Synergistic voltaglue adhesive mechanisms with alternating electric fields
Voltage-activated adhesion is a relatively new discovery that relies on direct currents for initiation of cross-linking. Previous investigations have found that direct currents are linearly correlated to the migration rates of electrocuring, but this is limited by high voltages exceeding 100 V with...
| Main Authors: | , , , , , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2020
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| Online Access: | https://hdl.handle.net/10356/142878 |
| _version_ | 1826118481430446080 |
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| author | Singh, Manisha Yin, Cheong See Page, Samuel J. Liu, Yuqing Wicaksono, Gautama Pujar, Rajashekhar Choudhary, Shyam Kumar Kulkarni, Giridhar U. Chen, Jun Hanna, John V. Webster, Richard David Steele, Terry W. J. |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering Singh, Manisha Yin, Cheong See Page, Samuel J. Liu, Yuqing Wicaksono, Gautama Pujar, Rajashekhar Choudhary, Shyam Kumar Kulkarni, Giridhar U. Chen, Jun Hanna, John V. Webster, Richard David Steele, Terry W. J. |
| author_sort | Singh, Manisha |
| collection | NTU |
| description | Voltage-activated adhesion is a relatively new discovery that relies on direct currents for initiation of cross-linking. Previous investigations have found that direct currents are linearly correlated to the migration rates of electrocuring, but this is limited by high voltages exceeding 100 V with instances of incomplete curing of voltage-activated adhesives on semiconducting substrates. Practical applications of electrocuring would benefit from lower voltages to mitigate high-voltage risks, especially with regard to potential medical applications. Alternative electrocuring strategies based on alternating current (AC), electrolyte ionic radius, and temperature are evaluated herein. Square-waveform AC electric field is hypothesized to initiate a two-sided curing progression of voltage-activated adhesive (PAMAM-g-diazirine, aka Voltaglue), where initiation occurs at the cathode terminal. Structure–activity relationships of Voltaglue as a function of AC frequency at currents of 1–3 mA are evaluated against direct currents, migration rate, storage modulus, and lap-shear adhesion on ex vivo tissue mimics. Numerous improvements in electrocuring are observed with AC stimulation vs direct current, including a 35% decrease in maximum voltage, 180% improvement in kinetic rates, and 100% increase in lap-shear adhesion at 2 mA. Li+ ion electrolytes and curing at 4 °C shifts curing kinetics by +104% and −22% respectively, with respect to the control ion (Na+ ion at 24 °C), suggesting that electrolyte migration is the rate-limiting step. Li+ ion electrolytes and curing at 50 °C improve storage modulus by 110% and 470%, respectively. Further evaluations of electrocured matrices with 19F NMR, solid-state NMR, and infrared spectroscopy provide insights into the probable cross-linking mechanisms. |
| first_indexed | 2024-10-01T04:44:07Z |
| format | Journal Article |
| id | ntu-10356/142878 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T04:44:07Z |
| publishDate | 2020 |
| record_format | dspace |
| spelling | ntu-10356/1428782023-07-14T15:59:53Z Synergistic voltaglue adhesive mechanisms with alternating electric fields Singh, Manisha Yin, Cheong See Page, Samuel J. Liu, Yuqing Wicaksono, Gautama Pujar, Rajashekhar Choudhary, Shyam Kumar Kulkarni, Giridhar U. Chen, Jun Hanna, John V. Webster, Richard David Steele, Terry W. J. School of Materials Science and Engineering School of Physical and Mathematical Sciences Interdisciplinary Graduate School (IGS) NTU-Northwestern Institute for Nanomedicine Engineering::Materials Voltaglue Adhesion Voltage-activated adhesion is a relatively new discovery that relies on direct currents for initiation of cross-linking. Previous investigations have found that direct currents are linearly correlated to the migration rates of electrocuring, but this is limited by high voltages exceeding 100 V with instances of incomplete curing of voltage-activated adhesives on semiconducting substrates. Practical applications of electrocuring would benefit from lower voltages to mitigate high-voltage risks, especially with regard to potential medical applications. Alternative electrocuring strategies based on alternating current (AC), electrolyte ionic radius, and temperature are evaluated herein. Square-waveform AC electric field is hypothesized to initiate a two-sided curing progression of voltage-activated adhesive (PAMAM-g-diazirine, aka Voltaglue), where initiation occurs at the cathode terminal. Structure–activity relationships of Voltaglue as a function of AC frequency at currents of 1–3 mA are evaluated against direct currents, migration rate, storage modulus, and lap-shear adhesion on ex vivo tissue mimics. Numerous improvements in electrocuring are observed with AC stimulation vs direct current, including a 35% decrease in maximum voltage, 180% improvement in kinetic rates, and 100% increase in lap-shear adhesion at 2 mA. Li+ ion electrolytes and curing at 4 °C shifts curing kinetics by +104% and −22% respectively, with respect to the control ion (Na+ ion at 24 °C), suggesting that electrolyte migration is the rate-limiting step. Li+ ion electrolytes and curing at 50 °C improve storage modulus by 110% and 470%, respectively. Further evaluations of electrocured matrices with 19F NMR, solid-state NMR, and infrared spectroscopy provide insights into the probable cross-linking mechanisms. ASTAR (Agency for Sci., Tech. and Research, S’pore) MOE (Min. of Education, S’pore) Accepted version 2020-07-06T08:45:29Z 2020-07-06T08:45:29Z 2020 Journal Article Singh, M., Yin, C. S., Page, S. J., Liu, Y., Wicaksono, G., Pujar, R., . . . Steele, T. W. J. (2020). Synergistic voltaglue adhesive mechanisms with alternating electric fields. Chemistry of Materials, 32(6), 2440-2449. doi:10.1021/acs.chemmater.9b04962 0897-4756 https://hdl.handle.net/10356/142878 10.1021/acs.chemmater.9b04962 6 32 2440 2449 en Chemistry of Materials This document is the Accepted Manuscript version of a Published Work that appeared in final form in Chemistry of Materials, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.chemmater.9b04962 application/pdf |
| spellingShingle | Engineering::Materials Voltaglue Adhesion Singh, Manisha Yin, Cheong See Page, Samuel J. Liu, Yuqing Wicaksono, Gautama Pujar, Rajashekhar Choudhary, Shyam Kumar Kulkarni, Giridhar U. Chen, Jun Hanna, John V. Webster, Richard David Steele, Terry W. J. Synergistic voltaglue adhesive mechanisms with alternating electric fields |
| title | Synergistic voltaglue adhesive mechanisms with alternating electric fields |
| title_full | Synergistic voltaglue adhesive mechanisms with alternating electric fields |
| title_fullStr | Synergistic voltaglue adhesive mechanisms with alternating electric fields |
| title_full_unstemmed | Synergistic voltaglue adhesive mechanisms with alternating electric fields |
| title_short | Synergistic voltaglue adhesive mechanisms with alternating electric fields |
| title_sort | synergistic voltaglue adhesive mechanisms with alternating electric fields |
| topic | Engineering::Materials Voltaglue Adhesion |
| url | https://hdl.handle.net/10356/142878 |
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