Development of Active and Stable Low Nickel Content Catalysts for Dry Reforming of Methane

Abstract

Methane dry reforming (DRM) was investigated over highly active Ni catalysts with low metal content (2.5 wt %) supported on Mg-Al mixed oxide. The aim was to minimize carbon deposition and metal sites agglomeration on the working catalyst which are known to cause catalyst deactivation. The solids were characterized using N 2 adsorption, X-ray diffraction, temperature-programmed reduction, X-ray photoelectron spectroscopy, and UV-Vis diffuse reflectance spectroscopy. The results showed that MgO-Al 2 O 3 solid solution phases are obtained when calcining Mg-Al hydrotalcite precursor in the temperature range of 550-800 • C. Such phases contribute to the high activity of catalysts with low Ni content even at low temperature (500 • C). Modifying the catalyst preparation with citric acid significantly slows the coking rate and reduces the size of large octahedrally coordinated NiO-like domains, which may easily agglomerate on the surface during DRM. The most effective Ni catalyst shows a stable DRM course over 60 h at high weight hourly space velocity with very low coke deposition. This is a promising result for considering such catalyst systems for further development of an industrial DRM technology.

Development of Highly Stable Low Ni Content Catalyst for Dry Reforming of CH4‐Rich Feedstocks

“…This effect is attributed to the presence of La that promotes the oxygen mobility and/or formation of defect structures where MgO is doped with Ni 2+ . On the other side,sample La.Ni(CA)/Mg 1.3 AlO x .1000 exposes the β peak at a temperature similar to that of La.Ni(CA)/Mg 1.3 AlO x and an additional split γ peak at very high temperature (980 °C) assigned to Ni in strong interaction with the support …”

“…[12,24] On the other side,sample La.Ni (CA)/Mg 1.3 AlO x .1000 exposes the β peak at a temperature similar to that of La.Ni(CA)/Mg 1.3 AlO x and an additional split γ peak at very high temperature (980°C) assigned to Ni in strong interaction with the support . [25] These β and γ Ni 2 + species are poorly reduced in usual pretreatment and therefore La.Ni(CA)/Mg 1.3 AlO x .1000 is only partially reduced before DRM. The Ni metal fraction after in situ reduction was evaluated in a two-step experiment: first, the reduction at 700°C was made, directly followed by a regular TPR experiment up to 1000°C.…”

Commemorative Issue in Honor of Professor Calvin H. Bartholomew’s 75th Birthday

“…Tu et al's contribution on palladium catalysts supported on titania for hydrogen peroxide production [16] also touches on themes of this metal and support in Dr. Bartholomew's work. Ha et al's paper on nickel catalysts for (dry) methane reforming and carbon deactivation [17] go back to Dr. Bartholomew's early work on both nickel and methane reforming. Türks et al's work on CO 2 methanation on nickel catalysts builds on these major themes of Dr. Bartholomew's research [18].…”

CO2 Reforming of Methane over LaNiO3 Perovskite Supported Catalysts: Influence of Silica Support

“…It is reported that the insertion of nickel into a well-defined structure, like the perovskites [8], hexaaluminates [9], spinels [10] or in a solid solutions [11], can reduce its deactivation. In dry reforming reaction, the active site is metallic transition metal [12].…”