单钯原子对氧加氢生成羟基具有高活性和选择性。

High activity and selectivity of single palladium atom for oxygen hydrogenation to HO.

作者信息

Yu Shiming, Cheng Xing, Wang Yueshuai, Xiao Bo, Xing Yiran, Ren Jun, Lu Yue, Li Hongyi, Zhuang Chunqiang, Chen Ge

机构信息

Beijing Key Laboratory for Green Catalysis and Separation, Faculty of Environment and Life, Beijing University of Technology, Beijing, 100124, P. R. China.

Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100124, P. R. China.

出版信息

Nat Commun. 2022 Aug 12;13(1):4737. doi: 10.1038/s41467-022-32450-6.

Nanosized palladium (Pd)-based catalysts are widely used in the direct hydrogen peroxide (HO) synthesis from H and O, while its selectivity and yield remain inferior because of the O-O bond cleavage from both the reactant O and the produced HO, which is assumed to have originated from various O adsorption configurations on the Pd nanoparticles. Herein, single Pd atom catalyst with high activity and selectivity is reported. Density functional theory calculations certify that the O-O bond breaking is significantly inhibited on the single Pd atom and the O is easier to be activated to form *OOH, which is a key intermediate for HO synthesis; in addition, HO degradation is shut down. Here, we show single Pd atom catalyst displays a remarkable HO yield of 115 mol/g/h and HO selectivity higher than 99%; while the concentration of HO reaches 1.07 wt.% in a batch.

纳米钯（Pd）基催化剂广泛应用于由氢气（H₂）和氧气（O₂）直接合成过氧化氢（H₂O₂）的反应中，然而由于反应物O₂以及生成的H₂O₂中O-O键的断裂，其选择性和产率仍然较低，据推测这源于Pd纳米颗粒上各种O的吸附构型。在此，报道了具有高活性和选择性的单原子Pd催化剂。密度泛函理论计算证明，在单原子Pd上O-O键的断裂受到显著抑制，且O更容易被活化形成*OOH，这是H₂O₂合成的关键中间体；此外，H₂O₂的降解也被抑制。在此，我们展示了单原子Pd催化剂具有115 mol/g/h的显著H₂O₂产率以及高于99%的H₂O₂选择性；在间歇反应中，H₂O₂的浓度达到了1.07 wt.%。