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UiO-66 derived Ru/ZrO2@C as a highly stable catalyst for hydrogenation of levulinic acid to gamma-valerolactone
Cao, Wenxiu1,2; Luo, Wenhao1; Ge, Hongguang2; Su, Yang1; Wang, Aiqin1; Zhang, Tao1
刊名GREEN CHEMISTRY
2017-05-07
DOI10.1039/c7gc00512a
19期:9页:2201-2211
收录类别SCI
文章类型Article
WOS标题词Science & Technology ; Physical Sciences
类目[WOS]Chemistry, Multidisciplinary
研究领域[WOS]Chemistry
关键词[WOS]AQUEOUS-PHASE HYDROGENATION ; SELECTIVE HYDROGENATION ; LIGNOCELLULOSIC BIOMASS ; RU CATALYST ; CARBON ; CONVERSION ; CHEMICALS ; PLATFORM ; FUELS ; RUTHENIUM
英文摘要The hydrogenation of levulinic acid (LA) to gamma-valerolactone (GVL) is a crucial reaction included in many biorefinery schemes for the production of renewable chemicals and fuels. The development of highly stable supported Ru-based catalysts in the polar protic liquid phase under hydrothermal conditions is still a major challenge. Here, we prepared a 0.85 wt% Ru/ZrO2@C catalyst using a new stabilization strategy based on the UiO-66 (Zr-MOF) material. The catalytic performance of this Ru/ZrO2@C in LA-to-GVL was tested and compared with commercial 5 wt% Ru/C at 10 bar H-2, 413 K in water and also in high protic aqueous solution (pH = 1). The full conversion of LA and quantitative yield of GVL were achieved with both catalysts. However, the 5 wt% Ru/C showed poor resistance to deactivation already after the first run. ICP, XPS, HRTEM, AC-STEM, TPR and physisorption data showed that quick deactivation of Ru/C was mainly caused by the leaching of ruthenium in addition to the loss of surface area via carbonaceous deposition in micro-pores. In contrast, the self-prepared Ru/ZrO2@C catalyst showed no apparent drop in catalytic performance either in water or in high protic aqueous solution upon multiple recycling, and no leaching of ruthenium was found even under harsh conditions (pH = 1). Remarkably, in the Ru/ZrO2@C catalyst, Ru (probable single-atom) was highly dispersed on nanotetragonal ZrO2 (3.3 nm), embedded in the amorphous carbon, and no apparent Ru nanoclusters were observed even after reactions. TPR results indicated that this excellent stability might be attributed to strong metal-support interaction between Ru and nanotetragonal ZrO2.
语种英语
WOS记录号WOS:000400836500022
引用统计
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/152003
专题中国科学院大连化学物理研究所
作者单位1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
2.Shaanxi Univ Technol, Sch Chem & Environm Sci, Shaanxi Key Lab Catalysis, Hanzhong 723001, Shaanxi, Peoples R China
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Cao, Wenxiu,Luo, Wenhao,Ge, Hongguang,et al. UiO-66 derived Ru/ZrO2@C as a highly stable catalyst for hydrogenation of levulinic acid to gamma-valerolactone[J]. GREEN CHEMISTRY,2017,19(9):2201-2211.
APA Cao, Wenxiu,Luo, Wenhao,Ge, Hongguang,Su, Yang,Wang, Aiqin,&Zhang, Tao.(2017).UiO-66 derived Ru/ZrO2@C as a highly stable catalyst for hydrogenation of levulinic acid to gamma-valerolactone.GREEN CHEMISTRY,19(9),2201-2211.
MLA Cao, Wenxiu,et al."UiO-66 derived Ru/ZrO2@C as a highly stable catalyst for hydrogenation of levulinic acid to gamma-valerolactone".GREEN CHEMISTRY 19.9(2017):2201-2211.
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