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Department of Chemistry and Centre for Surface Analysis and Research, Hong
Kong Baptist University, Kowloon Tong, Hong Kong, China
Background
Methane is available in huge quantity, besides burning,
there are many way to utilize it .
catalyst
CO2 reforming :
CH4 + CO2 2CO +2H2
Steam reforming:
CH4 + H2O CO + 3H2
Synthesis gas
Synthesis gas
Coupling reaction:
CH4 + CH4 C2H6 + etc
Aromatization:
nCH4 C6H6 , C10H8 +
Background
Numerous studies on CH4/CO2 reforming reaction using
Ni-based catalysts.
cat.
Synthesis gas
Our studies:
Reverse water-gas shift (RWGS) reaction over La2NiO4
catalyst during CH4/CO2 reforming by continuous wave
cavity enhanced absorption spectroscopy (CEAS).
Associated
reaction:
CO2 + H2 CO + H2O
Experimental Conditions:
Catalyst:
Ni(NO3)2 6 H2O + HNO3 + La2O3 La2NiO4 +
50 mg La2NiO4 sol-gel-generated catalyst at >500 oC
Laser system:
Tunable diode laser: 1279-1341 nm, 5 mW
Linewidth: 5 MHz
High reflective mirror: R > 0.99995
Results
CEA spectra of CH4 and H2O obtained at different pulsing rate (of
CH4/CO2 reaction. (Temperature = 700 oC)
= H2 O
= CH4
2000 s
1500 s
1000 s
500 s
7510.5
7510.8
7511.1
7511.4
-1
Wavenumber (cm )
CH4
H2O
Absorption (cm-1)
7510.59 7511.20
Vibrational
transition
Rotational
210 310
J =0 (Q
branch)
7511.30
110 310
J = 5, Ka = 0, Kc= 5
J = 6, Ka = 2, Kc= 4
Results
CEA spectra of CH4 and H2O obtained at different pulsing rate (of
CH4/CO2 reaction. (Temperature = 700 oC)
= H2 O
= CH4
2000 s
1500 s
1000 s
500 s
7510.5
7510.8
7511.1
7511.4
-1
Wavenumber (cm )
CH4
H2 O
225 min
95 min
15 min
0 min
7510.6
7510.8
7511.0
7511.2
Wavenumber (cm
-1
7511.4
After long
reaction time,
deactivation of
catalyst
Results
(1) The conversion of CO2 over La2NiO4 catalyst was
nearly 8.0 % higher than that of methane,
attributable to the contribution of RWGS reaction:
CO2 + H2 CO + H2O
H = + 41 kJ/mol
(a)
(b)
CO2
CO
700 C
Signal
600 C
500 C
400 C
CO2
CO2
room temp.
6357.0
6357.5
6358.0
6358.5
Wavenumber /cm
-1
6359.0
6359.5