，导致d-电子缺位1.30 e，这增加了愈伤木酚加氢脱氧过程中2-甲氧基环己醇中间体的去甲氧基化，从而提高了对环己醇和甲醇的选择性。这项工作强调了在生物质中实现完全碳利用的可扩展方法，推动了可持续生物燃料和化学品的发展。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

A d-Electron Deficient Ru Single-Atom Catalyst that Increases the Carbon Utilization of Lignin Derivatives for the Production of Green Cyclohexanol and Methanol

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A d-Electron Deficient Ru Single-Atom Catalyst that Increases the Carbon Utilization of Lignin Derivatives for the Production of Green Cyclohexanol and Methanol

The direct conversion of biomass to biofuels without byproducts is a big challenge. We report the synthesis of a d-electron deficient Ru single-atom catalyst supported on an ordered mesoporous titania/carbon composite (OMTC) to address this. The catalyst demonstrated complete conversion of guaiacol to cyclohexanol and methanol under mild conditions (1 MPa H₂, water as solvent) with exclusive selectivity. Structural and spectroscopic analyses revealed atomically dispersed Ru in the OMTC support, resulting in a d-electron deficiency of 1.30 e, which increased the demethoxylation of the 2-methoxycyclohexanol intermediate during guaiacol hydrodeoxygenation and therefore increased the selectivity to cyclohexanol and methanol. This work highlights a scalable approach to achieving full carbon utilization in the biomass, advancing the development of sustainable biofuels and chemicals.

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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.