Carbonyl-anchored single-atom palladium achieved on waste printing paper-derived carbon material by impregnation method: remarkable performance in selective oxidation of benzyl alcohol

苯甲醛 苯甲醇 催化作用 吸附 化学 酒精氧化 X射线光电子能谱 选择性 金属 碳纤维 煅烧 无机化学 有机化学 材料科学 化学工程 复合数 复合材料 工程类
作者
Yongbo Zhou,Chaojie Ma,X. Wang,Zhonghua Xiang,Chun‐Yang Yin,Wei Yan,Wei He,Y. Liu,Chunshan Lu,X. Li
出处
期刊:Materials Today Chemistry [Elsevier BV]
卷期号:28: 101340-101340 被引量:10
标识
DOI:10.1016/j.mtchem.2022.101340
摘要

N element can form various forms of coordination with metals, so it is used in the preparation of single-atom catalysts widely. However, the strong coordination bond between N and metals will inhibit the catalytic activity of the metal atoms. In this work, the waste printing paper was used to prepare a new type of carbon material by calcining at high temperature in water vapor atmosphere (PC-900). The waste printing paper-derived carbon presented the only carbonyl groups, which resulted in the loading of palladium (Pd) as single atoms (Pd/PC-900). X-ray photoelectron spectroscopy characterization and density function theory simulation proved that the Pd atom coordinated with two carbonyl groups. In the oxidation of benzyl alcohol, the adsorption energy of benzyl alcohol on Pd single atom was higher than benzaldehyde. The reaction selectivity of Pd/PC-900 to benzaldehyde was over 99.3% and the reaction rate of Pd/PC-900 (TOF = 19.9 × 103 h−1) was about twice of conventional Pd/AC (TOF = 9.7 × 103 h−1) at 140 °C in 0.1 MPa oxygen. After four runs, the activity and selectivity of Pd/PC-900 remained unchanged. Several analysis methods demonstrated that benzyl alcohol was oxidized to benzaldehyde with the alternate catalysis of Pd2+ and Pd0.
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