Process of preparing high purity hydrogen with liquid hydrocarbon in a palladium film reactor

A liquid hydrocarbon and reactor technology, which is applied in the field of producing high-purity hydrogen in a high-performance composite metal palladium membrane reactor, can solve the problems of high hydrogen selectivity and low methane selectivity, and achieve the effect of avoiding methanation reaction

Inactive Publication Date: 2007-03-21
DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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Problems solved by technology

However, the use of Ni-based catalysts with high activity at low temperatures enables the conversion of liquid hydrocarbons to be close to 100% at low temperatures and high space velocities, and the use of high-performance composite metal palladium membranes enables the steam reforming of liquid hydrocarbons to generate The hydrogen is separated in time to avoid the occurrence of methanation reaction, so as to obtain lower methane selectivity and higher hydrogen selectivity.

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  • Process of preparing high purity hydrogen with liquid hydrocarbon in a palladium film reactor

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Embodiment 1

[0028] With Ni(NO 3 ) 2 ·6H 2 O and Al(NO 3 ) 3 9H 2 O is the raw material, using (NH 4 ) 2 CO 3 As a precipitating agent, the temperature of the two solutions is controlled at room temperature for co-precipitation, and the pH is maintained at 8.0-8.5 during the precipitation process. After the precipitation is completed, it is aged for 2 hours, then washed, dried at 120 ° C, and roasted at 600 ° C for 4 hours. Control the NiO content in the catalyst at 40wt%, Al 2 o 3 is 60wt%. Take 5.5 g of the above catalyst, dilute it with quartz sand, and put it into a palladium membrane reactor with a bed height of 100 mm. The hydrogen permeation rate of the selected composite metal membrane is 52m 3 m -2 bar -1 h -1 , H 2 / N 2The separation factor is above 10,000. Using 6# solvent oil produced in Daqing as raw material, the fuel injection rate is 0.34ml / min, and the water injection rate is 0.80ml / min. The reaction was carried out at 550°C and 1.1 MPa, and the purge gas...

Embodiment 2

[0030] With Ni(NO 3 ) 2 ·6H 2 O, Al(NO 3 ) 3 9H 2 O and La(NO 3 ) 3 ·6H 2 Ni / La-Al prepared by co-precipitation method with O as raw material 2 o 3 Catalyst to NH 3 ·H 2 O is a precipitating agent, and the pH of the precipitation process is controlled to be about 8.0. After the precipitation process is completed, it is aged for 1 hour, washed by centrifugation, then dried at 120°C, and roasted at 600°C for 4 hours to prepare a composition of 50wt% NiO and 42wt% Al 2 o 3 , and 8 wt% La 2 o 3 catalyst. In a conventional fixed-bed reactor, using isooctane as a raw material, the performance of the catalyst was measured at 450°C, 500°C, and 550°C respectively. During the reaction, S / C=2.73 and pressure P=0.8MPa. The results in Table 1 show that the prepared catalyst has good low-temperature steam reforming activity, even if the carbon space velocity is as high as 30,000h -1 , at the temperature of 450°C, 500°C and 550°C, the conversion rate of liquid hydrocarbons ca...

Embodiment 3

[0034] With Ni(NO 3 ) 2 ·6H 2 O, Al(NO 3 ) 3 9H 2 O and Mg(NO 3 ) 2 ·6H 2 O is the raw material, using (NH 4 ) 2 CO 3 As a precipitant, control the temperature of the two solutions at room temperature for co-precipitation, maintain the pH at 8.0-8.5 during the precipitation process, age for 2 hours after the precipitation, then wash, dry at 120 ° C, and roast at 700 ° C for 4 hours. The composition of the catalyst is 36 wt% NiO, 12 wt% MgO and 52 wt% Al 2 o 3 , the prepared catalyst was crushed and sieved after being pressed into tablets, and Ni / MgO-Al with a particle size of 420-630 μm was taken 2 o 3 5.5g of the catalyst was diluted with quartz sand and loaded into a palladium membrane reactor with a bed height of 100mm. The hydrogen permeation rate of the selected composite metal membrane is 65m 3 m -2 bar -1 h -1 , H 2 / N 2 The separation factor is above 10,000. Using isooctane as a raw material, the carbon space velocity of the reaction in liquid hydr...

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Abstract

The process of preparing high purity hydrogen with liquid hydrocarbon in a palladium film reactor adopts Ni base catalyst with high activity at low temperature to obtain liquid hydrocarbon converting rate near 100 % at the conditions of 450-550 deg.c temperature and carbon space velocity as high as 30,000/hr, and uses high performance composite metal palladium film simultaneously at the conditions of 500-600 deg.c temperature and carbon space velocity as high as 2000/hr for timely separating hydrogen generated through water vapor reformation of liquid hydrocarbon to avoid methanation reaction, so as to obtain methane selectivity lower than 3 % and hydrogen selectivity higher than 97 % and obtain high pure hydrogen in the permeation side of the palladium film. The present invention has low hydrogen producing cost and may be used widely in hydrogen refilling station and small dispersed power station.

Description

technical field [0001] The invention relates to a method for preparing high-purity hydrogen from liquid hydrocarbons in a palladium membrane reactor. Specifically, a Ni-based hydrocarbon steam reforming catalyst with high activity at low temperature is used in a high-performance composite metal palladium membrane. High-purity hydrogen is produced in the reactor. This method for producing high-purity hydrogen will be widely used in small-scale hydrogen production in hydrogen refueling stations and distributed power stations, and provide cheap hydrogen production technology for hydrogen refueling stations and distributed power stations. Background technique [0002] Energy shortage, low energy utilization efficiency and the resulting environmental pollution are becoming important constraints to the sustainable development of human society. Actively developing new energy and renewable energy is the fundamental way to solve energy problems. As a secondary energy carrier, hydro...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C01B3/26
Inventor 徐恒泳陈亚中王玉忠
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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