Solving the Water Hypersensitive Challenge of Sulfated Solid Superacid in Acid-Catalyzed Reactions

Li, Licheng; Yue, Haiqin; Zhang, Suoying; Huang, Yao‐Bing; Zhang, Weina; Wu, Peng; Ji, Yongxin; Huo, Fengwei

doi:10.1021/acsami.8b20506

Cited by 15 publications

(5 citation statements)

References 32 publications

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“…All the supports and catalysts show typical type IV adsorption isotherms with a noticeable hysteresis loop. This indicates the presence of mesoporous structures in all samples, as is also demonstrated by their pore-size distribution patterns [44,45]. Further, it can be observed from Figure 3a that TiO 2 with different pH values have remarkably different shapes of hysteresis loops.…”

Section: Structural Propertiessupporting

confidence: 58%

Complete Hydrodesulfurization of Dibenzothiophene via Direct Desulfurization Pathway over Mesoporous TiO2-Supported NiMo Catalyst Incorporated with Potassium

Song²,

Yue

et al. 2019

Catalysts

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Mesoporous TiO2 containing different potassium content was prepared from potassium titanate by mediating the pH value of the ion exchange, which was used as catalytic support to load NiMo for hydrodesulfurization of dibenzothiophene. The as-prepared samples were characterized by X-ray diffraction, N2 physical adsorption/desorption, temperature-programmed reduction, scanning electron microscope/energy dispersive X-ray mapping analysis, high resolution transmission electron microscopy, and pyridine-adsorbed Fourier transform infrared spectroscopy. The characterization results showed that NiO and MoO3 were well dispersed on mesoporous TiO2 with varying potassium content. A crystal NiMoO4 phase was formed on the TiO2 with relatively high potassium content, which could decrease the reduction temperature of oxidized active species. The evaluation results from the hydrodesulfurization displayed that as the potassium content of the catalyst increased, the dibenzothiophene conversion firstly increased and then slightly decreased when potassium content exceeded 6.41 wt %. By contrast, the direct desulfurization selectivity could continuously increase along with the potassium content of catalyst. Furthermore, the change in direct desulfurization selectivity of a TiO2-supported NiMo catalyst was independent of the reaction condition. The mesoporous TiO2-supported NiMo catalyst incorporated with potassium could have near both 100% of dibenzothiophene and 100% of direct desulfurization selectivity. According to the structure–performance relationship discussion, the incorporation of potassium species could benefit the formation of more sulfided active species on mesoporous TiO2. Moreover, excessive free potassium species may poison the active sites of the hydrogenation pathway. Both factors determined the characteristics of complete hydrodesulfurization of dibenzothiophene via a direct desulfurization pathway for potassium-incorporated mesoporous TiO2 supported NiMo catalysts.

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Section: Structural Propertiessupporting

confidence: 58%

Complete Hydrodesulfurization of Dibenzothiophene via Direct Desulfurization Pathway over Mesoporous TiO2-Supported NiMo Catalyst Incorporated with Potassium

Song²,

Yue

et al. 2019

Catalysts

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“…Interestingly, TiO 2 predecoration could effectively reduce the interaction between sulfate and MnO x ; the SO 4 2− −TiO 2 @ MnO x catalyst showed a strong MnO 2 diffraction peak intensity (Figure 3A). The results of the FT-IR spectra showed that the modification of sulfate and TiO 2 did not change the basic structural unit of MnO 6 in MnO 2 , 38 and the S species was effectively introduced by treating with ammonium sulfate (1125 cm −1 for the symmetric stretching band of S O) 39 (Figure 3B). The sulfate radical treatment of the MnO x catalyst resulted in a diminution in the specific surface area according to the results of the nitrogen adsorption−desorption isotherm and pore size distribution (Figure 3C,D and Table S1).…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Converting Poisonous Sulfate Species to an Active Promoter on TiO₂ Predecorated MnO_x Catalysts for the NH₃-SCR Reaction

Kang

et al. 2021

ACS Appl. Mater. Interfaces

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MnO x -based catalysts possess excellent low-temperature NH3 selective catalytic reduction (NH3-SCR) activity, but the poor SO2/sulfate poisoning resistance and the narrow active-temperature window limit their application for NO x removal. Herein, TiO2 nanoparticles and sulfate were successively introduced into MnO x -based catalysts to modulate the NH3-SCR activity, and the active-temperature window (NO conversion above 80%, T 80) was significantly broadened to 100–350 °C (SO4 2––TiO2@MnO x ) compared to that of the pristine MnO x catalyst (ca. T 80: 100–268 °C). Combined with advanced characterizations and control experiments, it was clearly shown that the poisonous effects of sulfate on the MnO x catalyst could be efficiently inhibited in the presence of TiO2 species due to the interaction between sulfate and TiO2 to form a solid superacid (SO4 2––TiO2) species as NH3 adsorption sites for the low-temperature process. Furthermore, such solid superacid (SO4 2––TiO2) species could weaken the redox ability to inhibit the excessive oxidation of NH3 and thus enhance the high-temperature activity significantly. This work not only puts forward the TiO2 predecoration strategy that converts sulfate to a promoter to broaden the active temperature window but also experimentally proves that the requirement of redox ability and acidity in the MnO x -based NH3-SCR catalyst was dependent on the reaction temperature range.

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“…(2) Improving the water tolerance of catalysts is also important. Water, one of the byproducts of hexose dehydration, poisons solid acids catalysts because of its strong adsorption on the active sites, leading to site blocking and active sites leaching. , A water-tolerant phosphate-immobilized TiO 2 solid acid was reported by Noma et al, where phosphate/TiO 2 was used for glucose conversion. 34% of HMF yield at 49% of glucose conversion was achieved at 120 °C after 4 h. Also, they suggested that the continuous extraction of HMF increased HMF selectivity, even using a high concentration of glucose solution (40 wt %) as the substrate since the side reactions occurred between HMF and intermediates could be prevented.…”

Section: Thermal Catalytic Transformations Of Biomass-derived Glucosementioning

confidence: 99%

Thermal Catalytic Conversion of Biomass-Derived Glucose to Fine Chemicals

Wang

Huang

et al. 2021

Energy Fuels

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The energy crisis is a major challenge for the 21st century due to fossil fuel depletion. Biomass, the waste material from plants or animals containing renewable and abundant carbon resources, is considered as an ideal alternative for fossil fuels. Glucose, as a building unit of cellulose, is the most widely used monosaccharide that has wide applications ranging from pharmaceuticals and food industries. The conversion of biomassderived glucose has become a major and multidisciplinary field of research. Various catalytic transformation processes have been used in the thermochemical conversion of glucose. Numerous nanocatalysts have been developed to selectively convert biomassderived glucose into fine chemicals. This review mainly summarizes the recent achievements of developing catalytic systems for glucose conversion into high-value chemicals. The catalyst structure−activity relationships and underlying reaction mechanisms are also discussed.

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Solving the Water Hypersensitive Challenge of Sulfated Solid Superacid in Acid-Catalyzed Reactions

Cited by 15 publications

References 32 publications

Complete Hydrodesulfurization of Dibenzothiophene via Direct Desulfurization Pathway over Mesoporous TiO2-Supported NiMo Catalyst Incorporated with Potassium

Complete Hydrodesulfurization of Dibenzothiophene via Direct Desulfurization Pathway over Mesoporous TiO2-Supported NiMo Catalyst Incorporated with Potassium

Converting Poisonous Sulfate Species to an Active Promoter on TiO₂ Predecorated MnO_x Catalysts for the NH₃-SCR Reaction

Thermal Catalytic Conversion of Biomass-Derived Glucose to Fine Chemicals

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Solving the Water Hypersensitive Challenge of Sulfated Solid Superacid in Acid-Catalyzed Reactions

Cited by 15 publications

References 32 publications

Complete Hydrodesulfurization of Dibenzothiophene via Direct Desulfurization Pathway over Mesoporous TiO2-Supported NiMo Catalyst Incorporated with Potassium

Complete Hydrodesulfurization of Dibenzothiophene via Direct Desulfurization Pathway over Mesoporous TiO2-Supported NiMo Catalyst Incorporated with Potassium

Converting Poisonous Sulfate Species to an Active Promoter on TiO2 Predecorated MnOx Catalysts for the NH3-SCR Reaction

Thermal Catalytic Conversion of Biomass-Derived Glucose to Fine Chemicals

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Converting Poisonous Sulfate Species to an Active Promoter on TiO₂ Predecorated MnO_x Catalysts for the NH₃-SCR Reaction