(296h) One Step, Steady State Catalytic Conversion of Methane to Methanol Using Copper Zeolites: Kinetics and Site Requirements

Authors: 
Sullivan, M., Massachusetts Institute of Technology
Meyer, R., ExxonMobil Research and Engineering
Dinh, K., Massachusetts Institute of Technology
Román-Leshkov, Y., Massachusetts Institute of Technology
Serna, P., ExxonMobil
Abundant stores of natural gas have driven desire for effective utilization of CH4 within the current petrochemical infrastructure. Methane-derived methanol production typically proceeds through a high temperature (~1173 K), energy-intensive two step upgrading process. This work demonstrates a low temperature (~493 – 573 K), single step, steady state methanol production process over copper-based zeolitic catalysts. We utilize transient and steady state kinetic measurements as well as in situ titration in conjunction with infrared spectroscopic experiments in order to propose a C-H activation mechanism, subsequent conversion pathways, and reaction energetics as well as providing methods to identify and quantify active site motifs. The current work represents the first kinetic investigation and characterization of Cu-based catalysts for the steady state conversion of methane to methanol in zeolitic catalysts.