Dataset Information

Solvent-Activated Hafnium-Containing Zeolites Enable Selective and Continuous Glucose-Fructose Isomerisation.

ABSTRACT: The isomerisation of glucose to fructose is a critical step towards manufacturing petroleum-free chemicals from lignocellulosic biomass. Herein we show that Hf-containing zeolites are unique catalysts for this reaction, enabling true thermodynamic equilibrium to be achieved in a single step during intensified continuous operation, which no chemical or biological catalyst has yet been able to achieve. Unprecedented single-pass yields of 58?% are observed at a fructose selectivity of 94?%, and continuous operation for over 100?hours is demonstrated. The unexpected performance of the catalyst is realised following a period of activation within the reactor, during which time interaction with the solvent generates a state of activity that is absent in the synthesised catalyst. Mechanistic studies by X-ray absorption spectroscopy, chemisorption FTIR, operando UV/Vis and ¹ H-¹³ C HSQC?NMR spectroscopy indicate that activity arises from isolated Hf^IV atoms with monofunctional acidic properties.

SUBMITTER: Botti L

PROVIDER: S-EPMC7818259 | biostudies-literature | 2020 Nov

REPOSITORIES: biostudies-literature

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Solvent-Activated Hafnium-Containing Zeolites Enable Selective and Continuous Glucose-Fructose Isomerisation.

Botti Luca L Kondrat Simon A SA Navar Ricardo R Padovan Daniele D Martinez-Espin Juan S JS Meier Sebastian S Hammond Ceri C

Angewandte Chemie (International ed. in English) 20200831 45

The isomerisation of glucose to fructose is a critical step towards manufacturing petroleum-free chemicals from lignocellulosic biomass. Herein we show that Hf-containing zeolites are unique catalysts for this reaction, enabling true thermodynamic equilibrium to be achieved in a single step during intensified continuous operation, which no chemical or biological catalyst has yet been able to achieve. Unprecedented single-pass yields of 58 % are observed at a fructose selectivity of 94 %, and con ...[more]

PMID: 32686886

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Project description:RATIONALE:Cross-sectional studies have linked intake of high-fructose corn syrup-sweetened beverages with asthma in schoolchildren. OBJECTIVES:To examine associations of maternal prenatal and early childhood intake of sugar-sweetened beverages and fructose with current asthma in midchildhood (median age, 7.7 yr). METHODS:We assessed maternal pregnancy (first- and second-trimester average) and child (median age, 3.3 yr) intake of sugar-sweetened beverages and total fructose using food frequency questionnaires in 1,068 mother-child pairs from Project Viva, a prospective prebirth cohort. In a multivariable analysis, we examined associations of quartiles of maternal and child sugar-sweetened beverage, juice, and total fructose intake with child current asthma in midchildhood, assessed by questionnaire as ever having doctor-diagnosed asthma plus taking asthma medications or reporting wheezing in the past 12 months. RESULTS:Higher maternal pregnancy sugar-sweetened beverage consumption (mean, 0.6 servings/d; range, 0-5) was associated with younger maternal age, nonwhite race/ethnicity, lower education and income, and higher prepregnancy body mass index. Adjusting for prepregnancy body mass index and other covariates, comparing quartile 4 with quartile 1, higher maternal pregnancy intake of sugar-sweetened beverages (odds ratio, 1.70; 95% confidence interval, 1.08-2.67) and total fructose (odds ratio, 1.58; 95% confidence interval, 0.98-2.53) were associated with greater odds of midchildhood current asthma (prevalence, 19%). Higher early childhood fructose intake (quartile 4 vs. quartile 1) was also associated with midchildhood current asthma in models adjusted for maternal sugar-sweetened beverages (odds ratio, 1.79; 95% confidence interval, 1.07-2.97) and after additional adjustment for midchildhood body mass index z-score (odds ratio, 1.77; 95% confidence interval, 1.06-2.95). CONCLUSIONS:Higher sugar-sweetened beverage and fructose intake during pregnancy and in early childhood was associated with childhood asthma development independent of adiposity.

Dataset Information

Solvent-Activated Hafnium-Containing Zeolites Enable Selective and Continuous Glucose-Fructose Isomerisation.

Publications

Solvent-Activated Hafnium-Containing Zeolites Enable Selective and Continuous Glucose-Fructose Isomerisation.

Similar Datasets

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