Study of mesoporous catalysts for conversion of 2,3-butanediol to butenes

Zheng, Qunhao; Grossardt, Jason; Almkhelfe, Haider; Xu, Jiayi; Grady, Brian P.; Douglas, Justin T.; Amama, Placidus B.; Hohn, Keith L.

doi:10.1016/j.jcat.2017.08.017

Cited by 22 publications

(18 citation statements)

References 72 publications

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“…Then, the C 8 ketone can be converted to C 8 alkenes and C 8 alkanes, which can be used as gasoline blended components. This work extends previous work in our laboratory to convert 2,3 BDO and MEK to light alkenes (butene) [18][19][20], an intermediate to higher alkenes, and MEK to chemicals such as C 8 ketone [21].…”

Section: Introductionsupporting

confidence: 80%

Conversion of 5-Methyl-3-Heptanone to C8 Alkenes and Alkane over Bifunctional Catalysts

Al-Auda

Al-Atabi

et al. 2019

Catalysts

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A one-step catalytic process was used to catalyze the hydrodeoxygenation of 5-methyl-3-heptanone (C8 ketone) to a mixture of 5-methyl-3-heptene, 5-methyl-2-heptene (C8 alkenes), and 3-methyl heptane (C8 alkane). High conversion of C8 ketone to the desired products was achieved over a single bed of a supported catalyst (bifunctional heterogeneous catalyst) consisting of one transition metal (copper (Cu) or platinum (Pt)) loaded on alumina (Al2O3) under mild operating conditions (reaction temperatures were varied between 180 °C to 260 °C, and the pressure was 1 atm). The C8 ketone was hydrogenated to 5-methyl-3-heptanol (C8 alcohol) over metal sites, followed by dehydration of the latter on acid sites on the support to obtain a mixture of C8 alkenes. These C8 alkenes can be further hydrogenated on metal sites to make a C8 alkane. The results showed that the main products over copper loaded on alumina (20 wt% Cu–Al2O3) were a mixture of C8 alkenes and C8 alkane in different amounts depending on the operating conditions (the highest selectivity for C8 alkenes (~82%) was obtained at 220 °C and a H2/C8 ketone molar ratio of 2). However, over platinum supported on alumina (1 wt% Pt–Al2O3), the major product was a C8 alkane with a selectivity up to 97% and a conversion of 99.9% at different temperatures and all H2/C8 ketone ratios.

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Section: Introductionsupporting

confidence: 80%

Conversion of 5-Methyl-3-Heptanone to C8 Alkenes and Alkane over Bifunctional Catalysts

Al-Auda

Al-Atabi

et al. 2019

Catalysts

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“…Besides, the C-Ni/Al-SiO 2 catalyst has a H3 hysteresis loop, which indicates that the mesoporous structure of C-Ni/Al-SiO 2 includes unevenly distributed tubular pores and densely packed spherical interstitial pores, proving its crisscrossed mesoporous structure. P-Ni/Al-SiO 2 shows a H1 hysteresis loop with capillary condensation between the two inflection points, indicating that there are uniform parallel bundles, while for N-Ni/Al-SiO 2 , the nonmesoporous structure is confirmed by its large and increasing hysteresis loop, which cannot reach a constant value even when the relative pressure P / P 0 is close to 1 …”

Section: Results and Discussionmentioning

confidence: 96%

“…Then, 8.5 g of TEOS and the required amount of Al(O-CH(CH 3 ) 2 ) 3 were added to the above solution. The mixture was stirred at 40 °C for 24 h, and thereafter, the slurry was transferred into a PTFE bottle and heated at 100 °C in an oven for 48 h. The solid obtained was filtered and washed several times with water, dried at 60 °C for 24 h, and calcined at 550 °C for 6 h . The obtained sample was denoted as P-Al-SiO 2 .…”

Section: Methodsmentioning

confidence: 99%

Effect of Pore Structures on 1,4-Butynediol Hydrogenation over Mesoporous Ni/Al₂O₃-SiO₂ Catalysts

Wang

Jiang

Bai

et al. 2021

Ind. Eng. Chem. Res.

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This work describes the 1,4-butynediol (BYD) hydrogenation to 1,4-butanediol (BDO) performance over supported Ni/Al2O3-SiO2 catalysts with different mesoporous structures (cross pore C-Ni/Al-SiO2, parallel pore P-Ni/Al-SiO2, and nonmesoporous structured N-Ni/Al-SiO2). To illustrate the pore structure effects on the catalyst texture, metal–support interaction, and surface acidity, the obtained catalysts were characterized using BET, inductively coupled plasma (ICP), transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), H2 temperature-programed reduction (H2-TPR), and H2/NH3-temperature-programmed desorption (H2/NH3-TPD). Based on this, we proposed the structure–activity relationship between the pore structures and the hydrogenation performance. It was found that C-Ni/Al-SiO2 had short-range staggered and cross mesopores throughout the support, which can provide a larger surface area and pore volume for the fixation of highly dispersed active sites, thus enhancing the H2 activation ability. On the other hand, the cross channels have rich hole loops and surface defects for exposing assistant acid sites that are beneficial for the 1,4-butynediol (BYD) adsorption/activation, thus promising a superior hydrogenation ability. However, the narrow and long parallel pore structure of P-Ni/Al-SiO2 may limit the rapid diffusion of long-carbon-chain BYD in the pores, thus partially decreasing the accessibility of active sites and the catalytic activity. As for N-Ni/Al-SiO2, which has no mesoporous structure, its nickel particles are prone to aggregate seriously on the support surface, which weakens the interaction with the support and is not conducive to catalytic hydrogenation.

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“…In relation to the catalytic tests, the pure silica SBA-15 sample showed very low activity due to the presence of only silanol (Si-OH) groups, which are very weak acidic sites. According to microcalorimetric studies of ammonia desorption by Kumaran et al 25 and Zheng et al 26 , the number of acidic sites and the acid strength of SBA-15 are very low or almost inactive compared with those of Si-SBA-15. The aluminum insertion in the mesoporous structure increased the catalytic activity because there was a gradual increase in the ethanol conversion with the decrease in the Si/Al ratio, consequently, an increase in the amount of Al.…”

Section: Discussionmentioning

confidence: 99%

Incorporating Aluminum Into the Structure of SBA-15 by Adjusting the pH and Adding NaF

et al. 2019

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The Al incorporation on SBA-15 type material and the effects of pH adjusting and presence of NaF were studied. The direct synthesis method was performed for comparison. The following parameters were evaluated: the Si/Al ratio, pH increase, and amount of NaF added. These parameters have a great influence on the synthesis of the mesoporous Al/SBA-15 type, but the pH the most influential parameter for the incorporation of Al into the SBA-15 structure. The formation of the SBA-15 structure was observed through the direct synthesis method. However, aluminum is not present in the material. The increase in pH contributed to the formation of a disorganized material. By EDX, it was observed that synthesis with a Si/Al = 5 ratio and pH approximately 4 provides materials containing aluminum. When the amount of aluminum during the synthesis is lower, a pH of approximately 8 is required to incorporate aluminum into the final material. The Al-NMR analysis showed that it was possible to insert aluminum in the structure of SBA-15, but with the presence of aluminum hexa and pentacoordinated. In the catalytic test of the dehydration reaction of ethanol, the samples with higher aluminum contents showed better catalytic performance due to its higher acidity.

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Study of mesoporous catalysts for conversion of 2,3-butanediol to butenes

Cited by 22 publications

References 72 publications

Conversion of 5-Methyl-3-Heptanone to C8 Alkenes and Alkane over Bifunctional Catalysts

Conversion of 5-Methyl-3-Heptanone to C8 Alkenes and Alkane over Bifunctional Catalysts

Effect of Pore Structures on 1,4-Butynediol Hydrogenation over Mesoporous Ni/Al₂O₃-SiO₂ Catalysts

Incorporating Aluminum Into the Structure of SBA-15 by Adjusting the pH and Adding NaF

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Study of mesoporous catalysts for conversion of 2,3-butanediol to butenes

Cited by 22 publications

References 72 publications

Conversion of 5-Methyl-3-Heptanone to C8 Alkenes and Alkane over Bifunctional Catalysts

Conversion of 5-Methyl-3-Heptanone to C8 Alkenes and Alkane over Bifunctional Catalysts

Effect of Pore Structures on 1,4-Butynediol Hydrogenation over Mesoporous Ni/Al2O3-SiO2 Catalysts

Incorporating Aluminum Into the Structure of SBA-15 by Adjusting the pH and Adding NaF

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Effect of Pore Structures on 1,4-Butynediol Hydrogenation over Mesoporous Ni/Al₂O₃-SiO₂ Catalysts