Zheqiong Wu

Fabrication of High‐Performance Flexible Alkaline Batteries by Implementing Multiwalled Carbon Nanotubes and Copolymer Separator

A flexible alkaline battery with multiwalled carbon nanotube (MWCNT) enhanced composite electrodes and polyvinyl alcohol (PVA)-poly (acrylic acid) (PAA) copolymer separator has been developed. Purified MWCNTs appear to be the most effective conductive additive, while the flexible copolymer separator not only enhances flexibility but also serves as electrolyte storage.

Instillation versus Inhalation of Multiwalled Carbon Nanotubes: Exposure-Related Health Effects, Clearance, and the Role of Particle Characteristics

Inhaled multiwalled carbon nanotubes (MWCNTs) may cause adverse pulmonary responses due to their nanoscale, fibrous morphology and/or biopersistance. This study tested multiple factors (dose, time, physicochemical characteristics, and administration method) shown to affect MWCNT toxicity with the hypothesis that these factors will influence significantly different responses upon MWCNT exposure. The study is unique in that (1) multiple administration methods were tested using particles from the same stock; (2) bulk MWCNT formulations had few differences (metal content, surface area/functionalization); and (3) MWCNT retention was quantified using a specialized approach for measuring unlabeled MWCNTs in rodent lungs. Male Sprague–Dawley rats were exposed to original (O), purified (P), and carboxylic acid functionalized (F) MWCNTs via intratracheal instillation and inhalation. Blood, bronchoalveolar lavage fluid (BALF), and lung tissues were collected at postexposure days 1 and 21 for quantifying biological responses and MWCNTs in lung tissues by programmed thermal analysis. At day 1, MWCNT instillation produced significant BALF neutrophilia and MWCNT-positive macrophages. Instilled O- and P-MWCNTs produced significant inflammation in lung tissues, which resolved by day 21 despite MWCNT retention. MWCNT inhalation produced no BALF neutrophilia and no significant histopathology past day 1. However, on days 1 and 21 postinhalation of nebulized MWCNTs, significantly increased numbers of MWCNT-positive macrophages were observed in BALF. Results suggest (1) MWCNTs produce transient inflammation if any despite persistence in the lungs; (2) instilled O-MWCNTs cause more inflammation than P- or F-MWCNTs; and (3) MWCNT suspension media produce strikingly different effects on physicochemical particle characteristics and pulmonary responses.

Water defluoridation using a nanostructured diatom–ZrO2 composite synthesized from algal Biomass

Frustules or the rigid amorphous silica cell wall of unicellular, photosynthetic microalgae with unique porous architecture has been used to synthesize a composite by immobilizing ZrO2 on its surface and in the pores. This was effective in water defluoridation. The average diameter of the composite was 80±2 nm and surface area was 140 m(2)/g. The adsorption isotherms followed both Langmuir and Freundlich models, and the composite was regenerable. Adsorption kinetics followed second order model and the adsorption capacity was as high as 11.32 mg/g, while the Langmuir maximum adsorption capacity (q(m)) reached 15.53 mg/g. The research findings highlight the potential of diatoms as hosts for nanomaterials for use in water treatment.

Length reduction of multi-walled carbon nanotubes via high energy ultrasonication and its effect on their dispersibility

Length dependent dispersibility of carboxylated multiwalled carbon nanotubes is presented using a novel approach that ensures the same diameter and the degree of functionalization. The longer multiwalled nanotubes were reduced in length by ultrasonication and then their dispersibility was studied in comparison to the original tubes. Colloidal studies showed dependence on the length where the shorter tubes showed higher aggregation in terms of larger particle size, zeta potential and lower critical coagulation concentrations in the presence of electrolytes. It is hypothesized that the longer tubes entangled more leading to a more complex electrostatic double layer that increased their stability.

Enhanced charge-carrier transport through shorter carbon nanotubes in organic photovoltaics.

We demonstrate for the first time the efficiency improvement of organic photovoltaics by the addition of shorter multiwalled carbon nanotubes (MWNTs) generated by size sorting. The different size MWNTs were generated by size sorting a batch of carboxylated MWNTs and were introduced as charge carriers in poly(3-hexylthiophene) (P3HT):phenyl-C61-butyric acid methyl ester (PCBM) bulk heterojunction photovoltaic cells. As compared to a control with only PCBM, the addition of the long and short MWNT resulted in 12 and 34% improvement in short circuit current density (Jsc) respectively. The results indicate that length of carbon nanotubes is an important consideration in photovoltaic and possibly other nanoelectronic devices.

Effects of Multiwalled Carbon Nanotube Surface Modification and Purification on Bovine Serum Albumin Binding and Biological Responses

The potential diagnostic and therapeutic applications such as drug delivery of multi-walled carbon nanotubes (MWCNTs) are being increasingly explored due to their unique mechanical, chemical and biological properties. Carboxylation of MWCNTs has been widely used to improve the solubility in aqueous systems, and for further functionalization with biologically active moieties. Purity of carboxylated MWCNTs is of great importance in nanomedicine. An important consideration is that oxidation debris is generated during the process of carboxylation, which can be removed by base washing. We hypothesized that surface modification as well as further purification by debris removal may alter physicochemical properties of MWCNTs and their ability to bind proteins. In this study, we utilized pristine MWCNT carboxylated MWCNTs (F-MWCNTs) and base-washed carboxylated MWCNTs (BW-F-MWCNTs) to examine formation of a bovine serum albumin (BSA) protein corona and impact on biological responses. We found that carboxylation increased the capability of F-MWCNTs to bind BSA, and base washing further increased this binding by 41% implying that purification of F-MWCNTs is an important consideration in biological applications. The BSA protein corona decreased the hydrodynamic size of MWCNTs by nearly 50% because the coating improved colloidal behavior. The effect was significantly less pronounced for F-MWCNTs and BW-F-MWCNTs because they were highly dispersible to begin with. Functionalization increased cellular uptake by both rat aortic endothelial cells (RAEC) and macrophage-like murine cells (RAW264.7), while base washing showed results similar to the functionalized analog. Interestingly, BSA binding downregulated mRNA levels of interleukin-6 (IL-6) and heme oxygenase 1 (Hmox1) in RAEC cells but upregulated the expression of IL-6 and Hmox1 in RAW264.7 cells, indicating the dependence of cell types in biological responses to MWCNTs. Overall, our study demonstrated that surface modification as well as further purification impacted the interaction of MWCNTs with proteins and subsequent cellular responses. Interestingly, while the corona associated with the F-MWCNTs and BW-F-MWCNTs were significantly different, their respective cellular uptake and biological responses were similar. This implied that surface functionalization played a more important role than surface corona.

The Effects of Varying Degree of MWCNT Carboxylation on Bioactivity in Various In Vivo and In Vitro Exposure Models

Functionalization has been shown to alter toxicity of multi-walled carbon nanotube (MWCNT) in several studies. This study varied the degree of functionalization (viz., amount of MWCNT surface carboxylation) to define the relationship between the extent of carboxylation and effects in a variety of in vitro cell models and short-term ex vivo/in vivo particle exposures. Studies with vitamin D3 plus phorbol ester transformed THP-1 macrophages demonstrated that functionalization, regardless of amount, corresponded with profoundly decreased NLRP3 inflammasome activation. However, all MWCNT variants were slightly toxic in this model. Alternatively, studies with A549 epithelial cells showed some varied effects. For example, IL-33 and TNF-α release were related to varying amounts of functionalization. For in vivo particle exposures, autophagy of alveolar macrophages, measured using green fluorescent protein (GFP)- fused-LC3 transgenic mice, increased for all MWCNT tested three days after exposure, but, by Day 7, autophagy was clearly dependent on the amount of carboxylation. The instilled source MWCNT continued to produce cellular injury in alveolar macrophages over seven days. In contrast, the more functionalized MWCNT initially showed similar effects, but reduced over time. Dark-field imaging showed the more functionalized MWCNTs were distributed more uniformly throughout the lung and not isolated to macrophages. Taken together, the results indicated that in vitro and in vivo bioactivity of MWCNT decreased with increased carboxylation. Functionalization by carboxylation eliminated the bioactive potential of the MWCNT in the exposure models tested. The observation that maximally functionalized MWCNT distribute more freely throughout the lung with the absence of cellular damage, and extended deposition, may establish a practical use for these particles as a safer alternative for unmodified MWCNT.