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Enzyme Printed Fabrics: Bio‐functionalisation of Synthetic Textiles by Digital Inkjet Printing
University of Borås, Faculty of Textiles, Engineering and Business.ORCID iD: 0000-0003-2412-9004
2022 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis explores the possibilities of printing enzymes using resource-efficient technologies to promote the binding of other proteins and biomaterials on synthetic textiles. This strategy can be used to develop advanced textiles for applications, for example, in antimicrobial, drug delivery and biosensing. Digital inkjet printing was combined with enzyme technology to ensure minimum use of water, chemicals and energy in textile manufacturing processes.  

Inks containing two enzymes, lysozyme and tyrosinase, were formulated by adjusting several rheological and ionic properties. The activity of these enzymes was optimised while being printed through two different industrial grade piezoelectric printheads. The theoretical printability of the prepared inks was calculated. The effect of printhead temperature and number of printing passes on the activity was evaluated. Polyester (polyethylene terephthalate) and polyamide-6,6 were pre-treated through several techniques to understand their effect on enzyme adhesion, binding and activity retention. Tyrosinase was used to bind lysozyme on plasma activated polyamide-6,6 surface. The effects of printing these two enzymes in various sequences, i.e. tyrosinase before lysozyme and vice-versa on binding stability and activity, were studied. Influence of the printing process on enzyme kinetics was evaluated. Ability to store and reuse printed fabrics was also studied.  

Lysozyme and tyrosinase containing inks showed activity retention of 85% and 60%, respectively. Activity of lysozyme containing ink was optimum at 10–15 mPa.s when glycerol was used as a viscosity modifier. However, the optimum viscosity for tyrosinase containing ink was at 6–9 mPa.s, and carboxymethyl cellulose was found to be the most favourable modifier. For both inks, a surfactant amount below the critical micelle concentration was considered to be the most effective for printing. Among the studied fabric pre-treatment methods (alkaline, cutinase and plasma), it was found that the activity and stability of the enzyme were dependent on the nature of the pretreatment processes, which can be beneficial for different application areas, e.g. drug release and bio-sensing. Upon printing both inks on a plasma treated polyamide-6,6, tyrosinase was able to catalyse lysozyme protein to bind it on fabric. A maximum of 68% lytic activity was retained by lysozyme when it was printed after tyrosinase. This fabric showed inhibition of bacterial growth and retained almost half of its initial activity when cold stored for a month. 

Place, publisher, year, edition, pages
Borås: Högskolan i Borås, 2022.
Series
Skrifter från Högskolan i Borås, ISSN 0280-381X ; 135
Keywords [en]
Digital printing, inkjet, enzyme, printhead, rheology, immobilisation, piezoelectric, drop-on-demand, resource-efficient textiles, biological ink, lysozyme, tyrosinase, polyphenol oxidase, polyethylene terephthalate, polyester, polyamide-6, 6, nylon, surface modification, plasma, antimicrobial, antibacterial
National Category
Textile, Rubber and Polymeric Materials
Research subject
Textiles and Fashion (General)
Identifiers
URN: urn:nbn:se:hb:diva-29001ISBN: 978-91-89271-87-6 (print)ISBN: 978-91-89271-88-3 (electronic)OAI: oai:DiVA.org:hb-29001DiVA, id: diva2:1715338
Public defence
2023-02-28, M404, Allégatan 1, Borås, 09:00 (English)
Opponent
Supervisors
Available from: 2023-01-31 Created: 2022-12-01 Last updated: 2023-03-06Bibliographically approved
List of papers
1. Inkjetting of Enzymes: Chapter 12
Open this publication in new window or tab >>Inkjetting of Enzymes: Chapter 12
2019 (English)In: Advance in Textile Biotechnology 2nd edition / [ed] Artur Cavaco-Paulo, Vincent Nierstrasz, Qiang Wang, Elsevier, 2019Chapter in book (Refereed)
Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
inkjetting of enzymes
National Category
Textile, Rubber and Polymeric Materials
Research subject
Textiles and Fashion (General)
Identifiers
urn:nbn:se:hb:diva-21597 (URN)978-0-08-102632-8 (ISBN)978-0-08-102770-7 (ISBN)
Available from: 2019-08-13 Created: 2019-08-13 Last updated: 2023-01-11Bibliographically approved
2. Effects of ink characteristics and piezo-electric inkjetting parameters on lysozyme activity
Open this publication in new window or tab >>Effects of ink characteristics and piezo-electric inkjetting parameters on lysozyme activity
2019 (English)In: Scientific Reports, E-ISSN 2045-2322, Vol. 9, no 18252Article in journal (Refereed) Published
Abstract [en]

Inkjet printing of enzymes can facilitate many novel applications where a small amount of materials need to be deposited in a precise and flexible manner. However, maintaining the satisfactory activity of inkjet printed enzyme is a challenging task due to the requirements of ink rheology and printhead parameters. Thus to find optimum inkjetting conditions we studied the effects of several ink formulation and jetting parameters on lysozyme activity using a piezoelectric printhead. Within linear activity range of protein concentrations ink containing 50 µg/mL lysozyme showed a satisfactory activity retention of 85%. An acceptable activity of jetted ink was found at pH 6.2 and ionic strength of 0.06 molar. Glycerol was found to be an effective viscosity modifier (10–15 mPa.s), humectant and protein structure stabilizer for the prepared ink. A non-ionic surfactant when used just below critical micelle concentration was found to be favourable for the jetted inks. An increase in activity retention was observed for inks jetted after 24 hours of room temperature incubation. However, no additional activity was seen for inkjetting above the room temperature. Findings of this study would be useful for formulating other protein-based inks and setting their inkjet printing parameters without highly compromising the functionality.

Keywords
biological ink, lysozyme, inkjet printing, piezoelectric
National Category
Textile, Rubber and Polymeric Materials
Research subject
Textiles and Fashion (General)
Identifiers
urn:nbn:se:hb:diva-22771 (URN)10.1038/s41598-019-54723-9 (DOI)000501310300001 ()2-s2.0-85075948827 (Scopus ID)
Available from: 2020-02-03 Created: 2020-02-03 Last updated: 2023-01-11Bibliographically approved
3. Effective Pretreatment Routes of Polyethylene Terephthalate Fabric for Digital Inkjet Printing of Enzyme
Open this publication in new window or tab >>Effective Pretreatment Routes of Polyethylene Terephthalate Fabric for Digital Inkjet Printing of Enzyme
2021 (English)In: Materials Science & Engineering: B. Solid-state Materials for Advanced Technology, ISSN 0921-5107, E-ISSN 1873-4944Article in journal (Refereed) Published
Abstract [en]

Enzymes immobilized on synthetic polyethylene terephthalate (PET) textile surface by resource‐efficient inkjet printing technology can promote developments for various novel applications. Synthetic fabrics often require adequate pretreatments to facilitate such printing process. This work discusses PET–woven fabric pretreatment routes to improve wettability by alkaline, enzymatic, and plasma processes for effective printing of lysozyme using an industrial piezoelectric printhead. Results indicate that all pretreated samples contain a similar amount of enzymes upon printing. Plasma treated fabrics show relatively more hydrophilic surface characteristics, better protein binding stability, and lower retained activity. Alkali and cutinase‐treated samples possess relatively higher activity due to the greater amount of enzyme desorption to substrate solution. Depending on respective enzyme‐binding stability, a combination of a well-pretreated surface and inkjet as preferential placement technology, the approach of this study can be used as a facile enzyme immobilization method for suitable applications, for example, controlled‐release and bio‐sensing.

Keywords
biomaterials inkjet printing, lysozyme, polyethylene terephthalate (PET), pretreatment routes
National Category
Textile, Rubber and Polymeric Materials Other Biological Topics Polymer Chemistry Physical Chemistry
Research subject
Textiles and Fashion (General)
Identifiers
urn:nbn:se:hb:diva-24895 (URN)10.1002/admi.202001882 (DOI)000611092100001 ()2-s2.0-85099740075 (Scopus ID)
Note

Correction to article published 23 November 2021: https://doi.org/10.1002/admi.202101935

Available from: 2021-01-28 Created: 2021-01-28 Last updated: 2023-01-11Bibliographically approved
4. Piezoelectric inkjet printing of tyrosinase (polyphenol oxidase) enzyme on atmospheric plasma treated polyamide fabric
Open this publication in new window or tab >>Piezoelectric inkjet printing of tyrosinase (polyphenol oxidase) enzyme on atmospheric plasma treated polyamide fabric
2022 (English)In: Scientific Reports, E-ISSN 2045-2322, Vol. 12, no 1, article id 6828Article in journal (Refereed) Published
Abstract [en]

Tyrosinase enzyme was digitally printed on plasma pretreated polyamide-6,6 fabric using several sustainable technologies. Ink containing carboxymethyl cellulose was found to be the most suitable viscosity modifier for this enzyme. Before and after being deposited on the fabric surface, the printed inks retained enzyme activity of 69% and 60%, respectively, compared to activity prior printing process. A good number of the printed enzyme was found to be strongly adsorbed on the fabric surface even after several rinsing cycles due to surface activation by plasma treatment. Rinsed out fabrics retained a maximum activity of 34% resulting from the well-adsorbed enzymes. The activity of tyrosinase on printed fabrics was more stable than ink solution for at least 60 days. Effects of pH, temperature and enzyme kinetics on ink solution and printed fabrics were assessed. Tyrosinase printed synthetic fabrics can be utilized for a range of applications from biosensing and wastewater treatment to cultural heritage works.

Keywords
covalent immobilization, biosensor, adsorption
National Category
Textile, Rubber and Polymeric Materials
Research subject
Textiles and Fashion (General)
Identifiers
urn:nbn:se:hb:diva-27875 (URN)10.1038/s41598-022-10852-2 (DOI)000787775900070 ()2-s2.0-85128933473 (Scopus ID)
Available from: 2022-05-16 Created: 2022-05-16 Last updated: 2023-01-11Bibliographically approved
5. Sequential Inkjet Printing of Lysozyme and Tyrosinase on Polyamide Fabric: Sustainable Enzyme Binding on Textile Surface
Open this publication in new window or tab >>Sequential Inkjet Printing of Lysozyme and Tyrosinase on Polyamide Fabric: Sustainable Enzyme Binding on Textile Surface
2022 (English)In: Advanced Materials Interfaces, ISSN 2196-7350, Vol. 9, no 22, article id 2200723Article in journal (Refereed) Published
Abstract [en]

An ink containing tyrosinase catalyzes the tyrosine residues on lysozyme protein to bind it on a plasma-treated polyamide-6,6 (PA) fabric. Inkjet printing enables controlled and sequential deposition of two enzymes on PA which is necessary for proper binding. The effect of different printing sequences on crosslinking stability and enzymatic activity is presented. The lysozyme bound on the fabric shows satisfactory antimicrobial activity. The printed fabric retains about 68% of the ink activity when tyrosinase is printed before lysozyme. Further, this fabric retains about 24% of the initial activity up to four reuses. The fabric shows acceptable inhibition of bacterial growth and retains almost half of its initial activity when cold stored for a month. This work shows the potential of protein binding on textile surface using various means of sustainable technologies, namely enzyme, inkjet, and plasma. 

Place, publisher, year, edition, pages
John Wiley & Sons, 2022
National Category
Materials Chemistry Physical Chemistry
Identifiers
urn:nbn:se:hb:diva-28241 (URN)10.1002/admi.202200723 (DOI)000819562000001 ()2-s2.0-85133156944 (Scopus ID)
Note

This work was financially supported by the research school at the University of Borås. The authors are thankful for the support from TEKO (Sveriges Textil- och Modeföretag) and Sparbanksstiftelsen Sjuhärad.

Available from: 2022-07-08 Created: 2022-07-08 Last updated: 2023-02-07Bibliographically approved

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