Acid-based co-catalysis for oxidative dehydrogenation of ethylbenzene to styrene with CO<sub>2</sub> over X zeolite modified by alkali metal cation exchange

Zhao, Guoqing; Chen, Huanhui; Li, Junhui; Wang, Qunlong; Wang, Yanan; Ma, Shuwen; Zhu, Zhirong

doi:10.1039/c5ra13107c

Cited by 7 publications

(6 citation statements)

References 43 publications

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“…The presence of isolated Cs ions is known to be critical to ensure high selectivity and various modification strategies have been screened in attempts to improve the side chain methylation activity, which is the biggest challenge for the commercial viability of this technology. Cs and K exchanged zeolites also catalyze the less-explored oxidative dehydrogenation of ethylbenzene, a common by-product of toluene methylation, to styrene with CO 2 . Sodium-exchanged NaY and NaZSM-5 and analogues commodified with alkaline-earth metals and other additives are also among the best catalysts for the dehydration of lactic acid, a biogenic platform molecule, to acrylic acid. − Alkali metal exchanged zeolites have also been investigated in model reactions for the refinement of biofuels, such as the aldol condensation of propanal and the deoxygenation of methylesters .…”

Section: Alkali and Alkaline Earth Metalsmentioning

confidence: 99%

“…Cs and K exchanged zeolites also catalyze the less-explored oxidative dehydrogenation of ethylbenzene, a common by-product of toluene methylation, to styrene with CO 2 . 156 Sodium-exchanged NaY and NaZSM-5 and analogues commodified with alkaline-earth metals and other additives are also among the best catalysts for the dehydration of lactic acid, a biogenic platform molecule, to acrylic acid. 157−160 Alkali metal exchanged zeolites have also been investigated in model reactions for the refinement of biofuels, such as the aldol condensation of propanal 161 and the deoxygenation of methylesters.…”

Section: Alkali Metalsmentioning

confidence: 99%

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Single-Atom Catalysts across the Periodic Table

et al. 2020

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Isolated atoms featuring unique reactivity are at the heart of enzymatic and homogeneous catalysts. In contrast, although the concept has long existed, single-atom heterogeneous catalysts (SACs) have only recently gained prominence. Host materials have similar functions to ligands in homogeneous catalysts, determining the stability, local environment, and electronic properties of isolated atoms and thus providing a platform for tailoring heterogeneous catalysts for targeted applications. Within just a decade, we have witnessed many examples of SACs both disrupting diverse fields of heterogeneous catalysis with their distinctive reactivity and substantially enriching our understanding of molecular processes on surfaces. To date, the term SAC mostly refers to late transition metal-based systems, but numerous examples exist in which isolated atoms of other elements play key catalytic roles. This review provides a compositional encyclopedia of SACs, celebrating the 10th anniversary of the introduction of this term. By defining single-atom catalysis in the broadest sense, we explore the full elemental diversity, joining different areas across the whole periodic table, and discussing historical milestones and recent developments. In particular, we examine the coordination structures and associated properties accessed through distinct single-atom−host combinations and relate them to their main applications in thermo-, electro-, and photocatalysis, revealing trends in element-specific evolution, host design, and uses. Finally, we highlight frontiers in the field, including multimetallic SACs, atom proximity control, and possible applications for multistep and cascade reactions, identifying challenges, and propose directions for future development in this flourishing field.

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Section: Alkali and Alkaline Earth Metalsmentioning

confidence: 99%

Section: Alkali Metalsmentioning

confidence: 99%

Single-Atom Catalysts across the Periodic Table

et al. 2020

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“…It is very likely that these sites are those active when NaX is used as a "basic" catalyst such as, e.g. for the side-methylation of toluene with methanol [61], for aldol condensation reactions [62] and for dehydrogenations with CO 2 [63].…”

Section: Acido-basic Sites Of Cationic Zeolitesmentioning

confidence: 99%

Acidity and basicity of zeolites: A fundamental approach

Busca

2017

Microporous and Mesoporous Materials

229

124

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“…Moreover, this K–Fe catalyst faces the obstacle of low ethylbenzene conversion, high cost, and easy sintering owing to the high temperature of the reaction. Some issues with the catalyst such as potassium loss, instability of Fe 3+ , and the effect of Cr 3+ also limit the practical application of K–Fe catalyst. , Despite many efforts including the introduction of different metal elements and the use of different supports, − these problems have not yet been solved effectively. Metal-free catalyst such as carbon material has shown promising catalytic performance for dehydrogenation reactions. − Therefore, the development of a highly efficient carbon-based metal-free catalyst has great potential for DDH of ethylbenzene to styrene under oxidant- and steam-free conditions.…”

Section: Introductionmentioning

confidence: 99%

Defect-Enriched N,O-Codoped Nanodiamond/Carbon Nanotube Catalysts for Styrene Production via Dehydrogenation of Ethylbenzene

Zhou

Guo

Song

et al. 2019

ACS Appl. Nano Mater.

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Owing to the unique structure and enriched surface ketonic carbonyl group, nanodiamond (ND) shows excellent catalytic performance for dehydrogenation reaction. However, the agglomeration of predispersed ND aggregate by surface bonding force suppresses its catalytic activity. In this work, a nitrogen and oxygen codoped nanodiamond/carbon nanotube hybrid catalyst with the enriched structural defects (N,O-ND/CNT-d) has been fabricated by a facile two-step strategy including the hexamethylenetetramine (HTM)-assisted wet chemical approach and pyrolysis process, and the subsequent HNO 3 treatment process. The prepared N,O-ND/CNT-d hybrid catalyst gives 16.8% styrene yield with 98.7%f selectivity and 5.2 mmol g −1 h −1 of steady-state styrene formation rate. It not only shows 4.7 and 1.9 times high steady-state styrene rate as compared to the parent oxidized carbon nanotube (CNT-o) and oxidized ND (ND-o), respectively, but also exhibits higher catalytic performance than the previously reported carbon-based catalysts. This is ascribed to the more accessible catalytic active sites from the isolating effect of CNT by the formation of a hybrid and the dual roles of HTM as dispersant in the wet chemical process and as nitrogen precursor in the pyrolysis process and also to the oxygen doping by HNO 3 treatment, apart from the improved nucleophilicity of surface kenotic carbonyl groups and basic properties by the nitrogen doping. This work not only produces a novel and highly efficient metal-free catalyst with outstanding catalytic performance for clean and energy-efficient styrene synthesis through direct dehydrogenation of ethylbenzene under steam-and oxidant-free conditions but also presents a facile two-step strategy to fabricate other hybrids from dispersion-required carbon parents toward a variety of applications.

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Acid-based co-catalysis for oxidative dehydrogenation of ethylbenzene to styrene with CO₂ over X zeolite modified by alkali metal cation exchange

Abstract: A variety of the modified X zeolites were used to catalyse the oxidative dehydrogenation of ethylbenzene to styrene with CO2 for the first time.

Cited by 7 publications

References 43 publications

Single-Atom Catalysts across the Periodic Table

Single-Atom Catalysts across the Periodic Table

Acidity and basicity of zeolites: A fundamental approach

Defect-Enriched N,O-Codoped Nanodiamond/Carbon Nanotube Catalysts for Styrene Production via Dehydrogenation of Ethylbenzene

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Acid-based co-catalysis for oxidative dehydrogenation of ethylbenzene to styrene with CO2 over X zeolite modified by alkali metal cation exchange

Abstract: A variety of the modified X zeolites were used to catalyse the oxidative dehydrogenation of ethylbenzene to styrene with CO2 for the first time.

Cited by 7 publications

References 43 publications

Single-Atom Catalysts across the Periodic Table

Single-Atom Catalysts across the Periodic Table

Acidity and basicity of zeolites: A fundamental approach

Defect-Enriched N,O-Codoped Nanodiamond/Carbon Nanotube Catalysts for Styrene Production via Dehydrogenation of Ethylbenzene

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Acid-based co-catalysis for oxidative dehydrogenation of ethylbenzene to styrene with CO₂ over X zeolite modified by alkali metal cation exchange