scholarly journals Toward scalable biocatalytic conversion of 5-hydroxymethylfurfural by galactose oxidase using coordinated reaction and enzyme engineering

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
William R. Birmingham ◽  
Asbjørn Toftgaard Pedersen ◽  
Mafalda Dias Gomes ◽  
Mathias Bøje Madsen ◽  
Michael Breuer ◽  
...  

Abstract5-Hydroxymethylfurfural (HMF) has emerged as a crucial bio-based chemical building block in the drive towards developing materials from renewable resources, due to its direct preparation from sugars and its readily diversifiable scaffold. A key obstacle in transitioning to bio-based plastic production lies in meeting the necessary industrial production efficiency, particularly in the cost-effective conversion of HMF to valuable intermediates. Toward addressing the challenge of developing scalable technology for oxidizing crude HMF to more valuable chemicals, here we report coordinated reaction and enzyme engineering to provide a galactose oxidase (GOase) variant with remarkably high activity toward HMF, improved O2 binding and excellent productivity (>1,000,000 TTN). The biocatalyst and reaction conditions presented here for GOase catalysed selective oxidation of HMF to 2,5-diformylfuran offers a productive blueprint for further development, giving hope for the creation of a biocatalytic route to scalable production of furan-based chemical building blocks from sustainable feedstocks.

2020 ◽  
Author(s):  
William Birmingham ◽  
Asbjørn Toftgaard Pedersen ◽  
Mafalda Dias Gomes ◽  
Mathias Bøje Madsen ◽  
Michael Breuer ◽  
...  

5-Hydroxymethylfurfural (HMF) has emerged as a crucial bio-based chemical building block in the drive towards developing materials from renewable resources, due to its direct preparation from sugars and its readily diversifiable scaffold. A key obstacle in transitioning to bio-based plastic production lies in meeting the necessary industrial production efficiency, particularly in the cost-effective conversion of HMF to valuable intermediates. To address the challenge of developing scalable technology for oxidizing crude HMF to more valuable chemicals, we have integrated process and enzyme engineering to provide a galactose oxidase (GOase) variant with remarkably high activity toward HMF, improved O2 binding and excellent productivity (>1,000,000 TTN). The process concept presented here for GOase catalysed selective oxidation of HMF to 2,5-diformylfuran offers a productive and efficient platform for further development, thereby laying the groundwork for a biocatalytic route to scalable production of furan-based chemical building blocks from sustainable feedstocks.<br>


2020 ◽  
Author(s):  
William Birmingham ◽  
Asbjørn Toftgaard Pedersen ◽  
Mafalda Dias Gomes ◽  
Mathias Bøje Madsen ◽  
Michael Breuer ◽  
...  

5-Hydroxymethylfurfural (HMF) has emerged as a crucial bio-based chemical building block in the drive towards developing materials from renewable resources, due to its direct preparation from sugars and its readily diversifiable scaffold. A key obstacle in transitioning to bio-based plastic production lies in meeting the necessary industrial production efficiency, particularly in the cost-effective conversion of HMF to valuable intermediates. To address the challenge of developing scalable technology for oxidizing crude HMF to more valuable chemicals, we have integrated process and enzyme engineering to provide a galactose oxidase (GOase) variant with remarkably high activity toward HMF, improved O2 binding and excellent productivity (>1,000,000 TTN). The process concept presented here for GOase catalysed selective oxidation of HMF to 2,5-diformylfuran offers a productive and efficient platform for further development, thereby laying the groundwork for a biocatalytic route to scalable production of furan-based chemical building blocks from sustainable feedstocks.<br>


2015 ◽  
Author(s):  
Marcin Cybulski ◽  
Adam Formela ◽  
Katarzyna Sidoryk ◽  
Olga Michalak ◽  
Anna Rosa ◽  
...  

One of the anthraquinone classes comprises compounds with a carbonyl group. These natural or synthetic anthraquinones find their application as building blocks in the synthesis of the compounds with a biological activity. Recently, 4-substituted anthra-9,10-quinone-1-carboxylic acids (2) have been used as key intermediates in the synthesis of patented compounds (3) with anticancer activity against multidrug resistant cell lines. Although 2,7-dihydro-3H-dibenz[de,h]cinnolin-3,7-diones (3) were successfully synthetized in a small laboratory scale, several problems were observed during the preparation of their acid intermediates (2) in a multi-gram scale. The known methods for the preparation of 2 are based on the oxidation of the methyl group in anthra-9,10-quinones (1). The most common are: the oxidation with the diluted nitric acid under high pressure in a sealed tube at the temperature of 195-220 oC, the oxidation in nitrobenzene by passing chlorine gas through the reaction mixture at the temperature of 160-170 oC or in a presence of the fuming sulphuric acid. The mentioned methods require aggressive reagents and specific reaction conditions including high pressure and temperature. Thus, there was a need to find a new efficient, cost-effective and reproducible synthetic method of preparation of 2. While searching literature it was found that the direct oxidation of alkylarenes mediated by the sodium periodate/lithium bromide combination produces benzyl acetates throughout benzyl bromides in the acetic acid, or benzylic acids in the diluted inorganic acid. Based on these results we examined a variety of reaction conditions with or without the bromine source and the oxidizing anion. As a result, a novel procedure for the preparation of highly pure 4-substituted anthra-9,10-quinone-1-carboxylic acids (HPLC > 99.5%) using oxidizing anion/ brominating reagent system was developed. It enabled 2 isolation by the simple filtration of the reaction mixture and was applied in the scale-up of 2,7-dihydro-3H-dibenz[de,h]cinnolin-3,7-dione derivatives.


Author(s):  
John Masani Nduko ◽  
Seiichi Taguchi

Polyhydroxyalkanoates (PHAs) are naturally occurring biopolymers produced by microorganisms. PHAs have become attractive research biomaterials in the past few decades owing to their extensive potential industrial applications, especially as sustainable alternatives to the fossil fuel feedstock-derived products such as plastics. Among the biopolymers are the bioplastics and oligomers produced from the fermentation of renewable plant biomass. Bioplastics are intracellularly accumulated by microorganisms as carbon and energy reserves. The bioplastics, however, can also be produced through a biochemistry process that combines fermentative secretory production of monomers and/or oligomers and chemical synthesis to generate a repertoire of biopolymers. PHAs are particularly biodegradable and biocompatible, making them a part of today’s commercial polymer industry. Their physicochemical properties that are similar to those of petrochemical-based plastics render them potential renewable plastic replacements. The design of efficient tractable processes using renewable biomass holds key to enhance their usage and adoption. In 2008, a lactate-polymerizing enzyme was developed to create new category of polyester, lactic acid (LA)–based polymer and related polymers. This review aims to introduce different strategies including metabolic and enzyme engineering to produce LA-based biopolymers and related oligomers that can act as precursors for catalytic synthesis of polylactic acid. As the cost of PHA production is prohibitive, the review emphasizes attempts to use the inexpensive plant biomass as substrates for LA-based polymer and oligomer production. Future prospects and challenges in LA-based polymer and oligomer production are also highlighted.


2015 ◽  
Author(s):  
Marcin Cybulski ◽  
Adam Formela ◽  
Katarzyna Sidoryk ◽  
Olga Michalak ◽  
Anna Rosa ◽  
...  

One of the anthraquinone classes comprises compounds with a carbonyl group. These natural or synthetic anthraquinones find their application as building blocks in the synthesis of the compounds with a biological activity. Recently, 4-substituted anthra-9,10-quinone-1-carboxylic acids (2) have been used as key intermediates in the synthesis of patented compounds (3) with anticancer activity against multidrug resistant cell lines. Although 2,7-dihydro-3H-dibenz[de,h]cinnolin-3,7-diones (3) were successfully synthetized in a small laboratory scale, several problems were observed during the preparation of their acid intermediates (2) in a multi-gram scale. The known methods for the preparation of 2 are based on the oxidation of the methyl group in anthra-9,10-quinones (1). The most common are: the oxidation with the diluted nitric acid under high pressure in a sealed tube at the temperature of 195-220 oC, the oxidation in nitrobenzene by passing chlorine gas through the reaction mixture at the temperature of 160-170 oC or in a presence of the fuming sulphuric acid. The mentioned methods require aggressive reagents and specific reaction conditions including high pressure and temperature. Thus, there was a need to find a new efficient, cost-effective and reproducible synthetic method of preparation of 2. While searching literature it was found that the direct oxidation of alkylarenes mediated by the sodium periodate/lithium bromide combination produces benzyl acetates throughout benzyl bromides in the acetic acid, or benzylic acids in the diluted inorganic acid. Based on these results we examined a variety of reaction conditions with or without the bromine source and the oxidizing anion. As a result, a novel procedure for the preparation of highly pure 4-substituted anthra-9,10-quinone-1-carboxylic acids (HPLC > 99.5%) using oxidizing anion/ brominating reagent system was developed. It enabled 2 isolation by the simple filtration of the reaction mixture and was applied in the scale-up of 2,7-dihydro-3H-dibenz[de,h]cinnolin-3,7-dione derivatives.


Author(s):  
Hui Qiao ◽  
Mingqi He ◽  
Qiushi Wang ◽  
Shuaishuai Han ◽  
Haiqian Zhao ◽  
...  

Abstract Traditional electro-Fenton systems must continuously supply oxygen to the cathode, which leads to extensive volatilisation of benzene in solutions. In this study, we adopted a floating cathode electro-Fenton system without bubbling oxygen into the solution to treat benzene-containing wastewater. The effects of the floating cathode position and main reaction parameters on benzene degradation were analysed, and the degradation cost was estimated. The results indicated that the electro-Fenton system with floating cathode can effectively degrade benzene in solutions. For the cathode, the complete utilisation of air and oxygen released from the anode is crucial. The benzene degradation rate increased with an increase in benzene concentrations. Additionally, pH mainly affected the existing ionic state of iron and production ratio of active substances. The current intensity significantly influenced the reaction activity. Using the floating cathode electro-Fenton method, the benzene removal ratio in the solution can reach 74.80% after 60 min under the optimum reaction conditions. For floating cathode electro-Fenton system, the cost of treating benzene-containing sewage per cubic metre was $1.2187, which is significantly lower than that for traditional electro-Fenton technology ($1.4000). Hence, the floating cathode electro-Fenton system is an economical and efficient method for benzene degradation in solutions.


Author(s):  
James F. Mancuso

IBM PC compatible computers are widely used in microscopy for applications ranging from control to image acquisition and analysis. The choice of IBM-PC based systems over competing computer platforms can be based on technical merit alone or on a number of factors relating to economics, availability of peripherals, management dictum, or simple personal preference.IBM-PC got a strong “head start” by first dominating clerical, document processing and financial applications. The use of these computers spilled into the laboratory where the DOS based IBM-PC replaced mini-computers. Compared to minicomputer, the PC provided a more for cost-effective platform for applications in numerical analysis, engineering and design, instrument control, image acquisition and image processing. In addition, the sitewide use of a common PC platform could reduce the cost of training and support services relative to cases where many different computer platforms were used. This could be especially true for the microscopists who must use computers in both the laboratory and the office.


Phlebologie ◽  
2007 ◽  
Vol 36 (06) ◽  
pp. 309-312 ◽  
Author(s):  
T. Schulz ◽  
M. Jünger ◽  
M. Hahn

Summary Objective: The goal of the study was to assess the effectiveness and patient tolerability of single-session, sonographically guided, transcatheter foam sclerotherapy and to evaluate its economic impact. Patients, methods: We treated 20 patients with a total of 22 varicoses of the great saphenous vein (GSV) in Hach stage III-IV, clinical stage C2-C5 and a mean GSV diameter of 9 mm (range: 7 to 13 mm). We used 10 ml 3% Aethoxysklerol®. Additional varicoses of the auxiliary veins of the GSV were sclerosed immediately afterwards. Results: The occlusion rate in the treated GSVs was 100% one week after therapy as demonstrated with duplex sonography. The cost of the procedure was 207.91 E including follow-up visit, with an average loss of working time of 0.6 days. After one year one patient showed clinical signs of recurrent varicosis in the GSV; duplex sonography showed reflux in the region of the saphenofemoral junction in a total of seven patients (32% of the treated GSVs). Conclusion: Transcatheter foam sclerotherapy of the GSV is a cost-effective, safe method of treating varicoses of GSV and broadens the spectrum of therapeutic options. Relapses can be re-treated inexpensively with sclerotherapy.


2019 ◽  
Vol 2 (4) ◽  
pp. 260-266
Author(s):  
Haru Purnomo Ipung ◽  
Amin Soetomo

This research proposed a model to assist the design of the associated data architecture and data analytic to support talent forecast in the current accelerating changes in economy, industry and business change due to the accelerating pace of technological change. The emerging and re-emerging economy model were available, such as Industrial revolution 4.0, platform economy, sharing economy and token economy. Those were driven by new business model and technology innovation. An increase capability of technology to automate more jobs will cause a shift in talent pool and workforce. New business model emerge as the availabilityand the cost effective emerging technology, and as a result of emerging or re-emerging economic models. Both, new business model and technology innovation, create new jobs and works that have not been existed decades ago. The future workers will be faced by jobs that may not exist today. A dynamics model of inter-correlation of economy, industry, business model and talent forecast were proposed. A collection of literature review were conducted to initially validate the model.


The choice of cost-effective method of anticorrosive protection of steel structures is an urgent and time consuming task, considering the significant number of protection ways, differing from each other in the complex of technological, physical, chemical and economic characteristics. To reduce the complexity of solving this problem, the author proposes a computational tool that can be considered as a subsystem of computer-aided design and used at the stage of variant and detailed design of steel structures. As a criterion of the effectiveness of the anti-corrosion protection method, the cost of the protective coating during the service life is accepted. The analysis of existing methods of steel protection against corrosion is performed, the possibility of their use for the protection of the most common steel structures is established, as well as the estimated period of effective operation of the coating. The developed computational tool makes it possible to choose the best method of protection of steel structures against corrosion, taking into account the operating conditions of the protected structure and the possibility of using a protective coating.


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