Atomically dispersed nickel as coke-resistant active sites for methane dry reforming

Mohcin Akri; Shu Zhao; Xiaoyu Li; Ketao Zang; Adam F. Lee; Mark A. Isaacs; Wei Xi; Yuvaraj Gangarajula; Jun Luo; Yujing Ren; Yi Tao Cui; Lei Li; Yang Su; Xiaoli Pan; Wu Wen; Yang Pan; Karen Wilson; Lin Li; Botao Qiao; Hirofumi Ishii; Yen Fa Liao; Aiqin Wang; Xiaodong Wang; Tao Zhang

doi:10.1038/s41467-019-12843-w

Atomically dispersed nickel as coke-resistant active sites for methane dry reforming

Mohcin Akri, Shu Zhao, Xiaoyu Li, Ketao Zang, Adam F. Lee, Mark A. Isaacs, Wei Xi, Yuvaraj Gangarajula, Jun Luo, Yujing Ren, Yi Tao Cui, Lei Li, Yang Su, Xiaoli Pan, Wu Wen, Yang Pan, Karen Wilson, Lin Li, Botao Qiao, Hirofumi IshiiYen Fa Liao, Aiqin Wang, Xiaodong Wang, Tao Zhang

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

488 Scopus citations

Abstract

Dry reforming of methane (DRM) is an attractive route to utilize CO₂ as a chemical feedstock with which to convert CH₄ into valuable syngas and simultaneously mitigate both greenhouse gases. Ni-based DRM catalysts are promising due to their high activity and low cost, but suffer from poor stability due to coke formation which has hindered their commercialization. Herein, we report that atomically dispersed Ni single atoms, stabilized by interaction with Ce-doped hydroxyapatite, are highly active and coke-resistant catalytic sites for DRM. Experimental and computational studies reveal that isolated Ni atoms are intrinsically coke-resistant due to their unique ability to only activate the first C-H bond in CH₄, thus avoiding methane deep decomposition into carbon. This discovery offers new opportunities to develop large-scale DRM processes using earth abundant catalysts.

Original language	English
Article number	5181
Journal	Nature Communications
Volume	10
Issue number	1
DOIs	https://doi.org/10.1038/s41467-019-12843-w
State	Published - 1 Dec 2019
Externally published	Yes

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Akri, M., Zhao, S., Li, X., Zang, K., Lee, A. F., Isaacs, M. A., Xi, W., Gangarajula, Y., Luo, J., Ren, Y., Cui, Y. T., Li, L., Su, Y., Pan, X., Wen, W., Pan, Y., Wilson, K., Li, L., Qiao, B., ... Zhang, T. (2019). Atomically dispersed nickel as coke-resistant active sites for methane dry reforming. Nature Communications, 10(1), Article 5181. https://doi.org/10.1038/s41467-019-12843-w

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title = "Atomically dispersed nickel as coke-resistant active sites for methane dry reforming",

abstract = "Dry reforming of methane (DRM) is an attractive route to utilize CO2 as a chemical feedstock with which to convert CH4 into valuable syngas and simultaneously mitigate both greenhouse gases. Ni-based DRM catalysts are promising due to their high activity and low cost, but suffer from poor stability due to coke formation which has hindered their commercialization. Herein, we report that atomically dispersed Ni single atoms, stabilized by interaction with Ce-doped hydroxyapatite, are highly active and coke-resistant catalytic sites for DRM. Experimental and computational studies reveal that isolated Ni atoms are intrinsically coke-resistant due to their unique ability to only activate the first C-H bond in CH4, thus avoiding methane deep decomposition into carbon. This discovery offers new opportunities to develop large-scale DRM processes using earth abundant catalysts.",

author = "Mohcin Akri and Shu Zhao and Xiaoyu Li and Ketao Zang and Lee, {Adam F.} and Isaacs, {Mark A.} and Wei Xi and Yuvaraj Gangarajula and Jun Luo and Yujing Ren and Cui, {Yi Tao} and Lei Li and Yang Su and Xiaoli Pan and Wu Wen and Yang Pan and Karen Wilson and Lin Li and Botao Qiao and Hirofumi Ishii and Liao, {Yen Fa} and Aiqin Wang and Xiaodong Wang and Tao Zhang",

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doi = "10.1038/s41467-019-12843-w",

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Akri, M, Zhao, S, Li, X, Zang, K, Lee, AF, Isaacs, MA, Xi, W, Gangarajula, Y, Luo, J, Ren, Y, Cui, YT, Li, L, Su, Y, Pan, X, Wen, W, Pan, Y, Wilson, K, Li, L, Qiao, B, Ishii, H, Liao, YF, Wang, A, Wang, X & Zhang, T 2019, 'Atomically dispersed nickel as coke-resistant active sites for methane dry reforming', Nature Communications, vol. 10, no. 1, 5181. https://doi.org/10.1038/s41467-019-12843-w

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T1 - Atomically dispersed nickel as coke-resistant active sites for methane dry reforming

AU - Akri, Mohcin

AU - Zhao, Shu

AU - Li, Xiaoyu

AU - Zang, Ketao

AU - Lee, Adam F.

AU - Isaacs, Mark A.

AU - Xi, Wei

AU - Gangarajula, Yuvaraj

AU - Luo, Jun

AU - Ren, Yujing

AU - Cui, Yi Tao

AU - Li, Lei

AU - Su, Yang

AU - Pan, Xiaoli

AU - Wen, Wu

AU - Pan, Yang

AU - Wilson, Karen

AU - Li, Lin

AU - Qiao, Botao

AU - Ishii, Hirofumi

AU - Liao, Yen Fa

AU - Wang, Aiqin

AU - Wang, Xiaodong

AU - Zhang, Tao

PY - 2019/12/1

Y1 - 2019/12/1

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AB - Dry reforming of methane (DRM) is an attractive route to utilize CO2 as a chemical feedstock with which to convert CH4 into valuable syngas and simultaneously mitigate both greenhouse gases. Ni-based DRM catalysts are promising due to their high activity and low cost, but suffer from poor stability due to coke formation which has hindered their commercialization. Herein, we report that atomically dispersed Ni single atoms, stabilized by interaction with Ce-doped hydroxyapatite, are highly active and coke-resistant catalytic sites for DRM. Experimental and computational studies reveal that isolated Ni atoms are intrinsically coke-resistant due to their unique ability to only activate the first C-H bond in CH4, thus avoiding methane deep decomposition into carbon. This discovery offers new opportunities to develop large-scale DRM processes using earth abundant catalysts.

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VL - 10

JO - Nature Communications

JF - Nature Communications

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ER -

Atomically dispersed nickel as coke-resistant active sites for methane dry reforming

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