Poisoning Effects of H 2 S, CS 2 , and COS on Hydrogen Oxidation Reaction over Pt/C Catalysts

作者：Wenyan Dong, Cong Xu, Wenhui Zhao, Mudi Xin, Yanjuan Xiang, Aiguo Zheng, Meiling Dou, Shaojie Ke, Juncai Dong, Limei Qiu, Guangtong Xu · 发表于：ACS Applied Energy Materials · 年份：2022 · DOI：10.1021/acsaem.2c02284 · 被引用次数：35 · 研究领域：Electrocatalysts for Energy Conversion、Fuel Cells and Related Materials、Catalytic Processes in Materials Science

Hydrogen used in proton exchange membrane fuel cells (PEMFCs) mainly originates from refinery resources in which inevitable S-containing impurities possibly reduce the fuel cell life. Herein, the poisonous influence of trace impurities of H 2 S, carbon disulfide (CS 2 ), and carbonyl sulfide (COS) on the performance of Pt/C catalysts in hydrogen oxidation reaction (HOR) is investigated by a combination of electrochemical measurements, structural characterization, and DFT calculations. Rotating disk electrode (RDE) half-cell electrochemical experiments were used to determine the impact of H 2 S, CS 2, and COS on the HOR activity and the recovery capability of a commercial Pt/C catalyst. The experimental results indicate that CS 2 even poses a more severe threat to the HOR activity than H 2 S, while COS poses a weaker threat than H 2 S. Moreover, all of H 2 S, CS 2, and COS have a deteriorative impact on the regeneration of Pt/C catalysts. The theoretical calculation results reveal that CS 2 and COS can decrease the activity of HOR by decreasing the d-band center of Pt atoms except for occupying the active sites of Pt, while H 2 S deactivates the catalyst solely by occupying the active sites. Based on the analysis, the presence of trace CS 2 and COS, as well as H 2 S, will result in the serious degeneration of the Pt/C catalysts. These results provide insights into the deactivation mechanism of Pt-based catalysts and are significant for the practical applications of PEMFCs.