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1.
Artículo en Inglés | MEDLINE | ID: mdl-38649609

RESUMEN

Mercury (Hg) tailings are hazardous solid wastes because of their high Hg concentrations. Modified phosphogypsum (PG) can decrease the bioactivity and mobility of heavy metals through chemisorption or electrostatic interactions. In this study, PG whiskers were modified by ZnCl2 and S, chitosan-hydrochloric acid, and thioglycolic materials; the resulting modified whiskers were used to decontaminate Hg tailings. Leaching tests and orthogonal experiments were conducted to optimize the modification parameters, including modifier quantity, pH, reaction temperature, and reaction time. The structure and physicochemical properties of the whiskers before and after modification were characterized through X-ray diffraction (XRD), scanning electron microscopy (SEM), and Fourier transform infrared spectroscopy (FTIR). The stabilization efficiency of the modified PG whiskers ranged from 93.05 to 97.50%, demonstrating excellent stabilization effects. The stabilization was achieved through chemisorption or complexation. The decontamination process using modified whiskers reduced the pH and total nitrogen of the tailings; increased the cation exchange, total phosphorus, organic carbon, and total carbon; and made the tailings suitable for planting. In addition, the modified PG promoted the morphological transformation of Hg in the tailings, thereby significantly decreasing the Hg content in the effective states and mitigating the risk of Hg contamination.

2.
Langmuir ; 2024 Feb 05.
Artículo en Inglés | MEDLINE | ID: mdl-38316545

RESUMEN

Loading cocatalysts to promote spatial charge separation has been confirmed as an effective method for improving photocatalytic hydrogen production. This article reports that the synthesis of Ni(OH)2/Cd0.9Zn0.1S nanorod photocatalyst is suitable for photocatalytic H2 generation under visible light. It can be proven that the binary photocatalyst exhibits a one-dimensional nanorod morphological structure. Ni(OH)2 nanosheets occupy the top area of Cd0.9Zn0.1S nanorods. The photocatalytic H2 production rate can reach 132.93 mmol·h-1·g-1, which corresponds to an apparent quantum efficiency of up to 76.5% at a wavelength of 460 nm. In addition, the Ni(OH)2 nanosheet can aggregate the light-incited electrons of Cd0.9Zn0.1S, inhibiting the confluence of electrons and holes. The detailed analysis of its mechanism through characterization methods such as photoluminescence and electrochemical measurement shows that the significant improvement in photocatalytic performance derives from the effective spatial separation of photo-induced charge carriers. Therefore, this synthesis strategy of one-dimensional materials may bring new prospects for more efficient, stable, and sustainable photocatalysis for water splitting.

3.
Environ Sci Pollut Res Int ; 30(59): 123497-123506, 2023 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-37987978

RESUMEN

With the continuous emission of greenhouse gases, climate issues such as global warming have attracted widespread attention. As the largest CO2 emitter, China proposes the target of reaching the CO2 emissions peak by 2030 at the 75th United Nations General Assembly. To determine whether China can realize the goal, we construct an assessment system consisting of a new discrete grey prediction model on the basis of a rolling mechanism and an improved IPCC method. First, the new grey prediction model is used to predict the CO2 emissions and GDP from 2021 to 2030, and then, the enhanced IPCC method is used to obtain the carbon intensity from 2021 to 2030. In line with the direct judgment based on CO2 emissions and the indirect judgment based on the comparison between the AADR of carbon intensity and the AAIR of GDP, we find that China faces great challenges and difficulties in achieving its carbon peaking target by 2030. Finally, based on the forecast data and China's current situation, some policy recommendations are put forward to accelerate China's CO2 peak goal.


Asunto(s)
Dióxido de Carbono , Gases de Efecto Invernadero , Dióxido de Carbono/análisis , Gases de Efecto Invernadero/análisis , Calentamiento Global , China , Carbono
4.
Environ Sci Pollut Res Int ; 30(29): 74127-74140, 2023 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-37204567

RESUMEN

Biochar is regarded as an effective adsorbent for heavy metal pollution treatment, and functional optimization is still needed to improve its performance. We created raw biochar (BC and BP) from corn straw and pine sawdust, which were modified to produce sulfhydryl-modified biochar (MBC and MBP). Isothermal adsorption experiments and adsorption kinetics experiments as well as the related model fitting were performed to evaluate the adsorption performance of biochar on Hg(II). According to the results of the Langmuir model fitting, the maximum adsorption capacities of sulfhydryl-modified biochar were 193.05 mg/g (MBC) and 178.04 mg/g (MBP), respectively, which were approximately 1.6 times higher than the raw biochar. The results showed that adding sulfhydryl groups to biochar can improve its adsorption performance. The prompt effect resulted from the sulfhydryl modification providing additional functional groups and enhanced chemisorption and physical adsorption properties.


Asunto(s)
Mercurio , Metales Pesados , Contaminantes Químicos del Agua , Carbón Orgánico , Agua , Adsorción , Contaminantes Químicos del Agua/análisis , Cinética
5.
Environ Sci Pollut Res Int ; 30(18): 53492-53504, 2023 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-36859640

RESUMEN

Based on the unique technique property of grate-kiln pellet production process and its demand of ultra-low emission of NOx, a low energy-consumed embedded selective catalytic reduction (SCR) denitration technology was proposed. The temperature of the NOx-containing tributary flue gas was 350-500 °C, which basically accorded with the temperature range of SCR by V2O5-based catalyst. Considering the potential inhibition effect of high SO2 concentration (8000-10000 mg/m3) and metal-containing dust in the pelletizing flue gas, the catalyst compositions were optimized to V2O5 (0.5%) and WO3 (5%), giving NO conversion over 90% with low yield of N2O by-product. Compared with the low-medium temperature SCR technology, it was no longer necessary to reheat the flue gas, showing a remarkable CO2 emission reduction effect. The CO2 emission reduction ratios were 94% and 66% contributed by the decrease of fuel and electricity consumption for the embedded SCR technology, respectively. The operating cost was also greatly reduced from 11.4 CNY/t-pellet to 3.1 CNY/t-pellet (Chinese Yuan).


Asunto(s)
Dióxido de Carbono , Frío , Temperatura , Catálisis
6.
ACS Omega ; 7(19): 16352-16360, 2022 May 17.
Artículo en Inglés | MEDLINE | ID: mdl-35601292

RESUMEN

Novel Ce x Zr1-x O2 (x = 0.67, 0.8, 0.9, 1.0) catalysts were designed and synthesized by solvothermal, calcination, and sol-gel methods and were used to catalyze oxidation of soot from diesel vehicle exhaust. The influence of catalysts synthesized by different methods and Ce/Zr molar ratios on the performance was investigated. These catalysts were characterized by XRD, N2 adsorption-desorption, FT-IR, TEM, XPS, H2-temperature programmed reduction (TPR), and O2-temperature programmed desorption (TPD) techniques. The results indicated that Ce0.8Zr0.2O2 prepared by the calcination method has excellent activity and stability at low temperature. The soot ignition point is 322 °C, and the ratio of soot conversion reaches 90% at 497 °C, which is lower than that from the solvothermal and sol-gel methods. The XRD, Raman, SEM, XPS and H2-TPR results reveal that the structure and oxygen adsorption properties are crucial to soot oxidation activity, and Zr4+ is successfully doped into the CeO2 lattice and forms a homogeneous solid solution. Nanostructured Ce0.8Zr0.2O2 with 110.2 m2/g surface areas is produced. The proportion of chemical oxygen and surface adsorbed oxygen in the catalyst prepared from the calcination method is the highest at 23.18%. The structure may lead to charge imbalance, unsaturated bonds, and oxygen vacancies, thus increasing the adsorption of oxygen on the catalyst surface.

7.
Langmuir ; 37(51): 14823-14832, 2021 Dec 28.
Artículo en Inglés | MEDLINE | ID: mdl-34915697

RESUMEN

A series of mesoporous CeZrTiOx catalysts were prepared by a facile hydrothermal method. Compared with CeTiOx catalysts synthesized under the same conditions, the catalytic activity and anti-SO2 performance of the Ce1Zr1TiOx catalyst are greatly improved, and at the gas hourly space velocity (GHSV) of 60 000 h-1, the NOx removal efficiency is maintained at 90% in the temperature range of 290-500 °C. The catalytic effect of ZrO2 on the Ce-Ti catalyst NH3-SCR activity was elucidated through a series of characterizations. The results revealed that the doping of Zr could significantly improve and optimize the structure of Ce-Ti catalysts. At the same time, due to the doping of Zr, the synergistic effect between Ce and Zr in the CeZrTiOx catalyst can effectively increase oxygen mobility, total acid content, and surface adsorbed oxygen species and lead to a larger pore volume. In addition, the introduction of ZrO2 made the transformation of Ce4+ into Ce3+ more obvious, and the 2Ce4+ + Zr2+ ↔ 2Ce3+ + Zr4+ reaction greatly improved the reducibility of Ce1Zr1TiOx. Among them, the improvement of SCR performance and H2O/SO2 tolerance is due to the electronic interaction between Zr and Ce.

8.
Environ Sci Pollut Res Int ; 28(20): 24847-24871, 2021 May.
Artículo en Inglés | MEDLINE | ID: mdl-33763831

RESUMEN

Carbon monoxide (CO) catalytic oxidation has gained increasing interest in recent years due to its application prospects. The noble metal catalysts commonly exhibit outstanding CO catalytic oxidation activity. Therefore, this article reviewed the recent research on the application of noble metal catalysts in the catalytic oxidation of CO. The effects of catalyst support, dopant, and physicochemical properties on the catalytic activity for CO oxidation are summarized. The influence of the presence of water vapor and sulfur dioxide in the reaction atmosphere on the catalytic activity in CO oxidation is emphatically discussed. Moreover, this paper discussed several reaction mechanisms of CO catalytic oxidation on noble metal catalysts. Finally, the challenges of removing CO by catalytic oxidation in practical industrial flue gas are proposed.


Asunto(s)
Monóxido de Carbono , Metales , Catálisis , Oxidación-Reducción , Dióxido de Azufre
9.
J Environ Sci (China) ; 96: 64-71, 2020 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-32819700

RESUMEN

Based on the demand of sintering/pelleting flue gas ultra-low emission, a semi-dry method using a spray dryer absorber (SDA) combined with O3 oxidation was proposed for simultaneous removal of SO2 and NO. Effects of O3 injection site, O3/NO molar ratio, and spray tower temperature on the removal efficiencies were investigated. It was revealed that both desulfurization and denitrification efficiencies could reach to 85% under the conditions of setting O3 injection site inside of tower, O3/NO molar ratio 1.8, spray tower temperature 85°C, Ca/(S + 2 N) molar ratio 2.5 and slurry flow rate 300 mL/hr. CaSO3/Ca(OH)2 mixture slurry was used as absorbent to simulate operating conditions in iron and steel industry. The result shows that the addition of CaSO3 weakens both removal efficiencies. In addition, the reaction mechanism of simultaneous removal of SO2 and NO using SDA combined with O3 oxidation was proposed.


Asunto(s)
Hierro , Dióxido de Azufre , Oxidación-Reducción , Temperatura
10.
ACS Omega ; 5(31): 19615-19624, 2020 Aug 11.
Artículo en Inglés | MEDLINE | ID: mdl-32803056

RESUMEN

Ag-decorated g-C3N4 (denoted as Ag/CN-x) was prepared by a one-step calcination method, and the influences of calcination time on structure, morphology, surface composition, photocatalytic performance, and catalytic reduction activity of the prepared Ag/CN-x samples were investigated. The tests showed that the Ag/CN-8 prepared through by calcination for 8 h exhibited the best photocatalytic degradation efficiency of methyl orange (98.7% within 2 h) and the best catalytic reduction property of 4-nitrophenol (100% within 70 s). Meanwhile, these Ag/CN-x samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Brunauer-Emmett-Teller (BET), X-ray photoelectron spectroscopy (XPS), UV-vis diffuse reflectance spectra (DRS), photoluminescence (PL), photocurrent response, and electrochemical impedance spectroscopy (EIS) Nyquist plots. It was found that the Ag/CN-8 prepared through calcination for 8 h had a higher specific surface area, higher dispersibility of silver nanoparticles (Ag NPs), the widest range of visible light response, and the lowest photogenerated electron-hole recombination rate. The results of the trapping experiments indicated that a superoxide radical plays a major role. Moreover, a possible mechanism of photocatalytic degradation in methyl orange and catalytic reduction 4-nitrophenol was proposed.

11.
Nanoscale Res Lett ; 15(1): 109, 2020 May 14.
Artículo en Inglés | MEDLINE | ID: mdl-32409877

RESUMEN

The rutile SnxTi1-xO2 (x = 0, 0.33, 0.5, 0.67, 1) solid solution was synthesized by a one-step hydrothermal method, in which tetrabutyl titanate and Tin (IV) chloride pentahydrate were used as raw materials. A series of Ru/SnxTi1-xO2 were then prepared by the impregnation process in RuCl3 to investigate the performance and stability of CO and C3H8 oxidation. These catalysts were characterized through XRD, N2 adsorption-desorption, FT-IR, TEM, XPS, H2-TPR, and O2-TPD techniques. The effect of Sn/Ti molar ratio and hydrothermal condition on the low-temperature catalytic oxidized performance and stability of Ru/SnxTi1-xO2 were investigated. The results indicated that Ru/Sn0.67Ti0.33O2 catalyst showed an excellent activity and stability at low temperatures. The CO conversion reached 50% at 180 °C and 90% at 240 °C. Besides, the C3H8 conversion reached 50% at 320 °C, the complete conversion of C3H8 realized at 500 °C, and no deactivation occurs after 12 h of catalytic reaction. The excellent low-temperature activity and stability of the Ru/Sn0.67Ti0.33O2 were attributed to the following factors. Firstly, XRD results showed that Sn4+ was successfully introduced into the lattice of TiO2 to replace Ti4+ forming a homogeneous solid solution (containing -Sn4+-O-Ti4+- species), which was consistent with TEM and N2 adsorption-desorption results. The introduction of Sn could suppress the growth of anatase crystal and promote the formation of rutile phase, and this phase transition was helpful to improve the low-temperature activity of the catalysts. Secondly, TEM images showed that ultrafine Ru nanoparticles (~ 5 nm) were dispersed on Sn0.67Ti0.33O2 support, suggesting that the formation of SnxTi1-xO2 solid solution was beneficial to the dispersion of Ru particles.

12.
Polymers (Basel) ; 12(2)2020 Feb 02.
Artículo en Inglés | MEDLINE | ID: mdl-32024255

RESUMEN

Ionic liquids found a wide application in catalysis and extraction due to their unique properties. Herein, ethylene glycol dimethacrylate as the cross-linker and 1-vinyl-3- butylimidazolium tetrafluoroborate as functional monomer via thermally initiated free-radical polymerization was prepared as a novel copolymer solid phase micro-extraction (SPME) coating. A surface modified stainless-steel wire was implemented as the substrate. Factors affecting the extraction performances of the copolymer, including the molar ratio of monomers to cross-linkers, the amount of porogen agent, and polymerization time were evaluated and optimized. To evaluate the extraction performance, five commonly seen polycyclic aromatic hydrocarbons (PAHs) were taken as the analytical targets. The potential factors affecting extraction efficiency were optimized. The as-prepared SPME device, coupled with gas chromatography, was successfully applied for the determination of PAHs in water samples. The wide linear range, low detection limit, good reproducibility, selectivity, and excellent thermal stability indicate the promising application of the newly developed SPME fiber in environmental monitoring as well as in other samples having complex matrices.

13.
J Sep Sci ; 43(5): 896-904, 2020 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-31840426

RESUMEN

In this study, a new covalent organic framework, consisting of tetra(4-aminophenyl)porphyrin and tris(4-formyl phenyl)amine, was layer-by-layer immobilized on stainless-steel wire as a coating for microextraction. The fabrication process was easy and controllable under mild conditions. The as-grown fiber was applied to extract polycyclic aromatic hydrocarbons in aqueous solution via head-space solid-phase microextraction. Furthermore, it was analyzed by gas chromatography with a flame ionization detector. A wide linear range (0.1-50 µg/L), low limits of detection (0.006-0.024 µg/L, signal-to-noise ratio = 3), good repeatability (intra-fiber, n = 6, 3.1-8.50%), and reproducibility (fiber to fiber; n = 3, 5.79-9.98%), expressed as relative standard deviations, demonstrate the applicability of the newly developed coating. This new material was successfully utilized in real sample extraction with a satisfactory result. Potential parameters affecting the extraction efficiency, including extraction temperature and extraction time, salt concentration, agitation speed, sample volume, desorption temperature, and time, were also optimized and discussed.

14.
ACS Omega ; 4(25): 21091-21099, 2019 Dec 17.
Artículo en Inglés | MEDLINE | ID: mdl-31867502

RESUMEN

Simultaneous removal of NO x and SO2 by MgO combined with O3 oxidation was studied. The effects of the O3/NO molar ratio, oxidation temperature, and oxidation residence time on N2O5 decomposition and O3 consumption distributions were systematically illustrated, which is of great significance for improving NO x removal efficiency and reducing O3 consumption in practical application. When the O3/NO molar ratio was greater than 1.0, the highest N2O5 yield was achieved at 90 °C. The NO x removal efficiency reached 96.5% at an O3/NO molar ratio of 1.8. The oxidation temperature increased from 90 to 130 °C, resulting in the decrease of N2O5 yield, the improvement of O3-ICC (O3 invalid cycle consumption) caused by N2O5 decomposition, and the decrease of NO x removal efficiency from 96.5 to 76%. Besides, the effects of pH, SO2 concentration, and MgSO3 addition on NO x removal efficiency were also investigated. The results showed that the removal efficiency of NO x decreased with the increase of SO2 concentration, while MgSO3 addition into MgO slurry could promote the absorption of NO2 due to the reaction between NO2 and SO3 2-.

15.
Nanoscale Res Lett ; 14(1): 302, 2019 Aug 30.
Artículo en Inglés | MEDLINE | ID: mdl-31471771

RESUMEN

Visible-light-driven stannic oxide was synthesized by facile one-pot solvothermal method from SnCl2·2H2O and methanol. The as-prepared powder was identified by XRD as the low crystalline phase of SnO2, and its absorption edge reached about 530 nm, presenting good potential to respond to visible light. Under visible light irradiation (λ > 420 nm), the as-prepared tin oxide showed good anodic photocurrent effects on FTO photoelectrode, and showed hydrogen and oxygen evolution activities under electron donor (methanol) and acceptor (AgNO3), respectively, even without any co-catalyst loading. The visible-light-driven mechanism for this SnO2-x maybe ascribed to Sn2+ self-doped into Sn4+ and formed an energy gap between the band gap of SnO2.

16.
RSC Adv ; 9(32): 18222-18231, 2019 Jun 10.
Artículo en Inglés | MEDLINE | ID: mdl-35515254

RESUMEN

A facile and green hydrothermal method has been developed for the synthesis of Ag3PO4 with a variety of morphologies, including cubic, rhombic dodecahedral, spherical and roughly spherical, by using Ag4P2O7 as a sacrificial precursor. The as-prepared catalysts were characterized by carrying out X-ray diffraction (XRD), scanning electron microscopy (SEM), UV-visible diffuse reflectance spectroscopy (UV-Vis DRS), Fourier transform infrared spectroscopy (FT-IR) and X-ray photoelectron spectroscopy (XPS). The morphology of Ag3PO4 was controlled by simply adjusting the hydrothermal reaction temperature and time, without adding any templates and organic additives. Kinetics studies and characterization results revealed that the transformation from P2O7 4- to a PO4 3- radical was a rate-determining step, and influenced the morphology of Ag3PO4. Different oxygen evolution rates were observed for samples subjected to different hydrothermal reaction times, and the highest initial rate of O2 evolution achieved was 582.55 µmol h-1 g-1. Furthermore, for the samples prepared using a hydrothermal reaction time of 96 h, as the hydrothermal reaction temperature was increased, the oxygen evolution rate of the resulting sample decreased first and then increased, and the highest initial rate of O2 evolution was 856.06 µmol h-1 g-1, about twice the 418.34 µmol h-1 g-1 value for the sample prepared using the coprecipitation method. A possible mechanism has been proposed to explain how the hydrothermal reaction temperature and time influenced the Ag3PO4 morphology. Our method provides a guiding hydrothermal strategy for the synthesis of insoluble electrolytes with various morphologies from relatively soluble electrolytes without the need to use templates and organic additives.

17.
Molecules ; 23(1)2018 Jan 15.
Artículo en Inglés | MEDLINE | ID: mdl-29342978

RESUMEN

The host-guest interaction of a series of cyclohexyl-appended guests with cucurbit[8]uril (Q[8]) was studied by ¹H NMR spectroscopy, isothermal titration calorimetry (ITC), and X-ray crystallography. The X-ray structure revealed that two cycloalkane moieties can be simultaneously encapsulated in the hydrophobic cavity of the Q[8] host to form a ternary complex for the first time.


Asunto(s)
Hidrocarburos Aromáticos con Puentes/química , Ciclohexilaminas/química , Imidazoles/química , Calorimetría , Cristalografía por Rayos X , Espectroscopía de Resonancia Magnética , Modelos Moleculares , Estructura Molecular , Termodinámica
18.
Bull Environ Contam Toxicol ; 93(6): 769-74, 2014 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-25227428

RESUMEN

A headspace solid phase microextraction (HS-SPME) technique using stainless steel fiber coated with 20 µm multi-walled carbon nanotubes (MWCNTs) and gas chromatography with thermionic specific detector (GC-TSD) was developed to determine organophosphorous pesticides (OPPs) in soil. Parameters affecting the extraction efficiency such as extraction time and temperature, ionic strength, the volume of water added to the soil, sample solution volume to headspace volume ratio, desorption time, and desorption temperature were investigated and optimized. Compared to commercial polydimethylsiloxane (PDMS, 7 µm) fiber, the PDMS fiber was better to be corrected as phorate, whereas the MWCNTs fiber gave slightly better results for methyl parathion, chlorpyrifos and parathion. The optimized SPME method was applied to analyze OPPs in spiked soil samples. The limits of detection (LODs, S/N = 3) for the four pesticides were <0.216 ng g(-1), and their calibration curves were all linear (r (2) ≥ 0.9908) in the range from 1 to 200 ng g(-1). The precision (RSD, n = 6) for peak areas was 6.5 %-8.8 %. The recovery of the OPPs spiked real soil samples at 50 and 150 ng g(-1) ranged from 89.7 % to 102.9 % and 94.3 % to 118.1 %, respectively.


Asunto(s)
Monitoreo del Ambiente/instrumentación , Monitoreo del Ambiente/métodos , Nanotubos de Carbono/química , Compuestos Organofosforados/análisis , Plaguicidas/análisis , Contaminantes del Suelo/análisis , Microextracción en Fase Sólida/métodos , Carbono/química , Cromatografía de Gases , Dimetilpolisiloxanos/química , Límite de Detección
19.
J Chromatogr A ; 1188(1): 43-9, 2008 Apr 18.
Artículo en Inglés | MEDLINE | ID: mdl-18037422

RESUMEN

Microwave irradiation can provide a viable alternative to the traditional means such as ultraviolet light and thermal initiation for the preparation of monolithic capillary columns. Polystyrene-based monolithic stationary phases were prepared in situ in fused-silica capillaries and simultaneously in vials. The column permeability, electrophoretic and chromatographic behavior were evaluated using pressure-assisted capillary electrochromatography (pCEC), capillary electrochromatography (CEC) and low pressure liquid chromatography (LPLC). With an optimal monolithic material, the largest theoretical plates for preparing the column could be close to 18,000 plates/m for thiourea in the mode of pCEC. Furthermore, the influence of the composition of the porogenic solvents (toluene/isooctane) on the morphology of organic-based monoliths [poly(styrene-divinylbenzene-methacrylic acid)] was systematically studied with mercury intrusion porosimetry and scanning electron microscopy. The monoliths which were prepared with a high content of isooctane had a bigger pore size and better permeability, and hence resulted in a faster separation.


Asunto(s)
Poliestirenos/química , Algoritmos , Electrocromatografía Capilar , Cromatografía Líquida de Alta Presión , Electroforesis Capilar , Microscopía Electrónica de Rastreo , Microondas , Poliestirenos/efectos de la radiación
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