Gontzal Lezcano, Shekhar R. Kulkarni, Vijay K. Velisoju, Natalia Realpe and Pedro Castaño
{"title":"喷雾干燥和SiC共负载对甲烷偶联Mn-Na2WO4 /SiO2催化剂的本征微动力学影响","authors":"Gontzal Lezcano, Shekhar R. Kulkarni, Vijay K. Velisoju, Natalia Realpe and Pedro Castaño","doi":"10.1039/D4RE00403E","DOIUrl":null,"url":null,"abstract":"<p >This paper presents a microkinetic model to evaluate the effects of a silicon carbide (SiC) co-support and the shaping method on Mn–Na<small><sub>2</sub></small>WO<small><sub>4</sub></small>/SiO<small><sub>2</sub></small> catalysts used for the oxidative coupling of methane. The model considers mass transfer, catalytic, and gas-phase kinetics, and it is trained with experimental values (product composition) of three Mn–Na<small><sub>2</sub></small>WO<small><sub>4</sub></small> catalysts for calculating the kinetic parameters using catalytic descriptors while maintaining thermodynamic consistency. The catalysts were an SiO<small><sub>2</sub></small>-supported catalyst prepared through impregnation and two SiO<small><sub>2</sub></small>–SiC-supported catalysts (with βSiC and α + βSiC) prepared <em>via</em> spray-drying. Our analysis shows how the type of SiC and preparation method affect the textural properties and result in distinct CH<small><sub>3</sub></small>˙ radical oxidation, HO<small><sub>2</sub></small>˙ quenching, C<small><sub>2</sub></small>H<small><sub>4</sub></small> oxidation, and CO<small><sub><em>X</em></sub></small> transformation pathways, eventually leading to CH<small><sub>4</sub></small> conversion and C<small><sub>2</sub></small> selectivity. Our approach facilitates the assessment of the effects of the promoter and support on individual and global reaction networks.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 5","pages":" 975-998"},"PeriodicalIF":3.4000,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/re/d4re00403e?page=search","citationCount":"0","resultStr":"{\"title\":\"Intrinsic microkinetic effects of spray-drying and SiC co-support on Mn–Na2WO4/SiO2 catalysts used in oxidative coupling of methane†\",\"authors\":\"Gontzal Lezcano, Shekhar R. Kulkarni, Vijay K. Velisoju, Natalia Realpe and Pedro Castaño\",\"doi\":\"10.1039/D4RE00403E\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >This paper presents a microkinetic model to evaluate the effects of a silicon carbide (SiC) co-support and the shaping method on Mn–Na<small><sub>2</sub></small>WO<small><sub>4</sub></small>/SiO<small><sub>2</sub></small> catalysts used for the oxidative coupling of methane. The model considers mass transfer, catalytic, and gas-phase kinetics, and it is trained with experimental values (product composition) of three Mn–Na<small><sub>2</sub></small>WO<small><sub>4</sub></small> catalysts for calculating the kinetic parameters using catalytic descriptors while maintaining thermodynamic consistency. The catalysts were an SiO<small><sub>2</sub></small>-supported catalyst prepared through impregnation and two SiO<small><sub>2</sub></small>–SiC-supported catalysts (with βSiC and α + βSiC) prepared <em>via</em> spray-drying. Our analysis shows how the type of SiC and preparation method affect the textural properties and result in distinct CH<small><sub>3</sub></small>˙ radical oxidation, HO<small><sub>2</sub></small>˙ quenching, C<small><sub>2</sub></small>H<small><sub>4</sub></small> oxidation, and CO<small><sub><em>X</em></sub></small> transformation pathways, eventually leading to CH<small><sub>4</sub></small> conversion and C<small><sub>2</sub></small> selectivity. 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Intrinsic microkinetic effects of spray-drying and SiC co-support on Mn–Na2WO4/SiO2 catalysts used in oxidative coupling of methane†
This paper presents a microkinetic model to evaluate the effects of a silicon carbide (SiC) co-support and the shaping method on Mn–Na2WO4/SiO2 catalysts used for the oxidative coupling of methane. The model considers mass transfer, catalytic, and gas-phase kinetics, and it is trained with experimental values (product composition) of three Mn–Na2WO4 catalysts for calculating the kinetic parameters using catalytic descriptors while maintaining thermodynamic consistency. The catalysts were an SiO2-supported catalyst prepared through impregnation and two SiO2–SiC-supported catalysts (with βSiC and α + βSiC) prepared via spray-drying. Our analysis shows how the type of SiC and preparation method affect the textural properties and result in distinct CH3˙ radical oxidation, HO2˙ quenching, C2H4 oxidation, and COX transformation pathways, eventually leading to CH4 conversion and C2 selectivity. Our approach facilitates the assessment of the effects of the promoter and support on individual and global reaction networks.
期刊介绍:
Reaction Chemistry & Engineering is a new journal reporting cutting edge research into all aspects of making molecules for the benefit of fundamental research, applied processes and wider society.
From fundamental, molecular-level chemistry to large scale chemical production, Reaction Chemistry & Engineering brings together communities of chemists and chemical engineers working to ensure the crucial role of reaction chemistry in today’s world.