The cognition of active sites in the Ni-based catalysts plays a vital role and remains a huge challenge in improving catalytic performance of low temperature CO
2
dry reforming of methane (LTDRM). In this work
typical catalysts of SiO
2
and
γ
-Al
2
O
3
supported Ni and Ni-Ce were designed and prepared. Importantly
the difference in the chemical speciations of active sites on the Ni-based catalysts is revealed by advanced characterizations and further estimates respective catalytic performance for LTDRM. Results show that larger[Ni
n
0
]
particles mixed with [Ni-O-Si
n
]
) species on the Ni/SiO
2
(R) make CH
4
excessive decomposition
leading to poor activity and stability. Once the Ce species is doped
however
superior activity (59.0% CH
4
and 59.8% CO
2
conversions)
stability and high H
2
/CO ratio (0.96) at 600?℃ can be achieved on the Ni-Ce/SiO
2
(R)
in comparison with other catalysts and even reported studies. The improved performance can be ascribed to the formation of integral ([Ni
n
0
]
-[Ce
III
-□-Ce
III
]
) species on the Ni-Ce/SiO
2
(R) catalyst
containing highly dispersed [Ni
n
0
]
particles and rich oxygen vacancies
which can synergistically establish a new stable ba
lance between gasification of carbon species and CO
2
dissociation. With respect to Ni-Ce/
γ
-Al
2
O
3
(R)
the Ni and Ce precursors are easily captured by extra-framework Al
n
-OH groups and further form stable isolated ([Ni
n
0
]
-[Ni-O-Al
n
]
) and [Ce
III
-O-Al
n
]
species. In such a case
both of them preferentially accelerate CO
2
adsorption and dissociation
causing more carbon deposition due to the disproportionation of superfluous CO product. This deep distinguishment of chemical speciations of active sites can guide us to further develop new efficient Ni-based catalysts for LTDRM in the future.
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Related Author
Shasha Feng
Mengdi Zhou
Feng Han
Zhaoxiang Zhong
Weihong Xing
Related Institution
State Key Laboratory of Materials-Oriented Chemical Engineering, National Engineering Research Center for Special Separation Membrane, Nanjing Tech University
Nanjing Industrial Technology Research Institute of Membrane Material Co. Ltd.