Methane/natural gas is an alternative feedstock to produce fuels, chemicals and electricity, but its use is limited by the profitability of the processes and transportation expenses. Currently, indirect methane reforming processes are used industrially, with nickel-based catalysts, at aggressive operating conditions. As such, the catalysts suffer from poor stability due to coking. Herein, we review quantum mechanical density functional theory (DFT)-based investigations in surface carbon formation and its destruction reactions on nickel. A summary of how nickel-based bimetallics and transition metal oxide supported nickel catalysts influence the energetics of these stability-related reactions is also provided. Next, we discuss the main challenges associated with the accuracy and scalability of DFT computations. Finally, we explore perspectives for catalytic methane conversion processes.

甲烷/天然气是生产燃料，化学药品和电力的替代原料，但其使用受到工艺利润和运输费用的限制。目前，工业上使用镍基催化剂的间接甲烷重整工艺是在苛刻的操作条件下进行的。这样，由于焦化，催化剂的稳定性差。本文中，我们回顾了基于量子力学密度泛函理论（DFT）的表面碳形成及其对镍的破坏反应的研究。还概述了镍基双金属化合物和过渡金属氧化物负载的镍催化剂如何影响这些与稳定性相关的反应的能量。接下来，我们讨论与DFT计算的准确性和可伸缩性相关的主要挑战。最后，