最近，张安琪同学硕士期间的工作，题为“Microenvironmental Regulation of PdCo Nanoclusters in Mesoporous Carbon Enhances Hydrogen Production from Formic Acid”发表在催化顶级期刊Applied Catalysis B: Environment and Energy（IF=20.3）。
摘要：
Formic acid (FA, HCOOH), a valuable liquid product of biomass processes and CO2 hydrogenation, has regarded as a promising liquid organic hydrogen carrier for renewable energy systems. However, developing highly efficient catalysts for additive-free FA dehydrogenation (FAD) is urgently desirable but extremely challenging. Herein, PdCo nanoclusters (0.85 nm) with modulated microenvironment by amino-functionalized oxidized mesoporous carbon (PdCo/NOMC) are successfully prepared for robust hydrogen (H2) from FA. The as-prepared PdCo/NOMC exhibits excellent catalytic performance with 100% H2 selectivity and an ultrahigh turnover frequency (TOF) value of 9815 h-1 for FAD at 323 K. Kinetic isotope effect (KIE) investigations and density functional theory (DFT) calculations clearly show that the dissociation of C-H bonds in FAD is more difficult than that of O-H bonds on PdCo catalyst. DFT calculations further demonstrate that H2 desorption is being the rate-determining step of FAD, and the strong electronic coupling between metal Pd and Co is favorable for the O-H bond dissociation, C-H bond cleavage, and H2 desorption during FAD. This work not only guides the fabrication of functional nanocluster catalysts, but also catches the insight reaction mechanism of FAD.