Herein,we fabricate an embedding structure at the interface between Pt nanoparticles(NPs)and CeO_(2)-{100}nanocubes with surface defect sites(CeO_(2)-SDS)through quenching and gas bubbling-assisted membrane reduction ...Herein,we fabricate an embedding structure at the interface between Pt nanoparticles(NPs)and CeO_(2)-{100}nanocubes with surface defect sites(CeO_(2)-SDS)through quenching and gas bubbling-assisted membrane reduction methods.The in-situ substitution of Pt NPs for atomic-layer Ce lattice significantly increases the amount of reactive oxygen species from 133.68μmol/g to 199.44μmol/g.As a result,the distinctive geometric structure of Pt/CeO_(2)-SDS catalyst substantially improves the catalytic activity and stability for soot oxidation compared with the catalyst with no quenching process,i.e.,its T_(50)and TOF values are 332°C and 2.915 h^(-1),respectively.Combined with the results of experimental investigations and density functional theory calculations,it is unveiled that the unique embedding structure of Pt/CeO_(2)-SDS catalyst can facilitate significantly electron transfer from Pt to the CeO_(2)-{100}support,and induce the formation of interfacial[Ce-O_(x)-Pt_(2)]bond chains,which plays a crucial role in enhancing the key step of soot oxidation through the dual activation of surface lattice oxygen and molecular O_(2).Such a fundamental revelation of the interfacial electronic transmission and corresponding modification strategy contributes a novel opportunity to develop high-efficient and stable noble metal catalysts at the atomic level.展开更多
Improving the photocatalytic efficiency for hydrogen evolution from water splitting plays a vital role for the feasible applications of clean and sustainable hydrogen energy production.A crystalline microporous Cu^(Ⅱ...Improving the photocatalytic efficiency for hydrogen evolution from water splitting plays a vital role for the feasible applications of clean and sustainable hydrogen energy production.A crystalline microporous Cu^(Ⅱ)-based metal-organic framework(Cu^(Ⅱ)-MOF)and a series of three Pt/Cu^(Ⅱ)-MOF nanoribbons decorated with different loadings of Pt nanoparticles(NPs)have been synthesized and used subsequently as photocatalysts for hydrogen production via water splitting.Resulting significantly from the synergistic effects between the catalytic active Cu^(Ⅱ)and Pt centers,the optimized Pt(4.38 wt%)/Cu^(Ⅱ)-MOF nanoribbon exhibits an enhanced hydrogen generation rate up to 2.51 mmol g^(−1)h^(−1),remarkably higher by 4.7 and 1.9 times than those of the referential Pt NP and Cu^(Ⅱ)-MOF.The electronic interactions between the Pt and Cu^(Ⅱ)sites in the composite favorably dominate the potential of the conductive band and decrease the charge transfer resistance.These interesting results highlight an effective strategy for the rational design of a highly robust and microporous MOF-based composite with multiple photoactive metal sites.展开更多
基金supported by the Beijing Nova Program(No.20220484215)National Key Research and Development Program of China(Nos.2022YFB3504100,2022YFB3506200,2021YFA1500300 and 2022YFA1500146)National Natural Science Foundation of China(Nos.22376217,22208373,22272090 and 22272106)。
文摘Herein,we fabricate an embedding structure at the interface between Pt nanoparticles(NPs)and CeO_(2)-{100}nanocubes with surface defect sites(CeO_(2)-SDS)through quenching and gas bubbling-assisted membrane reduction methods.The in-situ substitution of Pt NPs for atomic-layer Ce lattice significantly increases the amount of reactive oxygen species from 133.68μmol/g to 199.44μmol/g.As a result,the distinctive geometric structure of Pt/CeO_(2)-SDS catalyst substantially improves the catalytic activity and stability for soot oxidation compared with the catalyst with no quenching process,i.e.,its T_(50)and TOF values are 332°C and 2.915 h^(-1),respectively.Combined with the results of experimental investigations and density functional theory calculations,it is unveiled that the unique embedding structure of Pt/CeO_(2)-SDS catalyst can facilitate significantly electron transfer from Pt to the CeO_(2)-{100}support,and induce the formation of interfacial[Ce-O_(x)-Pt_(2)]bond chains,which plays a crucial role in enhancing the key step of soot oxidation through the dual activation of surface lattice oxygen and molecular O_(2).Such a fundamental revelation of the interfacial electronic transmission and corresponding modification strategy contributes a novel opportunity to develop high-efficient and stable noble metal catalysts at the atomic level.
基金support was provided from the National Natural Science Finance of China(Grants 21671149,21571140 and 21531005)the Program for Innovative Research Team in University of Tianjin(TD13-5074)。
文摘Improving the photocatalytic efficiency for hydrogen evolution from water splitting plays a vital role for the feasible applications of clean and sustainable hydrogen energy production.A crystalline microporous Cu^(Ⅱ)-based metal-organic framework(Cu^(Ⅱ)-MOF)and a series of three Pt/Cu^(Ⅱ)-MOF nanoribbons decorated with different loadings of Pt nanoparticles(NPs)have been synthesized and used subsequently as photocatalysts for hydrogen production via water splitting.Resulting significantly from the synergistic effects between the catalytic active Cu^(Ⅱ)and Pt centers,the optimized Pt(4.38 wt%)/Cu^(Ⅱ)-MOF nanoribbon exhibits an enhanced hydrogen generation rate up to 2.51 mmol g^(−1)h^(−1),remarkably higher by 4.7 and 1.9 times than those of the referential Pt NP and Cu^(Ⅱ)-MOF.The electronic interactions between the Pt and Cu^(Ⅱ)sites in the composite favorably dominate the potential of the conductive band and decrease the charge transfer resistance.These interesting results highlight an effective strategy for the rational design of a highly robust and microporous MOF-based composite with multiple photoactive metal sites.
