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1.
J Colloid Interface Sci ; 651: 726-733, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37567116

RESUMO

Carbon nitride is an attractive non-metallic photocatalyst due to its small surface area, rapid electron-hole recombination, and low absorption of visible light. In this study, one-dimensional carbon nitride nanotubes were successfully synthesized by supramolecular self-assembly method for photocatalytic reduction of CO2 under mild conditions. The material demonstrates significantly improved CO2-to-CO activity compared to bulk carbon nitride under visible light irradiation, with a rate of 12.58 µmol g-1h-1, which is 3.37 times higher than that of pristine carbon nitride. This enhanced activity can be attributed to the abundant oxygen defects and nitrogen vacancies in the unique tubular carbon nitride structure, which results in the generation of more active sites and the efficient acceleration of the migration of photogenerated electron-hole pairs. Various characterizations collectively support the presence of these defects and vacancies. Moreover, in situ DRIFTS spectroscopy supported the proposed reaction mechanism for the photoreduction of CO2. This eco-friendly design approach provides novel insights into utilizing solar energy for the production of value-added products.

2.
R Soc Open Sci ; 10(6): 221213, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-37325598

RESUMO

Copper-doped ZnO-ZrO2 solid solution catalysts were synthesized via co-precipitation for promoting CH3OH synthesis via hydrogenation of CO2. Various testing methods were applied to investigate the effect of various copper contents on the catalysts. The catalytic performance was evaluated by a fixed bed reactor. XRD, HRTEM and Raman spectra collectively indicated that a ZnO-ZrO2 solid solution catalyst with 3% Cu had a higher Cu dispersion, while the H2-TPR results confirmed that a catalyst with 3% Cu had more Cu active sites under low temperature H2 pretreatment. When the copper content increased to 5% and 10%, the catalyst showed a better Cu crystallinity and a worse Cu dispersion, which could have a negative effect. Therefore, the CO2 conversion and methanol yield with a 3% CuZnO-ZrO2 catalyst at 5 MPa, 250°C and 12 000 ml/(g h) increased by 8.6% and 7.6%, respectively. Moreover, the CH3OH selectivity and catalytic stability of the solid solution catalyst were better than those of the traditional CZA catalyst.

3.
Front Chem ; 11: 1187762, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37288077

RESUMO

Cu1In2Zr4-O-C catalysts with Cu2In alloy structure were prepared by using the sol-gel method. Cu1In2Zr4-O-PC and Cu1In2Zr4-O-CP catalysts were obtained from plasma-modified Cu1In2Zr4-O-C before and after calcination, respectively. Under the conditions of reaction temperature 270°C, reaction pressure 2 MPa, CO2/H2 = 1/3, and GHSV = 12,000 mL/(g h), Cu1In2Zr4-O-PC catalyst has a high CO2 conversion of 13.3%, methanol selectivity of 74.3%, and CH3OH space-time yield of 3.26 mmol/gcat/h. The characterization results of X-ray diffraction (XRD), scanning electron microscopy (SEM), and temperature-programmed reduction chemisorption (H2-TPR) showed that the plasma-modified catalyst had a low crystallinity, small particle size, good dispersion, and excellent reduction performance, leading to a better activity and selectivity. Through plasma modification, the strong interaction between Cu and In in Cu1In2Zr4-O-CP catalyst, the shift of Cu 2p orbital binding energy to a lower position, and the decrease in reduction temperature all indicate that the reduction ability of Cu1In2Zr4-O-CP catalyst is enhanced, and the CO2 hydrogenation activity is improved.

4.
Environ Sci Pollut Res Int ; 28(20): 25949-25958, 2021 May.
Artigo em Inglês | MEDLINE | ID: mdl-33479875

RESUMO

A series of CQDs/Bi2WO6 (CBW) hybrid materials with different loading amounts of carbon quantum dots (CQDs) were prepared via a facile in situ hydrothermal method. As determined by multiple techniques including XRD, TEM, UV-vis, PL, TPR, and XPS, the CBW possessed expanded visible light response interval, decreased recombination rate of the photogenerated electron hole, and enhanced oxidation ability as compared with the pristine Bi2WO6. In addition, with different loading amounts of CQDs, the optical and electronic properties of the corresponding CBW were different. These CBW materials performed superior activities to the pristine Bi2WO6 in the photodegradation of VOCs under visible light, among which the CBW-2 demonstrated the best activity of almost complete degradation within only 120 min. Moreover, the CBW-2 exhibited high stability and reusability after five cycles.


Assuntos
Pontos Quânticos , Compostos Orgânicos Voláteis , Carbono , Catálise , Luz
5.
RSC Adv ; 11(17): 9865-9873, 2021 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-35423482

RESUMO

In this study, an AgBr/Ag3PO4 (ABAP) photocatalyst has been prepared via a facile one-pot anion-exchange method. SEM, XRD, XPS and UV-Vis DRS characterization techniques are carried out to study the structural and physicochemical characteristics of the AgBr/Ag3PO4 composites. The ABAP photocatalyst exhibited outstanding photocatalytic capability for the photodegradation of rhodamine B (RhB) under visible light irradiation. The optimal ABAP-48% composite displayed the highest photocatalytic activity; a complete degradation was attained in 25 min under visible light irradiation. The excellent stability and reusability of ABAP catalysts were examined by five subsequent runs. A probable degradation mechanism of ABAP composites was carefully surveyed. Furthermore, radical trapping experiments confirmed that the ˙O2 - radical was the main active species in the photodegradation reaction.

6.
Sci Total Environ ; 712: 135635, 2020 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-31806306

RESUMO

The support effect on CeO2 supported CuO catalysts are extensively investigated, but few studies have been reported in volatile organic compounds (VOCs) oxidation. Herein, CuO was impregnated on three conventional method synthesized CeO2 to study its impact on toluene total oxidation over CeO2 at low temperature (≤280 °C). Characterization results demonstrated that the shape and specific surface area of CeO2 affected the degree of CuO dispersion, which determine the interaction between CuO and CeO2. CuO significantly enhanced the toluene adsorption capacity of CeO2, but lots of oxygen vacancies were lost during its loading. Although strong CuCe interaction induced new oxygen vacancies, the increase or decrease of final amount was related to the original surface properties of CeO2. Mechanism analysis suggested that the activation of oxygen on oxygen vacancies controlled the toluene oxidation reaction rate. Therefore, the promotion or inhibition effect of CuO on CeO2 for toluene oxidation depends on physical and chemical properties. Through this study, we have drawn some valuable information in guiding the synthesis and design of CuO-CeO2 based catalysts.

7.
Chemosphere ; 235: 1146-1153, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-31561305

RESUMO

Waste is a misplaced resource. Herein, anionic (orange II sodium salt and Ponceau 2R) and cationic (Rhodamine B and Methylene blue) dye wastewater assisted photo-treatment (referred as DAPT) method was developed to modify sol-gel synthesized CeO2-TiO2 (CeTi) mixed oxide catalyst. Catalytic activity test results showed that both anionic and cationic dye wastewater could be used as "fuel" of photo-treatment to enhance the activity of CeTi catalyst in NO reduction and dichloromethane oxidation. Characterization and DFT calculation results revealed that DAPT process increased the amount of Ce3+ ions on CeTi samples, which could induce the formation of Ce-VO-Ti (oxygen vacancy (VO) in Ce-O-Ti short range structure). These Ce-VO-Ti defects not only could be adsorption sites for NH3, dichloromethane and oxygen, but also promoted the redox shift of Ce3++ Ti4+ ⇋ Ce4++ Ti3+ by enhancing the oxidizability of Ce4+ and Ti4+ species. Furthermore, defects changed the polarity of Ce-O and Ti-O, which was conducive to the activation of lattice oxygen. All these improvements contributed to the excellent catalytic activity of CeTi catalysts. We expected this work to be instructive on constructing structure-activity over CeO2-TiO2 based catalysts and utilizing dye wastewater.


Assuntos
Cério/química , Cloreto de Metileno/química , Óxido Nítrico/química , Titânio/química , Águas Residuárias/química , Adsorção , Catálise , Corantes , Oxirredução , Oxigênio/química
8.
Materials (Basel) ; 11(4)2018 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-29641476

RESUMO

In this work, a new composite materials of graphene oxide (GO)-incorporated metal-organic framework (MOF)(UiO-66-NH2/GO) were in-situ synthesized, and were found to exhibit enhanced high performances for CO2 capture. X-ray diffraction (XRD), scanning electron microscope (SEM), N2 physical adsorption, and thermogravimetric analysis (TGA) were applied to investigate the crystalline structure, pore structure, thermal stability, and the exterior morphology of the composite. We aimed to investigate the influence of the introduction of GO on the stability of the crystal skeleton and pore structure. Water, acid, and alkali resistances were tested for physical and chemical properties of the new composites. CO2 adsorption isotherms of UiO-66, UiO-66-NH2, UiO-66/GO, and UiO-66-NH2/GO were measured at 273 K, 298 K, and 318 K. The composite UiO-66-NH2/GO exhibited better optimized CO2 uptake of 6.41 mmol/g at 273 K, which was 5.1% higher than that of UiO-66/GO (6.10 mmol/g). CO2 adsorption heat and CO2/N2 selectivity were then calculated to further evaluate the CO2 adsorption performance. The results indicated that UiO-66-NH2/GO composites have a potential application in CO2 capture technologies to alleviate the increase in temperature of the earth's atmosphere.

9.
Environ Technol ; 34(9-12): 1405-10, 2013.
Artigo em Inglês | MEDLINE | ID: mdl-24191473

RESUMO

Titanium-based adsorbents for CO2 capture were prepared through impregnating the as-synthesized TiO2 nanotubes (TiNT) with four kinds of amines, namely monoethanolamine (MEA), ethylenediamine (EDA), triethylenetetramine (TETA) and tetraethylenepentamine (TEPA). The resultant samples were characterized by X-ray diffraction, low-temperature N2 adsorption as well as transmission electron microscopy. The absorption of CO2 was carried out in a dynamic packed column. The sample impregnated with TEPA showed a better adsorption capacity due to its higher amino groups content. In addition, CO2 adsorption capacity increases as the amount of amine loaded increases. Therefore, TiNT-TEPA-69 showed the highest CO2 adsorption capacity among the three samples impregnated with TETA; approximately 4.10 mmol/g at 30 degrees C. In addition, the dynamic adsorption/desorption performance was investigated. The adsorption capacity of TiNT-TEPA-69 dropped slightly (about 2%) during a total of five cycles. The TiNT-TEPA-69 adsorbent exhibited excellent CO2 adsorption/desorption performance.


Assuntos
Poluentes Atmosféricos/isolamento & purificação , Aminas/química , Dióxido de Carbono/isolamento & purificação , Nanotubos/química , Titânio/química , Adsorção , Poluentes Atmosféricos/química , Dióxido de Carbono/química , Recuperação e Remediação Ambiental
10.
J Environ Sci (China) ; 25(3): 554-60, 2013 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-23923429

RESUMO

TiO2 nanotubes (TiNT) were prepared by a hydrothermal treatment and modified by three kinds of amines, namely ethylenediamine, polyetherimide and tetraethylenepentamine (TEPA), to study their CO2 adsorption properties from gas streams. The resultant samples were characterized by X-ray diffraction, transmission electron microscopy, and infrared spectroscopy, as well as low temperature N2 adsorption. CO2 capture was investigated in a dynamic packed column at 30 degrees C. TEPA-modified TiO2 nanotubes showed the highest adsorption capacity of 167.64 mg/g because it had the highest amino-group content among the three amines. CO2 fixation on TiNT impregnated by TEPA was investigated at 30, 50, and 70 degrees C, and the adsorption capacity increased slightly with temperature. Following the adsorption step, the sorbents were regenerated by temperature programmed desorption, and the TiNT-TEPA sample, as CO2 sorbent, was found to be readily regenerated and energy-efficient. The cycle test also revealed that the TiNT-TEPA adsorbent is fairly stable, with only a 5% drop in the adsorption capacity after 10 adsorption/desorption cycles. In addition, the CO2 adsorption behavior was investigated with the deactivation model, and which showed an excellent prediction for the TiNT-TEPA breakthrough curves.


Assuntos
Aminas/química , Dióxido de Carbono/isolamento & purificação , Nanotubos/química , Titânio/química , Adsorção , Etilenodiaminas/química , Cinética , Modelos Químicos , Nanotubos/ultraestrutura , Espectrofotometria Infravermelho , Temperatura , Difração de Raios X
11.
J Environ Sci (China) ; 25(10): 2081-7, 2013 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-24494495

RESUMO

Carbon dioxide (CO2) adsorption on a standard metal-organic framework Mg2(dobdc) (Mg/DOBDC or Mg-MOF-74) and a tetraethylenepentamine (TEPA) modified Mg2(dobdc) (TEPA-Mg/DOBDC) were investigated and compared. The structural information, surface chemistry and thermal behavior of the adsorbent samples were characterized by X-ray powder diffraction (XRD), infrared spectroscopy (IR), thermogravimetric analysis (TGA) and nitrogen adsorption-desorption isotherm analysis. CO2 adsorption capacity was measured by dynamic adsorption experiments with N2-CO2 mixed gases at 60 degrees C. Results showed that the CO2 adsorption capacity of Mg/DOBDC was significantly improved after amine modification, with an increase from 2.67 to 6.06 mmol CO2/g adsorbent. Moreover, CO2 adsorption on the TEPA-Mg/DOBDC adsorbent was promoted by water vapor, and the adsorption capacity was enhanced to 8.31 mmol CO2/g absorbent. The adsorption capacity of the TEPA-Mg/DOBDC adsorbent dropped only 3% after 5 consecutive adsorption/desorption cycles. Therefore, this kind of adsorbent can be considered as a promising material for the capture of CO2 from flue gas.


Assuntos
Dióxido de Carbono/química , Etilenodiaminas/química , Gases/química , Compostos de Magnésio/química , Espectrofotometria Infravermelho , Água
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