Atomically Dispersed Ni-Based Anti-Coking Catalysts for Methanol Dehydrogenation in a Fixed-Bed Reactor
Jing‐Tan Han, Zhong‐Hua Xue, Ke Zhang, Honghui Wang, Xin‐Hao Li, Jie‐Sheng Chen
Abstract
Transition metal-based catalysts usually suffer from poor coke resistance during the dehydrogenation processes of hydrocarbon compounds in gas–solid heterogeneous systems, including methanol dehydrogenation. Herein, atomically dispersed Ni sites have been rationally anchored in nitrogen-doped carbon sheets (Ni–N4/NC), which could act as an integrated, active, and anticoking catalyst for methanol dehydrogenation with a high selectivity toward hydrogen and CO under 15 h–1 (weight hourly space velocities, WHSV) in a fixed-bed reactor. Both experimental and computational results reveal that the electronic structures of Ni–N4 sites promote the desorption of deep dehydrogenation product ethylene to release the Ni active centers, simultaneously giving a remarkably high H2 yield rate (1800 mol H2 mol–1 Ni h–1) and a high anticoking performance even under critical conditions.