Abstract
The transition metal nanocatalysts containing disordered active sites can potentially achieve efficient Sabatier reactions with high selectivity. However, it remains a challenge to maintain the stability of these active sites in such an exothermic reaction. Here, a thermal management approach is reported to address this challenge. Specifically, an efficient and stable catalytic system is developed by integrating urchin-like Ru nanoparticles with disordered active sites (d-RuNUs) and multi-walled carbon nanotubes (MWCNTs) as heat transfer framework, which achieves a CH(4) yield of 3.3 mol g(-1) h(-1) with nearly 100% selectivity in 12 h. The characterizations reveal that the thermal-induced crystallization seriously weakens the adsorption of CO(2), leading to significant degradation of catalytic performance. The heat transfer simulation confirms that the MWCNTs with high thermal conductivity play a key role in rapidly redistributing the reaction heat, thereby preventing the crystallization of disordered structures. This work elucidates the deactivation mechanism of disordered active sites in exothermic reactions and opens the avenue for local thermal management of non-thermal equilibrium reactions.