Nickel-lanthanum oxide catalyst for methane dry reforming and preparation method thereof

Abstract

The invention relates to a nickel-lanthanum oxide catalyst for methane dry reforming, the active component of the catalyst is metal Ni, the carrier is La2O3, and an obvious Ni-La interface is formed between the active component and the carrier; the weight percentage of the active component Ni is 1.0-5.0%, and the size of Ni nano-particles is about 20 nm; and the weight percentage of the carrier La2O3 is 95.0 to 99.0 percent. Meanwhile, the invention also discloses a preparation method of the catalyst. The catalyst shows very high catalytic stability, so that the problems of high-temperature sintering and carbon deposition of active components are effectively solved.

Description

technical field

[0001] The invention relates to the technical field of heterogeneous catalysis, in particular to a nickel-lanthanum oxide catalyst for dry reforming of methane and a preparation method thereof. Background technique

[0002] Methane dry reforming is the simultaneous conversion of two very stable carbon-one molecule CH 4 and CO 2 for syngas (CO and H 2 )the process of. Therefore, from a theoretical perspective, this reaction is a very challenging and important research topic in carbon-chemistry. From a practical point of view, this process is not only an important process for natural gas conversion, but also a large-scale chemical utilization of CO 2 Therefore, it is of great practical significance to alleviate the energy crisis and improve the living environment of human beings.

[0003] At present, the catalysts used for this reaction can be classified into two categories: noble metals and non-precious metals, among which non-precious metal Ni-based cata...

Examples

Embodiment 1

[0032] Carrier preparation: In a 1 L beaker, 13 g La (NO 3 ) 3 ·6H 2 O was dissolved in 200 mL of water with stirring, and then 1.0 mol·L was added dropwise. -1 NH 4 HCO 3 The precipitant adjusts the pH of the mixed slurry to 8.0. After continuing to stir for 0.5 h, the reactant was filtered and washed until the pH of the filtrate was 7.0, dried in an oven at 120 °C overnight, and finally calcined in a muffle furnace at 600 °C for 2.0 h to obtain the catalyst carrier La 2 O 2 CO 3 ;

[0033] Catalyst preparation: 3.0 g of the above La was added to a 50 mL crucible under infrared light irradiation 2 O 2 CO 3 carrier, weigh 0.30g Ni (NO 3 ) 2 ·6H 2 O was dissolved in 7 mL of water to obtain a precursor solution. The precursor solution was added to the crucible and immersed while stirring. After the solvent was evaporated to dryness, it was dried in an oven at 120 °C overnight, and calcined in a muffle furnace at 750 °C for 2.0 h. in tube furnace H 2 / N 2 (volume...

Embodiment 2

[0035] Carrier preparation: In a 1 L beaker, at room temperature (around 25 °C), 24 g La (CH 3 COO) 3 ·5H 2 O was dissolved in 200 mL of water with stirring, and then 0.5 mol L was added dropwise. -1 NH 3 ·H 2 O precipitant adjusts the pH of the mixed slurry to 8.0. After stirring for 0.5 h, the reactant was filtered and washed until the pH of the filtrate was 7.0, dried in an oven at 120 °C overnight, and finally calcined in a muffle furnace at 600 °C for 3.0 h to obtain the catalyst carrier La 2 O 2 CO 3 ;

[0036] Catalyst preparation: 3.0 g of the above La was added to a 50 mL crucible under infrared light irradiation 2 O 2 CO 3 carrier, weigh 0.40g Ni (CH 3 COO) 2 ·4H 2 O was dissolved in 7 mL of water to obtain a precursor solution. The precursor solution was added to the crucible and immersed while stirring. After the solvent was evaporated to dryness, it was dried in an oven at 120 °C overnight, and calcined in a muffle furnace at 800 °C for 2.0 h. in tu...

Embodiment 3

[0038] Carrier preparation: In a 1 L beaker, add 10 g LaCl at room temperature (around 25 °C) 3 Stir to dissolve in 200 mL of water, and then dropwise add 2.0 mol L -1 (NH 4 ) 2 CO 3 The precipitant adjusts the pH of the mixed slurry to 9.0. After continuing to stir for 0.5 h, the reactant was filtered and washed until the pH of the filtrate was 7.0, dried in an oven at 120 °C overnight, and finally calcined in a muffle furnace at 600 °C for 4.0 h to obtain the catalyst carrier La 2 O 2 CO 3 ;

[0039] Catalyst preparation: 3.0 g of the above La was added to a 50 mL crucible under infrared light irradiation 2 O 2 CO 3 Carrier, weigh 0.43g NiCl 2 ·6H 2 O was dissolved in 7 mL of water to obtain a precursor solution. The precursor solution was added to the crucible and immersed while stirring. After the solvent was evaporated to dryness, it was dried in an oven at 120 °C overnight, and calcined in a muffle furnace at 600 °C for 2.0 h. in tube furnace H 2 / N 2 (vol...

technical field

[0001] The invention relates to the technical field of heterogeneous catalysis, in particular to a nickel-lanthanum oxide catalyst for dry reforming of methane and a preparation method thereof. Background technique

[0002] Methane dry reforming is the simultaneous conversion of two very stable carbon-one molecule CH 4 and CO 2 for syngas (CO and H 2 )the process of. Therefore, from a theoretical perspective, this reaction is a very challenging and important research topic in carbon-chemistry. From a practical point of view, this process is not only an important process for natural gas conversion, but also a large-scale chemical utilization of CO 2 Therefore, it is of great practical significance to alleviate the energy crisis and improve the living environment of human beings.

[0003] At present, the catalysts used for this reaction can be classified into two categories: noble metals and non-precious metals, among which non-precious metal Ni-based cata...

Examples

Embodiment 1

[0032] Carrier preparation: In a 1 L beaker, 13 g La (NO 3 ) 3 ·6H 2 O was dissolved in 200 mL of water with stirring, and then 1.0 mol·L was added dropwise. -1 NH 4 HCO 3 The precipitant adjusts the pH of the mixed slurry to 8.0. After continuing to stir for 0.5 h, the reactant was filtered and washed until the pH of the filtrate was 7.0, dried in an oven at 120 °C overnight, and finally calcined in a muffle furnace at 600 °C for 2.0 h to obtain the catalyst carrier La 2 O 2 CO 3 ;

[0033] Catalyst preparation: 3.0 g of the above La was added to a 50 mL crucible under infrared light irradiation 2 O 2 CO 3 carrier, weigh 0.30g Ni (NO 3 ) 2 ·6H 2 O was dissolved in 7 mL of water to obtain a precursor solution. The precursor solution was added to the crucible and immersed while stirring. After the solvent was evaporated to dryness, it was dried in an oven at 120 °C overnight, and calcined in a muffle furnace at 750 °C for 2.0 h. in tube furnace H 2 / N 2 (volume...

Embodiment 2

[0035] Carrier preparation: In a 1 L beaker, at room temperature (around 25 °C), 24 g La (CH 3 COO) 3 ·5H 2 O was dissolved in 200 mL of water with stirring, and then 0.5 mol L was added dropwise. -1 NH 3 ·H 2 O precipitant adjusts the pH of the mixed slurry to 8.0. After stirring for 0.5 h, the reactant was filtered and washed until the pH of the filtrate was 7.0, dried in an oven at 120 °C overnight, and finally calcined in a muffle furnace at 600 °C for 3.0 h to obtain the catalyst carrier La 2 O 2 CO 3 ;

[0036] Catalyst preparation: 3.0 g of the above La was added to a 50 mL crucible under infrared light irradiation 2 O 2 CO 3 carrier, weigh 0.40g Ni (CH 3 COO) 2 ·4H 2 O was dissolved in 7 mL of water to obtain a precursor solution. The precursor solution was added to the crucible and immersed while stirring. After the solvent was evaporated to dryness, it was dried in an oven at 120 °C overnight, and calcined in a muffle furnace at 800 °C for 2.0 h. in tu...

Embodiment 3

[0038] Carrier preparation: In a 1 L beaker, add 10 g LaCl at room temperature (around 25 °C) 3 Stir to dissolve in 200 mL of water, and then dropwise add 2.0 mol L -1 (NH 4 ) 2 CO 3 The precipitant adjusts the pH of the mixed slurry to 9.0. After continuing to stir for 0.5 h, the reactant was filtered and washed until the pH of the filtrate was 7.0, dried in an oven at 120 °C overnight, and finally calcined in a muffle furnace at 600 °C for 4.0 h to obtain the catalyst carrier La 2 O 2 CO 3 ;

[0039] Catalyst preparation: 3.0 g of the above La was added to a 50 mL crucible under infrared light irradiation 2 O 2 CO 3 Carrier, weigh 0.43g NiCl 2 ·6H 2 O was dissolved in 7 mL of water to obtain a precursor solution. The precursor solution was added to the crucible and immersed while stirring. After the solvent was evaporated to dryness, it was dried in an oven at 120 °C overnight, and calcined in a muffle furnace at 600 °C for 2.0 h. in tube furnace H 2 / N 2 (vol...

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