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result(s) for
"Ultrafines"
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Remarkable nucleation and growth of ultrafine particles from vehicular exhaust
by
Fang, Xin
,
Tang, Rongzhi
,
Zheng, Jing
in
Aerosols
,
Atmospheric conditions
,
Chemical speciation
2020
High levels of ultrafine particles (UFPs; diameter of less than 50 nm) are frequently produced from new particle formation under urban conditions, with profound implications on human health, weather, and climate. However, the fundamental mechanisms of new particle formation remain elusive, and few experimental studies have realistically replicated the relevant atmospheric conditions. Previous experimental studies simulated oxidation of one compound or a mixture of a few compounds, and extrapolation of the laboratory results to chemically complex air was uncertain. Here, we show striking formation of UFPs in urban air from combining ambient and chamber measurements. By capturing the ambient conditions (i.e., temperature, relative humidity, sunlight, and the types and abundances of chemical species), we elucidate the roles of existing particles, photochemistry, and synergy of multipollutants in new particle formation. Aerosol nucleation in urban air is limited by existing particles but negligibly by nitrogen oxides. Photooxidation of vehicular exhaust yields abundant precursors, and organics, rather than sulfuric acid or base species, dominate formation of UFPs under urban conditions. Recognition of this source of UFPs is essential to assessing their impacts and developing mitigation policies. Our results imply that reduction of primary particles or removal of existing particles without simultaneously limiting organics from automobile emissions is ineffective and can even exacerbate this problem.
Journal Article
Barely porous organic cages for hydrogen isotope separation
by
Ceriotti, Michele
,
Balderas-Xicohténcatl, Rafael
,
Cooper, Andrew I.
in
Adsorption
,
Apertures
,
Cage molecules
2019
The separation of hydrogen isotopes for applications such as nuclear fusion is a major challenge. Current technologies are energy intensive and inefficient. Nanoporous materials have the potential to separate hydrogen isotopes by kinetic quantum sieving, but high separation selectivity tends to correlate with low adsorption capacity, which can prohibit process scale-up. In this study, we use organic synthesis to modify the internal cavities of cage molecules to produce hybrid materials that are excellent quantum sieves. By combining small-pore and large-pore cages together in a single solid, we produce a material with optimal separation performance that combines an excellent deuterium/hydrogen selectivity (8.0) with a high deuterium uptake (4.7 millimoles per gram).
Journal Article
CO2 electrolysis to multicarbon products at activities greater than 1 A cm−2
by
de Arquer, F. Pelayo García
,
Kirmani, Ahmad R.
,
Richter, Lee J.
in
Architecture
,
Carbon dioxide
,
Catalysts
2020
Electrolysis offers an attractive route to upgrade greenhouse gases such as carbon dioxide (CO2) to valuable fuels and feedstocks; however, productivity is often limited by gas diffusion through a liquid electrolyte to the surface of the catalyst. Here, we present a catalyst:ionomer bulk heterojunction (CIBH) architecture that decouples gas, ion, and electron transport. The CIBH comprises a metal and a superfine ionomer layer with hydrophobic and hydrophilic functionalities that extend gas and ion transport from tens of nanometers to the micrometer scale. By applying this design strategy, we achieved CO2 electroreduction on copper in 7 M potassium hydroxide electrolyte (pH ≈ 15) with an ethylene partial current density of 1.3 amperes per square centimeter at 45% cathodic energy efficiency.
Journal Article
CEN standard \Harmonized counting of atmospheric ultrafine particles\ and UFP monitoring initiatives in Europe
2019
The paper is devoted the standard CEN/TS 16976 described a standardized measuring method with number concentration of UFP. As well as, described TSI 3750-CEN CPC which meet all of these requirements.
Journal Article
Oxygen‐Vacancy Abundant Ultrafine Co3O4/Graphene Composites for High‐Rate Supercapacitor Electrodes
by
Yang, Xiaopeng
,
Goddard, William A.
,
Cao, Bingqiang
in
graphene
,
laser irradiation
,
oxygen vacancies
2018
The metal oxides/graphene composites are one of the most promising supercapacitors (SCs) electrode materials. However, rational synthesis of such electrode materials with controllable conductivity and electrochemical activity is the topical challenge for high‐performance SCs. Here, the Co3O4/graphene composite is taken as a typical example and develops a novel/universal one‐step laser irradiation method that overcomes all these challenges and obtains the oxygen‐vacancy abundant ultrafine Co3O4 nanoparticles/graphene (UCNG) composites with high SCs performance. First‐principles calculations show that the surface oxygen vacancies can facilitate the electrochemical charge transfer by creating midgap electronic states. The specific capacitance of the UCNG electrode reaches 978.1 F g−1 (135.8 mA h g−1) at the current densities of 1 A g−1 and retains a high capacitance retention of 916.5 F g−1 (127.3 mA h g−1) even at current density up to 10 A g−1, showing remarkable rate capability (more than 93.7% capacitance retention). Additionally, 99.3% of the initial capacitance is maintained after consecutive 20 000 cycles, demonstrating enhanced cycling stability. Moreover, this proposed laser‐assisted growth strategy is demonstrated to be universal for other metal oxide/graphene composites with tuned electrical conductivity and electrochemical activity. A novel one‐step laser irradiation route through simultaneous laser‐induced reduction and fragmentation to prepare ultrafine Co3O4 nanoparticles/graphene (UCNG) composites is proposed for the first time. Because of the plentiful oxygen vacancies on the ultrafine Co3O4 nanoparticles surface and the tightly anchoring of Co3O4 nanoparticles on graphene, the UCNG composites exhibit outstanding electrochemical performance, especially for high‐rate capability (93.7%).
Journal Article
Defects enriched hollow porous Co-N-doped carbons embedded with ultrafine CoFe/Co nanoparticles as bifunctional oxygen electrocatalyst for rechargeable flexible solid zinc-air batteries
by
Mu, Shichun
,
Cheng, Niancai
,
Lei, Zhao
in
Alloys
,
Atomic/Molecular Structure and Spectra
,
Biomedicine
2021
The construction and design of highly efficient and inexpensive bifunctional oxygen electrocatalysts substitute for noble-metal-based catalysts is highly desirable for the development of rechargeable Zn-air battery (ZAB). In this work, a bifunctional oxygen electrocatalysts of based on ultrafine CoFe alloy (4-5 nm) dispersed in defects enriched hollow porous Co-N-doped carbons, made by annealing SiO
2
coated zeolitic imidazolate framework-67 (ZIF-67) encapsulated Fe ions. The hollow porous structure not only exposed the active sites inside ZIF-67, but also provided efficient charge and mass transfer. The strong synergetic coupling among high-density CoFe alloys and Co-N
x
sites in Co, N-doped carbon species ensures high oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) activity. First-principles simulations reveal that the synergistic promotion effect between CoFe alloy and Co-N site effectively reduced the formation energy of from O* to OH*. The optimized CoFe-Co@PNC exhibits outstanding electrocatalytic stability and activity with the overpotential of only 320 mV for OER at 10 mA·cm
−2
and the half-wave potential of 0.887 V for ORR, outperforming that of most recent reported bifunctional electrocatalysts. A rechargeable ZAB constructed with CoFe-Co@PNC as the air cathode displays long-term cyclability for over 200 h and high power density (152.8 mW·cm
−2
). Flexible solid-state ZAB with our CoFe-Co@PNC as the air cathode possesses a high open circuit potential (OCP) up to 1.46 V as well as good bending flexibility. This universal structure design provides an attractive and instructive model for the application of nanomaterials derived from MOF in the field of sustainable flexible energy applications device.
Journal Article
General synthesis of ultrafine metal oxide/reduced graphene oxide nanocomposites for ultrahigh-flux nanofiltration membrane
2022
Graphene-based membranes have great potential to revolutionize nanofiltration technology, but achieving high solute rejections at high water flux remains extremely challenging. Herein, a family of ultrafine metal oxide/reduced graphene oxide (rGO) nanocomposites are synthesized through a heterogenous nucleation and diffusion-controlled growth process for dye nanofiltration. The synthesis is based on the utilization of oxygen functional groups on GO surface as preferential active sites for heterogeneous nucleation, leading to the formation of sub-3 nm size, monodispersing as well as high-density loading of metal oxide nanoparticles. The anchored ultrafine nanoparticles could inhibit the wrinkling of the rGO nanosheet, forming highly stable colloidal solutions for the solution processing fabrication of nanofiltration membranes. By functioning as pillars, the nanoparticles remarkably increase both vertical interlayer spacing and lateral tortuous paths of the rGO membranes, offering a water permeability of 225 L m
−2
h
−1
bar
−1
and selectivity up to 98% in the size-exclusion separation of methyl blue.
Graphene oxide nanofiltration membranes with tunable interlayer spacing tend to be either unstable in water or have low water permeation rates. Here the authors report a general synthetic method to achieve ultrafine metal oxide - reduced graphene oxide nanocomposites for dye filtration, achieving high water permeability and selectivity.
Journal Article
Room-temperature high-precision printing of flexible wireless electronics based on MXene inks
2022
Wireless technologies-supported printed flexible electronics are crucial for the Internet of Things (IoTs), human-machine interaction, wearable and biomedical applications. However, the challenges to existing printing approaches remain, such as low printing precision, difficulty in conformal printing, complex ink formulations and processes. Here we present a room-temperature direct printing strategy for flexible wireless electronics, where distinct high-performance functional modules (e.g., antennas, micro-supercapacitors, and sensors) can be fabricated with high resolution and further integrated on various flat/curved substrates. The additive-free titanium carbide (Ti
3
C
2
T
x
) MXene aqueous inks are regulated with large single-layer ratio (>90%) and narrow flake size distribution, offering metallic conductivity (~6, 900 S cm
−1
) in the ultrafine-printed tracks (3 μm line gap and 0.43% spatial uniformity) without annealing. In particular, we build an all-MXene-printed integrated system capable of wireless communication, energy harvesting, and smart sensing. This work opens a door for high-precision additive manufacturing of printed wireless electronics at room temperature.
High-precision printing of flexible wireless electronics has not been achieved before. Here, the authors leverage a room-temperature direct printing strategy to realize an all-MXene-printed integrated system capable of wireless communication, energy harvesting, and smart sensing.
Journal Article
Ultrafine PVDF Nanofibers for Filtration of Air-Borne Particulate Matters: A Comprehensive Review
2021
The ongoing global pandemic has bestowed high priority uponthe separation of air-borne particulate matters (PMs), aerosols, etc. using nonwoven fibrous materials, especially for face masks as a means of personal protection. Although spunbond or meltblown nonwoven materials are amongst the forerunners for polymer microfiber-based face mask or air filter development in mass scale, relatively new process of nonwoven manufacturing such as electrospinning is gaining a lot of momentum amongst the filter membrane manufacturers for its scalability of nanofiber-based filter membrane fabrication. There are several nanofiber-based face masks developing industries, which claim a very high efficiency in filtration of particulate matters (PM0.1–10) as well as other aerosols for their products. Polyvinylidene fluoride (PVDF), which is commonly known for its use of tactile sensors and energy harvesters, due to its piezoelectric property, is slowly gaining popularity among researchers and developers as an air filter material. Electrospun PVDF nanofibers can be as fine as 50 nm in mass scale, which allows the membrane to have large surface area compared to its volume, enhancing nanofiber–PM interaction. At the same time, the breathability index can be improved through these PVDF nanofiber membranes due to their architectural uniqueness that promotes slip flow around the fibers. The conductive nature of PVDF makes it advantageous as a promising electret filter allowing better capturing of ultrafine particles. This review aims to provide a comprehensive overview of such PVDF nanofiber-based filter membranes and their roles in air filtration, especially its application in filtrate of air-borne PMs.
Journal Article
A polymer tethering strategy to achieve high metal loading on catalysts for Fenton reactions
2023
The development of heterogenous catalysts based on the synthesis of 2D carbon-supported metal nanocatalysts with high metal loading and dispersion is important. However, such practices remain challenging to develop. Here, we report a self-polymerization confinement strategy to fabricate a series of ultrafine metal embedded N-doped carbon nanosheets (M@N-C) with loadings of up to 30 wt%. Systematic investigation confirms that abundant catechol groups for anchoring metal ions and entangled polymer networks with the stable coordinate environment are essential for realizing high-loading M@N-C catalysts. As a demonstration, Fe@N-C exhibits the dual high-efficiency performance in Fenton reaction with both impressive catalytic activity (0.818 min
−1
) and H
2
O
2
utilization efficiency (84.1%) using sulfamethoxazole as the probe, which has not yet been achieved simultaneously. Theoretical calculations reveal that the abundant Fe nanocrystals increase the electron density of the N-doped carbon frameworks, thereby facilitating the continuous generation of long-lasting surface-bound
•
OH through lowering the energy barrier for H
2
O
2
activation. This facile and universal strategy paves the way for the fabrication of diverse high-loading heterogeneous catalysts for broad applications.
This work reports a self-polymerization confinement strategy to develop and synthesize carbon-supported metal catalysts with high metal loading. Efficient Fenton reactivity is observed for samples containing well dispersed iron sites.
Journal Article