Metallic nickel exsolved from a two-dimensional MWW-type zeolitic nickel silicate: An effective catalyst for ammonia decomposition

Abstract

Exsolution of active species from metal oxide materials is an effective strategy for preparing a highly active and stable catalyst. Here, we prepared two-dimensional nickel (Ni) silicate material with delaminated MWW layers (Ni-DMLs) by hydrothermal treatment of borosilicate MWW precursor (B-MWW(P)) with Ni nitrate solutions and applied on the catalytic decomposition of ammonia (NH3) via exsolution. The layered B-MWW(P) was transformed to a three-dimensional (3D) tectosilicate MWW, a two-dimensional (2D) Ni-DML, and a 2D phyllosilicate structures at temperature regions of 100–120 °C, 140–160 °C, and 170–180 °C, respectively. Meanwhile, the Ni contents on the samples increased from 3.6 to 37.6 wt.% as the hydrothermal temperature increased from 100 to 180 °C, owing to the substitution of framework B by Ni. The chemical state of Ni on each sample was characterized by various analytical tools and correlated with their catalytic properties of NH3 decomposition over the exsolved metallic Ni species. The NH3 decomposition over Ni-DMLs was evaluated in the temperature range of 300–600 °C, and the apparent activation energies were compared. The Ni-DML-160 exhibited the best catalytic activity, achieving an NH3 conversion of 70% at 500 °C and maintained 90% to initial conversion during 100 h on stream at 550 °C. The synergistic effect of the strong interaction between the exsolved metallic Ni and the zeolite support and the 2D nature of Ni-DMLs relieved the catalytic deactivation by sintering and coking, respectively.