Functionalized graphene oxide serves as a novel vaccine nano-adjuvant for robust stimulation of cellular immunity.

Benefiting from their unique physicochemical properties, graphene derivatives have attracted great attention in biomedicine. In this study, we carefully engineered graphene oxide (GO) as a vaccine adjuvant for immunotherapy using urease B (Ure B) as the model antigen. Ure B is a specific antigen for Helicobacter pylori, which is a class I carcinogen for gastric cancer. Polyethylene glycol (PEG) and various types of polyethylenimine (PEI) were used as coating polymers. Compared with single-polymer modified GOs (GO-PEG and GO-PEI), certain dual-polymer modified GOs (GO-PEG-PEI) can act as a positive modulator to promote the maturation of dendritic cells (DCs) and enhance their cytokine secretion through the activation of multiple toll-like receptor (TLR) pathways while showing low toxicity. Moreover, this GO-PEG-PEI can serve as an antigen carrier to effectively shuttle antigens into DCs. These two advantages enable GO-PEG-PEI to serve as a novel vaccine adjuvant. In the subsequent in vivo experiments, compared with free Ure B and clinically used aluminum-adjuvant-based vaccine (Alum-Ure B), GO-PEG-PEI-Ure B induces stronger cellular immunity via intradermal administration, suggesting promising applications in cancer immunotherapy. Our work not only presents a novel, highly effective GO-based vaccine nano-adjuvant, but also highlights the critical roles of surface chemistry for the rational design of nano-adjuvants.

Functionalized graphene oxide in microbial engineering: An effective stimulator for bacterial growth.

Whether graphene and graphene oxide (GO) would affect the activities of bacteria has been under debate. Nevertheless, how graphene derivatives with biocompatible coatings interact with microorganisms and the underlying mechanisms are important issues for nanobiotechnology, and remain to be further explored. Herein, three new types of nano-GOs functionalized with polyethylene glycol (nGO-PEGs) were synthesized by varying the PEGylation degree, and their effects on Escherichia coli (E. coli) were carefully investigated. Interestingly, nGO-PEG (1:1), the one with relatively lower PEGylation degree, could significantly stimulate bacterial growth, whereas as-made GO and the other two nGO-PEGs showed no effect. Further analysis revealed that nGO-PEG (1:1) treatment significantly accelerated FtsZ-ring assembly, shortening Phase 1 in the bacterial cell cycle. Both DNA synthesis and extracellular polymeric substance (EPS) secretion were also dramatically increased. This unique phenomenon suggests promising potentials in microbial engineering as well as in clinical detection of bacterial pathogens. As a proof-of-concept, nGO-PEG (1:1) treatment could remarkably enhance (up to 6-fold) recombinant protein production in engineered bacteria cells. To our best knowledge, this is the first demonstration of functionalized GO as a novel, positive regulator in microbial engineering. Moreover, our work highlights the critical role of surface chemistry in modulating the interactions between nanomaterials and microorganisms.

Graphene Oxide Selectively Enhances Thermostability of Trypsin.

In the past few years, graphene and its derivative, graphene oxide (GO), have been extensively studied for their applications in biotechnology. In our previous work, we reported certain PEGylated GOs (GO-PEGs) can selectively promote trypsin activity and enhance its thermostability. To further explore this, here we synthesized a series of GO-PEGs with varying PEGylation degrees. Enzymatic activity assay shows that both GO and GO-PEGs can protect trypsin, but not chymotrypsin, from thermal denaturation at high temperature. Surprisingly, the lower the PEGylation degree, the better the protection, and GO as well as the GO-PEG with the lowest PEGylation degree show the highest protection efficiency (∼70% retained activity at 70 °C). Fluorescence spectroscopy analysis shows that GO/GO-PEGs have strong interactions with trypsin. Molecular Dynamics (MD) simulation results reveal that trypsin is adsorbed onto the surface of GO through its cationic residues and hydrophilic residues. Different from chymotrypsin adsorbed on GO, the active site of trypsin is covered by GO. MD simulation at high temperature shows that, through such interaction with GO, trypsin's active site is therefore stabilized and protected by GO. Our work not only illustrates the promising potential of GO/GO-PEGs as efficient, selective modulators for trypsin, but also provides the interaction mechanism of GO with specific proteins at the nano-bio interface.

Graphene-based nanocomposite as an effective, multifunctional, and recyclable antibacterial agent.

The development of new antibacterial agents that are highly effective are of great interest. Herein, we present a recyclable and synergistic nanocomposite by growing both iron oxide nanoparticles (IONPs) and silver nanoparticles (AgNPs) on the surface of graphene oxide (GO), obtaining GO-IONP-Ag nanocomposite as a novel multifunctional antibacterial material. Compared with AgNPs, which have been widely used as antibacterial agents, our GO-IONP-Ag shows much higher antibacterial efficiency toward both Gram-negative bacteria Escherichia coli (E. coli) and Gram-positive bacteria Staphylococcus aureus (S. aureus). Taking the advantage of its strong near-infrared (NIR) absorbance, photothermal treatment is also conducted with GO-IONP-Ag, achieving a remarkable synergistic antibacterial effect to inhibit S. aureus at a rather low concentration of this agent. Moreover, with magnetic IONPs existing in the composite, we can easily recycle GO-IONP-Ag by magnetic separation, allowing its repeated use. Given the above advantages as well as its easy preparation and cheap cost, GO-IONP-Ag developed in this work may find potential applications as a useful antibacterial agent in the areas of healthcare and environmental engineering.

Silver and gold icosahedra: one-pot water-based synthesis and their superior performance in the electrocatalysis for oxygen reduction reactions in alkaline media.

Much effort has gone into generating polyhedral noble metal nanostructures because of their superior electrocatalytic activities for fuel cells. Herein, we report uniform, high-yield icosahedral silver and gold nanoparticles by using a facile one-pot, seedless, water-based approach that incorporates polyvinyl pyrrolidone and ammonia. Electrocatalysis of the oxygen-reduction reaction was carried out in alkaline media to evaluate the performance of the icosahedral nanoparticles. They showed excellent stability and much higher electrocatalytic activity than the spherelike nanoparticles; they display a positive shift in reduction peak potential for O(2) of 0.14 and 0.05 V, while the reduction peak currents of the silver and gold icosahedra are 1.5- and 1.6-fold, respectively, better than the spherelike nanoparticles. More importantly, the icosahedral nanoparticles display electrocatalytic activities comparable with commercial Pt/C electrocatalysts. The facile preparation of icosahedral silver and gold nanoparticles and their superior performance in the oxygen reduction reaction render them attractive replacements for Pt as cathode electrocatalysts in alkaline fuel cells.

Facile subsequently light-induced route to highly efficient and stable sunlight-driven Ag-AgBr plasmonic photocatalyst.

In this paper, we successfully fabricate a stable and highly efficient direct sunlight plasmonic photocatalyst Ag-AgBr through a facile hydrothermal and subsequently sunlight-induced route. The diffuse reflectance spectra of Ag-AgBr indicate strong absorption in both UV and visible light region. The obtained photocatalyst shows excellent sunlight-driven photocatalytic performance. It can decompose organic dye within several minutes under direct sunlight irradiation and maintain a high level even though used five times. In addition, both the scanning electron microscopy images and X-ray photoelectron spectroscopy dates reveal the as-prepared photocatalyst to be very stable. Moreover, the mechanism suggests that the high photocatalytic activity and excellent stability result from the super sensitivity of AgBr to light, the surface plasmon resonance of Ag nanoparticles in the region of visible light, and the complexation between Ag(+) and nitrogen atom. Thus, the facile preparation and super performance of Ag-AgBr will make it available to utilize sunlight efficiently to remove organic pollutants, destroy bacteria, and so forth.