Abstract

BackgroundCumulative reported evidence has indicated that renewable feedstocks are a promising alternative source to fossil platforms for the production of fuels and chemicals. In that regard, the development of new, highly active, selective, and easy to recover and reuse catalysts for biomass conversions is urgently needed. The combination of enzymatic and inorganic heterogeneous catalysis generates an unprecedented platform that combines the advantages of both, the catalytic efficiency and selectivity of enzymes with the ordered structure, high porosity, mechanical, thermal and chemical resistance of mesoporous materials to obtain enzymatic heterogeneous catalysts. Enzymatic mineralization with an organic silicon precursor (biosilicification) is a promising and emerging approach for the generation of solid hybrid biocatalysts with exceptional stability under severe use conditions. Herein, we assessed the putative advantages of the biosilicification technology for developing an improved efficient and stable biocatalyst for sustainable biofuel production.ResultsA series of solid enzymatic catalysts denominated LOBE (low ordered biosilicified enzyme) were synthesized from Pseudomonas fluorescens lipase and tetraethyl orthosilicate. The microscopic structure and physicochemical properties characterization revealed that the enzyme formed aggregates that were contained in the heart of silicon-covered micelles, providing active sites with the ability to process different raw materials (commercial sunflower and soybean oils, Jatropha excisa oil, waste frying oil, acid oil from soybean soapstock, and pork fat) to produce first- and second-generation biodiesel. Ester content ranged from 81 to 93% wt depending on the raw material used for biodiesel synthesis.ConclusionsA heterogeneous enzymatic biocatalyst, LOBE4, for efficient biodiesel production was successfully developed in a single-step synthesis reaction using biosilicification technology. LOBE4 showed to be highly efficient in converting refined, non-edible and residual oils (with high water and free fatty acid contents) and ethanol into biodiesel. Thus, LOBE4 emerges as a promising tool to produce second-generation biofuels, with significant implications for establishing a circular economy and reducing the carbon footprint.

Highlights

  • Cumulative reported evidence has indicated that renewable feedstocks are a promising alternative source to fossil platforms for the production of fuels and chemicals

  • Synthesis and evaluation of biosilicified Pseudomonas fluorescens lipase Based on previous reports [31,32,33, 35], biosilicified Pseudomonas fluorescens lipases were synthesized with different theoretical amounts of enzyme (0, 1, 5, 10, 50, 100 and 150 mg) and the activity of the obtained biocatalysts to produce biodiesel was evaluated

  • Biodiesel production was measured under initial rate conditions (2 h in our system and the enzymatic reaction showing linear behavior) in order to compare the different fatty acid ethyl esters (FAEE) contents obtained

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Summary

Introduction

Cumulative reported evidence has indicated that renewable feedstocks are a promising alternative source to fossil platforms for the production of fuels and chemicals. The enzymatic reaction avoids the use of protecting groups and minimizes side reactions in mild operating conditions, reducing environmental constraints Such practical applications are hindered by the fragile nature of enzymes, such as low thermal stability (reduced half-live at temperatures over 70 °C [13]), narrow optimum pH for activity (pepsin: 2, acid phosphatase: 5.7, and alkaline phosphatase: 10.5 [14]), low tolerance to most organic solvents (chymotrypsin activity decreases at the threshold concentrations of 23% and 33% v/v of 1-propanol and 2-propanol, respectively [15]; polyphenol oxidase and trypsin activities are reduced when the solution has a concentration of 50% v/v of tetrahydrofuran, dioxane, acetone, or acetonitrile [16]), and salt concentration in the medium (increased ionic strength decreases the S. solfataricus carboxypeptidase activity [17]). They can simplify the processes of biocatalyst recovery and reuse, and purification of the products [25, 29, 30]

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