Journal
CHEMSUSCHEM
Volume 14, Issue 2, Pages 642-654Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.202002357
Keywords
alcohols; biomass; heterogeneous catalysis; hydrogenolysis; polyols
Funding
- National Natural Science Foundation of China [21978224, 21676205]
- National Science Fund for Distinguished Young Scholars of China [51625804]
- International Exchange Program for Graduate Students, Tongji University [201902041]
- China Scholarship Council (CSC)
- JSPS KAKENHI [20H02519, 18H05247]
- Grants-in-Aid for Scientific Research [20H02519] Funding Source: KAKEN
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The study investigated partial hydrogenolysis of erythritol to 1,4-butanediol using Ir-ReOx/SiO2 and Ir-ReOx/rutile-TiO2 catalysts. The Ir-ReOx/TiO2 catalyst showed higher conversion rate and selectivity to 1,4-BuD than Ir-ReOx/SiO2, especially at low conversion levels, resulting in high 1,4-BuD productivity. The activity and selectivity of various triols, diols and mono-ols were compared between catalysts and substrates. Ir-ReOx/TiO2 catalyst exhibited higher activity in hydrogenolysis of C-OH bonds in 1,2- and 1,3-diols, while lower loading amounts of Ir on TiO2 decreased the activity and selectivity.
Partial hydrogenolysis of erythritol, which can be produced at large scale by fermentation, to 1,4-butanediol (1,4-BuD) is investigated with Ir-ReOx/SiO2 and Ir-ReOx/rutile-TiO2 catalysts. In addition to the higher conversion rate over Ir-ReOx/TiO2 than over Ir-ReOx/SiO2, which has been also reported for glycerol hydrogenolysis, Ir-ReOx/TiO2 showed higher selectivity to 1,4-BuD than Ir-ReOx/SiO2, especially at low conversion levels, leading to high 1,4-BuD productivity of 20 mmol(1,4-BuD) g(Ir)(-1) h(-1) at 373 K (36 % conversion, 33 % selectivity). The productivity based on the noble metal amount is higher than those reported previously, although the maximum yield of 1,4-BuD (23 %) is not higher than the highest reported values. The reactions of various triols, diols and mono-ols are tested and the selectivity and the reaction rates are compared between catalysts and between substrates. The Ir-ReOx/TiO2 catalyst showed about twofold higher activity than Ir-ReOx/SiO2 in hydrogenolysis of the C-OH bond at the 2- or 3-positions in 1,2- and 1,3-diols, respectively, whereas the hydrogenolysis of C-OH at the 1-position is less promoted by the TiO2 support. Lowering the loading amount of Ir on TiO2 (from 4 wt % to 2 or 1 wt %) decreases the Ir-based activity and 1,4-BuD selectivity. Similarly, increasing the loading amount on SiO2 from 4 wt % to 20 wt % increases the Ir-based activity and 1,4-BuD selectivity, although they remain lower than those for TiO2-supported catalyst with 4 wt % Ir. High metal loadings on the support seem to be important.
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