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Understanding the effect of spatially separated Cu and acid sites in zeolite catalysts on oxidation of methane.

ABSTRACT: Unraveling the effect of spatially separated bifunctional sites on catalytic reactions is significant yet challenging. In this report, we investigate the role of spatial separation on the oxidation of methane in a series of Cu-exchanged aluminosilicate zeolites. Regulation of the bifunctional sites is done either through studying a physical mixture of Cu-exchanged zeolites and acidic zeolites or by systematically varying the Cu and acid density within a family of zeolite materials. We show that separated Cu and acid sites are beneficial for the formation of hydrocarbons while high-density Cu sites, which are closer together, facilitate the production of CO₂. By contrast, a balance of the spatial separation of Cu and acid sites shows more favorable formation of methanol. This work will further guide approaches to methane oxidation to methanol and open an avenue for promoting hydrocarbon synthesis using methanol as an intermediate.

SUBMITTER: Xiao P

PROVIDER: S-EPMC10978981 | biostudies-literature | 2024 Mar

REPOSITORIES: biostudies-literature

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Understanding the effect of spatially separated Cu and acid sites in zeolite catalysts on oxidation of methane.

Xiao Peipei P Wang Yong Y Wang Lizhuo L Toyoda Hiroto H Nakamura Kengo K Bekhti Samya S Lu Yao Y Huang Jun J Gies Hermann H Yokoi Toshiyuki T

Nature communications 20240328 1

Unraveling the effect of spatially separated bifunctional sites on catalytic reactions is significant yet challenging. In this report, we investigate the role of spatial separation on the oxidation of methane in a series of Cu-exchanged aluminosilicate zeolites. Regulation of the bifunctional sites is done either through studying a physical mixture of Cu-exchanged zeolites and acidic zeolites or by systematically varying the Cu and acid density within a family of zeolite materials. We show that ...[more]

PMID: 38548724

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Project description:Zeolites with different structures (P1, sodalite, and X) were synthesized from coal fly ash by applying ultrasonically assisted hydrothermal and fusion-hydrothermal synthesis. Bimetallic catalysts, containing 5 wt.% Ni and 2.5 wt.% Cu, supported on the zeolites, were prepared by a post-synthesis incipient wetness impregnation method. The catalysts were characterized by X-ray powder diffraction (XRPD), N2 physisorption, transmission electron microscopy (TEM), Mössbauer and X-ray photoelectron spectroscopies (XPS), and H2-temperature-programmed reduction (H2-TPR) analyses. The XRPD results showed that crystalline Cu0 and NixCuy intermetallic nanoparticles were formed in the reduced catalysts. The presence of the intermetallic phase affected the reducibility of the nickel by shifting it to a lower temperature, as confirmed by the H2-TPR curves. Based on the Mössbauer spectroscopic results, it was established that the iron contamination of the coal fly ash zeolites (CFAZs) was distributed in ionic positions of the zeolite lattice and as a finely dispersed iron oxide phase on the external surface of the supports. The formation of the NiFe alloy, not detectable by XRPD, was also evidenced on the impregnated samples. The catalysts were studied in the upgrading of levulinic acid (LA), derived from lignocellulosic biomass, to γ-valerolactone (GVL), in a batch reactor under 30 bar H2 pressure at 150 and 200 °C, applying water as a solvent. The NiCu/SOD and NiCu/X catalysts showed total LA conversion and a high GVL yield (>75%) at a reaction temperature of 200 °C. It was found that the textural parameters of the catalysts have less influence on the catalytic activity, but rather the stable dispersion of metals during the reaction. The characterization of the spent catalyst found the rearrangement of the support structure. The high LA conversion and GVL yield can be attributed to the weak acidic character of the support and the moderate hydrogenation activity of the Ni-Cu sites with high dispersion.

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Understanding the effect of spatially separated Cu and acid sites in zeolite catalysts on oxidation of methane.

Publications

Understanding the effect of spatially separated Cu and acid sites in zeolite catalysts on oxidation of methane.

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