Search

For TiO2-based photoanodes, the interfacial coupling between TiO2 and conductive materials (e.g., carbon) plays a vital role in determining the electron transfer efficiency and thus photoelectrical performance. In this paper, we describe a facile approach to effectively engineering the interfacial coupling between reduced graphene oxide (RGO) and TiO2 in well-designed one-dimensional (1D) RGO-wrapped TiO2 nanofibers, which act as ultrafast electron transfer bridges when implanted in photoanodes. The 3–5 nm RGO nanoshells were hybridized with TiO2 nanofibers as an electron donor component via d–π electron orbital overlap between C and Ti atoms, by adopting a thermal reduction at 450 °C. Remarkable photoelectric improvement, in terms of high photocurrent density by 2.2-fold and ultralow charge transfer resistance (Rct) by 0.2-fold, is ascribed to the interfacial charge transfer. Completely reduced RGO in RGO/TiO2 nanofibers was not necessary at the expense of their hydrophilicity, as it led to unexpected isolation in the photoanodes. The thermal reduction temperature of RGO/TiO2 nanofibers was found to be critical, and a maximal photocurrent density could be achieved by 2.7-fold at 530 °C. An excess of RGO/TiO2 nanofibers of more than 5 wt% had a degrading effect on the photoelectrical activity, largely due to the light-block effect and isolation in the matrix. This strategy provides new insight for tuning the intrinsic chemical and/or physical properties of well-designed semiconductor nanostructures with promising photoactivities in highly efficient photovoltaic devices. [ABSTRACT FROM AUTHOR]

Ultrafine noble metals have emerged as advanced nanocatalysts in modern society but still suffer from unavoidable sintering at temperatures above 250 °C (e.g., Pt). In this work, closely packed CeO 2 grains were confined elegantly in fibrous nanostructures and served as a porous support for stabilizing sub-3 nm Pt clusters. Through precisely manipulating the asymmetry of obtained nanofibers, uneven strain was induced within C-shaped CeO 2 nanofibers with tensile strain at the outer side and compressive strain at the inner side. As a result, the enriched oxygen vacancies significantly improved adhesion of Pt to CeO 2 , thereby boosting the sinter-resistance of ultraclose sub-3 nm Pt clusters. Notably, no aggregation was observed even after exposure to humid air at 750 °C for 12 h, which is far beyond their Tammann temperature (sintering onset temperature, below 250 °C). In situ HAADF-STEM observation revealed a unique sintering mechanism, wherein Pt clusters initially migrate toward the grain boundaries with concentrated stain and undergo slight coalescence, followed by subsequent Ostwald ripening at higher temperatures. Moreover, the sinter-resistant Pt/C-shaped CeO 2 effectively catalyzed soot combustion (over 700 °C) in a durable manner. This work provides a new insight for developing sinter-resistant catalysts from the perspective of strain engineering within nano-oxides.

Photothermal heating and photocatalytic treatment are two solar-driven water processing approaches by harnessing NIR and UV-vis light, respectively, which can fully utilize solar energy if integrated. However, it remains a challenge to achieve high performance in both approaches when integrated in a material due to uncontrollable heat diffusion. Here, we report a demonstration of heat confinement on photothermal sites and fluid cooling on photocatalysis sites at the nanoscale, within a well-designed heat and fluid confinement nanofiber reactor. Photothermal and photocatalytic nanostructures were alternatively aligned in electrospun nanofibers for on-demand nanofluidic thermal management as well as easy folding into 3D structures with enhanced light utilization and mass transfer. Such a design showed simultaneously high photothermal evaporation rate (2.59 kg m -2 h -1 , exceeding the limit rate) and efficient photocatalytic upcycling of microplastics pollutant into valued products. Enabled by controlled photothermal heating, the valued main product (i.e., methyl acetate) can be evaporated out with 100% selectivity by in situ separation., Competing Interests: Competing interests statement:The authors declare no competing interest.

Airborne particulate matter (PM) primarily resulting from fossil fuel burning is an increasingly global issue. In this work, an intrinsically fragile TiO 2 nanofibrous mat was facilely engineered with good structural integrity, flexibility, foldability, and high-temperature resistance (~1300 °C), by suppressing the sintering ( i.e. , growth) of nanocrystallites in each single nanofiber. Such functionalization enables self-regenerative air filtration for PM capture and in situ catalytic elimination in a "one-stone-two-birds" approach. Finite element analysis simulation revealed the retained nanopores in each anti-sintering nanofiber could facilitate the air flow during filtration. Without any chemical or physical modification, this self-standing and lightweight (7.1 g m -2 ) fibrous mat showed 96.05% filtration efficiency for 3-5 μm NaCl particles, with a low pressure drop of only 18 Pa and high quality factor of 0.179 Pa -1 under an airflow velocity of 32 L min -1 . By utilizing its photocatalytic attribute, the nanofibrous mat in situ eliminated the captured particles from incense burning under one Sun irradiation in 4 h, and thereby spontaneously regenerated in an easy manner. The straightforward grafting of Au nanoparticles onto nanofibers could enable a quick degradation toward cigarette smoke, mainly due to the photothermally elevated local temperature by Au around the reactive sites. The plasmonic fibrous mat kept a high and stable filtration efficiency of PM 0.3 , PM 2.5 , and PM 10 over 98.62%, 99.76%, and 99.99% during an outdoor long-term filtration test for 12 h under sunlight irradiation (Nanjing, China, September, 26 th , 2020, 7:30 to 19:30). This work provides a solution for solving the airborne pollution from its source, prolonging the lifetime of the filter, and avoiding the risk of producing secondary pollution.

Recently, there has been strong interest in flexible and wearable electronics to meet the technological demands of modern society. Environmentally-friendly and scalable electronic textiles is a key area that is still significantly underdeveloped. Here, we describe a novel strain sensor composed of aligned cellulose acetate (CA) nanofibers with belt-like morphology and a reduced graphene oxide (RGO) layer. The unique spatial alignment, microstructure and wettability of CA nanofibrous membranes facilitate their close contact with deposited GO colloids. After a portable and fast hot-press process within 700 s at 150 °C, the GO on CA membrane can be facilely reduced to a conductive RGO layer. Moreover, the connection among contiguous CA nanofibers and the interaction between the GO and CA substrate were both highly enhanced, resulting in superior mechanical strength with Young's modulus of 1.3 GPa and small sheet resistance lower than 10 kΩ. Therefore, the conductive RGO/CA membrane was successfully utilized as a strain sensor in a broad deformation range and with versatile deformation types. Moreover, the distinctive mechanical strength under different stretch angles endowed the well-aligned RGO/CA film with intriguing sensitivity against stress direction. Such a cost-effective and environmentally-friendly method can be easily extended to the scalable production of graphene-based flexible electronic textiles.

Iron oxide nanoparticles (NPs) possessing peroxidase-like catalytic activity have been widely explored in recent decades, owing to their high stability against harsh conditions, low cost, flexibility in structure design and composition, adjustable activities and excellent biocompatibility in comparison with natural enzymes. Recently, a lot of great achievements have been made in this field of iron oxide nanozymes, however, this research has now reached a bottleneck in that the maximum activity enhancement is difficult to achieve via a material design. Hence, in this work, visible light was introduced to improve the peroxidase-like activity of Fe 2 O 3 NPs synthesized via a combination of electrospinning technology and hydrothermal reaction. Our results showed that with the assistance of visible light, Fe 2 O 3 NPs exhibited at least 2.2-fold higher peroxidase activity than those tested under darkness, confirming the superiorly visible light promoted peroxidase-like catalytic activity of Fe 2 O 3 NPs. Furthermore, the affinity and maximum reaction velocity of Fe 2 O 3 nanoflowers (bandgap = 1.78 eV) towards 3,3',5,5'-tetramethylbenanozymeidine (TMB) were at least over 3.7 and 4.3 times greater than in Fe 2 O 3 nanocubes (bandgap = 2.08 eV), suggesting that the reaction performance of semiconductors could be controlled by proper adjustment of the bandgap. Moreover, the Fe 2 O 3 NPs were also successfully utilized to detect glucose. Herein, we believe that the present work exhibits a fascinating perspective for peroxidase-like catalytic fields.

Developing a facile strategy to synthesize template-free TiO 2 membrane with stable super-hydrophilic surface is still a daunting challenge. In this work, super-hydrophilicity (close to 0°) and underwater super-oleophobicity (165°) have been successfully demonstrated on a hierarchical Al 2 O 3 /TiO 2 membrane, which is prepared via a facile electrospinning method followed by simple calcination in air. The precisely-tuned Al 2 O 3 heterojunctions grew in situ and dispersed uniformly on the TiO 2 surface, resulting in an 'island in the sea' configuration. Such a unique feature allows not only achieving super-hydrophilicity by maximizing the surface roughness and enhancing the hydrogen bonding, but also improving the adsorption capacity toward different toxic dyes utilizing the abundant adsorption sites protected by the hierarchical nanostructure during sintering. The new Al 2 O 3 /TiO 2 nanofibrous membrane can serve as a novel filter for gravity driven oil/water separation along with dye removal, achieving 97.7% of oil/water separation efficiency and 98% of dye capture, thanks to their superb wettability and the sophisticated adsorptive performance. Our presented fabrication strategy can be extended to a wide range of ceramic materials and inspires their advanced applications in water purification under harsh liquid-phase environments.

In this work, the rationally-designed sharp corners on Au nanorods tremendously improved the catalytic activity, particularly in the presence of visible light irradiation, towards the hydrogenation of 4-nitrophenol to 4-aminophenol. A strikingly increased rate constant of 50.6 g -1 s -1 L was achieved in M-Au-3, which was 41.8 times higher than that of parent Au nanorods under dark conditions. The enhanced activities were proportional to the extent of the protruding sharp corners. Furthermore, remarkably enhanced activities were achieved in novel ternary Au/RGO/TiO 2 sheets, which were endowed with a 52.0 times higher rate constant than that of straight Au nanorods. These remarkably enhanced activities were even higher than those of previously reported 3-5 nm Au and 3 nm Pt nanoparticles. It was systematically observed that there are three aspects to the synergistic effects between Au and RGO sheets: (i) electron transfer from RGO to Au, (ii) a high concentration of p-nitrophenol close to dumbbell-like Au nanorods on RGO sheets, and (iii) increased local reaction temperature from the photothermal effect of both dumbbell-like Au nanorods and RGO sheets.

Recently, hollow nanofibers could be fabricated by coaxis electrospinning method or template method. However, they are limited to applications because of the hardship in actual preparation. In this work, hollow γ-Al 2 O 3 nanofibers with loofah-like skins were first fabricated by using a single spinneret during electrospinning. These intriguing nanofibers were explored as new Pt supports with excellently sinter-resistant performance up to 500 °C, attributed to the unique loofah-like surface of γ-Al 2 O 3 nanofibers and the strong metal-support interactions between Pt and γ-Al 2 O 3 . When applied in the catalytic reduction of p-nitrophenol, the Pt/γ-Al 2 O 3 calcined at 500 °C exhibited 4-times higher reaction rate constant (6.8 s -1 ·mg -1 ) over free Pt nanocrystals.

Graphene sheets, a flexible 2D material with excellent absorptive capacity, have great potential as absorbing materials. However, this material has always suffered from irreversible aggregation and thus loses the abundant active sites and large surface area. In this paper, large-scale graphene oxide (GO) sheets were cut and reduced to tiny reduced graphene oxide (RGO) sheets by a cell-break sonicator, for producing numerous defects, which are the center of chemisorption. Furthermore, sodium titanate nanowires functioned as a framework to help to disperse the tiny RGO sheets uniformly. And, in turn, the flexible tiny RGO sheets glued robust nanowires into a free-standing membrane. This novel composite membrane exhibited an ultra-high decoloration efficiency of 99.8% of rhodamine B in a continuous flow mode, and an outstanding absorptive capability of 1.30 × 10 -2 mol g -1 correlated to RGO content in batch reaction, which is about two orders of magnitude higher than other reported graphene-based absorbents. In addition, an efficient and feasible method without any heat treatment for regenerating the membrane is illustrated, and the recycled membrane retains superior decoloration efficiency. The excellent absorptive performance indicates the framework-based disperse strategy has great potential for the construction and application of defect-rich graphene.