Bioengineered liver crosslinked with nano-graphene oxide enables efficient liver regeneration via MMP suppression and immunomodulation.

Decellularized extracellular matrix scaffold, widely utilized for organ engineering, often undergoes matrix decomposition after transplantation and produces byproducts that cause inflammation, leading to clinical failure. Here we propose a strategy using nano-graphene oxide to modify the biophysical properties of decellularized liver scaffolds. Notably, we demonstrate that scaffolds crosslinked with nano-graphene oxide show high resistance to enzymatic degradation via direct inhibition of matrix metalloproteinase activity and increased mechanical rigidity. We find that M2-like macrophage polarization is promoted within the crosslinked scaffolds, which reduces graft-elicited inflammation. Moreover, we show that low activities of matrix metalloproteinases, attributed to both nano-graphene oxide and tissue inhibitors of metalloproteinases expressed by M2c, can protect the crosslinked scaffolds against in vivo degradation. Lastly, we demonstrate that bioengineered livers fabricated with the crosslinked scaffolds remain functional, thereby effectively regenerating damaged livers after transplantation into liver failure mouse models. Overall, nano-graphene oxide crosslinking prolongs allograft survival and ultimately improves therapeutic effects of bioengineered livers, which offer an alternative for donor organs.

Application of nano-graphene oxide as nontoxic disinfectant against alpha and betacoronaviruses.

New viruses are continuously emerging and recently there have been many great concerns on severe acute respiratory syndrome coronavirus (SARS-CoV-2). Nanographene oxide (nanoGO) has received much attention and is widely investigated to be utilised in therapy for infectious diseases by viruses. Thus, antiviral activity of nanoGO was evaluated using the porcine epidemic diarrhoea virus (PEDV), bovine coronavirus (BCoV), and SARS-CoV-2, which are all Alpha- and Beta-coronavirus. In a virus inhibition assay, the three viruses were inhibited by nanoGO in a dose-dependent manner, including attempts in the presence of high serum solution which partially mimicked biological fluid.

Sheet Resistance Analysis of Interface-Engineered Multilayer Graphene: Mobility Versus Sheet Carrier Concentration.

Both interlayer-undoped and interlayer-doped multilayer graphenes were prepared by the multiple transfers of graphene layers with multiple Cu etching (either dopant-free or doped during etching) and transfer, and the effect of interface properties on the electrical properties of multilayer graphene was investigated by varying the number of layers from 1 to 12. In both the cases, the sheet resistance decreased with increasing number of layers from 700 to 104 Ω/sq for the interlayer-undoped graphene and from 280 to 25 Ω/sq for the interlayer-doped graphene. Further, Hall measurements revealed that the origins of the sheet resistance reduction in the two cases are different. In the interlayer-undoped graphene, the sheet resistance decreased because of the increase in mobility with the addition of inner layers, which has a low carrier density and a high carrier mobility. On the other hand, it decreased because of the increase in sheet carrier density in the interlayer-doped multilayer graphene. The mobility and carrier density variations in both the cases were confirmed by fitting with the model of Hall effect in the heterojunction. In addition, we found that surface property modification by the doping of the top layer and the formation of double-layer graphene with different partial coverages allow the separate control of carrier density and mobility. Our study provides an effective approach for controlling the properties of multilayer graphene for electronic applications.

Ultraclean patterned transfer of single-layer graphene by recyclable pressure sensitive adhesive films.

We report an ultraclean, cost-effective, and easily scalable method of transferring and patterning large-area graphene using pressure sensitive adhesive films (PSAFs) at room temperature. This simple transfer is enabled by the difference in wettability and adhesion energy of graphene with respect to PSAF and a target substrate. The PSAF-transferred graphene is found to be free from residues and shows excellent charge carrier mobility as high as ∼17,700 cm(2)/V·s with less doping compared to the graphene transferred by thermal release tape (TRT) or poly(methyl methacrylate) (PMMA) as well as good uniformity over large areas. In addition, the sheet resistance of graphene transferred by recycled PSAF does not change considerably up to 4 times, which would be advantageous for more cost-effective and environmentally friendly production of large-area graphene films for practical applications.

Graphene-induced unusual microstructural evolution in Ag plated Cu foils.

Graphene-induced abnormal grain growth of Cu with a grain size of more than 1 mm(2) was observed on Cu-Ag alloy foil, and this phenomenon occurred only with graphene synthesis and only on the Cu-Ag alloy among various types of Cu foils.

Synthesis of CVD-graphene on rapidly heated copper foils.

Most chemical vapor deposition (CVD) systems used for graphene growth mainly employ convection and radiation heat transfer between the heating source and the metal catalyst in order to reach the activation temperature of the reaction, which in general leads to a long synthesis time and poor energy efficiency. Here, we report a highly time- and energy-efficient CVD setup, in which the metal catalyst (Cu) is designed to be physically contacted with a heating source to give quick heat transfer by conduction. The induced conduction heating enabled the usual effects of the pretreatment and annealing of Cu (i.e., annihilation of surface defects, impurities and contaminants) to be achieved in a significantly shorter time compared to conventional CVD. Notably, the rapid heating was observed to lead to larger grains of Cu with high uniformity as compared to the Cu annealed by conventional CVD, which are believed to be beneficial for the growth of high quality graphene. Through this CVD setup, bundles of high quality (∼252 Ω per square) and large area (over 16 inch) graphenes were able to be readily synthesized in 40 min in a significantly efficient way. When considering ease of scalability, high energy effectiveness and considerable productivity, our method is expected to be welcomed by industrialists.

Highly uniform growth of monolayer graphene by chemical vapor deposition on Cu-Ag alloy catalysts.

One of the major challenges for the practical application of graphene is the large scale synthesis of uniform films with high quality at lower temperature. Here, we demonstrate the use of Ag-plated Cu substrates in the synthesis of high-quality graphene films via chemical vapor deposition (CVD) of methane gas at temperatures as low as 900 °C. Various experimental analyses show that the plated Ag diffuses into Cu to form a uniform Cu-Ag alloy that suppresses the formation of multilayer nucleation and decreases the activation energy of precursor formation, leading to a lower synthesis temperature with enhanced monolayer coverage. In addition, we also observed an unusual Ag-assisted abnormal grain growth of Cu into the cube texture with larger grain sizes and reduced grain boundaries, which is believed to provide the homogeneous environment needed for uniform graphene growth.

Vapor-phase molecular doping of graphene for high-performance transparent electrodes.

Doping is an essential process to engineer the conductivity and work-function of graphene for higher performance optoelectronic devices, which includes substitutional atomic doping by reactive gases, electrical/electrochemical doping by gate bias, and chemical doping by acids or reducing/oxidizing agents. Among these, the chemical doping has been widely used due to its simple process and high doping strength. However, it also has an instability problem in that the molecular dopants tend to gradually evaporate from the surface of graphene, leading to substantial decrease in doping effect with time. In particular, the instability problem is more serious for n-doped graphene because of undesirable reaction between dopants and oxygen or water in air. Here we report a simple method to tune the electrical properties of CVD graphene through n-doping by vaporized molecules at 70 °C, where the dopants in vapor phase are mildly adsorbed on graphene surface without direct contact with solution. To investigate the dependence on functional groups and molecular weights, we selected a series of ethylene amines as a model system, including ethylene diamine (EDA), diethylene triamine (DETA), and triethylene tetramine (TETA) with increasing number of amine groups showing different vapor pressures. We confirmed that the vapor-phase doping provides not only very high carrier concentration but also good long-term stability in air, which is particularly important for practical applications.

Fast synthesis of high-performance graphene films by hydrogen-free rapid thermal chemical vapor deposition.

The practical use of graphene in consumer electronics has not been demonstrated since the size, uniformity, and reliability problems are yet to be solved to satisfy industrial standards. Here we report mass-produced graphene films synthesized by hydrogen-free rapid thermal chemical vapor deposition (RT-CVD), roll-to-roll etching, and transfer methods, which enabled faster and larger production of homogeneous graphene films over 400 × 300 mm(2) area with a sheet resistance of 249 ± 17 Ω/sq without additional doping. The properties of RT-CVD graphene have been carefully characterized by high-resolution transmission electron microscopy, Raman spectroscopy, chemical grain boundary analysis, and various electrical device measurements, showing excellent uniformity and stability. In particular, we found no significant correlation between graphene domain sizes and electrical conductivity, unlike previous theoretical expectations for nanoscale graphene domains. Finally, the actual application of the RT-CVD films to capacitive multitouch devices installed in the most sophisticated mobile phone was demonstrated.

Efficient transfer of large-area graphene films onto rigid substrates by hot pressing.

Graphene films grown on metal substrates by chemical vapor deposition (CVD) method have to be safely transferred onto desired substrates for further applications. Recently, a roll-to-roll (R2R) method has been developed for large-area transfer, which is particularly efficient for flexible target substrates. However, in the case of rigid substrates such as glass or wafers, the roll-based method is found to induce considerable mechanical damages on graphene films during the transfer process, resulting in the degradation of electrical property. Here we introduce an improved dry transfer technique based on a hot-pressing method that can minimize damage on graphene by neutralizing mechanical stress. Thus, we enhanced the transfer efficiency of the large-area graphene films on a substrate with arbitrary thickness and rigidity, evidenced by scanning electron microscope (SEM) and atomic force microscope (AFM) images, Raman spectra, and various electrical characterizations. We also performed a theoretical multiscale simulation from continuum to atomic level to compare the mechanical stresses caused by the R2R and the hot-pressing methods, which also supports our conclusion. Consequently, we believe that the proposed hot-pressing method will be immediately useful for display and solar cell applications that currently require rigid and large substrates.