Ba2+ doping into Ni/Al2O3 nanofibers promotes CO2 methanation via alkaline modulation

Mengyuan Zhang; Xiaoyan Lu; Ying Qu; Chuandong He; Jiali Dong; Kongliang Luo; Jian Ye; Nana Lu; Qiang Niu; Pengfei Zhang; Sheng Dai

doi:10.1016/j.cej.2024.154872

Ba²⁺ doping into Ni/Al₂O₃ nanofibers promotes CO₂ methanation via alkaline modulation

Mengyuan Zhang, Xiaoyan Lu, Ying Qu, Chuandong He, Jiali Dong, Kongliang Luo, Jian Ye, Nana Lu, Qiang Niu, Pengfei Zhang, Sheng Dai

Chemical Sciences Division

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

Abstract

Ni-based catalysts are promising catalysts for CO₂ methanation due to low lost. However, the activity and selectivity of Ni-based catalysts in CO₂ methanation at low temperatures still need to be improved. Here, Ni₄Al₂Ba_mO_x (m = 0–0.5) nanofibers were prepared. Doping Ba²⁺ would increase alkaline sites and facilitate generating oxygen vacancies. Especially, Ni₄Al₂Ba_0.2O_x exhibited the high specific surface area with 127.1 m² g⁻¹, being potential for exposing more active sites. Indeed, compared with undoped Ni₄Al₂O_x catalysts (CO₂ conv. = 45 %, CH₄ select. = 92 % at 300 °C), Ba²⁺ doping significantly improved activity (CO₂ conv. = 74 %, CH₄ select. = 99 % at 300 °C) and stability within 200 h for Ni₄Al₂Ba_0.2O_x. Both EPR and O^1S XPS confirmed that Ni₄Al₂Ba_0.2O_x can form more oxygen vacancies and CO₂-TPD confirmed that Ni₄Al₂Ba_0.2O_x had stronger CO₂ adsorption capacity compared to Ni₄Al₂O_x. In-situ infrared spectroscopy and DFT calculations both indicated that Ba²⁺ doping can promote generating surface hydroxyl groups and formate pathways.

Original language	English
Article number	154872
Journal	Chemical Engineering Journal
Volume	497
DOIs	https://doi.org/10.1016/j.cej.2024.154872
State	Published - Oct 1 2024

Funding

This work was supported by the National Natural Science Foundation of China (grant no. 22178219), National Key R & D Program Plan (2022YFA1504803 and 2020YFB0606400), Inner Mongolia R &D Program Plan (2021ZD0042, 2021EEDSCXSFQZD006, 2021GG0350), Ordos R&D Program (2121HZ231-8). This work was supported by the National Natural Science Foundation of China (grant no. 22178219 ), National Key R & D Program Plan ( 2022YFA1504803 ), Inner Mongolia R &D Program Plan ( 2021ZD0042 , 2021EEDSCXSFQZD006 , 2021GG0350 ),Ordos R&D Program ( 2121HZ231-8 ). The Central Guidance for Local Scientific and Technological Development Funds of China (No. 2022FRD05017 ).

Keywords

Ba doping
CO adsorption capacity
CO methanation
DFT calculations
Nanofiber

Access to Document

10.1016/j.cej.2024.154872

Cite this

@article{50ec2b3e92524844b29a2ddece281fe2,

title = "Ba2+ doping into Ni/Al2O3 nanofibers promotes CO2 methanation via alkaline modulation",

abstract = "Ni-based catalysts are promising catalysts for CO2 methanation due to low lost. However, the activity and selectivity of Ni-based catalysts in CO2 methanation at low temperatures still need to be improved. Here, Ni4Al2BamOx (m = 0–0.5) nanofibers were prepared. Doping Ba2+ would increase alkaline sites and facilitate generating oxygen vacancies. Especially, Ni4Al2Ba0.2Ox exhibited the high specific surface area with 127.1 m2 g−1, being potential for exposing more active sites. Indeed, compared with undoped Ni4Al2Ox catalysts (CO2 conv. = 45 %, CH4 select. = 92 % at 300 °C), Ba2+ doping significantly improved activity (CO2 conv. = 74 %, CH4 select. = 99 % at 300 °C) and stability within 200 h for Ni4Al2Ba0.2Ox. Both EPR and O1S XPS confirmed that Ni4Al2Ba0.2Ox can form more oxygen vacancies and CO2-TPD confirmed that Ni4Al2Ba0.2Ox had stronger CO2 adsorption capacity compared to Ni4Al2Ox. In-situ infrared spectroscopy and DFT calculations both indicated that Ba2+ doping can promote generating surface hydroxyl groups and formate pathways.",

keywords = "Ba doping, CO adsorption capacity, CO methanation, DFT calculations, Nanofiber",

author = "Mengyuan Zhang and Xiaoyan Lu and Ying Qu and Chuandong He and Jiali Dong and Kongliang Luo and Jian Ye and Nana Lu and Qiang Niu and Pengfei Zhang and Sheng Dai",

note = "Publisher Copyright: {\textcopyright} 2024 Elsevier B.V.",

year = "2024",

month = oct,

day = "1",

doi = "10.1016/j.cej.2024.154872",

language = "English",

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T1 - Ba2+ doping into Ni/Al2O3 nanofibers promotes CO2 methanation via alkaline modulation

AU - Zhang, Mengyuan

AU - Lu, Xiaoyan

AU - Qu, Ying

AU - He, Chuandong

AU - Dong, Jiali

AU - Luo, Kongliang

AU - Ye, Jian

AU - Lu, Nana

AU - Niu, Qiang

AU - Zhang, Pengfei

AU - Dai, Sheng

PY - 2024/10/1

Y1 - 2024/10/1

N2 - Ni-based catalysts are promising catalysts for CO2 methanation due to low lost. However, the activity and selectivity of Ni-based catalysts in CO2 methanation at low temperatures still need to be improved. Here, Ni4Al2BamOx (m = 0–0.5) nanofibers were prepared. Doping Ba2+ would increase alkaline sites and facilitate generating oxygen vacancies. Especially, Ni4Al2Ba0.2Ox exhibited the high specific surface area with 127.1 m2 g−1, being potential for exposing more active sites. Indeed, compared with undoped Ni4Al2Ox catalysts (CO2 conv. = 45 %, CH4 select. = 92 % at 300 °C), Ba2+ doping significantly improved activity (CO2 conv. = 74 %, CH4 select. = 99 % at 300 °C) and stability within 200 h for Ni4Al2Ba0.2Ox. Both EPR and O1S XPS confirmed that Ni4Al2Ba0.2Ox can form more oxygen vacancies and CO2-TPD confirmed that Ni4Al2Ba0.2Ox had stronger CO2 adsorption capacity compared to Ni4Al2Ox. In-situ infrared spectroscopy and DFT calculations both indicated that Ba2+ doping can promote generating surface hydroxyl groups and formate pathways.

AB - Ni-based catalysts are promising catalysts for CO2 methanation due to low lost. However, the activity and selectivity of Ni-based catalysts in CO2 methanation at low temperatures still need to be improved. Here, Ni4Al2BamOx (m = 0–0.5) nanofibers were prepared. Doping Ba2+ would increase alkaline sites and facilitate generating oxygen vacancies. Especially, Ni4Al2Ba0.2Ox exhibited the high specific surface area with 127.1 m2 g−1, being potential for exposing more active sites. Indeed, compared with undoped Ni4Al2Ox catalysts (CO2 conv. = 45 %, CH4 select. = 92 % at 300 °C), Ba2+ doping significantly improved activity (CO2 conv. = 74 %, CH4 select. = 99 % at 300 °C) and stability within 200 h for Ni4Al2Ba0.2Ox. Both EPR and O1S XPS confirmed that Ni4Al2Ba0.2Ox can form more oxygen vacancies and CO2-TPD confirmed that Ni4Al2Ba0.2Ox had stronger CO2 adsorption capacity compared to Ni4Al2Ox. In-situ infrared spectroscopy and DFT calculations both indicated that Ba2+ doping can promote generating surface hydroxyl groups and formate pathways.

KW - Ba doping

KW - CO adsorption capacity

KW - CO methanation

KW - DFT calculations

KW - Nanofiber

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