Periodic Reporting for period 3 - GREENSENSE (Sustainable, Wireless, Autonomous Nanocellulose-based Quantitative DoA Biosensing Platform)
Reporting period: 2021-01-01 to 2022-03-31
Printed Electronics is, together with additive manufacturing, one of the fastest growing technological field attracting interest in a variety of industries as diverse as consumer goods, healthcare, aerospace, media and transport. Paper and plastics are widely used as substrates in the development of flexible electronic devices. On the contrary to those based on more conventional plastic substrates, paper-based electronics can be expected to have a positive impact to the environment by reducing "electronic trash" and to the European economy by providing new opportunities to the pulp/paper manufacturing industry. Unfortunately, the surface properties of conventional paper are not suitable for printed electronics and, typically plastic coatings, based on fossil-oil polymers or inorganic additives are needed. Nevertheless, this approach is disfavored by limitations in fossil-oil reserves and lack of biodegradation of the coated paper, which create environmental and economic concerns. From a sustainablility point of view, this has augmented the interest in alternative biodegradable biopolymer films and coatings with similar properties. Among the different alternatives, nanocellulose NC-based films and coating presenting qualities such as strength, transparency, low porosity and low surface roughness are a promising potential alternative. On the other hand, the push for distributed diagnostic and on-site quantitative/semi-quantitative testing is driving the growth of the market of the point of care (PoC) diagnostic. In GREENSENSE, we merge PoC diagnostic and printed electronics in the form of a fully integrated biosensing platform. The biosensing platform relies on newly developed printed biosensors, NC-based printed electronic components and a single microchip to offer energy autonomy, wireless communication and user-friendly interface. The proposed biosensing platform is expected to open new routes for the development of several diagnostic applications based on inexpensive and sustainable materials. The project has fulfilled the following specific objectives:
•Cost-efficient production of nanocellulose at pilot scale.
•Pilot scale fabrication of NC-based films (NC-coated paper) and NC free-standing films.
•Formulation of different NC-based functional inks at pilot scale: conductive nanoinks, electrochemical inks and electrolytes.
• Production of NC-based printed electronic components that provide functionalities to the biosensing platform: display, energy storage components (supercapacitor and primary battery) and a NFC RF component.
• Development of biosensors to detect morphine.
•Fabrication of a monolithically integrated microchip with all required electronic functionalities.
•Fabrication of the components using sheet to sheet semi-automatic screen-printing processes.
•Integration of all components to produce the final biosensing platforms.
•Performance assessment.
•Sustainability assessment.
•Cost-benefit analysis.
•Cost-efficient production of nanocellulose at pilot scale.
•Pilot scale fabrication of NC-based films (NC-coated paper) and NC free-standing films.
•Formulation of different NC-based functional inks at pilot scale: conductive nanoinks, electrochemical inks and electrolytes.
• Production of NC-based printed electronic components that provide functionalities to the biosensing platform: display, energy storage components (supercapacitor and primary battery) and a NFC RF component.
• Development of biosensors to detect morphine.
•Fabrication of a monolithically integrated microchip with all required electronic functionalities.
•Fabrication of the components using sheet to sheet semi-automatic screen-printing processes.
•Integration of all components to produce the final biosensing platforms.
•Performance assessment.
•Sustainability assessment.
•Cost-benefit analysis.
In GREENSENSE project following targets have been achieved:
- Different types of nanocellulose have been fabricated, functionalized and characterized: carboxymethylated CNF, cationized CNF, aminosilylated CNF/CNC, sulfonated CNC and acetylated CNC, first at lab scale, and, finally, at pilot (potentially up to tons per year).
- Free-standing NC films and NC-coated paper boards have been produced and characterized (physical, optical, thermal, mechanical, etc.) at large scale.
- Different types of NC-based inks have been produced at large scale (up to 50 kg/batch): conductive (with conductivity up to 107 S/m), electrochemical, electrolytes for electrochromic display and energy storage applications. They have been characterized accordingly to international standards for printed electronics (IEC 62899).
- Different types of NC-based printed electronic components have been fabricated at large scale (more than 1.500):
o NFC Antennas with a reading distance up to 6 cm and a Q factor up to 14.
o Supercapacitors with capacity >100 mF/cm2 at 2V, energy density > 400 mJ/cm2 and power density > 150mW/cm2, ESR= <2 Ohm, < 3 µA of leakage current.
o Primary batteries with a capacity 1.8 – 2.1 mAh, 4.0 – 4.2V an impedance 100 - 250 Ohms and a calculated half capacity lifetime of 27 month.
o Different architecture electrochromic Displays for heterogenous integration, with a color contrast of ΔE~25-30. Furthermore, displays with different colour shades as well as displays updated via passive matrix addressing protocols have also been demonstrated.
- Development of biosensors for drugs detection with a redox active ink and a hydrogel.
Moreover, a microchip with several interfaces (for power management, sensor, RFID with harvesting possibilities to charge connected energy storages and for displays) has been developed.
Functional biosensing platforms with different functionalities and components (namely GEN2 and GEN3) have been manufactured at large scale (up to 75 units) by semi-automated processes (screen-printing, pick and place and BioDOT processes) on substrates of ca. 300 x 350 mm (8 platforms/sheet). An application has been also developed for the operation of the platforms using a Smartphone.
Mechanical, adhesion and ageing tests were performed for some of the printed electronic components and the final biosensing platforms according to standards (IEC 62951). Assessment of the analytical performance of the developed biosensors including linearity, precision, specificity, Limit of Detection (LoD), Limit of Quantification (LoQ), measuring range and thermal stability has been done.
A LCA has been done with data collection from all partners. For the sustainability and recyclability assessment, the need for recycling of printed electronics at their End-of-Life (EoL) has been explored. Additionally, the possible applications for paper-based electronics have been explored and the competitiveness of each application in-terms of sustainability has been assessed with the MPAS method.
The business plans for the materials, components and processes development in each Work Package have been done. Discussions of a GREENSENSE follow-up agreement to keep the critical mass of the project and attempt market exploitation of the results has been performed.
Dissemination has been achieved by the publication of several articles to relevant journals and the attendance to several conferences and fares. Moreover, a patent is currently under progress.
- Different types of nanocellulose have been fabricated, functionalized and characterized: carboxymethylated CNF, cationized CNF, aminosilylated CNF/CNC, sulfonated CNC and acetylated CNC, first at lab scale, and, finally, at pilot (potentially up to tons per year).
- Free-standing NC films and NC-coated paper boards have been produced and characterized (physical, optical, thermal, mechanical, etc.) at large scale.
- Different types of NC-based inks have been produced at large scale (up to 50 kg/batch): conductive (with conductivity up to 107 S/m), electrochemical, electrolytes for electrochromic display and energy storage applications. They have been characterized accordingly to international standards for printed electronics (IEC 62899).
- Different types of NC-based printed electronic components have been fabricated at large scale (more than 1.500):
o NFC Antennas with a reading distance up to 6 cm and a Q factor up to 14.
o Supercapacitors with capacity >100 mF/cm2 at 2V, energy density > 400 mJ/cm2 and power density > 150mW/cm2, ESR= <2 Ohm, < 3 µA of leakage current.
o Primary batteries with a capacity 1.8 – 2.1 mAh, 4.0 – 4.2V an impedance 100 - 250 Ohms and a calculated half capacity lifetime of 27 month.
o Different architecture electrochromic Displays for heterogenous integration, with a color contrast of ΔE~25-30. Furthermore, displays with different colour shades as well as displays updated via passive matrix addressing protocols have also been demonstrated.
- Development of biosensors for drugs detection with a redox active ink and a hydrogel.
Moreover, a microchip with several interfaces (for power management, sensor, RFID with harvesting possibilities to charge connected energy storages and for displays) has been developed.
Functional biosensing platforms with different functionalities and components (namely GEN2 and GEN3) have been manufactured at large scale (up to 75 units) by semi-automated processes (screen-printing, pick and place and BioDOT processes) on substrates of ca. 300 x 350 mm (8 platforms/sheet). An application has been also developed for the operation of the platforms using a Smartphone.
Mechanical, adhesion and ageing tests were performed for some of the printed electronic components and the final biosensing platforms according to standards (IEC 62951). Assessment of the analytical performance of the developed biosensors including linearity, precision, specificity, Limit of Detection (LoD), Limit of Quantification (LoQ), measuring range and thermal stability has been done.
A LCA has been done with data collection from all partners. For the sustainability and recyclability assessment, the need for recycling of printed electronics at their End-of-Life (EoL) has been explored. Additionally, the possible applications for paper-based electronics have been explored and the competitiveness of each application in-terms of sustainability has been assessed with the MPAS method.
The business plans for the materials, components and processes development in each Work Package have been done. Discussions of a GREENSENSE follow-up agreement to keep the critical mass of the project and attempt market exploitation of the results has been performed.
Dissemination has been achieved by the publication of several articles to relevant journals and the attendance to several conferences and fares. Moreover, a patent is currently under progress.
Main results achieved beyond the state of the art are:
Production at pilot scale of different types of nanocellulose (with carboxy, amino, sulfonic, acetyl, negative or positive groups), NC-free standing films and NC-coated papers, NC-based inks (conductive, electrochemical, electrolyte and dielectric).
Application of all these up-scaled materials for the fabrication of the different printed electronic components: NFC antennas, supercaps, batteries, displays and biosensors.
Development of a microchip with ARM Cortex M0 as core unit and diverse memory storages with several interfaces (power management, sensor, RFID with harvesting possibilities and for displays).
Development of functional biosensing platforms (two architectures) with the new developed microchip on the NC-coated paperboard via the use of semi-automated processes (e.g. flip chip technology).
GREENSENSE platforms are stepping stones in the development of future quantitative multi-parameters single use sustainable PoC devices on paper.
Production at pilot scale of different types of nanocellulose (with carboxy, amino, sulfonic, acetyl, negative or positive groups), NC-free standing films and NC-coated papers, NC-based inks (conductive, electrochemical, electrolyte and dielectric).
Application of all these up-scaled materials for the fabrication of the different printed electronic components: NFC antennas, supercaps, batteries, displays and biosensors.
Development of a microchip with ARM Cortex M0 as core unit and diverse memory storages with several interfaces (power management, sensor, RFID with harvesting possibilities and for displays).
Development of functional biosensing platforms (two architectures) with the new developed microchip on the NC-coated paperboard via the use of semi-automated processes (e.g. flip chip technology).
GREENSENSE platforms are stepping stones in the development of future quantitative multi-parameters single use sustainable PoC devices on paper.