Two-dimensional(2 D) platinum(Pt)-based nanomaterials are considered as the ideal fuel cell catalysts, while their rational synthesis associated with phase control remains a formidable challenge. Herein, we firstly de...Two-dimensional(2 D) platinum(Pt)-based nanomaterials are considered as the ideal fuel cell catalysts, while their rational synthesis associated with phase control remains a formidable challenge. Herein, we firstly design the novel 2 D Pt-lead-sulphur heterophased nanosheets(Pt Pb S HPNSs) as efficient high-toleration electrocatalysts for methanol oxidation reaction(MOR).They exhibit much higher activity and more highlighted bifunctional antipoisoning abilities than Pt Pb NSs and commercial Pt/C.Further density functional theory(DFT) simulation verifies that the decreased electron density of Pt sites worked by Pb and S makes CO intermediate favorable to desorb, avoiding the formation of CO*-polluted Pt sites. Simultaneously, this heterophased interface effectively weakens the adsorption of S^(2-)-species and improves the S-poisoning tolerance, showing a route to realize nearly innoxious catalysis. The present work highlights the importance of heterophase control in tuning antipoisoning property for 2 D Pt-based nanomaterials, which is key for the rational design of efficient fuel cell anodic catalysts.展开更多
基金supported by the Ministry of Science and Technology of China (2017YFA0208200, 2016YFA0204100)the National Natural Science Foundation of China (22025108)the Start-Up support from Xiamen University。
文摘Two-dimensional(2 D) platinum(Pt)-based nanomaterials are considered as the ideal fuel cell catalysts, while their rational synthesis associated with phase control remains a formidable challenge. Herein, we firstly design the novel 2 D Pt-lead-sulphur heterophased nanosheets(Pt Pb S HPNSs) as efficient high-toleration electrocatalysts for methanol oxidation reaction(MOR).They exhibit much higher activity and more highlighted bifunctional antipoisoning abilities than Pt Pb NSs and commercial Pt/C.Further density functional theory(DFT) simulation verifies that the decreased electron density of Pt sites worked by Pb and S makes CO intermediate favorable to desorb, avoiding the formation of CO*-polluted Pt sites. Simultaneously, this heterophased interface effectively weakens the adsorption of S^(2-)-species and improves the S-poisoning tolerance, showing a route to realize nearly innoxious catalysis. The present work highlights the importance of heterophase control in tuning antipoisoning property for 2 D Pt-based nanomaterials, which is key for the rational design of efficient fuel cell anodic catalysts.
