Supporting Information

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SUPPORTING INFORMATION

Wearable Circuits Sintered at Room Temperature


Directly on the Skin Surface for Health
Monitoring

Ling Zhang,†,‡,§,& Hongjun Ji,†,‡, ‖ ,& Houbing Huang, ⊥ ,& Ning Yi,ǂ,& Xiaoming Shi, ⊥

Senpei Xie,‡,‖Yaoyin Li,‡,‖ Ziheng Ye,‖ Pengdong Feng,‡,‖ Tiesong Lin,† Xiangli Liu,‖

Xuesong Leng,† Mingyu Li,†,‡, ‖ Jiaheng Zhang,†,‡, ‖ Xing Ma,†,‡, ‖ Peng He,†* Weiwei

Zhao,†,‡,‖,* and Huanyu Cheng,§,ǂ,*


State Key Laboratory of Advanced Welding & Joining, Harbin Institute of Technology,
Shenzhen, 518055, People’s Republic of China

Flexible Printed Electronics Technology Center, Harbin Institute of Technology,
Shenzhen, 518055, People’s Republic of China
§
Department of Engineering Science and Mechanics, The Pennsylvania State University,
University Park, PA 16802, USA.

‖ The School of Material Science and Engineering, Harbin Institute of Technology,

Shenzhen, 518055, People’s Republic of China

⊥ Advanced Research Institute of Multidisciplinary Science, Beijing Institute of

Technology, Beijing 100081, China


ǂ
Department of Materials Science and Engineering, The Pennsylvania State University,
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University Park, PA 16802, USA.
*
To whom correspondence should be addressed. E-mail: Huanyu.Cheng@psu.edu (H.C.);

wzhao@hit.edu.cn (W.Z.); hithepeng@hit.edu.cn (P.H.).

&
These authors contributed equally to this work

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This PDF file includes:

Figure S1. Schematic diagrams for measurements from resistive and capacitive sensors

using the SL900A RF chip

Figure S2. Contact angle measurement of the paper with the Ag NP ink.

Figure S3. Surface roughness change in the copy paper after the sintering aid layer

consisting of PVA paste and TiO2 nanoadditive.

Figure S4. X-ray diffraction of the high-temperature-resistant paper.

Figure S5. Comparison of the electrical and electromechanical properties of the low-

temperature sintered NP ink between this work and literature reports.

Figure S6. Porous structure in various paper and textile substrates.

Figure S7. Reduced surface roughness in various substrates with the sintering aid layer

consisting of PVA paste and TiO2 nanoadditive.

Figure S8. SEM images of metal particles sintered on the coated paper substrates and their

measured sheet resistances.

Figure S9. Electromechanical performance of the sintered patterns upon mechanical

deformations of bending and folding.

Figure S10. Normalized sheet resistance of the sintered patterns with Ag NP inks on three

different fabric substrates as a function of bending cycles, soaking time, and for different

pH values.

Figure S11. Effects of the sintering aid layer formula and sintering temperature of the ink

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on the electromechanical performance of the sintered patterns by using 50 nm Ag NPs on

a copy paper.

Figure S12. Possible chemical interaction between PVA and TiO2 in the nanocomposite.

Figure S13. Effect of the radical inhibitor on the sintering of the Ag NP ink

Figure S14. Cross-sectional SEM images showing the interface between the sintering aid

layer on a copy paper substrate and the sintered patterns using different metal particle inks

Figure S15. SEM images

Figure S16. SEM images of the sintering aid layer with CaO3 nanoadditives

Figure S17. The sheet resistance of the sintered Ag patterns on the sintering aid layer with

CaCO3 nanoadditives and TiO2 nanoadditives versus sintering temperature.

Figure S18. SEM images of Ag NPs after (a) water removal at 90 °C for 3 h and sintered

at (b) 120, (c) 140, and (d) 160 °C for 1 h.

Figure S19. Optical images of the stamp-based transfer printing process

Figure S20. Contact angle measurements of the Ag NP ink on the surface of the papers

coated by the sintering aid layer with different nanoadditives, including Al2O3, MgO,

BaTiO3, TiO2, CaCO3, and Cu.

Figure S21. Optical image to show the drying process of the printed Ag NP ink with the

electric hair dryer.

Figure S22. Pattern designs of a temperature sensor, humidity sensor, and electrode to

measure EMG/ECG signals.

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Figure S23. Measured pulsating photoplethysmogram (PPG) voltage output signal from

the photodetector for the red and infrared LEDs for the calculation of the blood oxygen

level.

Figure S24. ECG signals collected from the arms of a healthy volunteer (top) before and

(bottom) after running exercise.

Figure S25. Demonstration of wireless detection from directly printed on-body sensors

Table S1. Effect of different nanoadditives (TiO2, Al2O3, MgO, CaCO3, BaTiO3, and Cu)

in the PVA paste on the sintering temperature of 50 nm Ag NP ink on the coated paper.

Table S2. Effect of different nanoadditives (CaCO3, Al2O3, MgO, TiO2, and BaTiO3) in the

PVA paste on the sintering temperature of 2 μm Ag MP ink on the coated paper.

Table S3. Comparison in the sensitivity from the temperature and humidity sensors

between this work and others based on the Ag NP ink in literature reports.

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Figure S1. Schematic diagrams for measurements from resistive and capacitive sensors using
the SL900A RF chip.

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Figure S2. Contact angle measurement of the paper with the Ag NP ink.

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Figure S3. Surface roughness change in the copy paper after the sintering aid layer consisting of
PVA paste and TiO2 nanoadditive. Atomic force microscope (AFM) images of the copy paper (a)
before and (b) after applying the sintering aid layer. The surface roughness reduces from 1573 nm to
412 nm. (c) SEM images of the sintering aid layer with TiO2 nanoadditives.

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Figure S4. X-ray diffraction of the high-temperature-resistant paper.

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Figure S5. Comparison of the (a) electrical and (b) electromechanical properties of the low-
temperature sintered NP ink between this work (red star: CaCO3 nanoadditives; red asterisk:
TiO2 nanoadditives) and literature reports.

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Figure S6. Porous structure in various paper and textile substrates. (a) Schematic illustration of
the flexible substrate with the scanning electron microscope (SEM) images of various substrate
materials, including (b) copy paper, (c) printing paper, (d) weighting paper, (e) cotton, (f) chemical
fabric, and (g) silk.

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Figure S7. Reduced surface roughness in various substrates with the sintering aid layer consisting
of PVA paste and TiO2 nanoadditive. (a) Schematic illustration of the flexible substrate with the
SEM images of various substrate materials after applying the sintering aid layer, including (b) copy
paper, (c) printing paper, (d) weighting paper, (e) cotton, (f) chemical fabric, and (g) silk.

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Figure S8. SEM images of metal particles sintered on the coated paper substrates and their
measured sheet resistances. (a) Schematic of the sintered pattern on the coated paper substrate with
(b) the TEM image of 50 nm Ag NPs and the SEM images of sintered patterns on a copy paper by using
(c) 50 nm Ag NP ink, (d) 2 μm Ag MP ink, and (e) 40 μm Ag MP ink. The sheet resistance (R0, Ω/□)
of sintered patterns with different metal particle inks on three different paper substrates: (f) copy paper,
(g) printing paper, and (h) weighting paper.

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Figure S9. Electromechanical performance of the sintered patterns upon mechanical
deformations of bending and folding. Normalized sheet resistance R/R0 of sintered patterns with
four different metal particle inks on (a) copy paper, (b) printing paper, and (c) weighting paper is
measured as a function of (i) bending cycles, followed by (ii) folding of the same samples.

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Figure S10. Normalized sheet resistance of the sintered patterns with Ag NP inks on three different
fabric substrates as a function of (a) bending cycles, (b) soaking time, and (c) for different pH
values.

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Figure S11. Effects of the sintering aid layer formula and sintering temperature of the ink on the
electromechanical performance of the sintered patterns by using 50 nm Ag NPs on a copy paper.
Normalized sheet resistance change as a function of bending cycles with (a) different ratios of PVA
powder to water (1:9, 3:17, and 1:4), (b) different ratios of TiO2 to PVA paste (i.e., 1:20, 1:15, 1:10, and
1:5), and (c) sintering temperatures (i.e., 120, 140, and 160 ºC).

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Figure S12. Possible chemical interaction between PVA and TiO2 in the nanocomposite.

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Figure S13. Effect of the radical inhibitor on the sintering of the Ag NP ink. Preparation of the
sintering aid layer with the radical inhibitor: (a) After stirring the PVA powder in the deionized
water for ~2h at 70 ºC, (b) L-ascorbic acid is added with (c) stirring for 3 min, followed by (d)
adding TiO2 and stirring for 15 min. (e) After printing the Ag NP ink on the paper coated with the
sintering aid layer with the radical inhibitor, followed by annealing at 120 ºC, the obtained Ag
pattern is still not conducive.

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Figure S14. Cross-sectional SEM images showing the interface between the sintering aid layer on
a copy paper substrate and the sintered patterns using different metal particle inks: (a) 2 μm Ag
MPs, (b) 40 μm Ag MPs, (c) 50 nm Ni/Ag core/shell NPs.

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Figure S15. SEM images of (a) 50 nm Ni/Ag core/shell NPs, (b) 50 nm Ag NPs, (c) 2 μm Ag MPs,
and (d) 40 μm Ag MPs sintered on (i) copy paper, (ii) printing paper, and (iii) weighting paper
coated with the sintering aid layer consisting of PVA paste and TiO2 nanoadditive.

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Figure S16. SEM image of the sintering aid layer with CaO3 nanoadditives.

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Figure S17. The sheet resistance of the sintered Ag patterns on the sintering aid layer with (a)
CaCO3 nanoadditives and (b) TiO2 nanoadditives versus the sintering temperature.

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Figure S18. SEM images of Ag NPs after (a) water removal at 90 ºC for 3 h and sintered at (b)
120, (c) 140, and (d) 160 ºC for 1 h.

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Figure S19. Optical images of the stamp-based transfer printing process. (a) A soft elastomeric
polymer shaped to the desired patterns on a wooden stamp is first dipped into a commercial Ag NP ink.
(b) After bringing the inked stamp in contact with the skin, pressing and then slowly retrieving of the
stamp leaves the patterned ink on the textured skin surface.

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Figure S20. Contact angle measurements of the Ag NP ink on the surface of the papers coated by
the sintering aid layer with different nanoadditives, including Al2O3, MgO, BaTiO3, TiO2, CaCO3,
and Cu.

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Figure S21. Optical image to show the drying process of the printed Ag NP ink with the electric
hair dryer.

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Figure S22. Pattern designs of (a) temperature sensor, (b) humidity sensor, and (c) electrode to
measure EMG/ECG signals.

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Figure S23. Measured pulsating photoplethysmogram (PPG) voltage output signal by the
photodetector from the red and infrared LEDs for the calculation of the blood oxygen level. The
peak−to−peak interval informs a pulse rate of 76 beats/min. Following the equations in the methods
section, the blood oxygen saturation SpO2 is calculated to be 95.2 % after exercise.

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Figure S24. ECG signals collected from the arms of a healthy volunteer before (top) and after
(bottom) running exercise, by the Ag metal electrode sintered on the sintering aid layer with 10
wt% PVA paste (magenta) or by the commercial electrodes (red).

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Figure S25. Demonstration of wireless detection from directly skin-printed on-body sensors.
(a) Read range of the SL900A chip versus the measurement frequency. Wirelessly measured (b)
temperature and (c) humidity from the FPCB with the SL900A chip. (d) Wirelessly measured
ECG signals from a commercial wireless module with a small footprint.

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Table S1. Effect of different nanoadditives (TiO2, Al2O3, MgO, CaCO3, BaTiO3, and Cu) in the PVA
paste on the sintering temperature of 50 nm Ag NP ink on the coated paper.
TiO2 Al2O3 MgO CaCO3 BaTiO3 Cu Paste

25 °C NA NA NA 0.5Ω NA NA NA

70 °C 0.3Ω 0.4Ω 1.7Ω 0.3Ω NA NA NA

100 °C 0.5Ω 0.4Ω 1.2Ω 0.3Ω 0.5Ω NA NA

120 °C 0.4Ω 0.4Ω 0.8Ω 0.4Ω 0.5Ω NA NA

Note: NA indicates the non-conductive pattern.

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Table S2. Effect of different nanoadditives (CaCO3, Al2O3, MgO, TiO2, and BaTiO3) in the PVA paste
on the sintering temperature of 2 μm Ag MP ink on the coated paper.
CaCO3 Paste Al2O3 MgO TiO2 BaTiO3

25 °C 20.5Ω NA NA NA NA NA

50 °C 10.2Ω NA NA NA NA NA

60 °C 0.3Ω 11.4Ω 0.5Ω 2.2Ω 1.4Ω NA

90 °C NA

100 °C 0.2Ω 0.3Ω 0.4Ω 2.0Ω

120 °C 0.6Ω

150 °C 1.7Ω

Note: NA indicates the non-conductive pattern.

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Table S3. Comparison in the sensitivity from the temperature and humidity sensors between this work and
others based on the Ag NP ink in literature reports.1-4

Temperature Humidity Annealing


Ref. Deposition Substrate Composition
(Sensitivity) (Sensitivity) Temperature

[S1] 0.08%/°C 1.7%/%RH Fully printed PET PEDOT: PSS 60 °C

[S2] 0.03%/°C NG Fully printed PET Pure 130 °C

[S3] 0.09%/°C 1.1%/%RH Fully printed Paper Pure 25 °C

[S4] NG 1.25%/%RH Fully printed Paper Pure 100-150 °C

Our Stamp-based Room


0.195%/°C 1.125%/%RH Skin Pure
work printed temperature

References:

S(1) Rivadeneyra Torres, A. & Fernández-Salmerón, J. Cost-Effective Pedot: Pss Temperature Sensors
Inkjetted on a Bendable Substrate by a Consumer Printer. 2019.
S(2) Kanao, K., Harada, S., Yamamoto, Y., Honda, W., Arie, T., Akita, S. & Takei, K. Highly Selective Flexible
Tactile Strain and Temperature Sensors against Substrate Bending for an Artificial Skin. RSC
Advances 2015 5, 30170-30174.
S(3) Barmpakos, D., Segkos, A., Tsamis, C. & Kaltsas, G. in Multidisciplinary Digital Publishing Institute
Proceedings. 977.
S(4) Andersson, H., Manuilskiy, A., Unander, T., Lidenmark, C., Forsberg, S. & Nilsson, H.-E. Inkjet Printed
Silver Nanoparticle Humidity Sensor with Memory Effect on Paper. IEEE Sensors Journal 2011 12,
1901-1905.

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