期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 6, 期 11, 页码 14704-14712出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.8b03268
关键词
Sorbitol dehydration; Solid acid; Sulfated zirconia; biorefining; platform chemicals
资金
- EPSRC
- UK Catalysis Hub [EP/K014749/1, EP/K014706/1]
- British Council through the Global Innovation Initiative under the GB3-Net project
- EPSRC [EP/K036548/1, EP/K014706/1, EP/J020184/2, EP/K036548/2, EP/K014749/1, EP/G007594/2] Funding Source: UKRI
Isosorbide is a widely touted intermediate for the production of biorenewable polymers and plastics, accessible through the aqueous phase cascade conversion of D-sorbitol to isosorbide via 1,4-sorbitan. However, existing routes to isosorbide typically employ mineral acids under forcing conditions, and hence alternative heterogeneously catalyzed processes are highly desirable. Aqueous phase D-sorbitol conversion was therefore investigated over families of sulfated zirconia (SZ) solid acid catalysts, with the effect of employing monoclinic, tetragonal ZrO2, or Zr(OH)(4) as the parent support compared. The cascade proceeds via a stepwise dehydration to 1,4-sorbitan and subsequently isosorbide, with the latter favored over stronger acid sites. Monoclinic SZ exhibits superior activity to tetragonal SZ, reflecting a higher acid site density and pyrosulfate formation at lower SO42- loadings than over the other supports. Isosorbide selectivity at iso-conversion was proportional to acid site density, but independent of zirconia phase.
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