Active Pd nanoclusters supported on nitrogen/amino co-functionalized carbon for highly efficient dehydrogenation of formic acid

Abstract

Supported noble metal catalysts have exhibited satisfactory catalytic performance in the dehydrogenation of liquid chemical hydrogen carriers, in which the supports play a paramount role in conditioning the nature of the active center and thus improving the overall reactivity. Herein, the specially designed nitrogen/amino co-functionalized carbon (NH2-NC) supports are prepared to load active Pd nanoclusters for efficient dehydrogenation of formic acid (FA). The nitrogen/amino co-functionalization of carbon not only facilitates the Pd nanoclusters evenly dispersed with a mean size of 1. 4 nm, but also provides a beneficial metal-support interaction to promote FA dehydrogenation. The as-prepared Pd@NH2-NC discloses a 100% conversion of FA into CO2 and H2 with a remarkable initial turnover frequency (TOFinitial) of 4,892 h-1 and a low activation energy (Ea) of 28.5 kJ mol-1 without additive at 298 K. The work proposes a co-functionalization strategy to reasonably design supports for heterogeneous catalysts and may be extended to develop other multi-functionalized supports with different compositions and nanostructures.