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1.
Environ Pollut ; 346: 123498, 2024 Apr 01.
Article in English | MEDLINE | ID: mdl-38342433

ABSTRACT

Heavy metals present a substantial threat to both the environment and human health. Considering the delicate ecological equilibrium of the Tibetan Plateau (TP) and its heightened susceptibility to anthropogenic impacts, scholarly attention has progressively turned toward the examination of heavy metal pollution within the plateau's environment. In this study, we conducted a comprehensive analysis of various heavy metals (As, Cr, Co, Ni, Cu, Mo, Cd, Pb, and Sb), utilizing topsoil samples collected from the TP during the period of 2018-2021. Additionally, snow and cryoconite samples obtained from TP glaciers during the same timeframe were also subjected to analysis. The results indicate elevated concentrations of total heavy metals in the eastern and western TP (328.7 µg/g), as opposed to the central and southern TP (145.7 µg/g). Most heavy metals exhibit a consistent spatial distribution pattern. High Enrichment Factors (EFs) and Geoaccumulation Index (Igeo) values for As and Cd suggest their enrichment in TP topsoil. Receptor modeling identified three primary sources of heavy metals within the topsoil: industrial sources (42.3%), inherent natural sources within the surface soil (20.6%), and vehicular emissions (14.2%). Substantial differences in heavy metal concentrations and spatial distribution were observed between the topsoil and the glacial snow-cryoconite matrix. The prominent presence of Sb in the snow-cryoconite matrix, in contrast to its low abundance in the topsoil, indicates distinct source influences of long-range transported materials between the two environments. Our inference suggests that the influence of heavy metals from distant pollutants undergo mixing and dilution in the topsoil due to the presence of local indigenous heavy metals, although such influence is notably observed on the glacier surface of the TP. Consequently, this underscores the significant impact of long-range transported sources on heavy metals, surpassing the influence of local TP soils, to the alpine glaciers and even other atmospheric sediments in Tibetan Plateau.


Subject(s)
Metals, Heavy , Soil Pollutants , Humans , Tibet , Ice Cover , Cadmium/analysis , Environmental Monitoring/methods , Metals, Heavy/analysis , Soil , Soil Pollutants/analysis , China , Risk Assessment
2.
J Alzheimers Dis ; 97(2): 609-620, 2024.
Article in English | MEDLINE | ID: mdl-38143355

ABSTRACT

BACKGROUND: Glyphosate is the most commonly used herbicide with potential neurotoxicity. However, limited epidemical evidence is found in the relationship between glyphosate and cognitive impairment, especially in the cognitive-disrupting sensitive elderly populations. OBJECTIVE: This study aimed to examine the association of urinary glyphosate exposure with cognitive impairment in the United State (US) older adults. METHODS: Cognitive impairment was determined by the following four tests: the Consortium to Establish a Registry for Alzheimer's disease (CERAD) Immediate Recall test (IR), the CERAD Delayed Recall tests (DR), the Animal Fluency (AF) test and the Digit Substitution test (DSST). Survey weighted logistic regression and restricted cubic splines were applied to evaluate and visualize the association between glyphosate and cognitive impairment. RESULTS: A total of 465 elderly adults were identified in the National Health and Nutrition Examination Survey (NHANES) 2013-2014 cycle, and among them, 83.87% individuals had detectable urinary levels of glyphosate (0.628 ng/mL in average). After adjusting for the potential covariates, glyphosate was significantly linked to increased DR and AF impairment, and the corresponding ORs were 1.52 (1.01 to 2.30, p = 0.049) and 1.69 (1.11 to 2.59, p = 0.019), respectively. No significant association was identified between glyphosate and IR or DSST impairment. The RCS plot further confirmed the linear and positive relationships between glyphosate and DR and AF impairment. CONCLUSIONS: These findings suggested that exposure to glyphosate might be associated with declined cognitive function in the elderly, and it might be prudent to evaluate cognitive outcomes for aged individuals with glyphosate exposures.


Subject(s)
Alzheimer Disease , Cognition Disorders , Cognitive Dysfunction , Aged , Humans , Nutrition Surveys , Glyphosate , Cognitive Dysfunction/chemically induced , Cognitive Dysfunction/epidemiology , Cognition , Cognition Disorders/chemically induced , Cognition Disorders/epidemiology
3.
Nano Lett ; 23(7): 2974-2980, 2023 Apr 12.
Article in English | MEDLINE | ID: mdl-36975136

ABSTRACT

Herein we report the synthesis and characterization of spinel copper gallate (CuGa2O4) nanocrystals (NCs) with an average size of 3.7 nm via a heat-up colloidal reaction. CuGa2O4 NCs have a band gap of ∼2.5 eV and marked p-type character, in agreement with ab initio simulations. These novel NCs are demonstrated to be photoactive, generating a clear and reproducible photocurrent under blue light irradiation when deposited as thin films. Crucially, the ability to adjust the Cu/Ga ratio within the NCs, and the effect of this on the optical and electronic properties of the NCs, was also demonstrated. These results position CuGa2O4 NCs as a novel material for optoelectronic applications, including hole transport and light harvesting.

4.
Int J Mol Sci ; 24(5)2023 Mar 06.
Article in English | MEDLINE | ID: mdl-36902459

ABSTRACT

Non-coding RNAs (ncRNAs) are transcribed from the genome and do not encode proteins. In recent years, ncRNAs have attracted increasing attention as critical participants in gene regulation and disease pathogenesis. Different categories of ncRNAs, which mainly include microRNAs (miRNAs), long non-coding RNAs (lncRNAs), and circular RNAs (circRNAs), are involved in the progression of pregnancy, while abnormal expression of placental ncRNAs impacts the onset and development of adverse pregnancy outcomes (APOs). Therefore, we reviewed the current status of research on placental ncRNAs and APOs to further understand the regulatory mechanisms of placental ncRNAs, which provides a new perspective for treating and preventing related diseases.


Subject(s)
MicroRNAs , RNA, Long Noncoding , Pregnancy , Humans , Female , Pregnancy Outcome , Placenta/metabolism , RNA, Untranslated/metabolism , MicroRNAs/genetics , RNA, Long Noncoding/genetics
5.
ACS Appl Mater Interfaces ; 14(9): 11768-11778, 2022 Mar 09.
Article in English | MEDLINE | ID: mdl-35213125

ABSTRACT

The development of high-performing p-type transparent conducting oxides will enable immense progress in the fabrication of optoelectronic devices including invisible electronics and all-oxide power electronics. While n-type transparent electrodes have already reached widespread industrial production, the lack of p-type counterparts with comparable transparency and conductivity has created a bottleneck for the development of next-generation optoelectronic devices. In this work, we present the fabrication of delafossite copper chromium oxide p-type transparent electrodes with outstanding optical and electrical properties. These layers were deposited using ultrasonic spray pyrolysis, a wet chemical method that is fast, simple, and scalable. Through careful screening of the deposition conditions, highly crystalline, dense, and smooth CuCrO2 coatings were obtained. A detailed investigation of the role played by the deposition temperature and the cation ratio enabled the properties of the prepared layers to be reliably tuned, as verified using X-ray diffraction, X-ray photoelectron spectroscopy, optical spectroscopy, Hall effect measurements, and electron and atomic force microscopies. We demonstrate record conductivities for solution-processed CuCrO2, exceeding 100 S cm-1, and we also obtained the highest value for two separate figures of merit for p-type transparent conducting oxides. These performances position solution-deposited CuCrO2 as the leading p-type transparent-conducting oxide currently available.

6.
Sci Total Environ ; 825: 153946, 2022 Jun 15.
Article in English | MEDLINE | ID: mdl-35189209

ABSTRACT

Iron (Fe) is an essential micronutrient in glacial ecosystems and modulates global biogeochemical cycles. To find out the deposition concentration, multiple origins and release form of iron in various glacier areas of central Asia, this study investigated the total Fe (TFe) and dissolved-Fe (dFe, diameter < 0.45 or <0.2 µm) deposition in glaciers and snowpack of northeast Tibetan Plateau, based on snow and meltwater sampling in ablation period of 2014-2017. The composition and concentration of dFe in the samples were measured, and the spatial distribution and temporal variations of dFe in glacial surface snow and meltwater runoff were investigated. Results showed that average TFe and dFe contents exhibited a generally heterogeneous geographic distribution that varied from north to south. The northern locations in eastern Tianshan Mountains (e.g. Miaoergou Glacier) showed the highest TFe and dFe values, followed by Yuzhufeng Glacier of eastern Kunlun Mountains, whereas the Qilian Mountains locations displayed relatively lower TFe and dFe contents spanning a wide range. Based on the good correlation between TFe and dFe, we infer that aeolian dust and anthropogenic aerosols, and their chemical interactions are likely the important origins for dFe deposition. In meltwater runoff the peak values of dFe release flux appeared in July, with maximum appeared earlier (the early of July) than TFe (the end of July). Moreover, the annual dFe release flux from Laohugou glacier terminus meltwater runoff is estimated to be 1740 kg yr-1 (with 9256 kg yr-1 for TFe), and meltwater showed higher mean concentration of dFe than that of glacier snowpack. We also provided a conceptual framework showing the multiple origins and transport dynamics of dissolved Fe along the atmosphere-glacier-meltwater runoff path. Compared to Fe release in other global glacier/ice-sheet, the TP glacier is an important potential dFe reservoir and may have a profound effect on regional downstream ecosystem through Fe biochemistry cycle.


Subject(s)
Ecosystem , Ice Cover , Environmental Monitoring/methods , Ice Cover/chemistry , Iron , Tibet
7.
Natl Sci Rev ; 8(7): nwaa144, 2021 Jul.
Article in English | MEDLINE | ID: mdl-34691679

ABSTRACT

Mineral dust can indirectly affect the climate by supplying bioavailable iron (Fe) to the ocean. Here, we present the records of dissolved Fe (DFe) and total Fe (TDFe) in North Greenland Eemian Ice Drilling (NEEM) ice core over the past 110 kyr BP. The Fe records are significantly negatively correlated with the carbon-dioxide (CO2) concentrations during cold periods. The results suggest that the changes in Fe fluxes over the past 110 kyr BP in the NEEM ice core are consistent with those in Chinese loess records because the mineral-dust distribution is controlled by the East Asian deserts. Furthermore, the variations in the dust input on a global scale are most likely driven by changes in solar radiation during the last glacial-interglacial cycle in response to Earth's orbital cycles. In the last glacial-interglacial cycle, the DFe/TDFe ratios were higher during the warm periods (following the post-Industrial Revolution and during the Holocene and last interglacial period) than during the main cold period (i.e. the last glacial maximum (LGM)), indicating that the aeolian input of iron and the iron fertilization effect on the oceans have a non-linear relationship during different periods. Although the burning of biomass aerosols has released large amounts of DFe since the Industrial Revolution, no significant responses are observed in the DFe and TDFe variations during this period, indicating that severe anthropogenic contamination has no significant effect on the DFe (TDFe) release in the NEEM ice core.

8.
Small ; 17(49): e2101666, 2021 Dec.
Article in English | MEDLINE | ID: mdl-34309208

ABSTRACT

Methods for the fabrication of thin films with well controlled structure and properties are of great importance for the development of functional devices for a large range of applications. SILAR, the acronym for Successive Ionic Layer Adsorption and Reaction, is an evolution and combination of two other deposition methods, the Atomic Layer Deposition and Chemical Bath Deposition. Due to a relative simplicity and low cost, this method has gained increasing interest in the scientific community. There are, however, several aspects related to the influence of the many parameters involved, which deserve further deepening. In this review article, the basis of the method, its application to the fabrication of thin films, the importance of experimental parameters, and some recent advances in the application of oxide films are reviewed. At first the fundamental theoretical bases and experimental concepts of SILAR are discussed. Then, the fabrication of chalcogenides and metal oxides is reviewed, with special emphasis to metal oxides, trying to extract general information on the effect of experimental parameters on structural, morphological and functional properties. Finally, recent advances in the application of oxide films prepared by SILAR are described, focusing on supercapacitors, transparent electrodes, solar cells, and photoelectrochemical devices.

9.
ChemSusChem ; 13(23): 6229-6245, 2020 Dec 07.
Article in English | MEDLINE | ID: mdl-33030250

ABSTRACT

The massive release of the greenhouse gas CO2 has resulted in numerous environmental issues. In searching for advanced technologies for CO2 capture/conversions, recent advances in electrochemical reduction of CO2 in molten salts shed a light on potential solutions to CO2 mitigation. Electro-reduction of CO2 in molten salts exhibits features like high selectivity and efficiency towards sustainable carbons and fuels, low toxicity, and possibility to combine with in situ CO2 capture. In this Minireview, we highlight the tuning of the products in this process and mainly discuss two categories of electrolyte, carbonate-based molten salts (CMS) and those based on halides (HMS). Depending on the synthetic conditions, fuels such as CO or hydrocarbons (in the presence of hydrogen source, i. e., LiOH, NaOH, or KOH in the electrolyte) as well as high-value nanostructured carbons including carbon nanotubes, carbon nanofibers, carbon nano-onions, and graphene can be obtained with high efficiency. The synthesis parameters are compared, and the applications of as-obtained carbons are briefly summarized. Additionally, some perspectives on this technology are also discussed.

10.
Environ Sci Technol ; 54(18): 11344-11355, 2020 09 15.
Article in English | MEDLINE | ID: mdl-32822538

ABSTRACT

Mercury (Hg) is a globally spread trace metal due to its long atmospheric residence time. Yet, our understanding of atmospheric processes (e.g., redox reactions and deposition) driving Hg cycling is still limited, especially in polar regions. The Antarctic continent, by virtue of its remoteness, is the perfect location to investigate Hg atmospheric processes in the absence of significant local anthropogenic impact. Here, we present the first 2 year record (2016-2017) of total suspended particulate mercury (PHg) concentrations along with a year-round determination of an Hg stable isotopic composition in particles collected at Zhongshan Station (ZSS), eastern Antarctic coast. The mean PHg concentration is 21.8 ± 32.1 pg/m3, ranging from 0.9 to 195.6 pg/m3, and peaks in spring and summer. The negative mass-independent fractionation of odd Hg isotopes (odd-MIF, average -0.38 ± 0.12‰ for Δ199Hg) and the slope of Δ199Hg/Δ201Hg with 0.91 ± 0.12 suggest that the springtime isotope variation of PHg is likely caused by in situ photo-oxidation and reduction reactions. On the other hand, the increase of PHg concentrations and the observed odd-MIF values in summer are attributed to the transport by katabatic winds of divalent species derived from the oxidation of elemental Hg in the inland Antarctic Plateau.


Subject(s)
Mercury , Antarctic Regions , Environmental Monitoring , Isotopes , Mercury/analysis , Mercury Isotopes/analysis , Seasons
11.
J Nanosci Nanotechnol ; 20(9): 5642-5647, 2020 09 01.
Article in English | MEDLINE | ID: mdl-32331150

ABSTRACT

Two Australian native wooden sources (Acacia Mangium and Eucalyptus Globulus) derived pulps were explored as raw feed stocks to prepare the valuable nanomaterial of cellulose nanocrystals (CNC). After bleaching and acid hydrolysis, cellulose nanocrystals were successfully produced with high yields of approximately 60% for both kraft pulps. According to the characterization of SEM and AFM, the as prepared CNC had a rod like structure with the length and diameter in the range of 200~1000 nm and 10~100 nm, respectively based on the initial wooden source. XRD confirmed the crystalline structure of the resulting CNC. Further characterisation by TGA showed that the chemical treatment of the wood pulp had impact upon the thermal stability, evidenced by a lower onset temperature of the thermal decomposition of CNC.

12.
RSC Adv ; 10(64): 39080-39086, 2020 Oct 21.
Article in English | MEDLINE | ID: mdl-35518441

ABSTRACT

Aiming at solving the issue of wastewater purification, this work synthesized NH2-MIL-88B (Fe α In1-α ) photocatalysts by a simple one-pot method, which was employed for photocatalytic reduction of Cr(vi) and oxidation of TC-HCl. Compared with traditional NH2-MIL-88B (Fe) photocatalysts, NH2-MIL-88B (Fe0.6In0.4) displayed excellent photocatalytic performance; the photocatalytic redox rate for Cr(vi) and TC-HCl reached 86.83% and 72.05%, respectively. The good photocatalytic performance might be attributed to the metal-to-metal charge transition (MMCT) between Fe-O clusters and In-O clusters formed by doping In(iii) into NH2-MIL-88B (Fe), which provides effective active sites for the photocatalytic reduction and oxidation routes. Besides, the synergistic effect of the ligand-to-metal charge transition (LMCT) and MMCT expands the separation and transfer of photogenerated carriers and inhibits the recombination of electron-hole pairs, thus effectively improving the photocatalytic performance. Therefore, this work could provide a new method for the construction of mixed metal MOFs for the photocatalytic degradation of pollutants.

13.
Acc Chem Res ; 52(11): 3177-3187, 2019 Nov 19.
Article in English | MEDLINE | ID: mdl-31697061

ABSTRACT

Climate change represents one of the most important environmental issues of our time. Due to high levels of anthropogenic CO2 emissions, atmospheric CO2 has for the first time ever exceeded 415 ppm and has increased from 315 ppm in 1950. An annual increase in atmospheric CO2 of ∼2 ppm is equal to a net increase of ∼15.6 billion tons of CO2. The combustion of fossil fuels for electricity and transportation is still the main reason accounting for the CO2 accumulation. On the top of that, fossil fuels are widely used in our modern industry for the productions of indispensable social staples. For instance, the millennia old thermal reduction of iron ore by charcoal or baked coal (3C + 2Fe2O3 → 4Fe + 3CO2) continues as the main method for the production of iron. The artificial fertilizer ammonia boosts the global population and is mainly produced from the Haber-Bosch process, in which hydrogen is generated via steam reforming of methane (CH4 + 2H2O → 4H2 + CO2). Sequestration and diminution of CO2 require the development of a portfolio of technologies on (1) efficient and long-term harvesting of renewable energy, that is, solar, not only for electricity but also directly as the energy force in vital chemical processes, wherever possible, (2) carbon-neutral processes to replace current industrial processes that emit vast amounts of CO2, such as iron and ammonia production, and (3) new, low-cost technologies for CO2 capture and conversion with particular interests in the exploration of CO2 as the feedstock for fuels or other valuable chemicals and materials. To this end, we conducted some studies on the sustainable synthesis of ammonia and iron with net-zero CO2 emissions and large-scale CO2 capture and conversion into fuels and high value nanocarbon products via electrolysis in molten salt(s) with the introduction of the Solar Thermal Electrochemical Process (STEP). In STEP, solar UV-visible energy is focused on a photovoltaic device that generates the electricity to drive the electrolysis, while concurrently the solar thermal energy is focused on a second system to generate heat for the electrolysis cell. The utilization of the full spectrum of sunlight in STEP results in a higher solar energy efficiency than other solar conversion processes. STEP has been applied to conduct (1) CO2-free ammonia synthesis from nitrogen and water with the aid of nano-Fe2O3 in a molten hydroxide electrolyte, (2) CO2-free production of iron via electrochemical reduction of iron ore in molten carbonate, (3) CO2 capture and conversion into nanostructured carbon products as well as fuels in molten or mixed molten electrolytes, and (4) organic electrosynthesis of benzoic acid from benzene without overoxidizing into CO2. In this Account, we highlight some recent achievements in these topics and propose that using STEP is a highly efficient strategy for saving energy and, consequently, the environment. STEP is an ideal tool that can theoretically be applied to all endothermic reactions.

14.
J Colloid Interface Sci ; 555: 342-351, 2019 Nov 01.
Article in English | MEDLINE | ID: mdl-31394321

ABSTRACT

An Ag/AgCl/NH2-UiO-66 hybridized photocatalyst was successfully constructed via facile solvothermal with UV reduction method for efficient photocatalytic Cr (VI) reduction. The photoelectrochemical data indicate that compared with the UiO-66, the charge separation and transfer efficiency of Ag/AgCl/NH2-UiO-66 heterojunction is significantly enhanced due to the introduction of amine functionalization and formation of inorganic-organic hybrid. The surface plasmon resonance (SPR) effect deriving from Ag nanoparticles (NPs) largely extends photo-response range whilst the separation efficiency of photo-generated electrons and holes is improved significantly. The synthesized Ag/AgCl/NH2-UiO-66 hybrid system shows ameliorated structural stability and superior photocatalytic activity for Cr (VI) reduction under visible light irradiation, which is 1.7 times higher than that of the bare UiO-66. Furthermore, the possible mechanism of Cr (VI) reduction is proposed by analyzing electron transfer path in the ternary Ag/AgCl/NH2-UiO-66 hybridized system.

15.
Sci Rep ; 8(1): 4172, 2018 03 08.
Article in English | MEDLINE | ID: mdl-29520016

ABSTRACT

The objective of this study is to investigate the effect of decreased permafrost stability on carbon storage of the alpine ecosystems in the northeastern margin of the Qinghai-Tibet Plateau. During July and August 2013, we selected 18 sites in five types of permafrost (stable, substable, transitional, unstable, and extremely unstable) regions. We measured aboveground phytomass carbon (APC) and soil respiration (SR), soil inorganic carbon (SIC), soil organic carbon (SOC), belowground phytomass carbon, and soil properties down to 50 cm at same types of soils and grasslands. The results indicated that ecosystem carbon in cold calcic soils first decreased and then increased as the permafrost stability declined. Overall, decreasing permafrost stability was expected to reduce ecosystem carbon in meadows, but it was not obvious in swamp meadows and steppes. APC decreased significantly, but SIC and SOC in steppes first decreased and then increased with declining permafrost stability. Soil clay fraction and soil moisture were the controls for site variations of ecosystem carbon. The spatial variations in SR were possibly controlled by soil moisture and precipitation. This meant that alpine ecosystems carbon reduction was strongly affected by permafrost degradation in meadows, but the effects were complex in swamp meadows and steppes.

16.
J Environ Sci (China) ; 46: 190-202, 2016 Aug.
Article in English | MEDLINE | ID: mdl-27521951

ABSTRACT

The spatiotemporal distribution pattern of marine-origin matter on the Antarctica ice sheet was used to study variations in the source regions, transport mechanisms and post-depositional influences. We present data on sea salt ions, sulfur components and stable isotopes from surface and snow pit samples collected along the transect route from Zhongshan Station to Dome A during the austral summer in 2012-2013. A general decreasing trend in the accumulation, sea salt ions and sulfur components occurred with increasing distance from the coast and increasing elevation. However, different sources of the marine components, transport pathways and post-depositional influences were responsible for their different spatial distribution patterns. The marine ions in the coastal snow pit varied seasonally, with higher sea salt ion concentrations in the winter and lower concentrations in the summer; the opposite pattern was found for the sulfur compounds. The sea ice area surrounding Antarctica was the main source region for the deposited sea salt and the open sea water for the sulfur compounds. No significant trends in the marine-origin components were detected during the past 3 decades. Several periods of elevated deposition of sea salt ions were associated with lower temperatures (based on δD and δ(18)O) or intensified wind fields. In comparison to the sea salt ions, the sulfur concentrations exhibited the opposite distribution patterns and were associated with changes in the surrounding sea ice extent.


Subject(s)
Environmental Monitoring , Environmental Pollutants/analysis , Snow/chemistry , Antarctic Regions , Seasons , Sulfur Compounds/analysis
17.
Sci Rep ; 6: 27760, 2016 06 09.
Article in English | MEDLINE | ID: mdl-27279594

ABSTRACT

Primary evidence of the direct uptake of atmospheric CO2 and direct transformation into carbon nanotubes, CNTs, is demonstrated through isotopic labeling, and provides a new high yield route to mitigate this greenhouse gas. CO2 is converted directly to CNTs and does not require pre-concentration of the airbone CO2. This C2CNT (CO2 to carbon nanotube) synthesis transforms CO2-gas dissolved in a 750 °C molten Li2CO3, by electrolysis, into O2-gas at a nickel electrode, and at a steel cathode into CNTs or carbon or nanofibers, CNFs. CNTs are synthesized at a 100-fold price reduction compared to conventional chemical vapour deposition, CVD, synthesis. The low cost conversion to a stable, value-added commodity incentivizes CO2 removal to mitigate climate change. The synthesis allows morphology control at the liquid/solid interface that is not available through conventional CVD synthesis at the gas/solid interface. Natural abundance (12)CO2 forms hollow CNTs, while equivalent synthetic conditions with heavier (13)CO2 favours closed core CNFs, as characterized by Raman, SEM and TEM. Production ease is demonstrated by the first synthesis of a pure (13)C multiwalled carbon nanofiber.

18.
ACS Cent Sci ; 2(3): 162-8, 2016 Mar 23.
Article in English | MEDLINE | ID: mdl-27163042

ABSTRACT

The cost and practicality of greenhouse gas removal processes, which are critical for environmental sustainability, pivot on high-value secondary applications derived from carbon capture and conversion techniques. Using the solar thermal electrochemical process (STEP), ambient CO2 captured in molten lithiated carbonates leads to the production of carbon nanofibers (CNFs) and carbon nanotubes (CNTs) at high yield through electrolysis using inexpensive steel electrodes. These low-cost CO2-derived CNTs and CNFs are demonstrated as high performance energy storage materials in both lithium-ion and sodium-ion batteries. Owing to synthetic control of sp(3) content in the synthesized nanostructures, optimized storage capacities are measured over 370 mAh g(-1) (lithium) and 130 mAh g(-1) (sodium) with no capacity fade under durability tests up to 200 and 600 cycles, respectively. This work demonstrates that ambient CO2, considered as an environmental pollutant, can be attributed economic value in grid-scale and portable energy storage systems with STEP scale-up practicality in the context of combined cycle natural gas electric power generation.

19.
ACS Appl Mater Interfaces ; 8(8): 5509-16, 2016 Mar 02.
Article in English | MEDLINE | ID: mdl-26849857

ABSTRACT

Nickel(II) sulfide (NiS) nanosheets with a thickness of 10 nm and a size of 200 nm were facilely grown on stainless steel (SLS) meshes via a one-pot hydrothermal method. This unique construction renders an excellent electrical contact between the porous film of active NiS sheets and the highly conductive substrate, which exhibits a superior catalytic activity toward oxygen evolution reaction (OER). The NiS@SLS electrocatalyst exhibits an unusually low overpotential of 297 mV (i.e., 1.524 V vs RHE) at a current density of 11 mA·cm(-2), and an extra small Tafel slope of only 47 mV·dec(-1) proves an even more competitive performance at high to very high current densities. This performance compares very favorably to other Ni-based catalysts and even to the precious state-of-the-art IrO2 or RuO2 catalyst.

20.
ChemSusChem ; 8(18): 3077-83, 2015 Sep 21.
Article in English | MEDLINE | ID: mdl-26373362

ABSTRACT

An ionothermal sol-gel strategy to synthesize hierarchically porous carbon aerogels doped with different heteroatoms is presented by using biomass precursors in a scalable process. Morphologically similar but chemically different materials are used to study the influence of heteroatoms in Li-S batteries. The materials show capacities as high as 1290 mAh g(-1) in the first cycle using 50 wt % S loading. Heteroatom doping reduces the capacity fading and the polarization throughout cycling. Zeta potential measurements reveal positive surface charges for heteroatom-doped carbons and indicate attractive interactions with polysulfides causing reduced fading. A polysulfide-selective sorption study reveals strongly different adsorption behavior depending on the carbon's chemical composition. Interestingly, the polysulfide fraction is also crucial. The results indicate that improved adsorption of long-chain polysulfides to doped carbons is related to improved capacity retention.


Subject(s)
Biomass , Carbon/chemistry , Electric Power Supplies , Lithium/chemistry , Salts/chemistry , Sulfur/chemistry , Chemistry Techniques, Synthetic , Gels , Porosity
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