Shuaidi Zhang

Self-Powered Electronic Skin with Biotactile Selectivity

Power-generating flexible thin films for facile detection of biotactile events are fabricated from patterned metal-graphene oxide biopaper. These tactile materials are mechanically robust with a consistent output of 1 V and high response rate of 20 Hz. It is demonstrated that the simple quadruple electronic skin sensitively and selectively recognizes nine spatial biotactile positions and can readily be expanded.

Ultrastrong Freestanding Graphene Oxide Nanomembranes with Surface-Enhanced Raman Scattering Functionality by Solvent-Assisted Single-Component Layer-by-Layer Assembly

We report single-component ultrathin reduced graphene oxide (rGO) nanomembranes fabricated via nonconventional layer-by-layer assembly (LbL) of graphene oxide flakes, using organic solvent instead of water to provide strong complementary interactions and to ensure the uniform layered growth. This unique approach does not require regular polymeric from the assembly process or intermediate surface chemical modification. The resulting ultrastrong freestanding graphene oxide (rGO) LbL nanomembranes with a very low thickness of 3 nm (three GO monolayers) can be transferred over a large surface area across tens of square centimeters by using a facile surface-tension-assisted release technique. These uniform and ultrasmooth nanomembranes with high transparency (up to 93% at 550 nm) and high electrical conductivity (up to 3000 S/m) also exhibit outstanding mechanical strength of 0.5 GPa and a Youngs modulus of 120 GPa, which are several times higher than that of other reported regular rGO films. Furthermore, up to 94 wt % of silver nanoplates can be sandwiched between 5 nm GO layers to construct a flexible freestanding protected noble metal monolayer with surface-enhanced Raman scattering properties. These flexible rGO/Ag/rGO nanomembranes can be transferred and conformally coat complex surfaces and show a cleaner Raman signature, enhanced wet stability, and lower oxidation compared to bare Ag nanostructures.

Interfacial Shear Strength and Adhesive Behavior of Silk Ionomer Surfaces

The interfacial shear strength between different layers in multilayered structures of layer-by-layer (LbL) microcapsules is a crucial mechanical property to ensure their robustness. In this work, we investigated the interfacial shear strength of modified silk fibroin ionomers utilized in LbL shells, an ionic-cationic pair with complementary ionic pairing, (SF)-poly-l-glutamic acid (Glu) and SF-poly-l-lysine (Lys), and a complementary pair with partially screened Coulombic interactions due to the presence of poly(ethylene glycol) (PEG) segments and SF-Glu/SF-Lys[PEG] pair. Shearing and adhesive behavior between these silk ionomer surfaces in the swollen state were probed at different spatial scales and pressure ranges by using functionalized atomic force microscopy (AFM) tips as well as functionalized colloidal probes. The results show that both approaches were consistent in analyzing the interfacial shear strength of LbL silk ionomers at different spatial scales from a nanoscale to a fraction of a micron. Surprisingly, the interfacial shear strength between SF-Glu and SF-Lys[PEG] pair with partially screened ionic pairing was greater than the interfacial shear strength of the SF-Glu and SF-Lys pair with a high density of complementary ionic groups. The difference in interfacial shear strength and adhesive strength is suggested to be predominantly facilitated by the interlayer hydrogen bonding of complementary amino acids and overlap of highly swollen PEG segments.

Ligand-Exchange Dynamics on Gold Nanocrystals: Direct Monitoring of Nanoscale Polyvinylpyrrolidone–Thiol Domain Surface Morphology

We report direct high-resolution monitoring of an evolving mixed nanodomain surface morphology during thiol adsorption on polyvinylpyrrolidone (PVP)-stabilized single crystal gold nanocrystals. The thiol adsorption and replacement dynamics are much more complex than a simple complete substitution of the initial polymer ligand. We observed that during ligand exchange with linear thiol, the nanocrystal surface evolved from an initial 1 nm uniform PVP coating into a remarkably stable network of globular PVP domains 20-100 nm in size and ∼4 nm in height surrounded by thiol self-assembled monolayers. The final stability of such a mixed thiol-PVP surface morphology can possibly be attributed to the interfacial energy reduction from partially solvophilic surfaces and the entropic gain from mixed ligand surface layers. The ligand-exchange dynamics and the unusual equilibrium morphology revealed here provide important insights into both displacement dynamics of surface-bound molecules and the nanoscale peculiarities of surface functionalization of colloidal metal substrates.

Biotactile Sensors: Self‐Powered Electronic Skin with Biotactile Selectivity (Adv. Mater. 18/2016)

On page 3549, V. V. Tsukruk and co-workers develop self-powered ultrathin flexible films for bio-tactile detection. Graphene oxide materials are engineered for robust self-powered tactile sensing applications harnessing their electrochemical reactivity. The simple quadruple electronic skin sensor can recognize nine spatial bio-tactile positions with high sensitivity and selectivity-an approach that can be expanded towards large-area flexible skin arrays.

Dual-Excitation Nanocellulose Plasmonic Membranes for Molecular and Cellular SERS Detection

We demonstrate that cellulose nanofiber (CNF) biomaterials with high transparency and mechanical robustness can be combined with gold nanorods to form a multifunctional porous membrane for dual-mode surface-enhanced Raman scattering (SERS) detection of both small molecules and cells. The nanoporous nature of the nanofiber membranes allows for effective molecular filtration and preconcentration of the analytes, further boosting the SERS performance. Specifically, because of the low fluorescence and Raman background of the CNF matrix, extremely low loading density of gold nanorods can be used. The nanorod assemblies within the CNF network can be resonantly driven by a 532 nm laser (transverse plasmonic mode) and near resonantly driven at by a 785 nm laser (longitudinal mode), facilitating dual operational modes at two excitation wavelengths. The shorter wavelength excitation mode yields better Raman scattering efficiency and has been demonstrated to be capable of detecting rhodamine 6G (R6G) dyes down to picomolar concentrations. On the other hand, the longer wavelength excitation mode provides autofluorescence suppression for the better detection of microorganisms such as Escherichia coli, shortening the required integration time from hours to minutes. Upon drastically lowering the spectral background noise and utilizing nanofiltration, the plasmonic CNF membranes reported here show significantly improved SERS sensitivity and detection fidelity as compared to traditional metal, metal oxide, synthetic polymer, and paper SERS substrates.