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Received August 2, 2021
Accepted October 31, 2021
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The effect of Zn doping on active Cu species and its location of Cu-exchanged mordenite for the stepwise oxidation of methane to methanol
Nutchapon Chotigkrai1†
Phakpum Tannititam1
Sunthon Piticharoenphun1
Narit Triamnak2
Supareak Praserthdam3 4
Piyasan Praserthdam3 4
1Department of Chemical Engineering, Faculty of Engineering and Industrial Technology, Silpakorn University, Nakhon Pathom, Thailand 73000 2Department of Materials Science and Engineering, Faculty of Engineering and Industrial Technology, Silpakorn University, Nakhon Pathom, Thailand 73000 3Department of Chemical Engineering, Faculty of Engineering, Chulalongkorn University, Bangkok, Thailand 10310 4Center of Excellence on Catalysis and Catalytic Reaction Engineering, Chulalongkorn University, Bangkok, Thailand 10330
chotigkrai_n@silpakorn.edu
Korean Journal of Chemical Engineering, April 2022, 39(4), 920-927(8), 10.1007/s11814-021-1001-3
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Abstract
The effect of Zn doping (0.5-3wt%) on Cu-exchanged mordenite (Cu-MOR) was investigated during the stepwise oxidation of methane to methanol. The strong interaction between Cu and ZnOx stabilized the highly-dispersed state of Cu2+ but reduced the Cu2+ bounded to extra-framework oxygen (active site), as demonstrated by the H2- TPR and XPS results. The Cu/Al and Zn/Al ratios suggested that Zn preferably bonded to the sites in the 8-MR channel, which led to highly dispersed Cu2+ anchored onto the highly accessible sites (12-MR and 8-MR side pocket). The reactivity indicated that highly dispersed Cu2+ can be gradually transformed into active Cu2+ species during contact with methane. Bimetallic Cu-ZnOx was also able to activate methane, resulting in a product complex. Although Zndoped Cu-MOR catalysts gave a lower methanol yield at 2 h, a higher methanol yield could be achieved at saturation methane loading time. Interestingly, 3 wt% Zn doping on Cu-MOR showed superior activity due to the increase of methanol yield up to 20% at 5 h of methane loading time. This work paves the way for the design of highly dispersed Cu2+ in the 12-MR channel of mordenite zeolite via the control of strong Cu-ZnOx interaction.
Keywords
References
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Merkx M, Kopp DA, Sazinsky MH, Blazyk JL, Müller J, Lippard SJ, Angew. Chem.-Int. Edit., 40, 2782 (2001)
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Geng H, Yang Z, Zhang L, Ran J, Yan Y, Energy Conv. Manag., 132, 339 (2017)
Zhao Y, Shan B, Wang Y, Zhou J, Wang S, Ma X, Ind. Eng. Chem. Res., 57, 4526 (2018)
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Gong T, Qin L, Lu J, Feng H, Phys. Chem. Chem. Phys., 18, 601 (2016)
Narsimhan K, Iyoki K, Dinh K, Román-Leshkov Y, ACS Cent. Sci., 2, 424 (2016)
Tamiyakul S, Ubolcharoen W, Tungasmita DN, Jongpatiwut S, Catal. Today, 256, 325 (2015)
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Fu Z, Yin D, Yang Y, Guo X, Appl. Catal. A: Gen., 124, 59 (1995)
Popov AG, Smirnov AV, Knyazeva EE, Yuschenko VV, Kalistratova EA, Klementiev KV, Grünert W, Ivanova II, Microporous Mesoporous Mater., 134, 124 (2010)
Lunkenbein T, Schumann J, Behrens M, Schlögl R, Willinger MG, Angew. Chem.-Int. Edit., 54, 4544 (2015)
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Liu Q, Zhao Z, Arai M, Zhang C, Liu K, Shi R, Wu P, Wang Z, Lin W, Cheng H, Zhao F, Catal. Sci. Technol., 10, 4412 (2020)
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Niu X, Gao J, Miao Q, Dong M, Wang G, Fan W, Qin Z, Wang J, Microporous Mesoporous Mater., 197, 252 (2014)
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Kulkarni AR, Zhao ZJ, Siahrostami S, Nørskov JK, Studt F, ACS Catal., 6, 6531 (2016)
Pappas DK, Martini A, Dyballa M, Kvande K, Teketel S, Lomachenko KA, Baran R, Glatzel P, Arstad B, Berlier G, J. Am. Chem. Soc., 140, 15270 (2018)
Ikuno T, Grundner S, Jentys A, Li G, Pidko E, Fulton J, Sanchez-Sanchez M, Lercher JA, J. Phys. Chem. C, 123, 8759 (2019)
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Meyet J, Ashuiev A, Noh G, Newton MA, Klose D, Searles K, van Bavel AP, Horton AD, Jeschke G, van Bokhoven JA, Angew. Chem.-Int. Edit., 60, 16200 (2021)
Wang G, Huang L, Chen W, Zhou J, Zheng A, Phys. Chem. Chem. Phys., 20, 26522 (2018)
