One-Pot Synthesized Fe-AEI Zeolite Catalysts Contribute to Direct Oxidation of Methane

Xiao, Peipei; Nakamura, Kengo; Lu, Yao; Huang, Jun; Wang, Lizhuo; Osuga, Ryota; Nishibori, Maiko; Wang, Yong; Gies, Hermann; Yokoi, Toshiyuki

doi:10.1021/acscatal.3c04675

Cited by 5 publications

(3 citation statements)

References 50 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…However, when the Fe content was less than 0.02 wt %, the reactant conversion and methanol selectivity of Fe/FER were close to that of H-FER (Figure F,G). Only if the Fe content was high enough, here was higher than 0.47 wt %, the properties of Fe species were presented in the high N 2 O conversion and high CO x selectivity (Figure F,G), which has been reported in our recent work . Additionally, the relation of the Cu content with selectivity was available (Figure S19).…”

Section: Resultssupporting

confidence: 63%

“…However, 5Cu/FER was active using N 2 O or O 2 as an oxidant (Figure S36). It signified that aluminosilicate zeolite and Fe-containing zeolite might have a similar reaction mechanism in oxidation of methane using N 2 O as the oxidant. , Simultaneously, when N 2 O was adsorbed on H-FER zeolite, two bands belonging to Al-ONN at 2248 and 2226 cm –1 were observed in the FTIR spectrum (Figure A), which was similar to the Fe-containing zeolite but different from the Cu-containing zeolites that have been reported in our recent works. ,,− Thus, we concluded that the possible reaction pathway of aluminosilicate zeolite was similar to that of the Fe-containing zeolite. First N 2 O was adsorbed on the active Al sites as the Al-ONN motif.…”

Section: Resultsmentioning

confidence: 45%

“…Despite the reaction routes being diverse, the selection of catalysts was merely focused on precious metals such as Pt and Au , and transition metals such as Cu, Co, and Fe as catalytically active species . Particularly, the transition-metal-exchanged zeolites have widely been used in both gas- and liquid-phase reaction systems. − The single- or dual-nuclear transition-metal moieties have been reported as active sites, − inspired by the natural biocatalytic enzyme systems . Furthermore, no transition-metal loading made the preparation of catalysts simpler and easier to obtain.…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Direct Oxidation of Methane to Methanol over Transition-Metal-Free Ferrierite Zeolite Catalysts

Xiao,

Wang,

et al. 2024

J. Am. Chem. Soc.

Self Cite

View full text Add to dashboard Cite

Direct oxidation of methane to methanol was reported to be highly dependent on the transition-or noble-metal-loading catalysts in the past decades. Here, we show that the transition-metal-free aluminosilicate ferrierite (FER) zeolite effectively catalyzed methane and N 2 O to methanol for the first time. The distorted tetracoordinated Al in the framework and pentacoordinated Al on the extra framework formed during calcination, activation, and reaction processes were confirmed as the potential active centers. The possible reaction pathway similar to the Fe-containing zeolites was advocated based on the reaction results using different oxidants, N 2 O adsorption FTIR spectra, and 27 Al MAS NMR spectra. The stable and efficient methanol production capacity of FER zeolite was ascribed to the two-dimensional straight channels and its distinctive Al distribution of FER zeolite (CP914C) from Zeolyst. The transition-metal-free FER zeolite performed better than the record in the literature and our recent results using transition-metalcontaining catalysts in terms of selectivity and formation rate of methanol and stability. This work has great significance and prospects for utilizing CH 4 and N 2 O as resources and will open new avenues for methane oxidation.

show abstract

Section: Resultssupporting

confidence: 63%

Section: Resultsmentioning

confidence: 45%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Direct Oxidation of Methane to Methanol over Transition-Metal-Free Ferrierite Zeolite Catalysts

Xiao,

Wang,

et al. 2024

J. Am. Chem. Soc.

Self Cite

View full text Add to dashboard Cite

show abstract

Effect of different skeleton structures on N2O decomposition from ammonia-fueled engines using Fe-based zeolite catalysts

Li,

Wang,

Zhang

et al. 2024

Fuel

View full text Add to dashboard Cite

Roles of Acidic Proton for Fe-Containing Zeolite in Direct Oxidation of Methane

Xiao,

Toyoda,

Wang

et al. 2024

ACS Catal.

View full text Add to dashboard Cite

Fe-containing zeolite catalysts are active in N 2 O decomposition and direct oxidation of unreactive methane. Except for the well-known ability that acid sites realize the subsequent reaction of methanol to hydrocarbon, the roles of acidic protons in the direct oxidation of methane have not been studied regarding the formation of active Fe components and the reactivity in the reaction. Herein, on the premise of the comparable total Fe and Al contents, the acidity of one-pot synthesized Fe-AEI and ionexchanged Fe/AEI zeolites was adjusted by various Na contents, and the catalytic activity in methane oxidation reactions was compared under different conditions. Ultraviolet−visible (UV−vis) spectra at 25−500 °C of the as-synthesized Fe-AEI and the reaction performance at the corresponding conditions were combined to clarify the formation of potential active Fe species. Acidic proton was favorable for the formation of potential active Fe species for the one-pot synthesized Fe-AEI zeolite. However, for the H-type Fe/AEI zeolite, thermal treatment at high temperatures was prone to dealuminate, reduced the number of anchors for Fe 3+ attachment, and resulted in inactive Fe x O y . Furthermore, in contrast to the robust N 2 O adsorption capacity of Na + , the acidic proton exhibited weak competition with Fe 3+ for N 2 O adsorption and thus contributed to the higher activity in the methane oxidation reaction. Our findings highlighted the importance of the acidic proton for the formation of potential active Fe species, the frail competition of adsorption N 2 O with Fe species, and the feasibility of the tandem reaction of methane to methanol and methanol to hydrocarbon.

show abstract

One-Pot Synthesized Fe-AEI Zeolite Catalysts Contribute to Direct Oxidation of Methane

Cited by 5 publications

References 50 publications

Direct Oxidation of Methane to Methanol over Transition-Metal-Free Ferrierite Zeolite Catalysts

Direct Oxidation of Methane to Methanol over Transition-Metal-Free Ferrierite Zeolite Catalysts

Effect of different skeleton structures on N2O decomposition from ammonia-fueled engines using Fe-based zeolite catalysts

Roles of Acidic Proton for Fe-Containing Zeolite in Direct Oxidation of Methane

Contact Info

Product

Resources

About