Investigation of plant leaf-derived graphene quantum dot clusters via magnetic force microscopy.

Magnetic force microscopy (MFM) is utilized to characterize the magnetic moment in nanostructured plant leaf-derived graphene quantum dot clusters (GQDCs). The MFM signal reveals that the magnetic response of the GQDCs depends on the height and width of the GQDCs. However, individual GQDs, and smaller clusters with widths of less than 20 nm, have not shown any observable magnetic signal. Importantly, experimental analyses suggest that the magnetic signal of GQDCs distributed in a plane can be effectively detected at room temperature. These results could pave the way for future graphene-based magnetic storage media and spin manipulation quantum devices.

Green synthesis of catalytic gold/bismuth oxyiodide nanocomposites with oxygen vacancies for treatment of bacterial infections.

We have developed a simple and green solution for the synthesis of catalytic gold-doped bismuth oxyiodide (Au/BiOI) nanocomposites at room temperature from an aqueous mixture of gold ions, bismuth ions, and iodide ions. Au nanoparticles (NPs) were formed in situ and doped into BiOI nanosheets. The oxygen vacancies generated in BiOI give rise to its oxidase-like activity, and Au doping facilitated the reaction leading to a 4-fold higher oxidase-like activity of the Au/BiOI nanocomposite. The Au/BiOI nanocomposites showed wide spectrum antimicrobial activity not only against non-multidrug-resistant E. coli, K. pneumoniae, S. enteritidis, S. aureus, and B. subtilis bacteria, but also against multidrug-resistant bacteria, methicillin-resistant S. aureus (MRSA). The gold doping reduced the minimal inhibitory concentration value by ∼2000-fold for the Au/BiOI nanocomposite, in comparison with only BiOI nanoparticles. The bactericidal property of the Au/BiOI nanocomposite arose from the combined effect of the disruption of the bacterial membrane through a strong interaction of the nanocomposite with the bacteria and the generation of reactive oxygen species. Also, the Au/BiOI nanocomposite is highly biocompatible, which has been demonstrated in vitro by analysis of cytotoxicity and hemolysis, and in vivo by evaluating ocular tissue responses. Furthermore, intrastromal administration of Au/BiOI nanocomposites can effectively alleviate S. aureus-induced bacterial keratitis in rabbits, suggesting a significant disinfectant benefit in preclinical studies. The Au/BiOI nanocomposites show great potential for the inactivation of bacterial pathogens in an aqueous environment and treatment of bacterial infection-induced diseases.

Smart app-based on-field colorimetric quantification of mercury via analyte-induced enhancement of the photocatalytic activity of TiO2-Au nanospheres.

We have devised a unique strategy for highly sensitive, selective, and colorimetric detection of mercury based on analyte-induced enhancement of the photocatalytic activity of TiO2-Au nanospheres (TiO2-Au NSs) toward degradation of methylene blue (MB). Through electrostatic interactions, Au nanoparticles are attached to poly-(sodium 4-styreneulfonate)/poly(diallyldimethylammonium chloride) modified TiO2 nanoparticles, which then form an Au shell on each TiO2 core through reduction of Au3+ with ascorbic acid. Notably, the deposition of Hg species (Hg2+/CH3Hg+) onto TiO2-Au NSs through strong Au-Hg aurophilic interactions speeds up catalytic degradation of MB. The first-order degradation rates of MB by TiO2-Au NSs and TiO2-Au-Hg NSs are 1.4 × 10-2 min-1 and 2.1 × 10-2 min-1, respectively. Using a commercial absorption spectrometer, the TiO2-Au NSs/MB approach provides linearity (R2 = 0.98) for Hg2+ over a concentration range of 10.0 to 100.0 nM, with a limit of detection (LOD) of 1.5 nM. On the other hand, using a low-cost smartphone app that records the color changes (ΔRGB) of MB solution based on the red-blue-green (RGB) component values, the TiO2-Au NSs/MB approach provides an LOD of 2.0 nM for Hg2+ and 5.0 nM for CH3Hg+, respectively. Furthermore, the smartphone app sensing system has been validated for the analyses of various samples, including tap water, lake water, soil, and Dorm II, showing its great potential for on-line analysis of environmental and biological samples. Graphical Abstract ᅟ.

Facet- and structure-dependent catalytic activity of cuprous oxide/polypyrrole particles towards the efficient reduction of carbon dioxide to methanol.

The preparation of cost-effective, stable catalysts for the selective reduction of carbon dioxide (CO2) to C1 products such as methanol is extremely important because methanol can be used directly as a fuel or it can be converted into other value-added products. However, the catalysts currently used for the reduction of CO2 to methanol exhibit poor selectivity, poor stability and very low faradaic efficiency. Herein, we used low-cost, stable cuprous oxide/polypyrrole (Cu2O/Ppy) particles having structures of octahedra and icosahedra (microflowers) that were prepared on linen texture (LT) papers for the selective reduction of CO2 to form a value-added single C1 product, methanol. The Cu2O/Ppy particles possessing both octahedral and microflower shapes with exposed low-index (111) facets and high-index (311) and (211) facets are denoted as Cu2O(OL-MH)/Ppy particles. The as-prepared Cu2O(OL-MH)/Ppy particles exhibited high catalytic activity and selectivity towards the electrochemical reduction of CO2 at -0.85 V vs. RHE to form methanol, with a faradaic efficiency of 93 ± 1.2% and an average methanol formation rate of 1.61 ± 0.02 µmol m-2 s-1. The X-ray photoelectron spectroscopy (XPS) analysis revealed that the pyrrolic nitrogen atoms present in the Ppy shell played a dominant role as active sites for CO2 molecules. The Raman bands of Ppy and Cu2O did not shift even after being subjected to electrolysis for several hours, suggesting superior stability of the Cu2O(OL-MH)/Ppy particles. The high resolution microscopic, spectroscopic, diffraction and electrochemical analysis results clearly revealed that the Ppy shell protected the Cu2O particles and avoided corrosion, dissolution, and structural and crystal facet changes, leading to greater stability. The low-cost, durable, flexible, and catalytically active Cu2O(OL-MH)/Ppy LT paper holds great potential for catalytic, photocatalytic and energy storage applications.

Wrinkled 2D Materials: A Versatile Platform for Low-Threshold Stretchable Random Lasers.

A stretchable, flexible, and bendable random laser system capable of lasing in a wide range of spectrum will have many potential applications in next- generation technologies, such as visible-spectrum communication, superbright solid-state lighting, biomedical studies, fluorescence, etc. However, producing an appropriate cavity for such a wide spectral range remains a challenge owing to the rigidity of the resonator for the generation of coherent loops. 2D materials with wrinkled structures exhibit superior advantages of high stretchability and a suitable matrix for photon trapping in between the hill and valley geometries compared to their flat counterparts. Here, the intriguing functionalities of wrinkled reduced graphene oxide, single-layer graphene, and few-layer hexagonal boron nitride, respectively, are utilized to design highly stretchable and wearable random laser devices with ultralow threshold. Using methyl-ammonium lead bromide perovskite nanocrystals (PNC) to illustrate the working principle, the lasing threshold is found to be ≈10 µJ cm-2 , about two times less than the lowest value ever reported. In addition to PNC, it is demonstrated that the output lasing wavelength can be tuned using different active materials such as semiconductor quantum dots. Thus, this study is very useful for the future development of high-performance wearable optoelectronic devices.

Dirac point induced ultralow-threshold laser and giant optoelectronic quantum oscillations in graphene-based heterojunctions.

The occurrence of zero effective mass of electrons at the vicinity of the Dirac point is expected to create new paradigms for scientific research and technological applications, but the related discoveries are rather limited. Here, we demonstrate that a simple architecture composed of graphene quantum dots sandwiched by graphene layers can exhibit several intriguing features, including the Dirac point induced ultralow-threshold laser, giant peak-to-valley ratio (PVR) with ultra-narrow spectra of negative differential resistance and quantum oscillations of current as well as light emission intensity. In particular, the threshold of only 12.4 nA cm-2 is the lowest value ever reported on electrically driven lasers, and the PVR value of more than 100 also sets the highest record compared with all available reports on graphene-based devices. We show that all these intriguing phenomena can be interpreted based on the unique band structures of graphene quantum dots and graphene as well as resonant quantum tunneling.In graphene, electrons possess zero effective mass in proximity to the Dirac point, an unusual feature that could trigger the development of novel photonic devices. Here, the authors combine graphene quantum dots with two graphene layers and observe laser action with ultralow threshold.

Polymer/reduced graphene oxide functionalized sponges as superabsorbents for oil removal and recovery.

Polyurethane dish-washing (PU-DW) sponges are functionalized sequentially with polyethylenimine (PEI) and graphene oxide (GO) to form PEI/reduced graphene oxide (RGO) PU-DW sponges. The PEI/RGO PU-DW sponge consists of PEI/RGO sheets having numerous pores, with diameters ranging from 236 to 254nm. To further enhance hydrophobicity and absorption capacity of oil, PEI/RGO PU-DW sponge is further coated with 20% phenyltrimethoxysilane (PTMOS). The PTMOS/PEI/RGO PU-DW sponge absorbs various oils within 20s, with maximum absorption capacity values of 880% and 840% for bicycle chain oil and motorcycle engine oil, respectively. The absorbed oils were released completely by squeezing or immersed in hexane. The PTMOS/PEI/RGO PU-DW sponge efficiently separates oil/water mixtures through a flowing system. Having the advantages of faster absorption rate, reusability, and low cost, the PTMOS/PEI/RGO PU-DW sponge holds great potential as a superabsorbent for efficient removal and recovery of oil spills as well as for the separation of oil/water mixtures.

Synthesis, Optical Properties, and Sensing Applications of Gold Nanodots.

In this Personal Account, we briefly address our journey in developing photoluminescent nanomaterials for sensing purposes, with a focus on gold nanodots (Au NDs). Their synthetic strategies, optical properties, and sensing applications are emphasized. The Au NDs can be simply prepared from the etching of small-sized Au nanoparticles (<3 nm in diameter) by thiol compounds such as 11-mercaptoundecanoic acid under alkaline conditions. This simple approach allows the preparation of various functional Au NDs by choosing different thiol compounds as etching agents. Since the optical properties of Au NDs are highly dependent on the core and shell of each Au ND, the selection of etching reagents is important. Over the years we have developed various sensing systems using Au NDs for the detection of metal ions, anions, and proteins, based on analyte-induced photoluminescence quenching/enhancement of Au NDs as a result of changes in their oxidation state, shell composition, and structure.

Highly Stretchable and Sensitive Photodetectors Based on Hybrid Graphene and Graphene Quantum Dots.

Stretchable devices possess great potential in a wide range of applications, such as biomedical and wearable gadgets and smart skin, which can be integrated with the human body. Because of their excellent flexibility, two-dimensional (2D) materials are expected to play an important role in the fabrication of stretchable devices. However, only a limited number of reports have been devoted to investigating stretchable devices based on 2D materials, and the stretchabilities were restricted in a very small strain. Moreover, there is no report related to the stretchable photodetectors derived from 2D materials. Herein, we demonstrate a highly stretchable and sensitive photodetector based on hybrid graphene and graphene quantum dots (GQDs). A unique rippled structure of poly(dimethylsiloxane) is used to support the graphene layer, which can be stretched under an external strain far beyond published reports. The ripple of the device can overcome the native stretchability limit of graphene and enhance the carrier generation in GQDs due to multiple reflections of photons between the ripples. Our strategy presented here can be extended to many other material systems, including other 2D materials. It therefore paves a key step for the development of stretchable electronics and optical devices.