Isobutanol synthesis from syngas over K–Cu/ZrO 2 –La 2 O 3 ( x ) catalysts: Effect of La-loading

Wu, Yingquan; Xie, Hongmei; Tian, Shichao; Tsubaki, Noritatsu; Han, Yizhuo; Tan, Yisheng

doi:10.1016/j.molcata.2014.10.003

Cited by 45 publications

(37 citation statements)

References 47 publications

(37 reference statements)

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“…Further, by comparing to the Cu/SiO 2 catalyst, the Cu/Al 2 O 3 catalyst showed higher selectivities towards C 2+ alcohols. As reported [54][55][56], aldol condensation as one of the key steps for carbon-chain growth of alcohol products easily proceeded on basic oxide catalysts or acid oxide catalysts. The NH 3 -TPD result revealed that the surface acidity of the Cu/Al 2 O 3 catalyst was much stronger than that of the Cu/SiO 2 catalyst.…”

Section: Discussionmentioning

confidence: 80%

The Support Effects on the Direct Conversion of Syngas to Higher Alcohol Synthesis over Copper-Based Catalysts

Zhang

Zhang³

et al. 2019

Catalysts

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The types of supports employed profoundly influence the physicochemical properties and performances of as-prepared catalysts in almost all catalytic systems. Herein, Cu catalysts, with different supports (SiO2, Al2O3), were prepared by a facile impregnation method and used for the direct synthesis of higher alcohols from CO hydrogenation. The prepared catalysts were characterized using multiple techniques, such as X-ray diffraction (XRD), N2 sorption, H2-temperature-programmed reduction (H2-TPR), temperature-programmed desorption of ammonia (NH3-TPD), X-ray photoelectron spectroscopy (XPS) and in situ Fourier-transform infrared spectroscopy (FTIR), etc. Compared to the Cu/Al2O3 catalyst, the Cu/SiO2 catalyst easily promoted the formation of a higher amount of C1 oxygenate species on the surface, which is closely related to the formation of higher alcohols. Simultaneously, the Cu/Al2O3 and Cu/SiO2 catalysts showed obvious differences in the CO conversion, alcohol distribution, and CO2 selectivity, which were probably originated from differences in the structural and physicochemical properties, such as the types of copper species, the reduction behaviors, acidity, and electronic properties. Besides, it was also found that the gap in performances in two kinds of catalysts with the different supports could be narrowed by the addition of potassium because of its neutralization to surface acidy of Al2O3 and the creation of new basic sites, as well as the alteration of electronic properties.

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Section: Discussionmentioning

confidence: 80%

The Support Effects on the Direct Conversion of Syngas to Higher Alcohol Synthesis over Copper-Based Catalysts

Zhang

Zhang³

et al. 2019

Catalysts

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“…[1][2][3] The synthesis of higher alcohols via syngas (a mixture of H 2 and CO) derived from coal, renewable dry biomass, natural gas, shale gas and even waste, is a promising non-petroleum route to produce alternative clean liquid fuels and intermediates for important chemicals. [4][5][6][7][8] Generally, the CO hydrogenation process mainly proceeds on the four types of typical catalysts that are classified into noble Rh-based catalysts, [9,10] MoS 2 -based catalysts, [11,12] methanol catalysts (CuZn-or ZnCr-based) [13,14] and modified Fischer-Tropsch synthesis (FTS) catalysts (CuCo-or CuFe-based). [15][16][17] Although the Rh-based catalysts have displayed good activity and excellent C 2 + alcohols selectivity, its large-scale application in CO hydrogenation is restricted owing to the high cost and limited availability.…”

Section: Introductionmentioning

confidence: 99%

Direct Conversion of Syngas to Higher Alcohols over a CuCoAl|t‐ZrO₂ Multifunctional Catalyst

et al. 2021

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Selective synthesis of higher alcohols from syngas is promising but remains challenging owing to the low stability and selectivity towards higher alcohols. Here we introduce a CuCoAl j t-ZrO 2 (t denotes tetragonal crystal phase) multifunctional catalyst that can achieve an alcohol selectivity of 64.8 % with 79.6 % C 2 + OH, and a total selectivity of alcohols and olefins to 81.7 %. The proper proximity was tuned to increase selectivity towards alcohols and decrease the selectivity towards hydrocarbons. The lower surface [H*]/[C*] ratio due to the stronger basic sites of the CuCoAl j t-ZrO 2 limited alkyl (CH x ) species hydrogenation, and promoted CO insertion and carbon chain growth, resulting in improving the alcohols selectivity. Meanwhile, the weaker adsorption of bridge-type adsorbed CO and the lower decomposition rate of multi-bonded adsorbed CO over CuCoAl j t-ZrO 2 inhibited hydrocarbon generation. The selective promotion of the reaction route via the synergetic effect between CuCoAl and t-ZrO 2 was proposed to boost higher alcohols selectivity. This work may aid the rational design of effective multifunctional catalyst with synergistic effects for tuning selectivity.

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“…It has been reported that the carbon-based materials loaded with transition metals reveal high activity in NO x reduction by CO [16,50]. The physicochemical properties of the catalyst can affect the catalytic pathway [51,52]. The addition of La can be beneficial for NO conversion into N 2 and further enhancement of the catalytic activity [53,54].…”

Section: Catalytic Activity Evaluationmentioning

confidence: 99%

Promotional Effect of Manganese on Selective Catalytic Reduction of NO by CO in the Presence of Excess O2 over M@La–Fe/AC (M = Mn, Ce) Catalyst

Gholami

Martı́n

et al. 2020

Catalysts

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The catalytic performance of a series of La-Fe/AC catalysts was studied for the selective catalytic reduction (SCR) of NO by CO. With the increase in La content, the Fe2+/Fe3+ ratio and amount of surface oxygen vacancies (SOV) in the catalysts increased; thus the catalytic activity improved. Incorporating the promoters to La3-Fe1/active carbon (AC) catalyst could affect the catalyst activity by changing the electronic structure. The increase in Fe2+/Fe3+ ratio after the promoter addition is possibly due to the extra synergistic interaction of M (Mn and Ce) and Fe through the redox equilibrium of M3+ + Fe3+ ↔ M4+ + Fe2+. This phenomenon could have improved the redox cycle, enhanced the SOV formation, facilitated NO decomposition, and accelerated the CO-SCR process. The presence of O2 enhanced the formation of the C(O) complex and improved the activation of the metal site. Mn@La3-Fe1/AC catalyst revealed an excellent NO conversion of 93.8% at 400 °C in the presence of 10% oxygen. The high catalytic performance of MnOx and double exchange behavior of Mn3+ and Mn4+ can increase the number of SOV and improve the catalytic redox properties.

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Isobutanol synthesis from syngas over K–Cu/ZrO 2 –La 2 O 3 ( x ) catalysts: Effect of La-loading

Cited by 45 publications

References 47 publications

The Support Effects on the Direct Conversion of Syngas to Higher Alcohol Synthesis over Copper-Based Catalysts

The Support Effects on the Direct Conversion of Syngas to Higher Alcohol Synthesis over Copper-Based Catalysts

Direct Conversion of Syngas to Higher Alcohols over a CuCoAl|t‐ZrO₂ Multifunctional Catalyst

Promotional Effect of Manganese on Selective Catalytic Reduction of NO by CO in the Presence of Excess O2 over M@La–Fe/AC (M = Mn, Ce) Catalyst

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Isobutanol synthesis from syngas over K–Cu/ZrO 2 –La 2 O 3 ( x ) catalysts: Effect of La-loading

Cited by 45 publications

References 47 publications

The Support Effects on the Direct Conversion of Syngas to Higher Alcohol Synthesis over Copper-Based Catalysts

The Support Effects on the Direct Conversion of Syngas to Higher Alcohol Synthesis over Copper-Based Catalysts

Direct Conversion of Syngas to Higher Alcohols over a CuCoAl|t‐ZrO2 Multifunctional Catalyst

Promotional Effect of Manganese on Selective Catalytic Reduction of NO by CO in the Presence of Excess O2 over M@La–Fe/AC (M = Mn, Ce) Catalyst

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Direct Conversion of Syngas to Higher Alcohols over a CuCoAl|t‐ZrO₂ Multifunctional Catalyst