Pt-based catalysts are prone to oxidation and CO poisoning during the hydrogen oxidation reaction(HOR),leading to deactivation,which has presented significant challenges for the application of proton exchange membrane...Pt-based catalysts are prone to oxidation and CO poisoning during the hydrogen oxidation reaction(HOR),leading to deactivation,which has presented significant challenges for the application of proton exchange membrane fuel cells(PEMFC).Here,we propose a dual-protection strategy with the advantages of Pt-polyoxometalates(POMs)and carbon dots(CDs)to synthesize an advanced POMs-CDs based electrocatalyst,Pt-SiW_(12)-CDs,with Pt clusters dispersed on SiW_(12)-CDs substrates.It exhibited exceptional HOR performance,achieving a mass activity of 10.36 A mgPt^(−1)at an overpotential of 50 mV,which is over 54 times greater than that of Pt/C(0.19 A mgPt^(–1)).These catalysts also display impressive stability and CO tolerance.By employing X-ray absorption fine structure(XAFS)spectra,transient photovoltage(TPV),transient potential scanning(TPS),and density functional theory(DFT)calculation,the in-depth investigation suggested the muti-roles of SiW_(12)and CDs for synergistic enhancement of Pt electrocatalyst stability and activity in HOR process.CDs act as bridges,effectively and rapidly transferring protons and electrons to SiW_(12)from Pt clusters.CDs can effectively coordinate with Pt,regulating its electronic structure while pre-occupying Pt sites,thus hindering CO adsorption on Pt.The reduced SiW_(12)efficiently transfers electrons to Pt,inhibiting the oxidation of Pt.Additionally,SiW_(12)also serves as the driving force,maintaining the rapid progression of the HOR process.The dual-protection strategy provides new ideas and directions for design of efficient and stable heterogeneous catalyst.展开更多
基金supported by the National Key R&D Program of China(2024YFA1509300)the Natural Science Foundation of Jiangsu Province(BK20220028)+4 种基金the National Natural Science Foundation of China(52272043,52271223,52472049,52472230,52202107,22171041,22471030,22379024,and 21671036)the Science and Technology Development Fund,Macao SAR(0009/2022/ITP)State Key Laboratory of Catalysis(2024SKL-A-014)Collaborative Innovation Center of Suzhou Nano Science&Technology,the 111 ProjectSuzhou Key Laboratory of Functional Nano&Soft Materials.
文摘Pt-based catalysts are prone to oxidation and CO poisoning during the hydrogen oxidation reaction(HOR),leading to deactivation,which has presented significant challenges for the application of proton exchange membrane fuel cells(PEMFC).Here,we propose a dual-protection strategy with the advantages of Pt-polyoxometalates(POMs)and carbon dots(CDs)to synthesize an advanced POMs-CDs based electrocatalyst,Pt-SiW_(12)-CDs,with Pt clusters dispersed on SiW_(12)-CDs substrates.It exhibited exceptional HOR performance,achieving a mass activity of 10.36 A mgPt^(−1)at an overpotential of 50 mV,which is over 54 times greater than that of Pt/C(0.19 A mgPt^(–1)).These catalysts also display impressive stability and CO tolerance.By employing X-ray absorption fine structure(XAFS)spectra,transient photovoltage(TPV),transient potential scanning(TPS),and density functional theory(DFT)calculation,the in-depth investigation suggested the muti-roles of SiW_(12)and CDs for synergistic enhancement of Pt electrocatalyst stability and activity in HOR process.CDs act as bridges,effectively and rapidly transferring protons and electrons to SiW_(12)from Pt clusters.CDs can effectively coordinate with Pt,regulating its electronic structure while pre-occupying Pt sites,thus hindering CO adsorption on Pt.The reduced SiW_(12)efficiently transfers electrons to Pt,inhibiting the oxidation of Pt.Additionally,SiW_(12)also serves as the driving force,maintaining the rapid progression of the HOR process.The dual-protection strategy provides new ideas and directions for design of efficient and stable heterogeneous catalyst.
