Effect of N-doping on the catalytic decomposition of hydrogen iodide over activated carbon: Experimental and DFT studies

A series of N-doped activated carbon (NAC) with varying N contents were prepared to study the effect of N-doping on hydrogen iodide (HI) decomposition over activated carbon in sulfur-iodine (SI) cycle for hydrogen production . Element analysis , XPS and N 2 adsorption were performed for samples’ characterization. The HI conversion was proportional to the N content and the sample with 6.006% N content gave the highest HI conversion of 22.84%. Density functional theory (DFT) calculations confirmed the experimental results and elucidated the influence mechanism. The increase of N contents was favor to the decomposition of HI by enhancing the chemisorption of HI molecule on carbon structure. The role of N-doping was to remodel the local electronic density and charge distribution on the carbon surface . In addition, the effect of types of N-containing functional groups on HI decomposition was calculated. Results showed that the N-6 structure was conducive to the chemisorption of HI but N-5 and N-Q structures had a reverse effect. However, when the three N-containing functional groups exist simultaneously, the overall chemisorption of HI was enhanced, which, in turn, enhanced the decomposition of HI. This study can provide underlying guidance for preparing highly efficient NAC for HI decomposition.