Bioinspired ultra-stretchable and anti-freezing conductive hydrogel fibers with ordered and reversible polymer chain alignment

Abstract

High-performance stretchable conductive fibers are desired for the development of stretchable electronic devices. Here we show a simple spinning method to prepare conductive hydrogel fibers with ordered polymer chain alignment that mimics the hierarchically organized structure of spider silk. The as-prepared sodium polyacrylate hydrogel fiber is further coated with a thin layer of polymethyl acrylate to form a core–shell water-resistant MAPAH fiber. Owing to the coexistence and reversible transformation of crystalline and amorphous domains in the fibers, MAPAH fibers exhibit high tensile strength, large stretchability and fast resilience from large strain. MAPAH fiber can serve as a highly stretchable wire with a conductive hydrogel core and an insulating cover. The stretchability and conductivity of the MAPAH fiber are retained at −35 °C, indicating its anti-freezing property. As a prime example of stretchable conductive fibers, MAPAH fibers will shed light on the design of next generation textile-based stretchable electronic devices.

In Situ Grown Silver–Polymer Framework with Coordination Complexes for Functional Artificial Tissues

“…6), implying the presence of a strongly entangled and densely cross-linked PANSion network. These results are in accordance with other reports 25 and our AFM-SMFS data, affirming that [Ag(−C≡N)x] + complexes, as cross-linkers, cause structural changes to the PANSion network when compared to its antetype of PAN.…”

“…Furthermore, the gelation evolution for ϕ = 2.0 was manifested by the competing effect between the storage modulus (G′) and loss modulus (G″), where G′ became dominant once the gelation occurred (Figure S8, Supporting Information), implying the presence of a strongly entangled and densely cross-linked PANSion network. These results are in accordance with other reports [15] and our AFM-SMFS data, affirming that [Ag(N≡C−) x ] + complexes, as cross-linkers, bring structural changes to the PANSion network when compared to its antetype of PAN.…”

“…[13] Concomitantly, the molecular chain alignment was monitored to be strain-dependent (Figure 3f), where a larger strain produced a higher alignment degree, corresponding to a large value of Herman's orientation factor (f (H) ). [15] For instance, an f (H) value of 0.3427 for 𝜖 = 1, while an f (H) value 0.6331 for 𝜖 = 5, seems to substantiate our initial hypothesis. [13] The non-overlapping of f (H) between the first and second stretchingreleasing cycles might have arisen from the strain hysteresis or the reformation of the [Ag(N≡C−) x ] + complexes at different sites.…”

In Situ Grown Silver–Polymer Framework with Coordination Complexes for Functional Artificial Tissues

“…6), implying the presence of a strongly entangled and densely cross-linked PANSion network. These results are in accordance with other reports 25 and our AFM-SMFS data, affirming that [Ag(−C≡N)x] + complexes, as cross-linkers, cause structural changes to the PANSion network when compared to its antetype of PAN.…”

“…Furthermore, the gelation evolution for ϕ = 2.0 was manifested by the competing effect between the storage modulus (G′) and loss modulus (G″), where G′ became dominant once the gelation occurred (Figure S8, Supporting Information), implying the presence of a strongly entangled and densely cross-linked PANSion network. These results are in accordance with other reports [15] and our AFM-SMFS data, affirming that [Ag(N≡C−) x ] + complexes, as cross-linkers, bring structural changes to the PANSion network when compared to its antetype of PAN.…”

“…[13] Concomitantly, the molecular chain alignment was monitored to be strain-dependent (Figure 3f), where a larger strain produced a higher alignment degree, corresponding to a large value of Herman's orientation factor (f (H) ). [15] For instance, an f (H) value of 0.3427 for 𝜖 = 1, while an f (H) value 0.6331 for 𝜖 = 5, seems to substantiate our initial hypothesis. [13] The non-overlapping of f (H) between the first and second stretchingreleasing cycles might have arisen from the strain hysteresis or the reformation of the [Ag(N≡C−) x ] + complexes at different sites.…”

Engineering of Hierarchical Phase-Separated Nanodomains toward Elastic and Recyclable Shock-Absorbing Fibers with Exceptional Damage Tolerance and Damping Capacity

“…This behavior was attributed to the insufficient time available for the dissociation of reversible interactions under speed stretching, causing the entangled polymer chains to break instead. 10,54 These mechanical properties of PU−PCL 70 fibers are comparable to, or even superior to, those of previously reported SAFs (Figure 2b and Table S4, Supporting Information). 1−4,6−9, 12,17 The POM images in Figure 2c highlight that the half-cut PU−PCL 70 fiber can be elongated to a strain of 150% without propagating the cut, indicating its excellent damage tolerance.…”

Intelligent perceptual textiles based on ionic-conductive and strong silk fibers

“…Figure 3b shows the strain-stress curves of SIH fibers with varied stretching ratios. Stretching the fibers by 100% leads to the highest tensile strength of 55 MPa, which is several times higher than previously reported hydrogel fibers (less than 10 MPa) 35 – 40 . However, excessive stretching (stretching ratio ≥ 150%) decreased both strength and elongation, likely due to the introduction of defects.…”

In Situ Grown Silver–Polymer Framework with Coordination Complexes for Functional Artificial Tissues

“…6), implying the presence of a strongly entangled and densely cross-linked PANSion network. These results are in accordance with other reports 25 and our AFM-SMFS data, affirming that [Ag(−C≡N)x] + complexes, as cross-linkers, cause structural changes to the PANSion network when compared to its antetype of PAN.…”

“…Furthermore, the gelation evolution for ϕ = 2.0 was manifested by the competing effect between the storage modulus (G′) and loss modulus (G″), where G′ became dominant once the gelation occurred (Figure S8, Supporting Information), implying the presence of a strongly entangled and densely cross-linked PANSion network. These results are in accordance with other reports [15] and our AFM-SMFS data, affirming that [Ag(N≡C−) x ] + complexes, as cross-linkers, bring structural changes to the PANSion network when compared to its antetype of PAN.…”

“…[13] Concomitantly, the molecular chain alignment was monitored to be strain-dependent (Figure 3f), where a larger strain produced a higher alignment degree, corresponding to a large value of Herman's orientation factor (f (H) ). [15] For instance, an f (H) value of 0.3427 for 𝜖 = 1, while an f (H) value 0.6331 for 𝜖 = 5, seems to substantiate our initial hypothesis. [13] The non-overlapping of f (H) between the first and second stretchingreleasing cycles might have arisen from the strain hysteresis or the reformation of the [Ag(N≡C−) x ] + complexes at different sites.…”

Engineering of Hierarchical Phase-Separated Nanodomains toward Elastic and Recyclable Shock-Absorbing Fibers with Exceptional Damage Tolerance and Damping Capacity

“…This behavior was attributed to the insufficient time available for the dissociation of reversible interactions under speed stretching, causing the entangled polymer chains to break instead. 10,54 These mechanical properties of PU−PCL 70 fibers are comparable to, or even superior to, those of previously reported SAFs (Figure 2b and Table S4, Supporting Information). 1−4,6−9, 12,17 The POM images in Figure 2c highlight that the half-cut PU−PCL 70 fiber can be elongated to a strain of 150% without propagating the cut, indicating its excellent damage tolerance.…”

Intelligent perceptual textiles based on ionic-conductive and strong silk fibers

“…Figure 3b shows the strain-stress curves of SIH fibers with varied stretching ratios. Stretching the fibers by 100% leads to the highest tensile strength of 55 MPa, which is several times higher than previously reported hydrogel fibers (less than 10 MPa) 35 – 40 . However, excessive stretching (stretching ratio ≥ 150%) decreased both strength and elongation, likely due to the introduction of defects.…”

In Situ Grown Silver–Polymer Framework with Coordination Complexes for Functional Artificial Tissues

“…6), implying the presence of a strongly entangled and densely cross-linked PANSion network. These results are in accordance with other reports 25 and our AFM-SMFS data, affirming that [Ag(−C≡N)x] + complexes, as cross-linkers, cause structural changes to the PANSion network when compared to its antetype of PAN.…”

“…Furthermore, the gelation evolution for ϕ = 2.0 was manifested by the competing effect between the storage modulus (G′) and loss modulus (G″), where G′ became dominant once the gelation occurred (Figure S8, Supporting Information), implying the presence of a strongly entangled and densely cross-linked PANSion network. These results are in accordance with other reports [15] and our AFM-SMFS data, affirming that [Ag(N≡C−) x ] + complexes, as cross-linkers, bring structural changes to the PANSion network when compared to its antetype of PAN.…”

“…[13] Concomitantly, the molecular chain alignment was monitored to be strain-dependent (Figure 3f), where a larger strain produced a higher alignment degree, corresponding to a large value of Herman's orientation factor (f (H) ). [15] For instance, an f (H) value of 0.3427 for 𝜖 = 1, while an f (H) value 0.6331 for 𝜖 = 5, seems to substantiate our initial hypothesis. [13] The non-overlapping of f (H) between the first and second stretchingreleasing cycles might have arisen from the strain hysteresis or the reformation of the [Ag(N≡C−) x ] + complexes at different sites.…”

Engineering of Hierarchical Phase-Separated Nanodomains toward Elastic and Recyclable Shock-Absorbing Fibers with Exceptional Damage Tolerance and Damping Capacity

“…This behavior was attributed to the insufficient time available for the dissociation of reversible interactions under speed stretching, causing the entangled polymer chains to break instead. 10,54 These mechanical properties of PU−PCL 70 fibers are comparable to, or even superior to, those of previously reported SAFs (Figure 2b and Table S4, Supporting Information). 1−4,6−9, 12,17 The POM images in Figure 2c highlight that the half-cut PU−PCL 70 fiber can be elongated to a strain of 150% without propagating the cut, indicating its excellent damage tolerance.…”

Intelligent perceptual textiles based on ionic-conductive and strong silk fibers

“…Figure 3b shows the strain-stress curves of SIH fibers with varied stretching ratios. Stretching the fibers by 100% leads to the highest tensile strength of 55 MPa, which is several times higher than previously reported hydrogel fibers (less than 10 MPa) 35 – 40 . However, excessive stretching (stretching ratio ≥ 150%) decreased both strength and elongation, likely due to the introduction of defects.…”