Zn- and Na-modulated Fe catalysts were fabricated by a simple coprecipitation/washing method. Zn greatly changed the size of iron species, serving as the structural promoter, while the existence of Na on the surface of the Fe catalyst alters the electronic structure, making the catalyst very active for CO activation. Most importantly, the electronic structure of the catalyst surface suppresses the hydrogenation of double bonds and promotes desorption of products, which renders the catalyst unexpectedly reactive toward alkenes-especially C5+ alkenes (with more than 50% selectivity in hydrocarbons)-while lowering the selectivity for undesired products. This study enriches C1 chemistry and the design of highly selective new catalysts for high-value chemicals.
Zn‐ and Na‐modulated Fe catalysts were fabricated by a simple coprecipitation/washing method. Zn greatly changed the size of iron species, serving as the structural promoter, while the existence of Na on the surface of the Fe catalyst alters the electronic structure, making the catalyst very active for CO activation. Most importantly, the electronic structure of the catalyst surface suppresses the hydrogenation of double bonds and promotes desorption of products, which renders the catalyst unexpectedly reactive toward alkenes—especially C5+ alkenes (with more than 50% selectivity in hydrocarbons)—while lowering the selectivity for undesired products. This study enriches C1 chemistry and the design of highly selective new catalysts for high‐value chemicals.
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.
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