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

被引:3
作者
Xiao, Peipei [1 ]
Toyoda, Hiroto [1 ]
Wang, Yong [1 ]
Nakamura, Kengo [1 ]
Bekhti, Samya [1 ]
Osuga, Ryota [2 ]
Nishibori, Maiko [3 ]
Gies, Hermann [1 ]
Yokoi, Toshiyuki [1 ,4 ]
机构
[1] Tokyo Inst Technol, Inst Innovat Res, Yokohama 2268501, Japan
[2] Hokkaido Univ, Inst Catalysis, Sapporo, Hokkaido 268501, Japan
[3] Tohoku Univ, Int Ctr Synchrotron Radiat Innovat Smart, Sendai, Miyagi 9808572, Japan
[4] IPEACE223 Inc, Tokyo 1040045, Japan
基金
日本学术振兴会;
关键词
acidic proton; isomorphous substitution; Fe-zeolite; methane oxidation; tandem reaction; SELECTIVE OXIDATION; EXCHANGED ZEOLITES; DIRECT CONVERSION; COPPER; CU; INSIGHTS; SPECIATION; FE/SSZ-13; CATALYSTS; BENZENE;
D O I
10.1021/acscatal.4c04875
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Fe-containing zeolite catalysts are active in N2O 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 ion-exchanged 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 degrees 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 Fe3+ attachment, and resulted in inactive Fe x O y . Furthermore, in contrast to the robust N2O adsorption capacity of Na+, the acidic proton exhibited weak competition with Fe3+ for N2O 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 N2O with Fe species, and the feasibility of the tandem reaction of methane to methanol and methanol to hydrocarbon.
引用
收藏
页码:17434 / 17444
页数:11
相关论文
共 57 条
[1]   Mechanism of Hydrocarbon Formation in Methane and Methanol Conversion over Copper-Containing Mordenite [J].
Artsiusheuski, Mikalai A. ;
Verel, Rene ;
van Bokhoven, Jeroen A. ;
Sushkevich, Vitaly L. .
ACS CATALYSIS, 2023, 13 (09) :5864-5875
[2]   Methane Transformation over Copper-Exchanged Zeolites: From Partial Oxidation to C-C Coupling and Formation of Hydrocarbons [J].
Artsiusheuski, Mikalai A. ;
Verel, Rene ;
van Bokhoven, Jeroen A. ;
Sushkevich, Vitaly L. .
ACS CATALYSIS, 2021, 11 (20) :12543-12556
[3]   Selective Formation of α-Fe(II) Sites on Fe-Zeolites through One-Pot Synthesis [J].
Bols, Max L. ;
Devos, Julien ;
Rhoda, Hannah M. ;
Plessers, Dieter ;
Solomon, Edward, I ;
Schoonheydt, Robert A. ;
Sels, Bert F. ;
Dusselier, Michiel .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2021, 143 (39) :16243-16255
[4]   Fe-MOR and Fe-FER as catalysts for abatement of N2O with CH4: in situ UV-vis DRS and operando FTIR study [J].
Campa, Maria Cristina ;
Pietrogiacomi, Daniela ;
Catracchia, Carlotta ;
Morpurgo, Simone ;
Olszowka, Joanna ;
Mlekodaj, Kinga ;
Lemishka, Mariia ;
Dedecek, Jiri ;
Kornas, Agnieszka ;
Tabor, Edyta .
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY, 2024, 342
[5]   Insights into the Pyridine-Modified MOR Zeolite Catalysts for DME Carbonylation [J].
Cao, Kaipeng ;
Fan, Dong ;
Li, Lingyun ;
Fan, Benhan ;
Wang, Linying ;
Zhu, Dali ;
Wang, Quanyi ;
Tian, Peng ;
Liu, Zhongmin .
ACS CATALYSIS, 2020, 10 (05) :3372-3380
[6]   Investigating the influence of acid sites in continuous methane oxidation with N2O over Fe/MFI zeolites [J].
Chow, Ying Kit ;
Dummer, Nicholas F. ;
Carter, James H. ;
Williams, Christopher ;
Shaw, Greg ;
Willock, David J. ;
Taylor, Stuart H. ;
Yacob, Sara ;
Meyer, Randall J. ;
Bhasin, Madan M. ;
Hutchings, Graham J. .
CATALYSIS SCIENCE & TECHNOLOGY, 2018, 8 (01) :154-163
[7]   Continuous Partial Oxidation of Methane to Methanol Catalyzed by Diffusion-Paired Copper Dimers in Copper-Exchanged Zeolites [J].
Dinh, Kimberly T. ;
Sullivan, Mark M. ;
Narsimhan, Karthik ;
Serna, Pedro ;
Meyer, Randall J. ;
Dinca, Mircea ;
Roman-Leshkov, Yuriy .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2019, 141 (29) :11641-11650
[8]   Methane Oxidation to Methanol [J].
Dummer, Nicholas F. ;
Willock, David J. ;
He, Qian ;
Howard, Mark J. ;
Lewis, Richard J. ;
Qi, Guodong ;
Taylor, Stuart H. ;
Xu, Jun ;
Bethell, Don ;
Kiely, Christopher J. ;
Hutchings, Graham J. .
CHEMICAL REVIEWS, 2023, 123 (09) :6359-6411
[9]  
FREUDE D, 2002, HDB POROUS SOLIDS, V1, P465, DOI DOI 10.1002/9783527618286.CH14
[10]   Elucidating Zeolite Channel Geometry-Reaction Intermediate Relationships for the Methanol-to-Hydrocarbon Process [J].
Fu, Donglong ;
Paioni, Alessandra Lucini ;
Lian, Cheng ;
van der Heijden, Onno ;
Baldus, Marc ;
Weckhuysen, Bert M. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2020, 59 (45) :20024-20030