Christoph Lehmann*ab,
Deoraj Singh
a,
Maria Gastearena
ac and
Laura M. Comella
ad
aCluster of Excellence livMatS @ FIT – Freiburg Center for Interactive Materials and Bioinspired Technologies, University of Freiburg, Freiburg, Germany. E-mail: christoph.lehmann@livmats.uni-freiburg.de
bLaboratory for the Design of Microsystems, Department of Microsystems Engineering, University of Freiburg, Freiburg, Germany
cLaboratory for Chemistry and Physics of Interfaces, Department of Microsystems Engineering, University of Freiburg, Freiburg, Germany
dInstitute of Energy Efficient Mobility, Karlsruhe University of Applied Sciences, Karlsruhe, Germany
First published on 10th June 2025
Microfluidic devices, especially those utilizing polydimethylsiloxane (PDMS) structures, require reliable bonding methods to achieve durable, leak-proof seals. Current bonding techniques, including O2 plasma treatment, suffer from limitations related to material compatibility and surface roughness sensitivity, which compromise device stability and scalability in complex designs. In this study, we investigate the impact of surface roughness, wax contamination, and the presence of conductive materials on bonding strength in PDMS-based microfluidics. Additionally, we propose a novel bonding method using a flowable, one-component silicone rubber that forms robust seals without plasma treatment or silanization, effectively overcoming the challenges posed by increased surface roughness and material heterogeneity. The bonding method demonstrated significantly enhanced bond strengths across various substrate combinations (PDMS, copper, and FR4), with notable resilience under high pressure. This approach advances microfluidic fabrication by offering a scalable, versatile solution for multi-material bonding applicable in digital microfluidics and beyond.
While conventional microfluidics has proven valuable in the applications mentioned above, it faces certain limitations. The fixed nature of microchannels can restrict the degrees of freedom for fluid manipulation, and scaling up operations often requires complex redesigns.5,6 These challenges have led to the emergence of digital microfluidics. Unlike conventional microfluidics, digital microfluidics relies on an array of electrodes to manipulate discrete droplets or fluid phases on a planar surface.7 This electrode-based approach uses electrical fields to control droplet movement, merging, splitting, and mixing operations. Moreover, electrodes can be utilized to measure the electrical properties of the droplets, such as impedance8 or capacitance,9 enabling integrated sensing capabilities. This dual functionality of actuation and sensing makes digital microfluidics particularly attractive for lab-on-a-chip and lab-on-PCB applications, where fluid manipulation and analysis are required on a single platform.10,11
A microfluidic channel in both conventional and digital microfluidics can be implemented into a variety of materials, such as glass,12 silicones, and in particular polydimethylsiloxane (PDMS).13 Manufacturing microfluidic devices using PDMS offers easy fabrication, and enables features including optical transparency, biocompatibility, and versatile functionalization chemistries.13 Microfluidic devices that are fully PDMS-embedded offer additional advantages like being flexible and conformal to their environment, opening up applications in new areas in soft robotics and sensing in shape-changing environments.14–17 For fast prototyping and easy fabrication, lab-on-PCB devices offer the advantages of high integration, personalized design and easy mass production.11 However, integrating electrodes within digital microfluidic devices remains a significant challenge for the development of flexible sensing and manipulation capabilities. Conventional methods for embedding electrodes microfluidic devices often involve complex and time-consuming processes such as multi-step lithography, and large electrode sizes.8,9,18 Further, sometimes electrode materials with a high resistance are used, which can increase the error during signal acquisition.18
Regardless of the design and fabrication method, the fabricated open microchannels must be closed with another substrate to create a leakage-free device. This step in the fabrication process is especially critical in digital microfluidics since a tight and secure bond between various materials including silicone, metal, epoxy, and other polymers with a single bonding technique needs to be realized. As the microchannel dimensions approach low order micrometer scale and the network complexity increases, a bonding technique needs to be consistent over multiple length scales.19 To the best of our knowledge, a unified method for PDMS–PDMS, metal-PDMS, and epoxy-PDMS bonding has not been proposed yet. This limitation is significant because digital microfluidic devices often require the integration of these various materials to function effectively. Moreover, the incorporation of electrodes within flexible PDMS structures often necessitates trade-offs between mechanical flexibility and electrical functionality. Existing methods to address these challenges can involve labor-intensive and costly fabrication steps or require clean room facilities, limiting their scalability and accessibility for widespread.20
Conventional bonding methods in microfluidic device fabrication with PDMS typically involve oxygen plasma treatment, which temporarily renders the PDMS surface hydrophilic, allowing it to bond strongly with glass or another PDMS layer upon contact. However, the method does not work for bonding PDMS to metals, epoxies, or PMMA, having no silanol or hydroxyl groups to engage in a strong chemical bonding. Adhesion between the above-mentioned materials and PDMS can be improved by treating the surface with silane coupling agents (silanization), such as (3-aminopropyl)triethoxysilane (APTES) and (3-glycidyloxypropyl)trimethoxysilane (GPTMS), before the conformal contact to improve adhesion.21–23 Due to the strong reactivity of the silane coupling agents, the silane solution usually needs to be prepared immediately before the bonding process and cannot be used anymore after 30 to 60 min.24 Further, surfaces need to be free of any contamination to allow for a proper silanization of the surfaces.
Other bonding methods use a thin film of various kinds of adhesives that are applied by either spin-coating or a stamping method. After conformal contact, the adhesive film is cured. Agostini et al.25 used an ultraviolet (UV)-curable glue, whereas Li et al.26 explored the use of an epoxy-based adhesive. Here, the surfaces also needed to be plasma-treated or silanized before applying the adhesive thin film, followed by a curing step in a UV chamber or oven. Due to the chemical composition of the adhesive, the bonding can be compromised by certain basic fluids,27 leading to de-bonding depending on the application. Cao et al.28 proposed dimethyl-methylphenylmethoxy siloxane as an adhesive layer for bonding PDMS to glass. Chow et al.29 used a stamped uncured PDMS layer as an adhesive between PDMS and PMMA without any surface pretreatment, but could only achieve weak bonds.
Despite the high versatility of bonding techniques for digital microfluidics, several problems persist. Achieving uniform and reliable bonds over large areas remains challenging, especially as device designs become more complex and multiple material combinations need to be bonded together with one single technique.30 Furthermore, the proposed bonding methods do not give directions on the surface roughness and chemistry from further fabrication steps.20,31 Inconsistent bonding can lead to fluid leakage, reduced device performance, and failure.
These challenges are particularly pronounced in digital microfluidics, where the integration of different materials is crucial and the surface profile of all materials cannot be controlled jointly for all. For instance, additive manufacturing processes, such as 3D printing of molds for microfluidic devices, are likely to produce surfaces with significantly higher roughness than standard photolithography.32 Specifically, Fused Deposition Modeling (FDM) can yield surface roughnesses Sa > 10 μm. Similarly, lab-on-PCB integration11,33 often encounters inherent surface roughness due to the etching and lamination processes involved in PCB fabrication, where surface roughness can also reach tens of micrometers.
In this paper, we investigated how inhomogeneities and alterations in the fabrication process before the conformal bonding can affect the bonding strength of the interfacial layer that is needed to seal a microfluidic device. We investigated three steps in the fabrication process for PDMS-embedded digital microfluidics. As a reference for the integration of metal electrodes on PDMS, we used our recently proposed fabrication method for stretchable printed circuit boards based on PDMS and structured copper tracks.34 There, we identified three manufacturing steps and alterations, that deviated from conventional bonding methods and could affect the bonding strength: (1) the effect of previous wax contamination of the PDMS surface (2) a change in contact angle after O2 plasma treatment with conductive materials being present on the PDMS surface and (3) the effect of surface roughness of the surfaces to be bonded. We show, that previous wax contamination and the presence of conductive materials on the surface do not change the surface characteristics for a successful bonding using methods with O2 plasma treatment. On the other hand, bonding methods that involve O2 plasma treatment fail under increased surface roughness of the substrate. We produced substrates with varying surface roughness and quantified the effect of the surface roughness on the bonding strength using conventional O2 plasma treatment as the bonding method.
As a possible solution to this problem, we present a novel bonding method that addresses this critical issue by utilizing a flowable, one-component silicone rubber. The silicone can be applied as a thin film to the bonding area, cures at room temperature under the influence of atmospheric moisture, and forms a tight bond to various substrates. The bonding method does neither require O2 plasma treatment nor surface silanization and therefore is insensitive to deviations caused by the above-mentioned problems during the manufacturing process. We evaluated the bonding strength between PDMS and PDMS, copper and FR4 (fiberglass-epoxy composite material) with varying surface roughnesses and compared our results to the currently existing bonding methods.
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Fig. 1 1D and 2D surface profile of investigated PDMS surfaces with corresponding surface roughness of (a and b) Sa = 1.00 μm (c and d) Sa = 4.24 μm (e and f) Sa = 3.47 μm (g and h) Sa = 13.34 μm. |
To characterize possible contamination during fabrication processes, pristine PDMS samples were prepared as the base material. To simulate wax contamination, a wax layer (EM-Tec TempStick 135C, Micro to Nano, Netherlands) was melted onto the surface of select PDMS samples and left to fully cool. The wax-contaminated PDMS samples were then cleaned using acetone. Three sample types were prepared for Fourier transform infrared spectroscopy (FTIR) analysis: (i) pristine PDMS, (ii) waxed PDMS, and (iii) waxed PDMS cleaned with acetone. The FTIR measurements were performed using a spectrometer (Cary 630 FTIR, Agilent, USA) in transmission mode. Spectra were collected in the wavenumber range of 650 cm−1 to 4000 cm−1 to analyze the chemical composition of the surface materials. For each sample, transmittance data was recorded as a function of the wavenumber.
To investigate the bonding strength of the one-component silicone rubber, we applied a thin film of the silicone rubber on the surface of the PDMS specimen, as described in the preceding section and then brought it into contact with the second substrate. We tested the bonding strength of the material combinations PDMS–PDMS, PDMS–FR4, and PDMS–copper. Between the two substrates, the PDMS surface roughness was kept constant at Sa = 1.00 μm, whereas the roughness for respective PDMS, FR4, and copper surface was changed. For FR4 and copper, we used the metal and non-metal sides of pristine copper-clad laminate (35/00 Cu, Bungard, Germany). We achieved different surface roughnesses by sanding the surface with sandpaper, the pristine surface profile of FR4 and copper is shown in Fig. S2 (ESI).† The bonded substrates were clamped into the tensile test machine (Inspect Table, Hegewald & Peschke, Germany), see Fig. S3 (ESI).† For all tensile tests, the test speed was set to 10 mm s−1. Force and displacement were simultaneously recorded. The bonding strength was calculated from the maximum force and the cross-section of the bonded interface. The bonding strength values reported are the average of at least three measurements.
Specimen | Surface | Contact angle (°) | |
---|---|---|---|
Before PT | After PT | ||
1 | PDMS Sa = 1.0 μm | 112 ± 3 | 12 ± 3 |
2 | PDMS Sa = 4.24 μm | 128 ± 3 | 9 ± 2 |
3 | PDMS Sa = 4.24 μm with copper electrode | 125 ± 2 | 27 ± 9 |
4 | Copper Sa = 3.47 μm | 110 ± 3 | 27 ± 6 |
5 | Copper Sa = 13.34 μm | 143 ± 3 | 22 ± 4 |
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Fig. 5 Tensile strength of substrates bonded using an interfacial layer of one-component silicone rubber, with surface roughnesses RaPDMS = 2.44 μm. The error shows the 68% confidence on mean. |
The maximum achieved bonding strength with our proposed method is summarized together with other previously suggested bonding methods in Table 2. FR4 exhibited the highest bonding strength with PDMS with a maximum of (1078 ± 28) kPa, 183% more than the highest reported value.39 The maximum PDMS–PDMS bonding strength was (773 ± 123) kPa, 18% higher than the highest reported value. Similarly, the maximum bonding strength for PDMS and copper was achieved at (498 ± 162) kPa, 59% higher than the highest reported value. In addition to the higher bonding strength, our proposed method does not need any surface functionalization using corona or O2 plasma treatment and bonds well without any surface silanization. The curing time for our method, at 12 hours, is longer compared to the methods reported previously. In addition, as the silicone rubber film is thin, it cures within 2 min under atmospheric conditions. The curing time could be extended or stopped by reducing the humidity or working within inert conditions.
Reference | Bonded substrates | Bonding strength | Bonding method (kPa) | Temperature | Time |
---|---|---|---|---|---|
Our work | PDMS–PDMS (Sa = 1.00 μm/13.34 μm) | 773 ± 123 | One-component silicone rubber | RT | 12 h |
PDMS–FR4 (Sa = 1.00 μm/7.83 μm) | 1078 ± 28 | ||||
PDMS–Cu (Sa = 1.00 μm/9.02 μm) | 498 ± 162 | ||||
Wu et al.24 | PDMS–Cu | 236 | Corona discharge treatment followed by surface modification with 2% MPTMS | RT | ≤1 h |
Sunkara et al.21 | PDMS–Cu | 312 ± 57 | O2 plasma treatment followed by surface modification with 1% APTES | RT | ≤1 h |
Chang and Yu39 | PDMS–PDMS | 650 | Half-cured PDMS film | 65 °C | 30 min |
PDMS–FR4 | 380 | ||||
Lee and Chung23 | PDMS–PDMS | 184 | O2 plasma treatment followed by surface modification with 1% APTES and GPTMS | RT | 1 h |
Vlachopoulou et al.40 | PDMS–PDMS | 406 | O2 plasma treatment followed by surface modification with 5% APTES | RT | 1 h |
Samel et al.41 | PDMS–PDMS | 545 | Spin coating of PDMS curing agent | 65 °C | 4 h |
Agostini et al.25 | PDMS–PDMS | (2 bar) | O2 plasma treatment followed by surface modification with 1% APTES + spin coating of UV-curable glue | RT | ≤1 h |
Our newly proposed method uses a one-component silicone rubber which is applied as a thin film on the substrate and acts as a glue between the two substrates upon conformal contact. Since the used silicone rubber is flowable, it can compensate for increased surface roughnesses and inhomogeneities on the substrate surface, making it a useful bonding agent for various types of surfaces. We could show that the bonding method works between PDMS and PDMS, copper and FR4, making it ideal especially in the field of digital microfluidics. Further, it does not require prior O2 plasma treatment and surface modification. To the best of our knowledge, this is the first reported bonding method, that does not require prior plasma treatment and surface silanization and still achieved bonding strengths in the same order as previous reported methods.
Footnote |
† Electronic supplementary information (ESI) available. See DOI: https://doi.org/10.1039/d5ra02701b |
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