Active sites and mechanism of the direct conversion of methane and carbon dioxide to acetic acid over the zinc-modified H-ZSM-5 zeolite

Zhang, Peng; Yang, Xuejing; Hou, Xiuli; Mi, Jianli; Yuan, Zhefan; Huang, Jun; Stampfl, Catherine

doi:10.1039/c9cy01749f

Cited by 32 publications

(30 citation statements)

References 81 publications

(61 reference statements)

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“…72 The C− C coupling was pointed out as the rate-determining step for acetic acid production from CH 4 and CO 2 over Zn-ZSM-5 by other studies. 85,86 These results indicated that Zn 2+ showed high activity for the CH 4 activation and C−C coupling. While CO 2 can directly insert into the −[ZnCH 3 ] + intermediates, the desorption of acetic acid depends on both the Zn 2+ sites and the acidic sites from the catalyst supports.…”

Section: Catalytic Activity and Selectivitymentioning

confidence: 85%

“…Recently, two Zn sites, including isolated Zn 2+ located at the channel of HZSM-5 zeolite and small ZnO clusters on the surface of zeolite, were investigated for the conversion of CH 4 and CO 2 to acetic acid. 85 DFT calculations demonstrated that the local structure of Zn sites in HZSM-5 could influence the catalytic activity. Zn 2+ located at the five-membered ring in sinusoidal and straight channels showed better activity than on other sites and small ZnO clusters.…”

Section: Catalytic Activity and Selectivitymentioning

confidence: 99%

“…99 The same activation mechanism is also found in some heterogeneous catalysts. 63,85 However, CO 2 can be activated by multisites different from that for CH 4 activation or by the acid sites on the support. In some studies, the oxygen vacancy on the support can also activate CO 2 , such as defective In 2 O 3 .…”

Section: Catalytic Activity and Selectivitymentioning

confidence: 99%

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Insight into Acetic Acid Synthesis from the Reaction of CH₄ and CO₂

Nie

Chen

2021

ACS Catal.

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The reaction of CH 4 and CO 2 to produce acetic acid is an atom-efficient way for using carbon resources and for mitigating CO 2 emissions. This article provides a critical assessment of the progress in this catalytic reaction from the perspective of identifying and constructing the active sites. We elucidate how Cu-and Zn-based catalysts with different structures are used for the activation of CH 4 and CO 2 . The differences in the metal oxidation state may affect the adsorption of CH 4 and CO 2 and consequently change the activation barriers for the dissociation of the C−H bond of CH 4 and the C−C coupling reaction. We discuss how the active sites and transition states can be modified by the location of metal sites, the framework environment, and the promotion effect of different acid sites. We also compare different technologies, including catalyst pretreatment, preactivation with CO 2 , tandem reaction, and plasma-driven catalysis for the CH 4 and CO 2 conversion. We conclude by identifying opportunities for improving the efficiency of heterogeneous catalysts for this important reaction.

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Section: Catalytic Activity and Selectivitymentioning

confidence: 85%

Section: Catalytic Activity and Selectivitymentioning

confidence: 99%

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Insight into Acetic Acid Synthesis from the Reaction of CH₄ and CO₂

Nie

Chen

2021

ACS Catal.

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“…High usage of fossil fuels results in the emission of numerous greenhouse gases into the atmosphere, which has increased the average temperature of the Earth. CH 4 and CO 2 are two main contributors to the greenhouse effect; therefore, considerable attention is being paid to their conversion and utilization worldwide. − As a promising technology that can simultaneously convert CH 4 and CO 2 , there is increasing focus on methane dry reforming (MDR, CH 4 (g) + CO 2 (g) ⇌ 2CO(g) + 2H 2 (g), Δ H 298 = +247 kJ/mol). − The product syngas is an important chemical intermediate, which can be applied to synthesize energy chemicals like alkanes, olefins, and liquid hydrocarbons using the Fischer–Tropsch process. The contributions to both the environment and energy make MDR a very hot topic of industrially relevant catalyst research.…”

Section: Introductionmentioning

confidence: 99%

Ni/SiO₂ Catalyst Prepared by Strong Electrostatic Adsorption for a Low-Temperature Methane Dry Reforming Reaction

Wang

Han

et al. 2021

Ind. Eng. Chem. Res.

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Low-temperature methane dry reforming (MDR) over supported Ni catalysts is a more economical way to convert greenhouse gases than high-temperature MDR. However, sintering from Ni aggregation and carbon deposition from deep cracking of CH4 caused catalyst deactivation. In this study, we synthesized a supported Ni/SiO2-E catalyst by strong electrostatic adsorption for low-temperature MDR (673–773 K). Experimental results showed that the Ni/SiO2-E catalyst exhibited higher performance on using low-temperature MDR than the Ni/SiO2-I catalyst prepared by the conventional impregnation method. From characterizations of X-ray diffraction (XRD), transmission electron microscopy (TEM), hydrogen temperature-programmed reduction (H2-TPR), etc. in fresh catalysts and used catalysts, the excellent stable performance of MDR over the Ni/SiO2-E catalyst was associated with the smaller Ni size and the stronger Ni–SiO2 interaction. The former contributed to less formation of carbon deposits and the latter resulted in hardly any sintering of Ni nanoparticles.

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“…In addition, methane is also a basic feedstock to produce other value added chemicals. [11][12][13] Hydrogenation of CO 2 into methane, i.e., CO 2 methanation, is among the most important topics of CO 2 valorization. 14,15 CO 2 methanation is a reversible and strong exothermic reaction, and is thermodynamically favorable.…”

Section: Introductionmentioning

confidence: 99%

Low temperature methanation of CO₂ over an amorphous cobalt-based catalyst

Qian

et al. 2021

Chem. Sci.

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Active sites and mechanism of the direct conversion of methane and carbon dioxide to acetic acid over the zinc-modified H-ZSM-5 zeolite

Abstract: The catalytic activity of the conversion of CH4 and CO2 on zinc modified H-ZSM-5 is strongly dependent on the structure of the active sites.

Cited by 32 publications

References 81 publications

Insight into Acetic Acid Synthesis from the Reaction of CH₄ and CO₂

Insight into Acetic Acid Synthesis from the Reaction of CH₄ and CO₂

Ni/SiO₂ Catalyst Prepared by Strong Electrostatic Adsorption for a Low-Temperature Methane Dry Reforming Reaction

Low temperature methanation of CO₂ over an amorphous cobalt-based catalyst

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Active sites and mechanism of the direct conversion of methane and carbon dioxide to acetic acid over the zinc-modified H-ZSM-5 zeolite

Abstract: The catalytic activity of the conversion of CH4 and CO2 on zinc modified H-ZSM-5 is strongly dependent on the structure of the active sites.

Cited by 32 publications

References 81 publications

Insight into Acetic Acid Synthesis from the Reaction of CH4 and CO2

Insight into Acetic Acid Synthesis from the Reaction of CH4 and CO2

Ni/SiO2 Catalyst Prepared by Strong Electrostatic Adsorption for a Low-Temperature Methane Dry Reforming Reaction

Low temperature methanation of CO2 over an amorphous cobalt-based catalyst

Contact Info

Product

Resources

About

Insight into Acetic Acid Synthesis from the Reaction of CH₄ and CO₂

Insight into Acetic Acid Synthesis from the Reaction of CH₄ and CO₂

Ni/SiO₂ Catalyst Prepared by Strong Electrostatic Adsorption for a Low-Temperature Methane Dry Reforming Reaction

Low temperature methanation of CO₂ over an amorphous cobalt-based catalyst