Novel nickel‐based catalyst for low temperature hydrogen production from methane steam reforming in membrane reformer

Abstract

Hydrogen production from various hydrocarbon fuels, particularly biomass-derived fuels, has attracted worldwide attention due to its potential for application to fuel cells, a device which converts chemical energy into electricity efficiently and cleanly. However, current technology, such as natural gas steam reforming, could not meet the specific requirements of hydrogen for fuel cells. Therefore, novel processes are intensively investigated, aiming to develop economic and efficient ones for the specific purpose. An important direction is the integrated membrane reformer for one-step high-purity hydrogen production. However, for the commercial realization of this technology, there are still some difficulties to overcome. By comparison with previous investigations with a similar membrane, this work showed that catalyst also played an important role in determining membrane reformer performance. We proposed that when thickness of membrane was several micrometers, the permeance of membrane became less important than the kinetics of catalyst, due to the fact that under such conditions, hydrogen permeation rate was faster than the kinetics of steam reforming reaction when commercial catalyst was applied, but further evidence is indispensable. In this initial work, we focused on developing efficient nickel catalyst for low temperature steam reforming. Nickel-based catalyst was developed by deposition-coprecipitation and used as pre-reduced, showing high performance for methane steam reforming at low temperatures and good durability, which may find practical application for the integrated membrane reforming process. 

Supported nickel catalysts for low temperature methane steam reforming: comparison between metal additives and support modification

“…The main reason for the development of new classes of low temperature steam reforming catalysts is the increasing interest in proton exchanged membrane (PEM) fuel cells, as the most appropriate power source for future generation vehicles [5]. These fuel cells operate with on site generated hydrogen by hydrocarbon or oxygenated organics reforming technologies in a membrane reformer [6][7][8]. High reforming temperatures can damage the thin Pd membrane and increase the total cost of the produced hydrogen.…”

“…High reforming temperatures can damage the thin Pd membrane and increase the total cost of the produced hydrogen. Previous studies of low temperature MSR on nickel considered various catalysts: impregnated Ni/Al 2 O 3 , Ni/SiO 2 , Ni/ZrO 2 calcined at 700°C [9], Ni supported on Mg-La-Al mixed oxides prepared by coprecipitation-deposition and calcined at 900°C [7], Ni supported on Ce x Zr 1-x O 2 prepared by impregnation and calcined at 500°C [10]. The reaction temperatures were between 500 and 600°C and methane conversion at 500°C ranged from 10% for Ni/Ce 0.15 Zr 0.85 O 2 [10] to 25% for Ni/ZrO 2 [9].…”

High-Temperature Stability and Saturation Magnetization of Superparamagnetic Nickel Nanoparticles in Microporous Polysilazane-Derived Ceramics and their Gas Permeation Properties

“…In other words, a reason for the more pronounced enhancement in the hydrogen permeance at 300 °C compared to that of 25 °C after hydrothermal treatment could be related to the well-known hydrogen affinity of the metal nickel. − …”

Computational study of Pd-membrane CH4 steam reformer with fixed catalyst bed: Searching for a way to increase membrane efficiency

“…In order to overcome transport limitations and increase membrane efficiency a novel type of structured catalyst support, called CCFS [27] was incorporated in the MR model. The separation plate between the corrugated sheets in CCFS catalyst direct the fluid flow Gallucci et al [12] Fluidized-bed Roses et al [13] Tube-in-tube Chen et al [8,9] Tube-in-tube i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 9 ( 2 0 1 4 ) 2 0 0 7 2 e2 0 0 9 3 more efficiently between the heated wall and the membrane to improve overall heat and mass transfer coefficients. Inside the packing almost ideal transversal mixing is realized due to the monolithic type channels.…”

“…Hydrogen transport balance at the membrane: b W p m RT g $10 5 À P H 2 ;gap À P H 2 ;mbr Á ¼ p m J H 2 (9) The membrane parameters used to define J H 2 are provided in Table 2. Terms accounting for equilibrium:…”