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Supporting Information for
Robust DNA-bridged memristor for textile chip
This file includes:
Methods (Pages S2-S4)
Supplementary Figures 1 to 17 (Pages S5-S21)
Supplementary Tables 1(Page S22 )
Supplementary References (Pages S23-S24)
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1. Preparation of DNA solution
The preparation of DNA solution followed the previous report.[1] 10 mg
deoxyribonucleic acid sodium (ss-DNA,99%, Sigma-Aldrich) was dissolved in 5 mL
deionized water and sonicated for 30 min. Then, hexadecyltrimethylammonium
chloride (CTMA, 99%, Makun) was added to the DNA solution, maintaining a
DNA/CTMA weight ratio of 1/1. The resulting solution was sonicated for 30 min. The
production was centrifuged at 8000 rpm for 5 min, and the supernatant was discarded
and the precipitate was collected to be re-dispersed in n-butanol.
2. Deposition of DNA on Ag or Pt fibres through electrophoretic deposition
Two Ag fibers (99.99%, 50 μm, Alfa Aesar) or Pt fibers (99.99%, 50 μm, Alfa Aesar)
were connected to a direct current supply (Keithley 2400 Source Meter) and dipped into
the as-prepared solution. Depending on the time or the voltage applied, the film
thickness was controlled. A voltage of 1.8 V and a period of 3 min had been chosen
after careful experimental optimization.
3. Preparation of modified photoanode fiber
First, a Ti fiber (99.99%, 127 μm, Alfa Aesar) was sequentially sonicated by de-ionized
water, acetone and isopropanol each for 5 min, followed by anodic oxidation in a water
bath at 50 oC. Then, a mixture solvent of water and glycerol (volume ratio, 1/1)
containing 0.27 M NH4F was used as the electrolyte. The growth was operated in a two-
electrode system with a Ti fiber and a Pt plate as the anode and cathode at 20 V for 7
min, respectively. The resulting Ti fiber was washed by de-ionized and annealed at 500 oC for 60 min.
4. Preparation of aligned CNT sheet and fiber
CNT sheet was dry-drawn from spinnable CNT array synthesized by chemical vapor
deposition.[2] Al2O3 (3 nm) and Fe (1.2 nm) were deposited on silicon wafer by electron
beam evaporation as the catalyst. Ethylene (90 sccm), Ar (400 sccm) and H2 (30 sccm)
were used as carbon source, carrier gas and reduction gas, respectively. The spinnable
CNT array was grown at 750 °C in a quartz tube furnace for 10 min. CNT fiber was
prepared by further twisting the aligned CNT sheet.[3, 4]
5. Fabrication of fiber-shaped all-inorganic perovskite solar cell
The CsPbBr3 quantum dots were synthesized according to the previous literature.[5] A
modified photoanode fiber was dip-coated in the CsPbBr3 QDs solution and annealed
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at 300 oC, transforming QDs to large CsPbBr3 crystals and removing organic ligands.
This process was repeated for 20 to 100 times to obtain different thicknesses of active
layers. Finally, the aligned carbon nanotube sheet as the counter electrode was wrapped
onto the composite fiber to obtain a fiber-shaped all-inorganic perovskite solar cell. The
carbon nanotube (CNT) sheet was obtained from a spinnable CNT array synthesized by
chemical vapour deposition.
6. Fabrication of fiber-shaped Ni/Bi full battery[6]
A rGO/Bi/CNT hybrid fiber anode was first prepared. The rGO/Bi composite was
electro-co-deposited on the CNT fiber in a solution (40 mL) containing graphene oxide
(0.03 mg/mL), ethylenediaminetetraacetic acid disodium salt (EDTA·2Na, 0.1 M) and
Bi(NO3)3·5H2O (50 × 10−3 m). Carbon rod and Hg/HgO electrodes were used as counter
and reference electrodes, respectively. A potential of −1.2 V versus Hg/HgO electrode
was applied for 60 s. After electrodeposition, the sample was washed with water and
dried at 80 °C. Finally, the sample was dipped in graphene oxide solution (1.5 mg/mL)
for ten times and dried at 80 °C in air.
A rGO/Ni/NiO/CNT fibre cathode was then prepared. 12 mg of the rGO/Ni/NiO hybrid
was dispersed in 2 mL ethanol by ultrasonication at 60 °C for 10 min, followed by
immersion of eight stacked CNT sheets and later scrolled into an rGO/Ni/NiO/CNT
hybrid fibre.
The fiber‐shaped Ni//Bi battery can be finally fabricated. The rGO/Bi/CNT and
rGO/Ni/NiO/CNT fiber electrodes were twisted with a separator between them and then
inserted into a poly (tetrafluoroethylene) tube. After an electrolyte was injected into the
tube, both ends of the tube were sealed.
7. Fabrication of fiber-shaped light-emitting device
The ZnS:Cu and polydimethylsiloxane mixture was prepared by mixing
polydimethylsiloxane precursor, namely, a mixture of elastomer prepolymer and curing
agent with a weight ratio of 9/1, and ZnS:Cu microparticles at a weight ratio of 1/1.
Next, the obtained mixture was dip-coated onto a silver-plated nylon yarn (100 μm in
diameter) and then cured in the oil bath for 10 s at 160 oC. The obtained composite fiber
was washed with ethanol and then dried at 80 °C for 30 min. After that, an enamelled
copper fiber was spirally wound onto the resulting composite fiber to fabricate a fiber-
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shape light-emitting device.
8. Integration
The fiber-shaped perovskite solar cells were connected in series with fiber-shaped Ni/Bi
batteries and worked as the power supply for the computing unit. The direct current
voltage would be transformed into sweep pulses via a commercial transformer and
provided tunable pulse intensity (e.g., +0.2V, +0.4V and -0.2V).
9. Electrical measurements and characterizations
The electrical measurements of the memristors including direct current, pulse electrical
measurements and basic logic gates measurements were performed in the atmosphere
using semiconductor characterization system (Keithley 2400 and Agilent B1500 with
pulse generator unit). As for the memristor, the Pt fibers (99.99%,0.025 mm, Alfa Aesar)
were carefully interlaced with the Ag fibers coated with DNA. The Ag electrode was
applied with an external bias while the Pt electrode was kept as ground.
J–V curves of the fiber-shaped all-inorganic perovskite solar cell were recorded by a
Keithley 2400 Source Meter under the illumination (100 mW cm-2) of a simulated
AM1.5 solar light from a solar simulator (OrielSol3A 94023A equipped with a 450 W
Xe lamp and an AM1.5 filter). Current-voltage and galvanostatic charge/discharge
measurements were conducted using an electrochemical workstation (CHI 660D). The
light intensity of the fiber-shaped light-emitting device was carried out by a
Photoresearch PR-680 under an alternating current waveform using a function
generator (3312 A; Hewlett Packard) and a high-voltage amplifier (610 D; TREK Inc.).
The morphologies were characterized by field-emitting scanning electron microscopy
(Hitachi S-4800) and high-resolution transmission electron microscopy (JEOL, JEM-
2100F). The chemical composition and structure were confirmed by Fourier transform
infrared spectroscopy (Nicolet 6700) and laser Raman spectroscopy (XploRA). The
orientation of the DNA molecules was characterized by grazing incidence small angle
scattering (Xeuss2.0). Plan-view conductive filament mapping was characterized by
conducting atom force microscopy (Multimode V, Bruker Nano Surfaces) and Cr/Pt-
coated tips (Multi75E-G, Budget Sensors).
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Figure S1. Schematic illustration to DNA assembly via electrophoretic deposition with
simultaneous modification of Ag nanoparticles (AgNPs).
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Figure S2. Raman spectra of the DNA/AgNPs film prepared via electrophoretic
deposition.
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Figure S3. High-resolution cross-sectional transmission electron microscopy images
of the DNA/AgNP film prepared via electrophoretic deposition. Scale bars in a and b,
5 nm and 1 nm, respectively.
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Figure S4. X-ray photoelectron spectroscopy of the DNA/AgNP film prepared via
electrophoretic deposition.
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Figure S5. Capacitance–voltage characteristics of the DNA assembly process via
electrophoretic deposition with different electrodes. a) Platinum. b) Silver.
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Figure S6. Fourier transform infrared spectra of the DNA/AgNP layer.
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Figure S7. a) Schematic illustration of conducting atomic force microscopy test
method and plan-view conductive filament mapping by conductive atomic force
microscopy. b) Under set state. c) Reset state.
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Figure S8. Switching speed of the Pt/DNA/Ag memristor with homogeneously
distributed DNA prepared via dip coating.
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Figure S9. Small-area Fourier transform infrared spectra of the Pt/DNA/AgNPs/Ag
memristor prepared via electrophoretic deposition under original and set states.
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Figure S10. Scanning electron microscopy images of DNA assembly via
electrophoretic deposition with Pt electrode at increasing magnifications from left to
right. Scale bars in a, b and c, 10 μm, 1 μm and 200 nm, respectively.
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Figure S11. Current-voltage characteristics of the Pt/DNA/Ag memristor (inset is the
schematic illustration of the device structure).
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Figure S12. a) Fabrication process of fiber-shaped perovskite solar cell. b-d)
Corresponding scanning electron microscopy images in a. Scar bars in b, c and d, 200
nm, 200 nm and 5 μm, respectively.
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Figure S13. Current-voltage characteristic of the fiber-shaped solar cell.
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Figure S14. a) Fabrication process of fiber-shaped Ni/Bi full battery. b-c) Scanning
electron microscopy images of rGO/Bi/CNT fiber anode at low and high magnification,
respectively. d-e) Scanning electron microscopy images of rGO/Ni/NiO/CNT fiber
cathode at low and high magnification, respectively. Scale bars in b, c, d and e, 20 μm,
2 μm, 20 μm and 200 nm, respectively.
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Figure S15. a) Galvanostatic charge and discharge profiles of fiber-shaped Ni/Bi full
battery. b) Cycling performance for 10,000 cycles.
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Figure 16. a) Schematic diagram for the fabrication of electroluminescent fiber. b-d)
Corresponding Scanning electron microscopy images in a. Scale bars in b-d, 100 μm.
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Figure S17. a) Cross-sectional scanning electron microscopy image of the light-
emitting fiber. b-c) Luminescent properties under different bias and frequencies,
respectively. d) Photographs of the flexible light-emitting fiber under different bending
or twisting conditions. Scale bars in a and d, 100 μm and 1 cm, respectively.
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Supplementary Table 1. Comparison of the memristive performances of this work with the state-of-art organic memristors.
Device structure Set (V) Reset (V) Set power/reset
power (W) Retention time (s) On/off
Cycle
number (n) Reference
Ag/DNA:AgNPs/Pt 0.20.4 -0.05-0.2 10-10
/10-5
105 10
6 1000 This work
Al/GO–PVK/ITO -2 4 / 104 10
3 / [7]
Au/PI:PCBM/Al 3 -4 10-5
/10-2
104 10
3 300 [8]
ITO/RGO‐PFCF/Al -1.2 2 / 104 10
2 / [9]
Au/Co(III) polymer/Au -5 5 / 104 102 / [10]
Ag/PI/GO:PI/PI/ITO 2.54.5 -7 10-7
/10-3
1.6×103 10
3 130 [11]
Ag/(PAH/ferritin)15
/pt -1.5 2 10-3
/10-1
One year 102 300 [12]
Al/silk/ITO 14 -14 / 120 11 1000 [13]
Ag/sericin/Au 2.5 -0.5 10-7
/10-2
103 10
6 300 [14]
ITO/Al-chelated gelation/ITO -1.0 1.8~2.6 10-5
/10-1
105 10
4 60 [15]
Al/PVK/ITO 1 -3.1 10-4
/10-1
104 10
3 / [16]
Ag/WK@AuNCs–SF/ITO 0.4 -0.2 10-5
/10-3
1.4×104 10
2 100 [17]
Au/lignin/ITO/PET -0.5-0.7 0.50.7 10-4
/10-4
/ / 10 [18]
ITO/mer-
[Ru(L)3](PF
6)2:AuNc/ITO
0.490.55 -0.51-0.59 10-10
/8×10-7
3×106 10
310
5 10
12 [19]
Au/PS:PCBM/Al 3.04.0 -4 10-7
/10-2
104 10
3 500 [20]
Al/S-layer protein (Slp)/ITO 8 -8 10-3
/10-3
4×103 6.2 500 [21]
Ag/2DPBTA+PDA
/ITO 0.9 3 10-7
/10-3
3.6×104 10
5 200 [22]
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Supplementary References
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