Direct Conversion of Syngas to Ethanol within Zeolite Crystals

Wang, Chengtao; Zhang, Jian; Qin, Gangqiang; Wang, Liang; Zuidema, Erik; Yang, Qi; Dang, Shanshan; Yang, Chengguang; Xiao, Jianping; Meng, Xiangju; Mesters, C.M.A.M.; Xiao, Feng‐Shou

doi:10.1016/j.chempr.2019.12.007

Cited by 139 publications

(129 citation statements)

References 58 publications

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“…temperature benefit the fast C-O bond cleavage to form abundant CH x species that are strongly adsorbed on the catalyst surface, which hindered the transformation of more CO molecules for the continuous reaction. Similar viewpoint has been studied experimentally and theoretically [31,32]. A decreased temperature of 240°C led to a lower reaction rate at 4.1 mol CO mol Ru À1 h À1 and higher selectivity at 47.3% to C 12+ hydrocarbons (Table S3).…”

Section: Introductionsupporting

confidence: 78%

Fischer-Tropsch reaction within zeolite crystals for selective formation of gasoline-ranged hydrocarbons

Wang

Fang

Wang

et al. 2021

Journal of Energy Chemistry

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Section: Introductionsupporting

confidence: 78%

Fischer-Tropsch reaction within zeolite crystals for selective formation of gasoline-ranged hydrocarbons

Wang

Fang

Wang

et al. 2021

Journal of Energy Chemistry

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“…The advantages of the metal@zeolite structure are obviously observed in RhMn catalyzed syngas transformation, where RhMn@S-1 (RhMn nanoparticles fixed in S-1 zeolite) exhibited a 9-fold higher ethanol productivity than the supported RhMn nanoparticles catalysts. 114 Several reasons were identified for the unusual catalytic performances: the hindered hydrogen spillover in the siliceous zeolite, as discussed above, could hinder deep hydrogenation and contribute to the oxygenate production; the well-defined Rh-MnO x interfacial nanostructure is highly stable under the reaction conditions, thus maintaining the abundant active sites for oxygenate formation; the confinement effect of zeolite micropores weakens the intermediate adsorption and reduces the energy barriers for C–C coupling.…”

Section: Hydrogen Spillover-dependent Selective Catalysismentioning

confidence: 99%

Metal@Zeolite Hybrid Materials for Catalysis

2020

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The fixation of metal nanoparticles into zeolite crystals has emerged as a new series of heterogeneous catalysts, giving performances that steadily outperform the generally supported catalysts in many important reactions. In this outlook, we define different noble metal-in-zeolite structures (metal@zeolite) according to the size of the nanoparticles and their relative location to the micropores. The metal species within the micropores and those larger than the micropores are denoted as encapsulated and fixed structures, respectively. The development in the strategies for the construction of metal@zeolite hybrid materials is briefly summarized in this work, where the rational preparation and improved thermal stability of the metal nanostructures are particularly mentioned. More importantly, these metal@zeolite hybrid materials as catalysts exhibit excellent shape selectivity. Finally, we review the current challenges and future perspectives for these metal@zeolite catalysts.

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“…Single metal atoms can be stabilized by the O/N/C atoms in zeolites or MOFs. Therefore, the electronic structure (particularly the oxidation state, charge transfer, and d electron density) of SACs is different from that of metal clusters in such supports; [72,76,91,92] XAS can clearly distinguish Reproduced with permission. [83] Copyright 2016, Wiley-VCH.…”

Section: Electronic Propertiesmentioning

confidence: 99%

“…Single metal atoms can be stabilized by the O/N/C atoms in zeolites or MOFs. Therefore, the electronic structure (particularly the oxidation state, charge transfer, and d electron density) of SACs is different from that of metal clusters in such supports; [ 72,76,91,92 ] XAS can clearly distinguish these two types of active sites. In addition, linear combination fitting of XANES can provide quantitative information about the electronic properties in SACs.…”

Section: Xas Analysis Of Sacs Supported By Crystalline Porous Materialsmentioning

confidence: 99%

Single‐Atom Catalysts Supported by Crystalline Porous Materials: Views from the Inside

et al. 2020

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Reducing the size of nanoparticle catalysts is one desirable method that can improve their catalytic activity. Single-atom catalysts (SACs) represent the smallest possible size a catalyst can achieve with maximum atomic efficiency. [6] Moreover, recent studies have shown that the use of single-atom catalytic sites, rather than ensembles of atoms, is crucial in many catalytic reactions. [7] Without proper protection, however, single-atom sites in these catalysts are not stable since they tend to aggregate and form larger particles. [8-10] To solve this problem, many different protecting supports have been developed such as polymers and porous organic cages. [11,12] Crystalline porous materials, such as zeolites and metal-organic frameworks (MOFs), have been widely used to stabilize small metal species in catalytic reactions due to the controllable size, shape, and dimensions of their pores and channels. [13-15] Therefore, they are highly desirable in supporting SACs. [13] Despite the promising aspects of zeolite and MOF-supported SACs, their characterization remains challenging due to the single-atomic nature of their bonding environments; atomic-level resolution is needed for the structural characterization of these catalysts. X-ray absorption spectroscopy (XAS) is a powerful tool in studying the structure and properties of atoms in their coordination environments with subatomic resolution, [16,17] and thus is considered particularly suitable for the study of SACs. [16,17] In this contribution, a comprehensive review of representative works on zeolite-and MOF-protected SACs will be presented from the XAS perspective. The subatomic resolution (0.01 Å level) of synchrotron-based XAS technique allows for views from "inside" the SACs regarding their structure, electronic properties, and catalytic activities. The processed data from extended X-ray absorption fine structure (EXAFS) will be shown as a powerful tool to probe the atomic structure of SACs in zeolites and MOFs. Through the standard fitting analysis of EXAFS, together with the assistance of advanced analysis tools, detailed information concerning the local structure of SACs can be obtained. Additionally, it will be demonstrated that the X-ray absorption near-edge structure (XANES) can provide insight into the unique electronic properties of SACs. Furthermore, in situ/operando XAS techniques, coupled with state-of-the-art Single-atom catalysts (SACs) have recently emerged as an exciting system in heterogeneous catalysis showing outstanding performance in many catalytic reactions. Single-atom catalytic sites alone are not stable and thus require stabilization from substrates. Crystalline porous materials such as zeolites and metal-organic frameworks (MOFs) are excellent substrates for SACs, offering high stability with the potential to further enhance their performance due to synergistic effects. This review features recent work on the structure, electronic, and catalytic properties of zeolite and MOF-protected SACs, offering atomic-scale views from the "insid...

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Direct Conversion of Syngas to Ethanol within Zeolite Crystals

Cited by 139 publications

References 58 publications

Fischer-Tropsch reaction within zeolite crystals for selective formation of gasoline-ranged hydrocarbons

Fischer-Tropsch reaction within zeolite crystals for selective formation of gasoline-ranged hydrocarbons

Metal@Zeolite Hybrid Materials for Catalysis

Single‐Atom Catalysts Supported by Crystalline Porous Materials: Views from the Inside

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