Selectivity Descriptors of Methanol‐to‐Aromatics Process over 3‐Dimensional Zeolites DOI
Xin Zhang, Xuan Gong, Edy Abou‐Hamad

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Aug. 16, 2024

Abstract The zeolite‐catalyzed methanol‐to‐aromatics (MTA) process is a promising avenue for industrial decarbonization. This predominantly utilizes 3‐dimensional 10‐member ring (10‐MR) zeolites like ZSM‐5 and ZSM‐11, chosen their confinement effect essential aromatization. Current research mainly focuses on enhancing selectivity mitigating catalyst deactivation by modulating zeolites′ physicochemical properties. Despite the potential, MTA technology at low Technology Readiness Level, hindered mechanistic complexities in achieving desired towards liquid aromatics. To bridge this knowledge gap, study proposes roadmap catalysis strategically combining controlled catalytic experiments with advanced characterization methods (including operando conditions “mobility‐dependent” solid‐state NMR spectroscopy). It identifies descriptor‐role of Koch‐carbonylated intermediates, longer‐chain hydrocarbons, intersectional cavities yielding preferential aromatics selectivity. Understanding these descriptors architectural impacts vital, potentially advancing other emerging technologies.

Language: Английский

Recent progress in the deactivation mechanism of zeolite catalysts in methanol to olefins DOI
Sheng Fan, Han Wang, Sen Wang

et al.

Science China Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: June 3, 2024

Language: Английский

Citations

5
Efficacy of Ca/ZSM-5 zeolites derived from precipitated calcium carbonate in the methanol-to-olefin process DOI
Xinyu You, Xin Zhang, Shican Jiang

et al.

Chinese Journal of Structural Chemistry, Journal Year: 2024, Volume and Issue: 43(4), P. 100265 - 100265

Published: March 6, 2024

Language: Английский

Citations

4
Water-Controlled Coking Dynamics during High-Pressure Methanol-to-Olefins Reaction over SAPO-34 DOI
Chengwei Zhang, Xinqiang Wu, Yanan Zhang

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: 15(3), P. 1553 - 1562

Published: Jan. 13, 2025

Water, as a co-feed and decoking agent for catalyst regeneration, is increasingly recognized crucial component in methanol to olefins (MTO) catalysis over zeolites. In this study, water-controlled coking dynamics improved diffusion efficiency have been revealed high-pressure MTO reaction the SAPO-34 zeolite catalyst. Through gas chromatograph–mass spectrometry (GC-MS), matrix-assisted laser desorption/ionization Fourier-transform ion cyclotron resonance mass (MALDI FT-ICR MS), ultraviolet–visible spectroscopy (UV–vis), kinetic behavior of water-delayed has confirmed mainly two aspects: suppressing aging active hydrocarbon pool species (HCPs, e.g., phenyl, naphthyl species) form polyaromatic hydrocarbons (PAHs) within CHA cages hindering cross-linking PAHs between cages. For deactivated catalyst, restoration conversion from 5% 40% upon switching water–methanol 100% after steam treatment further confirms situ coke decomposition capability water under real conditions. Moreover, structured illumination microscopy (SIM) offers direct visualization retained organic their spatiotemporal distribution individual crystals influence water, thereby providing visual evidence process. Thus, mechanistic insights into unveiled study provide theoretical foundation application water-related techniques industry.

Language: Английский

Citations

0
Microenvironment perturbations driving methanol low-temperature conversion over zeolite DOI Creative Commons

F. Liu,

Xianfeng Yi,

Tangkang Liu

et al.

Science Advances, Journal Year: 2025, Volume and Issue: 11(8)

Published: Feb. 19, 2025

Compared to methanol, dimethyl ether (DME) is a more ideal and attractive raw material for industrial applications. Typically, the industrially zeolite-catalyzed methanol dehydration DME occurs at temperatures above 423 kelvin. Improving catalytic reactivity reducing energy consumption are urgently needed but remain challenging. Here, we report an unexplored associative strategy realize formation room temperature generation of olefins even 413 kelvin, which achieved by coinjecting basic acetone manipulate local chemical microenvironment reactant inside H-ZSM-5 zeolite. The crucial role in accelerating direct highlighted as obvious destabilization effect adsorbed cluster with strong hydrogen bonds subsequent traction water during formation. These findings offer insights into rational design reaction systems manipulating surroundings regulate performances should represent large step forward conversion technology.

Language: Английский

Citations

0
Methanol to Olefins (MTO): Understanding and Regulating Dynamic Complex Catalysis DOI
Shanfan Lin, Hua Li, Peng Tian

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: March 26, 2025

The research and development of methanol conversion into hydrocarbons have spanned more than 40 years. past four decades witnessed mutual promotion successive breakthroughs in both fundamental industrial process to olefins (MTO), demonstrating that MTO is an extremely dynamic, complex catalytic system. This Perspective summarizes the endeavors achievements Dalian Institute Chemical Physics, Chinese Academy Sciences, continuous study reaction mechanisms engineering It elucidates chemical issues concerning essence dynamic evolution cross-talk among diffusion, reaction, catalyst (coke modification), which are crucial for technology optimization. By integrating principles, reaction-diffusion model, coke formation kinetics MTO, a mechanism- model-driven modulation processes has been achieved. acquisition deepening understanding chemistry facilitated optimization upgrading catalysts processes.

Language: Английский

Citations

0
The role of C1 species in the methanol-to-hydrocarbons reaction: Beyond merely being reactants DOI
Yanan Zhang, Wenna Zhang, Chengwei Zhang

et al.

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Journal Year: 2025, Volume and Issue: 71, P. 169 - 178

Published: April 1, 2025

Language: Английский

Citations

0
Design of ZnFeAlO4/Zn-SAPO-34 composite catalyst for selective hydrogenation of CO2 to propane DOI
Xiaoyue Wang,

Xiaohong Guo,

Peixiang Shi

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 358, P. 124439 - 124439

Published: July 24, 2024

Language: Английский

Citations

3
Acid Catalysis Mediated by Aqueous Hydronium Ions Formed by Contacting Zeolite Crystals with Liquid Water DOI
Yue Liu, Chen Luo, Shuai Wang

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 11, 2024

Zeolites are crystalline microporous aluminosilicates widely used as solid acids in catalytic routes to clean and sustainable energy carriers chemicals from biogenic fossil feedstocks. This study addresses how zeolites act weak polyprotic dissociate form extra-crystalline hydronium (H3O+) ions liquid water. The extent of their dissociation depends on the required conjugate framework anions, which becomes unfavorable increases intracrystalline charge densities because repulsive interactions ultimately preclude detachment all protons catalytically relevant H3O+(aq) ions. is accurately described using electrostatic repulsion formalisms that account for aqueous H3O+ concentrations zeolite concentrations, Al densities, frameworks. Probed by hydrolysis cellulose, most abundant polymer, this demonstrates catalyze reaction exclusively through formation at rates strictly proportional phase, irrespective provenance differing structure or content, without purported involvement acid sites extracrystalline surfaces intervening smaller cellulose oligomers. results mechanistic interpretations seamlessly rigorously bridge chemistry media, while resolving enduring puzzle transformations substrates cannot enter voids where reside.

Language: Английский

Citations

3
Role of Phosphorus on ZSM-5 Zeolite for the Methanol-to-Hydrocarbon Reaction DOI Creative Commons
Song Lu, Juan Carlos Navarro de Miguel, Sarah Komaty

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 5623 - 5639

Published: March 21, 2025

Language: Английский

Citations

0
Relay Catalysis for Highly Selective Conversion of Methanol to Ethylene in Syngas DOI Creative Commons
Kuo Chen,

Fenfang Wang,

Yu Wang

et al.

JACS Au, Journal Year: 2023, Volume and Issue: 3(10), P. 2894 - 2904

Published: Oct. 15, 2023

The precise C-C coupling is a challenging goal in C1 chemistry. conversion of methanol, cheap and easily available feedstock, into value-added largely demanded olefins has been playing game-changing role the production olefins. current methanol-to-olefin (MTO) process, however, suffers from limited selectivity to specific olefin. Here, we present relay-catalysis route for high-selective methanol ethylene syngas (H2/CO) typically used synthesis. A bifunctional catalyst composed selectively dealuminated H-MOR zeolite ZnO-TiO2, which implemented carbonylation with CO acetic acid selective hydrogenation tandem, offered 85% at complete 583 K. removal Brønsted sites 12-membered ring channel favors CH3OH carbonylation. high capabilities ZnO-TiO2 adsorption activation H2 play key roles ethylene. Our work provides promising strategy C2 molecules.

Language: Английский

Citations

9