Ni-based catalysts derived from Ni-Zr-Al ternary hydrotalcites show outstanding catalytic properties for low-temperature CO₂ methanation

TY - JOUR

T1 - Ni-based catalysts derived from Ni-Zr-Al ternary hydrotalcites show outstanding catalytic properties for low-temperature CO2 methanation

AU - He, Feng

AU - Zhuang, Jiahao

AU - Lu, Bin

AU - Liu, Xianglin

AU - Zhang, Jianling

AU - Gu, Fangna

AU - Zhu, Minghui

AU - Xu, Jing

AU - Zhong, Ziyi

AU - Xu, Guangwen

AU - Su, Fabing

N1 - Publisher Copyright: © 2021 Elsevier B.V.

PY - 2021/9/15

Y1 - 2021/9/15

N2 - Developing Ni-based catalysts with high activity and stability in low-temperature methanation is necessary due to their sintering and coking at high temperatures. Here, we report our developed novel Ni-Zr-Al catalysts derived from Ni-Zr-Al ternary hydrotalcites synthesized by a hydrothermal process, followed by a reduction in hydrogen. Comparing with the Ni-Al catalyst derived from Ni-Al hydrotalcite and the commercial Ni-based catalyst, the Ni-Zr-Al catalysts show a remarkably higher low-temperature activity (210−270 °C) in CO2 methanation. Both the experimental and theoretical calculations confirmed the introduction of Zr into the Ni-Al binary hydrotalcite could generate synergetic effects between Ni and ZrO2, resulting in more surface oxygen vacancies, basic sites, and abundant mesopores. In-situ DRIFTS analysis showed the CO2 methanation to CH4 follows the intermediate formate route. This work provides a new theoretical understanding of CO2 activation and methanation, and a practical way to address the existing problem for Ni-based catalysts.

AB - Developing Ni-based catalysts with high activity and stability in low-temperature methanation is necessary due to their sintering and coking at high temperatures. Here, we report our developed novel Ni-Zr-Al catalysts derived from Ni-Zr-Al ternary hydrotalcites synthesized by a hydrothermal process, followed by a reduction in hydrogen. Comparing with the Ni-Al catalyst derived from Ni-Al hydrotalcite and the commercial Ni-based catalyst, the Ni-Zr-Al catalysts show a remarkably higher low-temperature activity (210−270 °C) in CO2 methanation. Both the experimental and theoretical calculations confirmed the introduction of Zr into the Ni-Al binary hydrotalcite could generate synergetic effects between Ni and ZrO2, resulting in more surface oxygen vacancies, basic sites, and abundant mesopores. In-situ DRIFTS analysis showed the CO2 methanation to CH4 follows the intermediate formate route. This work provides a new theoretical understanding of CO2 activation and methanation, and a practical way to address the existing problem for Ni-based catalysts.

KW - CO methanation

KW - High performance

KW - Mechanism

KW - Ni-Zr-Al hydroxides

KW - Ni-based catalyst

UR - http://www.scopus.com/inward/record.url?scp=85104661817&partnerID=8YFLogxK

U2 - 10.1016/j.apcatb.2021.120218

DO - 10.1016/j.apcatb.2021.120218

M3 - 文章

AN - SCOPUS:85104661817

SN - 0926-3373

VL - 293

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

M1 - 120218

ER -