A Newly Designed Core-Shell-Like Zeolite Capsule Catalyst for Synthesis of Light Olefins from Syngas via Fischer–Tropsch Synthesis Reaction

Di, Zuoxing; Zhao, Tiejian; Feng, Xuleng; Luo, Mingsheng

doi:10.1007/s10562-018-2624-9

Cited by 23 publications

(16 citation statements)

References 29 publications

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“…A similar work also reported that core–shell structured Fe@SAPO‐34 catalysts exhibited higher selectivity to light olefins than a bare Fe catalyst and a simple Fe/SAPO‐34 mixture. [ 26 ] In a recent work, Khodakov and co‐workers systematically studied the effects of the proximity between Ru sites and Brønsted acid sites on product distributions by generating core–shell structures in which the shell was a ZSM‐5 or silicalite‐1 zeolite. [ 27 ] The proximity between Ru sites and acid sites significantly improved the selectivity toward iso‐paraffins in low‐temperature FT systems.…”

Section: Syngas Conversion Over Zeolite‐based Catalystsmentioning

confidence: 99%

Applications of Zeolites to C1 Chemistry: Recent Advances, Challenges, and Opportunities

2020

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However, due to growing concerns regarding crude oil depletion and increasing environmental requirements, finding abundant fossil hydrocarbons with high H 2 /C ratios as well as alternative carbon resources has become crucial to maintaining sustainable, environmentally benign systems that can aid human development. [2] Thus, one-carbon (C1) chemistry, which is the chemistry of C1 molecules that can be derived from sources other than fossil hydrocarbons, including carbon monoxide (CO), carbon dioxide (CO 2), methane (CH 4), methanol (CH 3 OH), and formic acid (HCOOH), has emerged and plays important roles in the energy supply and high-value chemical preparation. [1,3] These C1 resources can be obtained from natural gas, shale gas, coal, biomass, solid wastes, and CO 2 emissions. [3a,4] Extensive studies have been dedicated to the catalytic conversion of C1 molecules, including production of dimethyl ether (DME) and liquid fuels from syngas (a mixture of CO and H 2); production of methanol, light olefins, and even aromatics from CH 4 ; and production of hydrogen from HCOOH. [5] All of these transformations require metallic catalytic species such as single atoms; clusters; or oxides, carbides, or alloy particles (e.g., Rh-, AuPd-, Fe 3 O 4-, and Fe 5 C 2-based catalysts). However, these isolated metallic species suffer from severe sintering due to a lack of confinement effects from supports, which leads to poor catalytic stability and decreased selectivities toward their target products. The efficient production of a specific range of hydrocarbons or oxygenates remains a difficult scientific and technical challenge. Overcoming product selectivity limitations and improving catalyst stabilities via catalyst designs are important areas of research. Zeolites are an important class of shape-selective catalysts with uniform micropores, tunable acidities, and high thermal and hydrothermal stabilities. Over the past decade, they have gained broad popularity and been applied to various industrially important catalytic processes. [6] In particular, the design and development of zeolite-based mono-, bi-, and multifunctional catalysts that combine the advantages of zeolites with those of metallic catalytic species have boosted the application of zeolites to C1 chemistry. As shown in Figure 1, value-added hydrocarbons and oxygenates can be produced from C1 molecules via various catalytic routes over zeolite-based catalysts. By May of 2020, the Structure Commission of the International C1 chemistry, which is the catalytic transformation of C1 molecules including CO, CO 2 , CH 4 , CH 3 OH, and HCOOH, plays an important role in providing energy and chemical supplies while meeting environmental requirements. Zeolites are highly efficient solid catalysts used in the chemical industry. The design and development of zeolite-based mono-, bi-, and multifunctional catalysts has led to a booming application of zeolite-based catalysts to C1 chemistry. Combining the advantages of zeolites and metallic catalytic species has promoted the catal...

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Section: Syngas Conversion Over Zeolite‐based Catalystsmentioning

confidence: 99%

Applications of Zeolites to C1 Chemistry: Recent Advances, Challenges, and Opportunities

2020

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“…图 8 不同 SAPO-34 含量 Fe@Si/S-34 催化剂的 FTO 性能 Figure 8 Catalytic performances of the Fe@Si/S-34 catalysts with different SAPO-34 content in FTO reaction 表 2 比较了 Fe@Si/S-34-2 与文献报道相似催化剂的催化性能. 从表中可以看出, 本工作制备的疏水性 Fe@Si/S-34-2 催化剂对 CO 2 的选择性显著低于文献报道的未疏水改性的催化剂, 这进一步说明疏水改性的确抑制了 WGS 反应, 减少了 CO 2 的生成, 使更多的 CO 转化为烃类产物, 提高了 CO 的利用效率; 从 C 2 ～C 4 烯烃选择性来看, Fe@Si/S-34-2 催化剂对 C 2 ～C 4 烯烃的选择性明显高于文献 [20], 略低于文献 [22,[31][32]报道的金属改性催化剂, 但从 C 2 ～C 4 烯烃收率来看, Fe@Si/S-34-2 催化剂的收率明显更高. 总体来看, Fe@Si/S-34-2 催化剂对 CO 转化率较高, 对 CO 2 的选择性最低, 对 C 2 ～C 4 烯烃的选择性较高, 该催化剂优异的催化性能主要归因于 Fe@Si 催化剂的疏水性抑制 WGS 反应和 SAPO-34 分子筛的裂解活性的协同耦合作用.…”

Section: Sapo-34 含量对催化剂 Fto 性能的影响unclassified

Preparation of Fe@Si/S-34 Catalysts and Its Catalytic Performance for Syngas to Olefins

Chen¹,

Meng²,

Lu³

et al. 2023

Acta Chimica Sinica

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The direct synthesis of light olefins from syngas via Fischer-Tropsch synthesis reaction is a promising technology for direct synthesis of olefins from syngas. The key is to improve the selectivity of light olefins through the regulation of product distribution. In this work, the hydrophobic Fe@Si catalyst was prepared by room temperature solid state method-Stöber-silylation method, and then the catalyst was combined with SAPO-34 molecular sieves with different contents to prepare Fe@Si/S-34 composite catalysts. The effects of SAPO-34 molecular sieve content on the physicochemical properties of the catalysts were investigated by X-ray diffraction, scanning electron microscopy, N2 adsorption-desorption, NH3 temperature programmed desorption and water contact angle measurement. The results showed that the content of SAPO-34 molecular sieve has significant influence on the surface area, pore volume, acidity and hydrophobicity of the catalysts. With the increase of SAPO-34 molecular sieve content, the specific surface area and total pore volume of the catalyst increased, the weak acid and medium-strong acid sites increased, and the hydrophobicity weakened. The catalytic performance evaluation results showed that the Fe@Si/S-34 composite catalyst decomposed C5+ hydrocarbons into light hydrocarbons, significantly reduced the selectivity of C5+ products and increased the selectivity of C2～C4 hydrocarbons. Appropriate SAPO-34 molecular sieve could significantly improve the selectivity of C2～C4 olefins. When the mass ratio of Fe@Si catalyst to SAPO-34 is 2, the C2～C4 olefin selectivity of Fe@Si/S-34 catalyst is the highest, the conversion of CO is 80.0%, the selectivity of CO2 in the product is 8.9%, and the selectivity of C2～C4 olefins is 31.1%. In this study, the hydrophobicity of Fe@Si catalyst and the cracking activity of SAPO-34 molecular sieve for C5+ hydrocarbon were coupled together to inhibit the water-gas shift (WGS) reaction, reduce the CO2 selectivity and obtain higher C2～C4 olefin selectivity, which provided a new strategy for the development of catalysts for Fischer-Tropsch synthesis to olefins.

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“…175 The nonzeolite core-shell catalyst design has also been explored for the FTO route to olefins. 176 The Fe 3 O 4 @MnO 2 core-shell is reported to show an exceptionally high lower olefin yield and a high lower olefin selectivity at high CO conversion. 176 The catalyst exhibited 79.60% total alkene selectivity and 64.95% for C 41 alkene selectivity at 75% CO conversion.…”

Section: Methanol Synthesismentioning

confidence: 99%

“…176 The Fe 3 O 4 @MnO 2 core-shell is reported to show an exceptionally high lower olefin yield and a high lower olefin selectivity at high CO conversion. 176 The catalyst exhibited 79.60% total alkene selectivity and 64.95% for C 41 alkene selectivity at 75% CO conversion. The performance of the catalyst was attributed to electron transfer from the MnO 2 shell to the Fe 3 O 4 core, which promotes dissociative adsorption of CO molecules on Fe 3 O 4 .…”

Section: Methanol Synthesismentioning

confidence: 99%

Chemicals and Fuels from Biomass via Fischer–Tropsch Synthesis: A Route to Sustainability

2022

Focus on Catalysts

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A Newly Designed Core-Shell-Like Zeolite Capsule Catalyst for Synthesis of Light Olefins from Syngas via Fischer–Tropsch Synthesis Reaction

Cited by 23 publications

References 29 publications

Applications of Zeolites to C1 Chemistry: Recent Advances, Challenges, and Opportunities

Applications of Zeolites to C1 Chemistry: Recent Advances, Challenges, and Opportunities

Preparation of Fe@Si/S-34 Catalysts and Its Catalytic Performance for Syngas to Olefins

Chemicals and Fuels from Biomass via Fischer–Tropsch Synthesis: A Route to Sustainability

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