Hierarchically porous γ-Al2O3 nanosheets: Facile template-free preparation and reaction mechanism for H2S selective oxidation

Shen, Lijuan; Zheng, Xiaohai; Lei, Ganchang; Li, Xiang; Cao, Yanning; Jiang, Lilong

doi:10.1016/j.cej.2018.03.157

Cited by 74 publications

(39 citation statements)

References 57 publications

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“…Alumina oxides contain tremendous acid sites due to the existence of empty orbitals, which can act as a Lewis acid [43]. In order to determine the acid-base properties of the as prepared samples, NH 3 -TPD (acid sites) and CO 2 -TPD (base sites) were chosen to study in this work.…”

Section: Acid-base Site Characterizationmentioning

confidence: 99%

Controllable Acid/Base Propriety of Sulfate Modified Mixed Metal Oxide Derived from Hydrotalcite for Synthesis of Propylene Carbonate

Ding

Zhang

et al. 2019

Catalysts

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Ammonium persulfate modified mixed metal oxide derived from hydrotalcite with tunable acid/base properties can be prepared via thermal decomposition of Mg-Al hydrotalcite-type precursors and ammonium persulfate. By controlling the ammonium persulfate content, these sulphur mutated samples, denoted as SMgAlO-y (y = 1; 3; 5; 7), were investigated in this research. The resulted materials were characterized by XRD, SEM, FT-IR spectra, Py-IR spectra, XPS, Hammett indicator, CO2-TPD, as well as NH3-TPD. Furthermore, the acid-base property of the sample surface was determined by inverse gas chromatography measurements (IGC). Among all the obtained outcomes, the target SMgAlO-5 demonstrated the maximal Ka/Kb value, and it presented the highest activity as a catalyst in the synthesis of propylene carbonate (PC) through 1,2-propylene glycol and urea, giving the yield of 97.2% at the optimized reaction condition, which indicated that the PC yield counted on the synergic effect of the acidity and basicity on catalysts.

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Section: Acid-base Site Characterizationmentioning

confidence: 99%

Controllable Acid/Base Propriety of Sulfate Modified Mixed Metal Oxide Derived from Hydrotalcite for Synthesis of Propylene Carbonate

Ding

Zhang

et al. 2019

Catalysts

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“…In Figure c, the Mo 2 C sample shows a sulfur yield of 94.0% at 130 °C. MC/CN exhibits the highest sulfur yield (99.0%) at 190 °C, much higher than that of CN . There is no doubt that the introduction of Mo 2 C contributes to the enhanced sulfur yield (160–250 °C).…”

Section: Resultsmentioning

confidence: 93%

“…Taking this into consideration, it is reasonable to combine the superior electronegativity of CN and outstanding electronic capture capability of Mo 2 C together. As expected, the composite showed a high sulfur selectivity of nearly 100% from 100 to 190 °C, sulfur yield of >99% at 190 °C, and H 2 S conversion stability of >95% for as long as 30 h, outperforming most of oxides. , We demonstrate for the first time the use of Mo 2 C and Mo 2 C-modified CN for H 2 S oxidation.…”

Section: Introductionmentioning

confidence: 99%

Enhanced Selective H₂S Oxidation Performance on Mo₂C-Modified g-C₃N₄

Lei

Zhou

Zheng

et al. 2019

ACS Sustainable Chem. Eng.

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Direct catalytic selective oxidation of H2S to sulfur at low temperature has been drawing attention. Molybdenum carbide (Mo2C), in which the excess occupied orbitals provide more back-donation chances for the adsorbents’ π-orbitals, shows activity in electrocatalysis, photocatalysis, thermocatalysis, etc. that are comparable to those of noble metals. This work reports for the time the use of Mo2C and Mo2C-modified g-C3N4 for catalytic selective oxidative desulfurization. The density functional theory calculation indicates that Mo2C facilitates the adsorption of H2S molecule and the HS group. Furthermore, the Mo2C-modified g-C3N4 shows a sulfur yield of as high as 99.0% at 190 °C, much higher than that of g-C3N4 (46.0%). The good stability of the catalyst was demonstrated by X-ray diffraction, Fourier transform infrared spectra, and so on. Remarkably, the H2S conversion of the Mo2C-modified g-C3N4 remains constant (95.0%) at 190 °C for as long as 30 h. As a first demonstration using carbides in selective H2S oxidation, this work provides an opportunity to develop a novel class of potential catalysts.

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“…The selective catalytic oxidation of H 2 S (H 2 S+1/2O 2 →1/n S n +H 2 O) is a technique that can eliminate H 2 S with sulfur being recovered as a useful resource. Specifically, this process is free from thermodynamic limitations and low in capital cost, thus offering practical advantages over current industrial routes for H 2 S elimination [6–11] …”

Section: Methodsmentioning

confidence: 99%

“…Specifically, this process is free from thermodynamic limitations and low in capital cost, thus offering practical advantages over current industrial routes for H 2 S elimination. [6][7][8][9][10][11] Metal oxides catalysts such as Fe 2 O 3 and Al 2 O 3 have been widely studied for H 2 S selective oxidation by their competitive cost and considerable catalytic performances. [12][13][14][15] Nonetheless, even after long-term research, the catalytic performance (i. e. selectivity, conversion, and stability) of these catalysts can still not satisfy simultaneously.…”

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confidence: 99%

Electronic Regulation of Bromophenyl Grafted Metal‐Free Carbon Nitride Catalysts for Enhanced Utilization of H₂S

et al. 2021

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Developing metal‐free heterogeneous catalysts with high efficiency for the elimination of H2S into eco‐friendly products are very important for both fundamental catalytic science and industrial chemistry. Herein, we design a new modified carbon nitride catalyst engrafted with Br‐substituted aromatic heterocycle (CNU−Br) through a simple copolymerization and exfoliation method. CNU−Br exhibits excellent H2S conversion efficiency, high sulfur selectivity, and outstanding stability in the catalytic desulfurization reaction, which is better than most of the reported catalysts. The experiments and theoretical calculations show that the grafting of bromophenyl groups into the fundamental carbon nitride structural network leads to π‐delocalization, surface modification, as well as enhances the basicity of the structural active N sites. The regulation of the H and S affinity of CNU−Br that mediate the facile cleavage of H2S hydrogen‐sulfur bonds and the release of S atoms in thermodynamics. Furthermore, the superior surface area and mass transfer over CNU−Br accelerate the adsorption and oxidation of H2S in kinetics compared with the ordinary carbon nitride.

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Hierarchically porous γ-Al2O3 nanosheets: Facile template-free preparation and reaction mechanism for H2S selective oxidation

Cited by 74 publications

References 57 publications

Controllable Acid/Base Propriety of Sulfate Modified Mixed Metal Oxide Derived from Hydrotalcite for Synthesis of Propylene Carbonate

Controllable Acid/Base Propriety of Sulfate Modified Mixed Metal Oxide Derived from Hydrotalcite for Synthesis of Propylene Carbonate

Enhanced Selective H₂S Oxidation Performance on Mo₂C-Modified g-C₃N₄

Electronic Regulation of Bromophenyl Grafted Metal‐Free Carbon Nitride Catalysts for Enhanced Utilization of H₂S

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Hierarchically porous γ-Al2O3 nanosheets: Facile template-free preparation and reaction mechanism for H2S selective oxidation

Cited by 74 publications

References 57 publications

Controllable Acid/Base Propriety of Sulfate Modified Mixed Metal Oxide Derived from Hydrotalcite for Synthesis of Propylene Carbonate

Controllable Acid/Base Propriety of Sulfate Modified Mixed Metal Oxide Derived from Hydrotalcite for Synthesis of Propylene Carbonate

Enhanced Selective H2S Oxidation Performance on Mo2C-Modified g-C3N4

Electronic Regulation of Bromophenyl Grafted Metal‐Free Carbon Nitride Catalysts for Enhanced Utilization of H2S

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Enhanced Selective H₂S Oxidation Performance on Mo₂C-Modified g-C₃N₄

Electronic Regulation of Bromophenyl Grafted Metal‐Free Carbon Nitride Catalysts for Enhanced Utilization of H₂S