Comparison of the Reactive Adsorption Desulfurization Performance of Ni/ZnO-Al2O3 Adsorbents Prepared by Different Methods

Rooh Ullah; Peng Bai; Pingping Wu; Zhanquan Zhang; Ziyi Zhong; U. J. Etim; Fazle Subhan; Zifeng Yan

doi:10.1021/acs.energyfuels.6b00232

Comparison of the Reactive Adsorption Desulfurization Performance of Ni/ZnO-Al₂O₃ Adsorbents Prepared by Different Methods

Rooh Ullah, Peng Bai^*, Pingping Wu, Zhanquan Zhang, Ziyi Zhong, U. J. Etim, Fazle Subhan, Zifeng Yan

^*Corresponding author for this work

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

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Abstract

In this study, a series of Ni/ZnO-Al₂O₃ mixed oxide (MO) adsorbents were prepared by the one-step homogeneous precipitation method and the cation-anion double hydrolysis (CADH) method for reactive adsorption desulfurization (RADS) using thiophene as a model fuel in a fixed bed reactor. The synthesized adsorbents were characterized by N₂ sorption, X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), H₂ temperature-programmed reduction (H₂-TPR), ultraviolet-visible (UV-vis) diffuse reflectance spectroscopy (DRS), and Raman spectroscopy. Results show that both Ni loading and the preparation method have a significant effect on the RADS activities of the adsorbent. Among the studied adsorbents, 10% Ni/ZnO-Al₂O₃ prepared by the one-step urea precipitation method showed the best RADS performance, with a thiophene conversion up to 96% and a sulfur adsorption capacity of 86 mg of S/g, which is 34% larger than that of CADH adsorbents. In addition, upon five RADS-regeneration cycles, sample 10% Ni/ZnO-Al₂O₃ exhibited a drop of only 3% in thiophene conversion, indicating the high stability of the Ni/ZnO-Al₂O₃ adsorbent prepared by homogeneous precipitation. Characterization results show that the one-step homogeneous precipitation method could facilitate the formation of small ZnO particles while suppressing the formation of inactive ZnAl₂O₄. On the other hand, by decreasing the formation of NiAl₂O₄, the homogeneous precipitation method could also generate high concentration of Ni⁰ sites, which are the active centers for the hydrogenolysis of C-S bonds. These findings indicate that a high-performance adsorbent for RADS can be obtained by employing a proper preparation method with good control on the adsorbent structure.

Original language	English
Pages (from-to)	2874-2881
Number of pages	8
Journal	Energy and Fuels
Volume	30
Issue number	4
DOIs	https://doi.org/10.1021/acs.energyfuels.6b00232
State	Published - 21 Apr 2016
Externally published	Yes

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10.1021/acs.energyfuels.6b00232

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@article{a4f24f01a54443c2a517e113435fd4ee,

title = "Comparison of the Reactive Adsorption Desulfurization Performance of Ni/ZnO-Al2O3 Adsorbents Prepared by Different Methods",

abstract = "In this study, a series of Ni/ZnO-Al2O3 mixed oxide (MO) adsorbents were prepared by the one-step homogeneous precipitation method and the cation-anion double hydrolysis (CADH) method for reactive adsorption desulfurization (RADS) using thiophene as a model fuel in a fixed bed reactor. The synthesized adsorbents were characterized by N2 sorption, X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), H2 temperature-programmed reduction (H2-TPR), ultraviolet-visible (UV-vis) diffuse reflectance spectroscopy (DRS), and Raman spectroscopy. Results show that both Ni loading and the preparation method have a significant effect on the RADS activities of the adsorbent. Among the studied adsorbents, 10% Ni/ZnO-Al2O3 prepared by the one-step urea precipitation method showed the best RADS performance, with a thiophene conversion up to 96% and a sulfur adsorption capacity of 86 mg of S/g, which is 34% larger than that of CADH adsorbents. In addition, upon five RADS-regeneration cycles, sample 10% Ni/ZnO-Al2O3 exhibited a drop of only 3% in thiophene conversion, indicating the high stability of the Ni/ZnO-Al2O3 adsorbent prepared by homogeneous precipitation. Characterization results show that the one-step homogeneous precipitation method could facilitate the formation of small ZnO particles while suppressing the formation of inactive ZnAl2O4. On the other hand, by decreasing the formation of NiAl2O4, the homogeneous precipitation method could also generate high concentration of Ni0 sites, which are the active centers for the hydrogenolysis of C-S bonds. These findings indicate that a high-performance adsorbent for RADS can be obtained by employing a proper preparation method with good control on the adsorbent structure.",

author = "Rooh Ullah and Peng Bai and Pingping Wu and Zhanquan Zhang and Ziyi Zhong and Etim, {U. J.} and Fazle Subhan and Zifeng Yan",

note = "Publisher Copyright: {\textcopyright} 2016 American Chemical Society.",

year = "2016",

month = apr,

day = "21",

doi = "10.1021/acs.energyfuels.6b00232",

language = "英语",

volume = "30",

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journal = "Energy and Fuels",

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T1 - Comparison of the Reactive Adsorption Desulfurization Performance of Ni/ZnO-Al2O3 Adsorbents Prepared by Different Methods

AU - Ullah, Rooh

AU - Bai, Peng

AU - Wu, Pingping

AU - Zhang, Zhanquan

AU - Zhong, Ziyi

AU - Etim, U. J.

AU - Subhan, Fazle

AU - Yan, Zifeng

PY - 2016/4/21

Y1 - 2016/4/21

N2 - In this study, a series of Ni/ZnO-Al2O3 mixed oxide (MO) adsorbents were prepared by the one-step homogeneous precipitation method and the cation-anion double hydrolysis (CADH) method for reactive adsorption desulfurization (RADS) using thiophene as a model fuel in a fixed bed reactor. The synthesized adsorbents were characterized by N2 sorption, X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), H2 temperature-programmed reduction (H2-TPR), ultraviolet-visible (UV-vis) diffuse reflectance spectroscopy (DRS), and Raman spectroscopy. Results show that both Ni loading and the preparation method have a significant effect on the RADS activities of the adsorbent. Among the studied adsorbents, 10% Ni/ZnO-Al2O3 prepared by the one-step urea precipitation method showed the best RADS performance, with a thiophene conversion up to 96% and a sulfur adsorption capacity of 86 mg of S/g, which is 34% larger than that of CADH adsorbents. In addition, upon five RADS-regeneration cycles, sample 10% Ni/ZnO-Al2O3 exhibited a drop of only 3% in thiophene conversion, indicating the high stability of the Ni/ZnO-Al2O3 adsorbent prepared by homogeneous precipitation. Characterization results show that the one-step homogeneous precipitation method could facilitate the formation of small ZnO particles while suppressing the formation of inactive ZnAl2O4. On the other hand, by decreasing the formation of NiAl2O4, the homogeneous precipitation method could also generate high concentration of Ni0 sites, which are the active centers for the hydrogenolysis of C-S bonds. These findings indicate that a high-performance adsorbent for RADS can be obtained by employing a proper preparation method with good control on the adsorbent structure.

AB - In this study, a series of Ni/ZnO-Al2O3 mixed oxide (MO) adsorbents were prepared by the one-step homogeneous precipitation method and the cation-anion double hydrolysis (CADH) method for reactive adsorption desulfurization (RADS) using thiophene as a model fuel in a fixed bed reactor. The synthesized adsorbents were characterized by N2 sorption, X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), H2 temperature-programmed reduction (H2-TPR), ultraviolet-visible (UV-vis) diffuse reflectance spectroscopy (DRS), and Raman spectroscopy. Results show that both Ni loading and the preparation method have a significant effect on the RADS activities of the adsorbent. Among the studied adsorbents, 10% Ni/ZnO-Al2O3 prepared by the one-step urea precipitation method showed the best RADS performance, with a thiophene conversion up to 96% and a sulfur adsorption capacity of 86 mg of S/g, which is 34% larger than that of CADH adsorbents. In addition, upon five RADS-regeneration cycles, sample 10% Ni/ZnO-Al2O3 exhibited a drop of only 3% in thiophene conversion, indicating the high stability of the Ni/ZnO-Al2O3 adsorbent prepared by homogeneous precipitation. Characterization results show that the one-step homogeneous precipitation method could facilitate the formation of small ZnO particles while suppressing the formation of inactive ZnAl2O4. On the other hand, by decreasing the formation of NiAl2O4, the homogeneous precipitation method could also generate high concentration of Ni0 sites, which are the active centers for the hydrogenolysis of C-S bonds. These findings indicate that a high-performance adsorbent for RADS can be obtained by employing a proper preparation method with good control on the adsorbent structure.

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U2 - 10.1021/acs.energyfuels.6b00232

DO - 10.1021/acs.energyfuels.6b00232

M3 - 文章

AN - SCOPUS:84966263994

SN - 0887-0624

VL - 30

SP - 2874

EP - 2881

JO - Energy and Fuels

JF - Energy and Fuels

IS - 4

ER -

Comparison of the Reactive Adsorption Desulfurization Performance of Ni/ZnO-Al₂O₃ Adsorbents Prepared by Different Methods

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