Efficient decomposition of formic acid into hydrogen on Pd nanoparticles anchored in amine-pyridine polymer networks without extra additives at ambient condition

• Published in: International journal of hydrogen energy Vol. 46; no. 12; pp. 8469 - 8476
• Main Authors: Wei, Rui-Lin, Huang, Min, Lan, Bing, Wang, Chao-Nan, Wang, Qiong-Lan, Yang, Yao-Yue
• Format: Journal Article
• Language: English
• Published: Elsevier Ltd 16.02.2021
• Subjects: Amine-pyridine polymer; CO free; Formic acid decomposition; Hydrogen production; Palladium; Amine-pyridine polymer; Palladium; CO free; Formic acid decomposition; Hydrogen production
• ISSN: 0360-3199; 1879-3487
• DOI: 10.1016/j.ijhydene.2020.11.260

Palladium (Pd) is considered as the most promising catalyst for hydrogen production from formic acid decomposition (FAD), but pristine Pd catalysts are less active and readily to perform activity decay by CO poisoning. Thus the modulation of Pd is critical for its application in H2 production from FAD. Here a Pd/APPNs catalysts by anchoring ca. 2.1 ± 0.3 nm Pd nanoparticles in the amino-pyridine polymer networks (designated as APPNs) was designed based on so-called metal-support interaction. The strong interaction between Pd and N of amine-pyridine unites was demonstrated by the X-ray photoelectron spectroscopic (XPS) analysis. It suggests the electron transfer between N and Pd, which could lower the d-band center of Pd and further effectively enhance the FAD catalysis performance. The initial FAD TOF value of 512 h−1 and the activation energy (Ea) of ca. 22.1 kJ mol−1 give a proper proof for the catalysis enhancement. And the third time FAD run still show a 442 h−1 TOF, indicating an excellent catalysis stability. In addition, the production analysis by Gas chromatography (GC) show that no CO was detected. This CO-free production was also confirmed through no observation of Surface-enhanced Adsorption Infrared Spectral (SEIRAS) band at 1700-2100 cm−1 (i.e. the COad species) on Pd/ANNPs surface. This work indicates that direct modification of Pd by the functionalized support (metal-support interaction) could effective enhance the FAD catalysis performance, although further work combined with other tuning means should be push forward. Pd Nanoparticles anchored in amine-pyridine polymer networks facilitate the formic acid decomposing into CO-free H2 at ambient condition. [Display omitted] •Facial catalysts preparation by anchoring Pd nanoparticles in the APPNs.•Highly efficient FAD catalysis performance on Pd/ANNPs without extra additives.•Pd and N interaction effective tuning the electronic structure of Pd.•No CO generating due to the surface modulation through metal-support interaction.