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

• DOI: 10.20517/cs.2023.13
• Publication Date: 2023-05-16T03:08:10Z
• Authors: Dan Liu; Cheng Zhou; Ge Wang; Yong Li; Zhimao Yang; Chuncai Kong; Ben Liu

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.