钌钨合金纳米颗粒催化呋喃醛串联加氢开环合成线性酮

doi:10.1016/S1872-2067(25)64911-4

催化学报 ›› 2026, Vol. 82: 337-347.DOI: 10.1016/S1872-2067(25)64911-4

钌钨合金纳米颗粒催化呋喃醛串联加氢开环合成线性酮

黄鹏^a, 谢志俊^a, 郭勇^a, 王珺^a, 邹吉军^b, 邓强^a^,^*()

^a南昌大学化学化工学院, 江西南昌 330031
^b天津大学化工学院, 天津 300072

收稿日期:2025-07-30 接受日期:2025-09-25 出版日期:2026-03-18 发布日期:2026-03-05
通讯作者: * 电子信箱: dengqiang@ncu.edu.cn (邓强).
基金资助:
国家自然科学基金(22178158);国家自然科学基金(52162014);江西省双千人才计划-青年项目(S2021GDQN0947);江西省自然科学基金重点项目(S2024ZRZDL0220)

Ruthenium-tungsten alloy nanoparticles accelerate the cascade hydrogenation-ring opening of furfurals to linear ketones

Peng Huang^a, Zhijun Xie^a, Yong Guo^a, Jun Wang^a, Ji-Jun Zou^b, Qiang Deng^a^,^*()

^aSchool of Chemistry and Chemical Engineering, Nanchang University, Nanchang 330031, Jiangxi, China
^bSchool of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China

Received:2025-07-30 Accepted:2025-09-25 Online:2026-03-18 Published:2026-03-05
Contact: * E-mail: dengqiang@ncu.edu.cn (Q. Deng).
Supported by:
National Natural Science Foundation of China(22178158);National Natural Science Foundation of China(52162014);Jiangxi Provincial Double Thousand Talents Plan-Youth Program(S2021GDQN0947);Key project of Jiangxi Provincial Natural Science Foundation(S2024ZRZDL0220)

摘要/Abstract

摘要：

将生物质转化为含氧精细化学品是实现可持续经济发展、降低化石能源依赖的关键路径, 呋喃类化合物(糠醛、5-羟甲基糠醛等)作为单糖脱水产物, 是生物质催化转化的重要平台分子. 其中, 呋喃类化合物经串联加氢开环反应制备的线性酮类化合物, 在医药、香料中间体及聚合物单体领域具有重要应用价值. 然而, 传统催化剂易引发过度加氢、过度酸催化反应等问题, 导致线性酮产率偏低, 且目前报道的反应体系所需温度较高(90-200 °C), 温和条件下的高效催化仍是该领域亟待突破的难点, 因此开发高选择性、高活性的双功能催化剂具有重要研究意义.

本文采用浸渍还原法制备了负载型钌钨(RuW)合金纳米颗粒催化剂, 其核心在于构建了RuW合金结构与RuW-WO_x界面, 可通过氢溢流效应原位形成H⁺-H^-对, 突破了传统双功能催化剂中金属位点与酸性位点空间分离的局限, 让加氢与开环反应能在邻近活性位点高效衔接, 实现双功能协同催化. X射线衍射、透射电镜、X射线光电子能谱、扩展X-射线吸收精细结构等表征证明, RuW合金纳米颗粒(约5 nm)均匀分散于载体表面, 且存在丰富的Ru-O-W界面, H₂在RuW合金位点解离为H原子后迁移至WO_x位点, 形成H^--Ru···O-H⁺物种. 催化性能测试表明, 在80 °C、1.0 MPa H₂的温和条件下, RuW/SiO₂催化糠醛加氢开环生成5-羟基-2-戊酮的产率高达86.2%, 碳平衡保持在97%以上, 抑制了过度加氢产物四氢糠醇及酸催化环重排产物环戊酮的生成; 该催化剂对5-甲基糠醛、5-羟甲基糠醛反应同样具有普适性, 分别高选择性生成2,5-己二酮、1-羟基-2,5-己二酮与2,5-己二酮, 且能稳定循环使用5次. 机理研究表明, 原位形成的H⁺-H^-对不仅作为糠醛C=O加氢的活性位, 而且作为呋喃醇开环活性位, 缩短中间体的扩散路径, 避免过度反应.

综上, 本研究通过氢溢流构建H⁺-H^-对的双功能催化策略, 为温和条件下生物质平台分子的高选择性转化提供了新思路, 有望推动呋喃类化合物定向制备线性酮的工业化应用, 也为其他串联反应催化剂的设计提供参考.

关键词: RuW-WO_x界面, 双功能催化, 呋喃醛, 线性酮, 氢溢流

Abstract:

The metal-acid bifunctional catalyzed conversion of furfurals to linear ketones is crucial but challenging for sustainable chemical synthesis owing to the tendency for over hydrogenation and overacid-catalyzed reaction pathways over traditional catalysts. Herein, ruthenium-tungsten (RuW) alloy nanoparticle-supported catalysts (such as, RuW/SiO₂, RuW/Al₂O₃, RuW/C) were prepared via incipient wetness impregnation followed by H₂ reduction, showing a cascade hydrogenation-ring opening transformation of furfural to 5-hydroxy-2-pentanone with an unprecedented yield of 86.2% at a mild temperature of 80 °C. Catalytic mechanism studies confirmed that hydrogen spillover from RuW alloy sites to WO_x sites generated H⁺-H^- pairs in situ, which functioned as atypical active sites for the furfural hydrogenation step and offered Brönsted acidic sites for the ring opening of furan alcohol, thereby facilitating the facile preparation of 5-hydroxy-2-pentanone. Furthermore, the catalyst exhibited broad applicability for synthesizing linear ketones from various furfurals (i.e., 5-methyl furfural and 5-hydroxymethyl furfural). This study demonstrated interesting bifunctional catalysis through harnessing hydrogen spillover to form transient H⁺-H^- pairs, enabling a challenging cascade reaction pathway toward an efficient linear ketone synthesis.

Key words: RuW-WO_x interface, Bifunctional catalysis, Furfurals, Linear ketones, Hydrogen spillover

黄鹏, 谢志俊, 郭勇, 王珺, 邹吉军, 邓强. 钌钨合金纳米颗粒催化呋喃醛串联加氢开环合成线性酮[J]. 催化学报, 2026, 82: 337-347.

Peng Huang, Zhijun Xie, Yong Guo, Jun Wang, Ji-Jun Zou, Qiang Deng. Ruthenium-tungsten alloy nanoparticles accelerate the cascade hydrogenation-ring opening of furfurals to linear ketones[J]. Chinese Journal of Catalysis, 2026, 82: 337-347.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(25)64911-4

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Fig. 1. (A) XRD patterns of RuW/SiO2 and Ru/SiO2. (B) TEM image of RuW/SiO2. Raman spectra (C), Ru 3p XPS spectra (D), W 4f XPS spectra (E), and EXAFS k2-weighted χ(k) analysis (F) of RuW/SiO2 and Ru/SiO2.

Fig. 2. (A) Reaction pathway of FFA reaction. Product distribution curve over time over Ru/SiO2 (B) and RuW/SiO2 (C). (D) Catalytic performance of FFA reaction over various catalysts. (E) Recycling performance of RuW/SiO2 in FFA reaction. Catalytic performance of 5-methyl furfural (F) and 5-hydroxymethyl furfural (G) over different catalysts. Reaction conditions: H2O (15 mL), temperature (80 °C), reactant (1 mmol), H2 (1.0 MPa), Ru/SiO2 (100 mg), RuW/SiO2 (100 mg); (D) time (12 h); (E) time (4 h); (F,G) time (12 h). The products were quantified by GC.

Fig. 3. (A) Catalytic performance of FFA reaction over various catalysts. (B) FFA hydrogenation kinetic experiments over Ru/SiO2 and RuW/SiO2 under different FFA concentrations and H2 pressure. (C) FFA hydrogenation rate over Ru/SiO2 and RuW/SiO2 under different atmospheres. In-situ DRIFT spectra (D) and W 4f and O 1s XPS analysis (E) in NAP-XPS of H2-activated RuW/SiO2. (F) PD hydrogenation rate over Ru/SiO2 and RuW/SiO2. Reaction conditions: H2O (15 mL), temperature (80 °C), reactant (1 mmol). (A) catalysts (100 mg), H2 (1.0 MPa), time (24 h); (B) catalysts (20 mg), H2 (1.0 MPa) time (0.5 h); (C) catalysts (20 mg), H2/D2 (1.0 MPa) time (0.5 h); (F) catalysts (20 mg), H2 (1.0 MPa), time (0.5 h). The products were quantified by GC.

Fig. 4. (A) FA ring opening rate over Ru/SiO2 and RuW/SiO2 under different atmospheres. NH3-TPD (B) and Py-FTIR (C) spectra of various catalysts. (D) In-situ DRIFT spectra of adsorbed FA on various catalysts. (E) The adsorption kinetics of FA over different catalysts. Adsorption conditions: H2O (150 mL), catalyst (100 mg), FA (0.05 mmol), temperature (30 °C). The FA concentrations were quantified by UV-Vis. (F) Catalytic performance of FFA reaction over physical mixture of Ru/SiO2 and different catalysts. Reaction conditions: H2O (15 mL), temperature (80 °C), reactant (1 mmol); (A) catalysts (100 mg), H2/N2 (1.0 MPa); (F) Ru/SiO2 (100 mg), HZSM-5 (11 mg), W/SiO2 (100 mg), time (24 h). The products were quantified by GC.

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钌钨合金纳米颗粒催化呋喃醛串联加氢开环合成线性酮

Ruthenium-tungsten alloy nanoparticles accelerate the cascade hydrogenation-ring opening of furfurals to linear ketones

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