Electron-deficient nickel tailored by boron for coke-free methane dry reforming

Abstract
Methane dry reforming (MDR) converts two major greenhouse gases (CO2 and CH4) into syngas (H2/CO) for synthesizing fuels and chemicals, which provides a process both economically viableand environmentally friendly, aligning with the goal of carbon neutrality. Ni is the most efficient andeconomic non-noble active metal for MDR but often suffers from deactivation caused by sintering orcoking due to the fast C-H activation but sluggish carbon removal. Herein, we reporta rather stableNi catalyst (Nin) derived from electrostatic-driven self- assembled 2D composites, which offered acoke-free manner for a prolonged stability (over 350 h) under typical MDR conditions. This outper-formed catalyst featured with homogeneously distributed spherical Ni nanoparticles (~6 nm) stabi-lized within mixed-oxide matrix. Partially electron-deficient Ni species are tailored by surroundedboron species through the Ni-0-B structure, which hindered the last C-H bond cleavage of methaneand accelerated CO2 reactivity, thus balancing elementary steps to enable a coke-free operation. It marks an important step forward for C-H bond manipulation and inspires material design in other applications.