Overcoming the kinetic and deactivation limitations of Ni catalyst by alloying it with Zn for the dry reforming of methane

Vijay Kumar Velisoju; Quaid Johar Samun Virpurwala; Yerrayya Attada; Xueqin Bai; Bambar Davaasuren; Mohamed Ben Hassine; Xueli Yao; Gontzal Lezcano; Shekhar Rajabhau Kulkarni; Pedro Castaño

doi:10.1016/j.jcou.2023.102573

Overcoming the kinetic and deactivation limitations of Ni catalyst by alloying it with Zn for the dry reforming of methane

Vijay Kumar Velisoju, Quaid Johar Samun Virpurwala, Yerrayya Attada, Xueqin Bai, Bambar Davaasuren, Mohamed Ben Hassine, Xueli Yao, Gontzal Lezcano, Shekhar Rajabhau Kulkarni, Pedro Castaño

Research output: Contribution to journal › Article › peer-review

19 Scopus citations

Abstract

Stimulated by the capacity of Zn to improve the adoption of CO2 and CH4, we doped a Ni-supported ZrO2 catalyst with Zn to enhance its performance and stability in the dry reforming of methane. We prepared a set of catalysts with different Ni:Zn:Zr proportions and conducted extensive ex situ and in situ characterizations to prove that a Ni–Zn alloy was formed at 750 °C under reductive conditions. Combining a tailored morphology of the alloy nanoparticles, strong metal–support (ZnO–ZrO2) interactions, and additional oxygen vacancies created by Zn inclusion resulted in an enhanced catalyst with 15% higher initial activity and higher stability for over 100 h on stream than Zn-free catalyst. Our experimental and modeling results demonstrated that the catalyst with adjusted Ni:Zn:Zr proportion improves the adsorption and reaction rates of CH4 and CO2 while extending its lifetime through enhanced coke precursor gasification compared to its Zn-free counterpart.

Original language	English (US)
Pages (from-to)	102573
Journal	Journal of CO2 Utilization
Volume	75
DOIs	https://doi.org/10.1016/j.jcou.2023.102573
State	Published - Aug 23 2023

Bibliographical note

KAUST Repository Item: Exported on 2023-08-31
Acknowledged KAUST grant number(s): BAS/1/1403
Acknowledgements: King Abdullah University of Science and Technology (KAUST) provided funding for this work: BAS/1/1403. The authors acknowledge the KAUST Supercomputing Laboratory for providing high-performance computational resources and the KAUST Core Labs for providing support.

ASJC Scopus subject areas

Waste Management and Disposal
Process Chemistry and Technology
Chemical Engineering (miscellaneous)

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10.1016/j.jcou.2023.102573

https://repository.kaust.edu.sa/bitstream/10754/693867/1/1-s2.0-S2212982023001841-main.pdf

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title = "Overcoming the kinetic and deactivation limitations of Ni catalyst by alloying it with Zn for the dry reforming of methane",

abstract = "Stimulated by the capacity of Zn to improve the adoption of CO2 and CH4, we doped a Ni-supported ZrO2 catalyst with Zn to enhance its performance and stability in the dry reforming of methane. We prepared a set of catalysts with different Ni:Zn:Zr proportions and conducted extensive ex situ and in situ characterizations to prove that a Ni–Zn alloy was formed at 750 °C under reductive conditions. Combining a tailored morphology of the alloy nanoparticles, strong metal–support (ZnO–ZrO2) interactions, and additional oxygen vacancies created by Zn inclusion resulted in an enhanced catalyst with 15% higher initial activity and higher stability for over 100 h on stream than Zn-free catalyst. Our experimental and modeling results demonstrated that the catalyst with adjusted Ni:Zn:Zr proportion improves the adsorption and reaction rates of CH4 and CO2 while extending its lifetime through enhanced coke precursor gasification compared to its Zn-free counterpart.",

author = "Velisoju, {Vijay Kumar} and Virpurwala, {Quaid Johar Samun} and Yerrayya Attada and Xueqin Bai and Bambar Davaasuren and {Ben Hassine}, Mohamed and Xueli Yao and Gontzal Lezcano and Kulkarni, {Shekhar Rajabhau} and Pedro Casta{\~n}o",

note = "KAUST Repository Item: Exported on 2023-08-31 Acknowledged KAUST grant number(s): BAS/1/1403 Acknowledgements: King Abdullah University of Science and Technology (KAUST) provided funding for this work: BAS/1/1403. The authors acknowledge the KAUST Supercomputing Laboratory for providing high-performance computational resources and the KAUST Core Labs for providing support.",

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doi = "10.1016/j.jcou.2023.102573",

language = "English (US)",

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T1 - Overcoming the kinetic and deactivation limitations of Ni catalyst by alloying it with Zn for the dry reforming of methane

AU - Velisoju, Vijay Kumar

AU - Virpurwala, Quaid Johar Samun

AU - Attada, Yerrayya

AU - Bai, Xueqin

AU - Davaasuren, Bambar

AU - Ben Hassine, Mohamed

AU - Yao, Xueli

AU - Lezcano, Gontzal

AU - Kulkarni, Shekhar Rajabhau

AU - Castaño, Pedro

N1 - KAUST Repository Item: Exported on 2023-08-31 Acknowledged KAUST grant number(s): BAS/1/1403 Acknowledgements: King Abdullah University of Science and Technology (KAUST) provided funding for this work: BAS/1/1403. The authors acknowledge the KAUST Supercomputing Laboratory for providing high-performance computational resources and the KAUST Core Labs for providing support.

PY - 2023/8/23

Y1 - 2023/8/23

N2 - Stimulated by the capacity of Zn to improve the adoption of CO2 and CH4, we doped a Ni-supported ZrO2 catalyst with Zn to enhance its performance and stability in the dry reforming of methane. We prepared a set of catalysts with different Ni:Zn:Zr proportions and conducted extensive ex situ and in situ characterizations to prove that a Ni–Zn alloy was formed at 750 °C under reductive conditions. Combining a tailored morphology of the alloy nanoparticles, strong metal–support (ZnO–ZrO2) interactions, and additional oxygen vacancies created by Zn inclusion resulted in an enhanced catalyst with 15% higher initial activity and higher stability for over 100 h on stream than Zn-free catalyst. Our experimental and modeling results demonstrated that the catalyst with adjusted Ni:Zn:Zr proportion improves the adsorption and reaction rates of CH4 and CO2 while extending its lifetime through enhanced coke precursor gasification compared to its Zn-free counterpart.

AB - Stimulated by the capacity of Zn to improve the adoption of CO2 and CH4, we doped a Ni-supported ZrO2 catalyst with Zn to enhance its performance and stability in the dry reforming of methane. We prepared a set of catalysts with different Ni:Zn:Zr proportions and conducted extensive ex situ and in situ characterizations to prove that a Ni–Zn alloy was formed at 750 °C under reductive conditions. Combining a tailored morphology of the alloy nanoparticles, strong metal–support (ZnO–ZrO2) interactions, and additional oxygen vacancies created by Zn inclusion resulted in an enhanced catalyst with 15% higher initial activity and higher stability for over 100 h on stream than Zn-free catalyst. Our experimental and modeling results demonstrated that the catalyst with adjusted Ni:Zn:Zr proportion improves the adsorption and reaction rates of CH4 and CO2 while extending its lifetime through enhanced coke precursor gasification compared to its Zn-free counterpart.

UR - http://hdl.handle.net/10754/693867

UR - https://linkinghub.elsevier.com/retrieve/pii/S2212982023001841

U2 - 10.1016/j.jcou.2023.102573

DO - 10.1016/j.jcou.2023.102573

M3 - Article

SN - 2212-9820

VL - 75

SP - 102573

JO - Journal of CO2 Utilization

JF - Journal of CO2 Utilization

ER -

Overcoming the kinetic and deactivation limitations of Ni catalyst by alloying it with Zn for the dry reforming of methane

Abstract

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