Plasma-Catalytic Direct Oxidation of Methane to Methanol Over Cu-Mor: Revealing the Zeolite-Confined Cu2+ Active Sites DOI

Huan Lv,

Shengyan Meng, Zhaolun Cui

и другие.

Опубликована: Янв. 1, 2024

Efficient methane conversion to methanol remains a significant challenge in chemical industry. This study investigates the direct oxidation of under mild conditions, employing synergy non-thermal plasma and Cu-MOR (Copper-Mordenite) catalysts. Catalytic tests demonstrate that IE-3 catalyst (i.e., prepared by three cycles ion exchange) exhibits superior catalytic performance (with 51% selectivity 7.9% conversion). Conversely, catalysts via wetness impregnation tend over-oxidize CH4 CO CO2. Through systematic characterizations (XRD, TPR, UV-Vis, HRTEM, XPS), we elucidate exchange mainly leads formation zeolite-confined Cu2+ species, while predominantly results CuO particles. Based on performance, in-situ FTIR spectra, conclude species serve as active sites for plasma-catalytic methanol.

Язык: Английский

Cu and Zn Bimetallic Co-Modified H-MOR Catalyst for Direct Oxidation of Low-Concentration Methane to Methanol DOI Creative Commons
Yan Fu,

Cunshuo Li,

Shengxin An

и другие.

ACS Omega, Год журнала: 2023, Номер 8(30), С. 27179 - 27189

Опубликована: Июль 18, 2023

The direct oxidation of low-concentration methane to value-added chemicals can not only reduce carbon emission but also provide an alternative production route for fossil fuels. Herein, we proposed a novel catalyst the methanol via impregnation method, which selected copper and zinc as co-modifiers modify MOR catalyst. highest yield 71.35 μmol·gcat-1·h-1 was obtained over bimetallic Cu0.5Zn0.35-MOR retained good activity after three cycles testing experiments, indicating recyclability. Based on results performance tests characterization studies, it confirmed that Cu species bound zeolite framework were main active sites oxidation. introduction Zn decreased generation octahedrally coordinated extra-framework aluminum, promoted dispersion within framework. In other words, more tetrahedrally FAl-stabilized presented in our CuZn-MOR system comparison monometallic Cu-MOR Benefiting from aforementioned modification, agglomerative sintering metal during reaction effectively prevented. This work may feasible guide future optimization Cu-based catalysts designed selective methane.

Язык: Английский

Процитировано

13
Plasma-catalytic direct oxidation of methane to methanol over Cu-MOR: Revealing the zeolite-confined Cu2+ active sites DOI

Huan Lv,

Shengyan Meng, Zhaolun Cui

и другие.

Chemical Engineering Journal, Год журнала: 2024, Номер 496, С. 154337 - 154337

Опубликована: Авг. 2, 2024

Язык: Английский

Процитировано

5
Preparation of Cu-Based Spherical Micromesoporous Material by Using Sepiolite Toward Methanol Production from Catalytic Oxidation of Low-Concentration Coalbed Methane DOI
Yishuang Wang,

Baolong Qin,

Mingqiang Chen

и другие.

Industrial & Engineering Chemistry Research, Год журнала: 2024, Номер unknown

Опубликована: Апрель 10, 2024

Direct catalytic oxidation (DCO) of coalbed methane to methanol has been considered as a significant technology for highly efficient and clean utilization coal resources. Herein, the Cu-based spherical micromesoporous material (Cu/SMMM) was successfully prepared by using sepiolite-derived silica source, DCO achieved under low-temperature gas-phase system. Under optimal reaction conditions, Cu/SMMM accomplished maximum production 69.3 μmol/gcat/h selectivity 81.2% with full activation at 450 °C in air 4 h, carried out 320 1 h. Various characterizations demonstrated that unique SMMM promoted dispersion copper oxides form more active species Lewis acidic sites (LAS). The variable-temperature FTIR, XAS, NO-IR analyses identified dispersed dimeric such ([Cu2(μ-O)]2+ or [(Cu2O2)2+]) major into methanol. Additionally, combined situ FTIR analysis, mechanism revealed, which adsorbed could be converted CH3* species. Subsequently, bound oxygen CH3O* species, then presence water.

Язык: Английский

Процитировано

3
Photothermal catalytic methane oxidation to methanol on Cu/Ti-ZSM-5 DOI
Wen-Jing Wang,

Jun-Cai Hao,

Lei Liu

и другие.

Fuel, Год журнала: 2024, Номер 376, С. 132720 - 132720

Опубликована: Авг. 8, 2024

Язык: Английский

Процитировано

3
Efficient CH4 oxidation to C1/C2 oxygenates over cluster-dispersing Rh decorated ZSM-5 DOI Creative Commons
Xin Zhang, Chao Hu,

Jingting Jin

и другие.

RSC Advances, Год журнала: 2025, Номер 15(2), С. 1301 - 1310

Опубликована: Янв. 1, 2025

Converting methane directly into liquid oxygenated products such as methanol and acetic acid is an energy-efficient method with significant potential for various industrial applications.

Язык: Английский

Процитировано

0
Fabrication of EDTA modified silica gel toward highly efficient adsorptive removal of copper ions from methanol DOI

Z. Yin,

Qidong Zhao,

Chuyi Xie

и другие.

Separation and Purification Technology, Год журнала: 2025, Номер unknown, С. 133225 - 133225

Опубликована: Апрель 1, 2025

Язык: Английский

Процитировано

0
ABO4 as an Active Catalyst Structure for Direct Partial CH4 Oxidation as Identified through Screening of Supported Catalysts DOI
Junya Ohyama,

Yuriko Yoshioka,

Masato TSUKAMOTO

и другие.

ACS Catalysis, Год журнала: 2024, Номер 15(2), С. 697 - 705

Опубликована: Дек. 24, 2024

In the present study, 76 different metal-oxide-supported-transition-metal catalysts were prepared using 11 metal oxides (MgO, Al2O3, SiO2, TiO2, V2O5, ZrO2, Nb2O5, MoO3, Ta2O5, WO3, and La2O3) seven 3d metals (V, Mn, Fe, Co, Ni, Cu, Zn). The supported catalysts, along with single oxides, screened to identify catalytically active lattice oxygen structures for partial oxidation of CH4 formaldehyde methanol. Fe/MoO3, Fe/V2O5, particularly Fe/Nb2O5 found be highly effective. Structural analysis Fe sites in was performed high-energy-resolution-fluorescence-detected K-edge X-ray absorption near-edge structure spectroscopy, revealing that FeNbO4, FeMoO4, FeVO4 species Fe/Nb2O5, respectively, are responsible their partial-oxidation activities. contrast, Fe2O3 formed Fe/Al2O3, Fe/SiO2, Fe/Ta2O5, Fe/WO3 complete CO2 than oxidation, as MgFe2O4, LaFeO3, TiFe2O5 Fe/MgO, Fe/La2O3, Fe/TiO2, interstitial solid solution Fe3+ ZrO2 generated Fe/ZrO2. Furthermore, while Fe/WO4 ineffective FeWO4 by a hydrothermal method exhibits high selectivity oxidation. Additionally, previous studies have shown CuWO4 CuMoO4 Accordingly, ABO4 (where A is B group 5 or 6 metal) indicated viable design basis development

Язык: Английский

Процитировано

2
Role of copper and cerium species in Cu/CeZSM catalysts for direct methane to methanol reaction: Insights of structure–activity relationship DOI

Pranay R. Chandewar,

Debaprasad Shee

Journal of Catalysis, Год журнала: 2024, Номер 442, С. 115916 - 115916

Опубликована: Дек. 20, 2024

Язык: Английский

Процитировано

1
Molybdate-Based Catalytic Systems for Aerobic Oxidation of Organic Substrates (A Review) DOI
Sofya Sh. Latypova, E. A. Eseva, N. A. Sinikova

и другие.

Petroleum Chemistry, Год журнала: 2023, Номер 63(11), С. 1274 - 1291

Опубликована: Дек. 1, 2023

Язык: Английский

Процитировано

3
Plasma-Catalytic Direct Oxidation of Methane to Methanol Over Cu-Mor: Revealing the Zeolite-Confined Cu2+ Active Sites DOI

Huan Lv,

Shengyan Meng, Zhaolun Cui

и другие.

Опубликована: Янв. 1, 2024

Efficient methane conversion to methanol remains a significant challenge in chemical industry. This study investigates the direct oxidation of under mild conditions, employing synergy non-thermal plasma and Cu-MOR (Copper-Mordenite) catalysts. Catalytic tests demonstrate that IE-3 catalyst (i.e., prepared by three cycles ion exchange) exhibits superior catalytic performance (with 51% selectivity 7.9% conversion). Conversely, catalysts via wetness impregnation tend over-oxidize CH4 CO CO2. Through systematic characterizations (XRD, TPR, UV-Vis, HRTEM, XPS), we elucidate exchange mainly leads formation zeolite-confined Cu2+ species, while predominantly results CuO particles. Based on performance, in-situ FTIR spectra, conclude species serve as active sites for plasma-catalytic methanol.

Язык: Английский

Процитировано

0