Dan My Nguyen

University of Delaware

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Thermo-reversible gelation of self-assembled conducting polymer colloids

Vidhika S. Damani Xinran Xie Rachel E. Daso Khushboo Suman Masoud Ghasemi

Electrically conductive hydrogels based on conducting polymers have found increased use in bioelectronics due to their low moduli that mimic biological tissues, their ability to transport both ionic and electronic charges, and their ease of processing in various form factors via printing or injection. Current approaches towards conductive hydrogels, however, rely on covalent and therefore irreversible crosslinking mechanisms. Here, we report a thermo-responsive conducting polymer (TR-CP) that undergoes a fully reversible non-covalent crosslinking at 35 °C within less than a minute to form conductive hydrogels. The TR-CP is based on a block polyelectrolyte complex, that self-assembles into well-defined colloidal particles in water which undergo an isovolumetric sol-gel transition just below physiological temperature. The hydrogels have tunable mechanical properties in the 20 to 200 Pa range, are stable at various pH and salt conditions, self-healing, injectable, and biocompatible in vitro and in vivo. We demonstrate that the TR-CPs can be used to fabricate sensitive, conformal and reusable electrodes for surface electromyography. This unique material provides exciting opportunities for stimuli-responsive and adaptive bioelectronics.

10.26434/chemrxiv-2024-g900w

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One Pot Photomediated Formation of Electrically Conductive Hydrogels

ACS Polymers Au (2023)

Dan My Nguyen Chun‐Yuan Lo Tianzheng Guo T. G. Choi Shalini Sundar

Electrically conductive hydrogels represent an innovative platform for the development of bioelectronic devices. While photolithography technologies have enabled the fabrication of complex architectures with high resolution, photoprinting conductive hydrogels is still a challenging task because the conductive polymer absorbs light which can outcompete photopolymerization of the insulating scaffold. In this study, we introduce an approach to synthesizing conductive hydrogels in one step. Our approach combines the simultaneous photo-cross-linking of a polymeric scaffold and the polymerization of 3,4-ethylene dioxythiophene (EDOT), without additional photocatalysts. This process involves the copolymerization of photo-cross-linkable coumarin-containing monomers with sodium styrenesulfonate to produce a water-soluble poly(styrenesulfonate-co-coumarin acrylate) (P(SS-co-CoumAc)) copolymer. Our findings reveal that optimizing the [SS]:[CoumAc] ratio at 100:5 results in hydrogels with the strain at break up to 16%. This mechanical resilience is coupled with an electronic conductivity of 9.2 S m–1 suitable for wearable electronics. Furthermore, the conductive hydrogels can be photopatterned to achieve micrometer-sized structures with high resolution. The photo-cross-linked hydrogels are used as electrodes to record stable and reliable surface electromyography (sEMG) signals. These novel photo-cross-linkable polymers combined with one-pot PEDOT (poly-EDOT) polymerization open possibilities for rapidly prototyping complex bioelectronic devices and creating custom-designed interfaces between electronics and biological systems.

10.1021/acspolymersau.3c00031

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Influence of the molecular weight and size distribution of PSS on mixed ionic-electronic transport in PEDOT:PSS

Polymer Chemistry (2022)

Chun‐Yuan Lo Yuhang Wu Elorm Awuyah Dilara Meli Dan My Nguyen

The commercially available polyelectrolyte complex poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) is ubiquitous in organic and hybrid electronics. As such, it has often been used as a benchmark material for fundamental studies and the development of new electronic devices. Yet, most studies on PEDOT:PSS have focused on its electronic conductivity in dry environments, with less consideration given to its ion transport, coupled ionic-electronic transport, and charge storage properties in aqueous environments. These properties are essential for applications in bioelectronics (sensors, actuators), charge storage devices, and electrochromic displays. Importantly, past studies on mixed ionic-electronic transport in PEDOT:PSS neglected to consider how the molecular structure of PSS affects mixed ionic-electronic transport. Herein, we therefore investigated the effect of the molecular weight and size distribution of PSS on the electronic properties and morphology of PEDOT:PSS both in dry and aqueous environments, and overall performance in organic electrochemical transistors (OECTs). Using reversible addition-fragmentation chain transfer (RAFT) polymerization with two different chain transfer agents, six PSS samples with monomodal, narrow (

10.1039/d2py00271j

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Imidazolium-Based Sulfonating Agent to Control the Degree of Sulfonation of Aromatic Polymers and Enable Plastics-to-Electronics Upgrading

JACS Au (2024)

Chun‐Yuan Lo Kelsey P. Koutsoukos Dan My Nguyen Yuhang Wu David Alejandro Angel Trujillo

The accumulation of plastic waste in the environment is a growing environmental, economic, and societal challenge. Plastic upgrading, the conversion of low-value polymers to high-value materials, could address this challenge. Among upgrading strategies, the sulfonation of aromatic polymers is a powerful approach to access high-value materials for a range of applications, such as ion-exchange resins and membranes, electronic materials, and pharmaceuticals. While many sulfonation methods have been reported, achieving high degrees of sulfonation while minimizing side reactions that lead to defects in the polymer chains remains challenging. Additionally, sulfonating agents are most often used in large excess, which prevents precise control over the degree of sulfonation of aromatic polymers and their functionality. Herein, we address these challenges using 1,3-disulfonic acid imidazolium chloride ([Dsim]Cl), a sulfonic acid-based ionic liquid, to sulfonate aromatic polymers and upgrade plastic waste to electronic materials. We show that stoichiometric [Dsim]Cl can effectively sulfonate model polystyrene up to 92% in high yields, with minimal defects and high regioselectivity for the

Polystyrene sulfonate

Sulfonic acid

10.1021/jacsau.4c00355

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Electronically Conductive Hydrogels by in Situ Polymerization of a Water‐Soluble EDOT‐Derived Monomer

Advanced Engineering Materials (2022)

Dan My Nguyen Yuhang Wu Abigail Nolin Chun‐Yuan Lo Tianzheng Guo

Electronically conductive hydrogels have gained popularity in bioelectronic interfaces because their mechanical properties are similar to biological tissues, potentially preventing scaring in implanted electronics. Hydrogels have low elastic moduli, due to their high water content, which facilitates their integration with biological tissues. To achieve electronically conductive hydrogels, however, requires the integration of conducting polymers or nanoparticles. These “hard” components increase the elastic modulus of the hydrogel, removing their desirable compatibility with biological tissues, or lead to the heterogeneous distribution of the conductive material in the hydrogel scaffold. A general strategy to transform hydrogels into electronically conductive hydrogels without affecting the mechanical properties of the parent hydrogel is still lacking. Herein, a two‐step method is reported for imparting conductivity to a range of different hydrogels by in‐situ polymerization of a water‐soluble and neutral conducting polymer precursor: 3,4–ethylenedioxythiophene diethylene glycol (EDOT‐DEG). The resulting conductive hydrogels are homogenous, have conductivities around 0.3 S m −1 , low impedance, and maintain an elastic modulus of 5–15 kPa, which is similar to the preformed hydrogel. The simple preparation and desirable properties of the conductive hydrogels are likely to lead to new materials and applications in tissue engineering, neural interfaces, biosensors, and electrostimulation.

Gelatin

Polypyrrole

In situ polymerization

10.1002/adem.202200280

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Combining Linker Design and Linker-Exchange Strategies for the Synthesis of a Stable Large-Pore Zr-Based Metal–Organic Framework

ACS Applied Materials & Interfaces (2018)

Hue Thi Nguyen Thach N. Tu My V. Nguyen Tien Nu Hoang Lo Hiroyasu Furukawa

A Zr(IV)-based metal–organic framework (MOF), termed reo-MOF-1 [Zr6O8(H2O)8(SNDC)4], composed of 4-sulfonaphthalene-2,6-dicarboxylate (HSNDC2–) linkers and Zr6O8(H2O)8(CO2)8 clusters was synthesized by solvothermal synthesis. Structural analysis revealed that reo-MOF-1 adopts the reo topology highlighted with large cuboctahedral cages (23 Å). This structure is similar to that found in DUT-52 (fcu topology), however, reo-MOF-1 lacks the body-centered packing of the 12-connected Zr6O4(OH)4(CO2)12 clusters, which is attributed to the subtle, but crucial influence in the bulkiness of functional groups on the linkers. The control experiments, where the ratio of H3SNDC/naphthalene-2,6-dicarboxylate linkers was varied, also support our finding that the bulky functionalities play a key role for defect-controlled synthesis. The reo-MOF-1A framework was obtained by linker exchange to yield a chemically and thermally stable material despite its large pores. Remarkably, reo-MOF-1A exhibits permanent porosity (Brunauer–Emmett–Teller and Langmuir surface areas of 2104 and 2203 m2 g–1, respectively). Owing to these remarkable structural features, reo-MOF-1A significantly enhances the yield in Brønsted acid-catalyzed reactions.

Linker

10.1021/acsami.8b11037

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Citations (27)