Effect of ZnO on acid–base properties and catalytic performances of ZnO/ZrO<sub>2</sub>–SiO<sub>2</sub> catalysts in 1,3-butadiene production from ethanol–water mixture

Larina, Olga V.; Kyriienko, Pavlo I.; Balakin, Dmytro Yu.; Vorokhta, Mykhailo; Khalakhan, Ivan; Nychiporuk, Y.M.; Matolín, Vladimı́r; Soloviev, Sergiy O.; Orlyk, S. M.

doi:10.1039/c9cy00991d

Cited by 36 publications

(33 citation statements)

References 72 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The lower binding energy (BE) component can be attributed to hydrocarbon [19] or CH 3 I [20] and the other component to C−N bonding in the methylammonium [19] . In the N 1 s level (Figure 1b) only one peak is detected at a BE of 402.6 eV, typical for nitrogen bonding in the MAPI film [6,18] . In the Pb 4 f spectrum (Figure 1c) only a doublet peak related to the MAPI film with the Pb 4 f 7 /2 position at 138.6 eV is observed, in agreement with previous studies [6,21] .…”

Section: Resultssupporting

confidence: 91%

In situ Near‐Ambient Pressure X‐ray Photoelectron Spectroscopy Reveals the Influence of Photon Flux and Water on the Stability of Halide Perovskite

et al. 2020

Self Cite

View full text Add to dashboard Cite

For several years, scientists have been trying to understand the mechanisms that reduce the long‐term stability of perovskite solar cells. In this work, we examined the effect of water and photon flux on the stability of CH3NH3PbI3 perovskite films and solar cells using in situ near‐ambient pressure X‐ray photoelectron spectroscopy (NAP‐XPS), field emission scanning electron microscopy (FESEM), and current density–voltage (J–V) characterization. The used amount of water vapor (up to 1 mbar) had a negligible impact on the perovskite film. The higher the photon flux, the more prominent were the changes in the NAP‐XPS and FESEM data; also, a faster decline in power conversion efficiency (PCE) and a more substantial hysteresis in the J‐V characteristics were observed. Based on our results, it can be concluded that the PCE decrease originates from the creation of Frenkel pair defects in the perovskite film under illumination. The stronger the illumination, the higher the number of Frenkel defects, leading to a faster PCE decline and more substantial hysteresis in the J‐V sweeps.

show abstract

Section: Resultssupporting

confidence: 91%

In situ Near‐Ambient Pressure X‐ray Photoelectron Spectroscopy Reveals the Influence of Photon Flux and Water on the Stability of Halide Perovskite

et al. 2020

Self Cite

View full text Add to dashboard Cite

show abstract

“…These results indicated that the Si−O−Zn and Si−O−Zr bonds were formed in ZnZr/SiO 2 and ZnZrTUD-1. 38 For the Zr 3d region, the Zr 3d peaks of ZnZr/SiO 2 and ZnZrTUD-1 shifted to higher binding energies than those of ZrTUD-1 (Figure S4), suggesting the interaction between Zn and Zr species. Therefore, the ZnZrTUD-1 catalyst, with a strong interaction among ZnO, ZrO 2 , and TUD-1, can enhance the synergies of various active centers to improve the production toward butadiene.…”

Section: ■ Results and Discussionmentioning

confidence: 98%

“…ZnZr/SiO 2 generated a higher amount of LASs than ZnZrTUD-1 (Table 2) owing to the part of the LAS of ZnZr/SiO 2 originating from the interaction of Zn species and silanols. 38 However, over ZnZrTUD-1, the LAS were formed via the interaction both Zr species and silanols. This suggests that the Zn species were mainly in the form of ZnO in ZnZrTUD-1.…”

Section: Table 1 Textural Properties Of the Synthesized Catalystsmentioning

confidence: 99%

One-Pot Hydrothermal Synthesis of Multifunctional ZnZrTUD-1 Catalysts for Highly Efficient Direct Synthesis of Butadiene from Ethanol

Wang

Guo

Gao

et al. 2021

ACS Sustainable Chem. Eng.

View full text Add to dashboard Cite

The direct conversion of ethanol to butadiene (ETB) is a promising approach for renewable butadiene production. However, simultaneous achievement of high butadiene selectivity and catalyst stability has always been a challenge. Here, the multifunctional ZnZrTUD-1 catalyst possesses both superior catalytic performance and stability in direct ETB conversion. To study the effect of the active centers of catalysts on the catalytic performance, the designed active centers of the catalysts were optimized and further characterized by multiple techniques. One-pot hydrothermal synthesis was utilized to improve the interaction among ZnO, ZrO2, and TUD-1 mesoporous silicate. The results demonstrated that the optimized ZnZrTUD-1 catalyst possessed an excellent ability of resistance to carbon deposition and exhibited a synergistic catalysis effect. When the reaction was conducted at 400 °C and a weight hourly space velocity of 0.38 h–1, the catalytic performance revealed that it generated an outstanding butadiene selectivity of 62.5% and an ethanol conversion of 84.6%, which still remained stable during 50 h on stream.

show abstract

“…It should be noted that higher 1,3-BD selectivity is achieved during the conversion of ethanolaqueous mixtures in the presence of ZnLaZr−KSKG as opposed to ZnZr−KSKG (see Table S2, 16 ). This may be attributed to the fact that Brønsted basic sites being active in aldol condensation [49][50][51] (including ETB process) 52 are formed during deposition of lanthanum oxide or hydroxide on SiO 2 .…”

Section: Water Vapor Effect On Catalytic Performance Of the Znlazrsi Oxide Systems For Etbprocessmentioning

confidence: 99%

“…9 Moreover, the presence of over 5-10 % water in the feed has been shown to significantly affect activity and selectivity of the ETB process catalysts. [15][16][17][18][19] Thus, development of the catalysts able to convert ethanol-aqueous mixtures containing 50-80 vol% ethanol into 1,3-BD is a very important task which is insufficiently studied now.…”

Section: Introductionmentioning

confidence: 99%

Design of Effective Catalysts Based on ZnLaZrSi Oxide Systems for Obtaining 1,3-Butadiene from Aqueous Ethanol

Larina

Shcherban

Kyriienko

et al. 2020

ACS Sustainable Chem. Eng.

Self Cite

View full text Add to dashboard Cite

ZnLaZrSi oxide systems prepared with a silica component of the different nature have been studied in 1,3-butadiene production from aqueous ethanol. The following silica materials were used: KSKG, A-175, A-380, SBA-15, MCM-41, MCM-48, MCF and dealuminated BEA zeolites. The characteristics of the porous structure of the silica support, such as porosity, pore size distribution, specific and external surface areas, were found not to be critical parameters for achieving a high 1,3-butadiene yield during the EtOH-H 2 O mixture conversion in the presence of ZnLaZrSi oxide catalysts. On the contrary, the quantity and strength of Lewis acid sites, which in turn differ depending on the choice of silica material, have a significant impact on 1,3-butadiene selectivity and yield. The highest values of the selectivity of 1,3-butadiene formation (up to 68 %) and yield as well as stability toward deactivation in the presence of H 2 O were achieved over ZnLaZr-KSKG, ZnLaZr-SBA-15 and ZnLa-Zr 1 SiBEA (with mononuclear isolated tetrahedral Zr(IV) species). The productivity of ZnLa-Zr 1 SiBEA catalyst accounts for 0.324 g 1,3-BD •g cat -1 •h -1 (T = 648К, WHSV = 2.88 h -1 , 80 vol% EtOH in water as an EtOH source). The main reason for the decrease in 1,3-butadiene yield in the presence of H 2 O in the reaction mixture was shown to be a deactivation of acetaldehyde condensation sites on the catalyst surface, while the rate of acetaldehyde formation decreases slightly. According to 1 H-13 C CP/MAS NMR spectroscopic results, the use of aqueous ethanol as the feed for ETB-process is very advantage to prevent the carburization of the catalysts.= 2.88 h -1 , 80 vol% EtOH in water as an EtOH source). Therefore, for industrial realization of ETB process the development of the effective catalysts based on dealuminated BEA zeolites is also promising. ASSOCIATED CONTENTSupporting Information. The following file is available free of charge. 29Si and 1 H -29 Si CP MAS NMR spectra of ZnLa-Zr 3 SiBEA sample, SEM images of the ZnLaZrSi samples at three magnifications, the indices of EtOH-water mixture conversion in the presence of ZnLaZrSi oxide systems, the indices of ETB process in the presence of 2 %ZnO/6 %ZrO 2 -KSKG (DOCX).

show abstract

Effect of ZnO on acid–base properties and catalytic performances of ZnO/ZrO₂–SiO₂ catalysts in 1,3-butadiene production from ethanol–water mixture

Abstract: The effect of ZnO and the preparation method of ZnO/ZrO2–SiO2 catalysts on their acid–base properties and catalytic performances in the conversion of diluted ethanol mixtures into 1,3-butadiene (BD) is presented.

Cited by 36 publications

References 72 publications

In situ Near‐Ambient Pressure X‐ray Photoelectron Spectroscopy Reveals the Influence of Photon Flux and Water on the Stability of Halide Perovskite

In situ Near‐Ambient Pressure X‐ray Photoelectron Spectroscopy Reveals the Influence of Photon Flux and Water on the Stability of Halide Perovskite

One-Pot Hydrothermal Synthesis of Multifunctional ZnZrTUD-1 Catalysts for Highly Efficient Direct Synthesis of Butadiene from Ethanol

Design of Effective Catalysts Based on ZnLaZrSi Oxide Systems for Obtaining 1,3-Butadiene from Aqueous Ethanol

Contact Info

Product

Resources

About

Effect of ZnO on acid–base properties and catalytic performances of ZnO/ZrO2–SiO2 catalysts in 1,3-butadiene production from ethanol–water mixture

Abstract: The effect of ZnO and the preparation method of ZnO/ZrO2–SiO2 catalysts on their acid–base properties and catalytic performances in the conversion of diluted ethanol mixtures into 1,3-butadiene (BD) is presented.

Cited by 36 publications

References 72 publications

In situ Near‐Ambient Pressure X‐ray Photoelectron Spectroscopy Reveals the Influence of Photon Flux and Water on the Stability of Halide Perovskite

In situ Near‐Ambient Pressure X‐ray Photoelectron Spectroscopy Reveals the Influence of Photon Flux and Water on the Stability of Halide Perovskite

One-Pot Hydrothermal Synthesis of Multifunctional ZnZrTUD-1 Catalysts for Highly Efficient Direct Synthesis of Butadiene from Ethanol

Design of Effective Catalysts Based on ZnLaZrSi Oxide Systems for Obtaining 1,3-Butadiene from Aqueous Ethanol

Contact Info

Product

Resources

About

Effect of ZnO on acid–base properties and catalytic performances of ZnO/ZrO₂–SiO₂ catalysts in 1,3-butadiene production from ethanol–water mixture