Abstract
Hydrogels, known for their mechanical and chemical similarity to biological tissues, are widely used in biotechnologies, whereas semiconductors provide advanced electronic and optoelectronic functionalities such as signal amplification, sensing, and photomodulation. Combining semiconducting properties with hydrogel designs can enhance biointeractive functions and intimacy at biointerfaces, but this is challenging owing to the low hydrophilicity of polymer semiconductors. We developed a solvent affinity–induced assembly method that incorporates water-insoluble polymer semiconductors into double-network hydrogels. These semiconductors exhibited tissue-level moduli as soft as 81 kilopascals, stretchability of 150% strain, and charge-carrier mobility up to 1.4 square centimeters per volt per second. When they are interfaced with biological tissues, their tissue-level modulus enables alleviated immune reactions. The hydrogel’s high porosity enhances molecular interactions at semiconductor-biofluid interfaces, resulting in photomodulation with higher response and volumetric biosensing with higher sensitivity.
| Original language | English |
|---|---|
| Pages (from-to) | 431-439 |
| Number of pages | 9 |
| Journal | Science |
| Volume | 386 |
| Issue number | 6720 |
| DOIs | |
| State | Published - Oct 25 2024 |
Funding
We thank the University of Chicago Animal Resources Center (RRID: SCR_021806) for animal housing and use of their facility and equipment. All the animal experiments performed in this research were approved by the Institutional Animal Care and Use Committee of the University of Chicago under the protocol ACUP 72702. This work used the Soft Matter Characterization Facility (SMCF) and the Materials Research Science and Engineering Center (MRSEC) at the University of Chicago. Parts of the diagrams were created with BioRender.com. This work was supported by the US National Institutes of Health Director\u2019s New Innovator Award (1DP2EB034563) and the US Office of Naval Research (N00014-21-1-2266). This work was partially supported by the start-up fund from the University of Chicago. This research used beamline 7.3.3 of the Advanced Light Source, which is a US Department of Energy (DOE) Office of Science User Facility under contract no. DE-AC02-05CH11231. Y.W. was supported in part by an ALS Doctoral Fellowship in Residence. Z.C., Y.W., and X.G. acknowledge financial aid from an NSF grant (DMR-2047689) that enabled the thin-film tensile testing of the samples. B.T. acknowledges grant support from the US Army Research Office (W911NF-24-1-0053). P.L. acknowledges the Grier Prize for Innovation Research in the Biophysical Sciences. Work performed at the Center for Nanoscale Materials, a US DOE Office of Science User Facility, was supported by the US DOE, Office of Basic Energy Sciences, under contract no. DE-AC02-06CH11357. S. Wang is a CZ Biohub Investigator. Engineering Center (MRSEC) at the University of Chicago. Parts of the diagrams were created with BioRender.com. Funding: This work was supported by the US National Institutes of Health Director\u2019s New Innovator Award (1DP2EB034563) and the US Office of Naval Research (N00014-21-1-2266). This work was partially supported by the start-up fund from the University of Chicago. This research used beamline 7.3.3 of the Advanced Light Source, which is a US Department of Energy (DOE) Office of Science User Facility under contract no. DE-AC02-05CH11231. Y.W. was supported in part by an ALS Doctoral Fellowship in Residence. Z.C., Y.W., and X.G. acknowledge financial aid from an NSF grant (DMR-2047689) that enabled the thin-film tensile testing of the samples. B.T. acknowledges grant support from the US Army Research Office (W911NF-24-1-0053). P.L. acknowledges the Grier Prize for Innovation Research in the Biophysical Sciences. Work performed at the Center for Nanoscale Materials, a US DOE Office of Science User Facility, was supported by the US DOE, Office of Basic Energy Sciences, under contract no. DE-AC02-06CH11357. S. Wang is a CZ Biohub Investigator. Author contributions: S. Wang supervised this work. Y.D. and S. Wang designed the experiments. Y.D. synthesized the polymers and hydro-SCs. N.L. and N.S. performed and analyzed NMR. Y.D., Y. Li, S. Li, and S.C. fabricated and tested the OECT. Y.D. and Yo.Liu performed the conformability test. S. Wai performed biocompatibility study. Yu.Liu, J.X., and H.C.F. performed and analyzed the cryo-EM results. M.H. performed the STEM-EDS (energy dispersive spectroscopy) imaging and elemental mapping. Y. Li performed SEM imaging. Y.D. and H.C.F. performed the liquid AFM for swelling ratio measurement. Y.W. and C. Zhu performed the GIXD characterizations. Z.C., Y.W., K.T., and X.G. performed the FOW measurements. W.L. measured the fluorescent spectroscopy. Y.D., P.L., J.S., S. Lee, and B.T. performed the measurements for studying the photoelectrochemical and photothermal effect. Y.D. and M.W. carried out the thickness measurement. Y.D. and N.S. performed the diffusion test on semiconductor. Y.D., N.S., and N.L. carried out the enzyme immobilization and sensing test. N.S. performed the QCM and infrared measurements. C. Zhang and S.S. helped analyze the results. Y.D. and S. Wang wrote the paper. All authors reviewed and commented on the manuscript. Competing interests: S. Wang and Y.D. are inventors on patent application no. UCHI 25-T-008 submitted by the University of Chicago. Data and materials availability: All data are available in the manuscript or the supplementary materials. License information: Copyright \u00A9 2024 the authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original US government works. https://www. science.org/about/science-licenses-journal-article-reuse