Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 314, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2022.121515
Keywords
Layered double hydroxides; Dual active sites; Catalytic transfer hydrogenation; Active hydrogen species; Synergetic catalysis
Funding
- National Natural Science Foundation of China [22172006, 22102006]
- National Key R&D Program of China [2021YFC2103501]
- Fundamental Research Funds for the Central Universities [XK1803-05, PT2021-04]
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This study prepared a Cu-based catalyst by transforming layered double hydroxides precursor, which showed promising catalytic behavior in the CTH reaction of furfural. The coexistence of Cu-0 and Cu+ on the catalyst surface and their synergistic effect were found to play a vital role in determining the catalytic behavior. The findings of this study provide important insights for other CTH reactions in the upgrading processes of biomass.
As a safe and environmentally friendly selective hydrogenation method, catalytic transfer hydrogenation (CTH) has aroused great interest in preparation of high-value-added products from biomass derived resources. Herein, a Cu-based catalyst (Cu/CuAl-MMO-400) was prepared by structural topological transformation of layered double hydroxides (LDHs) precursor, which displayed promising catalytic behavior toward CTH reaction of furfural (FAL) with 2-propanol (2-POL) as the hydrogen donor. Notably, the reaction rate is as high as 0.125 mol g(-1) h(-1), which is superior to previously reported non-noble metal catalysts. A combination investigation based on XPS, XANES and Bader charge confirms the co-existence of Cu-0 and Cu+ sites on the surface of Cu nanoparticles. Both experimental studies (in situ DRIFTS and isotope labelling MS) and DFT calculations reveal that the Cu-0 inverted exclexpressionmexpressiontion Cu+ synergistic effect plays a vital role in determining catalytic behavior: the Cu+ species acts as both dehydroge-nation and hydrogenation active site; while the Cu-0 site promotes the transfer of H atoms between adsorbed substrates. This work substantiates a Cu-0-Cu+ synergetic catalysis by establishing structure-property correlation and revealing reaction pathway, which could be extended to other CTH reactions in the upgrading processes of biomass.
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