Stretchable Wire-Shaped Asymmetric Supercapacitors Based on Pristine and MnO₂ Coated Carbon Nanotube Fibers

Abstract

While the emerging wire-shaped supercapacitors (WSS) have been demonstrated as promising energy storage devices to be implemented in smart textiles, challenges in achieving the combination of both high mechanical stretchability and excellent electrochemical performance still exist. Here, an asymmetric configuration is applied to the WSS, extending the potential window from 0.8 to 1.5 V, achieving tripled energy density and doubled power density compared to its asymmetric counterpart while accomplishing stretchability of up to 100% through the prestrainning-then-buckling approach. The stretchable asymmetric WSS constituted of MnO2/CNT hybrid fiber positive electrode, aerogel CNT fiber negative electrode and KOH-PVA electrolyte possesses a high specific capacitance of around 157.53 μF cm(-1) at 50 mV s(-1) and a high energy density varying from 17.26 to 46.59 nWh cm(-1) with the corresponding power density changing from 7.63 to 61.55 μW cm(-1). Remarkably, a cyclic tensile strain of up to 100% exerts negligible effects on the electrochemical performance of the stretchable asymmetric WSS. Moreover, after 10,000 galvanostatic charge-discharge cycles, the specific capacitance retains over 99%, demonstrating a long cyclic stability.

A General Electrode Design Strategy for Flexible Fiber Micro‐Pseudocapacitors Combining Ultrahigh Energy and Power Delivery

“…Various carbonaceous materials like activated carbon,9, 10 carbon nanotubes (CNTs),11, 12, 13 reduced graphene oxide (rGO),14, 15, 16 and our recently developed rGO/CNT hybrids17, 18 were exploited as active materials for fiber m‐SCs, yet their applications are restricted by the low capacitance of <200 mF cm −2 . Alternatively, incorporating pseudocapacitive materials into fiber m‐SCs is a superior solution to achieve high‐density energy due to 10–100 times higher theoretical capacitance than carbon materials 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36. Due to the poor conductivity for pseudocapacitive materials, composite electrode design by depositing active materials on one‐dimensional (1D) conductive scaffolds including carbon‐based fibers19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30 or metal‐based wires,31, 32, 33, 34, 35, 36 was employed to improve the electron transport.…”

“…Alternatively, incorporating pseudocapacitive materials into fiber m‐SCs is a superior solution to achieve high‐density energy due to 10–100 times higher theoretical capacitance than carbon materials 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36. Due to the poor conductivity for pseudocapacitive materials, composite electrode design by depositing active materials on one‐dimensional (1D) conductive scaffolds including carbon‐based fibers19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30 or metal‐based wires,31, 32, 33, 34, 35, 36 was employed to improve the electron transport. Despite some progresses, the improvements in the areal energy density for these fiber m‐SCs are still too modest to cater for many practical requirements and often come at the expense of sacrificing their rate capability or power density 1, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36.…”

“…Due to the poor conductivity for pseudocapacitive materials, composite electrode design by depositing active materials on one‐dimensional (1D) conductive scaffolds including carbon‐based fibers19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30 or metal‐based wires,31, 32, 33, 34, 35, 36 was employed to improve the electron transport. Despite some progresses, the improvements in the areal energy density for these fiber m‐SCs are still too modest to cater for many practical requirements and often come at the expense of sacrificing their rate capability or power density 1, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36. This impedes their broad practical applications where both high power and energy densities are required.…”

“…The widely employed scaffolds in the literature are mainly carbonaceous fibers such as CNT yarns, rGO fibers, and their composite fibers. But their conductivity is unsatisfactory for long‐range electron transport along the fiber 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30. Unlike macroscopic planar SCs, effective long‐distance electron transport is highly required for fiber m‐SCs due to the lack of extra metal current collectors within slender fiber electrodes.…”

“…Unlike macroscopic planar SCs, effective long‐distance electron transport is highly required for fiber m‐SCs due to the lack of extra metal current collectors within slender fiber electrodes. However, such crucial design concern is often ignored in previous carbon‐based fiber m‐SCs, thus leading to a major bottleneck in performance (typically <200 mF cm −2 and <1 mW cm −2 ) 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30. As compared, metallic scaffold was recognized as the best candidate for long‐range electron transport 31, 32, 33, 34, 35, 36.…”