Single-metal sites anchored in nitrogen-doped nanocarbons are recognized as potent electrocatalysts for applications in energy conversion and storage.Here,an innovative inorganic salt-mediated secondary calcination st...Single-metal sites anchored in nitrogen-doped nanocarbons are recognized as potent electrocatalysts for applications in energy conversion and storage.Here,an innovative inorganic salt-mediated secondary calcination strategy was developed to construct robust Pt single-atom catalysts on nitrogen-and oxygen-doped graphene nanosheets(Pt-N/O-GNs),thereby significantly enhancing the efficiency of the electrocatalytic oxygen reduction reaction(ORR).The ultrathin N/O-GNs,obtained by stripping Zn-ZIF with auxiliaries of KCl and LiCl,provide stable anchoring sites for highly exposed Pt-N_(3)O active structures.The Pt-N/O-GNs catalyst,featuring a low Pt loading of 0.44 wt%,demonstrates exceptional mass activity in the ORR process.It attains an impressive onset potential of 0.99 V and a half-wave potential of 0.88 V.The zinc-air battery driven by the Pt-N/O-GNs displays superior power density and cycle stability.Theoretical computational studies reveal that the structure of heteroatoms doped in few-layer graphene facilitates the stable anchoring of single-atom configurations.The findings provide new perspectives for the tailored design and fabrication of single-metal-site electrocatalysts.展开更多
The efficient conversion of lignin into mono-cycloalkanes via both C–O and C–C bonds cleavage are attractive,but challenging due to the high C–C bond dissociation energy.Previous studies have demonstrated that NbO_...The efficient conversion of lignin into mono-cycloalkanes via both C–O and C–C bonds cleavage are attractive,but challenging due to the high C–C bond dissociation energy.Previous studies have demonstrated that NbO_(x)-based catalysts exhibited exceptional capabilities for C_(Ar)–C bond cleavage and broken the limitation of lignin monomers.In this work,we presented an economical multifunctional Pt-Nb/MOR catalyst that achieved an impressive monomer yield of 147%during the depolymerization and hydrodeoxygenation of lignin into mono-cycloalkanes.Reaction pathway studies showed that unlike traditional NbO_(x)-based catalytic system,bicyclohexane was an important intermediate in this system and followed the C_(sp3)–C_(sp3)cleavage pathway after complete cyclic-hydrogenation.Deep investigations demonstrated that the doping of Nb in Pt/MOR not only enhanced the activation of hydrogen by Pt,but also increased the acidity of MOR,both of these are favor for the hydrogenolytic cleavage of C_(sp3)–C_(sp3)bonds.This work provides a low-cost catalyst to obtain high-yield monomers from lignin under relatively mild conditions and would help to design catalysts with higher activity for the valorization of lignin.展开更多
Carbon supported Pt-based intermetallic compounds(IMCs)with high activity and durability are the most competitive cathode catalysts for the commercialization of proton exchange membrane fuel cells(PEMFCs).The synthesi...Carbon supported Pt-based intermetallic compounds(IMCs)with high activity and durability are the most competitive cathode catalysts for the commercialization of proton exchange membrane fuel cells(PEMFCs).The synthesis of Pt-based intermetallics with a good balance between small size and high metal loading remains challenging because of the high-temperature annealing that is generally required to form intermetallic phases.We developed a sodium thiosulfate-assisted impregnation strategy to synthesize small-sized and highly ordered PtM IMCs catalysts(M=Co,Fe,Ni)with high-Pt-content(up to 44.5 wt%).During the impregnation process,thiosulfate could reduce H_(2)PtCl6 to form uniformly dispersed Pt colloid on carbon supports,which in turn prevents the aggregation of Pt at the low-temperature annealing stage.Additionally,the strong interaction between Pt and S inhibits particle sintering,ensuring the formation of small-sized and uniform PtM intermetallic catalysts at the high-temperature annealing stage.The optimized intermetallic PtCo catalyst delivered a high mass activity of 0.72 A mgPt^(–1)and a large power performance of 1.17 W·cm^(–2)at 0.65 V under H_(2)-air conditions,along with 74%mass activity retention after the accelerated stress test.展开更多
The influence of applied temperatures on the creep rupture life of the third-generation low-cost single crystal(SX)superalloy with Pt-Al coating was evaluated.The creep damage was observed under the conditions of 1100...The influence of applied temperatures on the creep rupture life of the third-generation low-cost single crystal(SX)superalloy with Pt-Al coating was evaluated.The creep damage was observed under the conditions of 1100℃/137 MPa,1120℃/137 MPa,and 1140℃/137 MPa.Results show that the properties of bare superalloy outperform those of coated superalloy under all test conditions.The most significant reduction in creep life reaches 50%when the test condition is 1100℃/137 MPa.At higher temperatures(1120 and 1140℃),the crack propagation rate in Pt-Al coatings to SX superalloy substrate decreases,thereby reducing the degradation degree of mechanical properties.Instead of the penetration into SX substrate,tip oxidation and Al diffusion of the coating cracks cause the formation of oxides,therefore leading to the slow degradation in microstructures of the substrate beneath the coating.At 1100℃,however,the microstructure of coating/SX superalloy substrate degrades due to the Al internal diffusion.This diffusion mechanism promotes the formation of harmful topologically close packed phases around 1100℃.At 1120 and 1140℃,the dislocation of SX superalloy substrate beneath the coating is relatively unchanged,compared to that in the inner superalloy.In contrast,the dislocation network of the substrate beneath the coating becomes sparse,and the number of superdislocations cutting intoγ′phases increases at 1100℃.展开更多
文摘Single-metal sites anchored in nitrogen-doped nanocarbons are recognized as potent electrocatalysts for applications in energy conversion and storage.Here,an innovative inorganic salt-mediated secondary calcination strategy was developed to construct robust Pt single-atom catalysts on nitrogen-and oxygen-doped graphene nanosheets(Pt-N/O-GNs),thereby significantly enhancing the efficiency of the electrocatalytic oxygen reduction reaction(ORR).The ultrathin N/O-GNs,obtained by stripping Zn-ZIF with auxiliaries of KCl and LiCl,provide stable anchoring sites for highly exposed Pt-N_(3)O active structures.The Pt-N/O-GNs catalyst,featuring a low Pt loading of 0.44 wt%,demonstrates exceptional mass activity in the ORR process.It attains an impressive onset potential of 0.99 V and a half-wave potential of 0.88 V.The zinc-air battery driven by the Pt-N/O-GNs displays superior power density and cycle stability.Theoretical computational studies reveal that the structure of heteroatoms doped in few-layer graphene facilitates the stable anchoring of single-atom configurations.The findings provide new perspectives for the tailored design and fabrication of single-metal-site electrocatalysts.
文摘The efficient conversion of lignin into mono-cycloalkanes via both C–O and C–C bonds cleavage are attractive,but challenging due to the high C–C bond dissociation energy.Previous studies have demonstrated that NbO_(x)-based catalysts exhibited exceptional capabilities for C_(Ar)–C bond cleavage and broken the limitation of lignin monomers.In this work,we presented an economical multifunctional Pt-Nb/MOR catalyst that achieved an impressive monomer yield of 147%during the depolymerization and hydrodeoxygenation of lignin into mono-cycloalkanes.Reaction pathway studies showed that unlike traditional NbO_(x)-based catalytic system,bicyclohexane was an important intermediate in this system and followed the C_(sp3)–C_(sp3)cleavage pathway after complete cyclic-hydrogenation.Deep investigations demonstrated that the doping of Nb in Pt/MOR not only enhanced the activation of hydrogen by Pt,but also increased the acidity of MOR,both of these are favor for the hydrogenolytic cleavage of C_(sp3)–C_(sp3)bonds.This work provides a low-cost catalyst to obtain high-yield monomers from lignin under relatively mild conditions and would help to design catalysts with higher activity for the valorization of lignin.
文摘Carbon supported Pt-based intermetallic compounds(IMCs)with high activity and durability are the most competitive cathode catalysts for the commercialization of proton exchange membrane fuel cells(PEMFCs).The synthesis of Pt-based intermetallics with a good balance between small size and high metal loading remains challenging because of the high-temperature annealing that is generally required to form intermetallic phases.We developed a sodium thiosulfate-assisted impregnation strategy to synthesize small-sized and highly ordered PtM IMCs catalysts(M=Co,Fe,Ni)with high-Pt-content(up to 44.5 wt%).During the impregnation process,thiosulfate could reduce H_(2)PtCl6 to form uniformly dispersed Pt colloid on carbon supports,which in turn prevents the aggregation of Pt at the low-temperature annealing stage.Additionally,the strong interaction between Pt and S inhibits particle sintering,ensuring the formation of small-sized and uniform PtM intermetallic catalysts at the high-temperature annealing stage.The optimized intermetallic PtCo catalyst delivered a high mass activity of 0.72 A mgPt^(–1)and a large power performance of 1.17 W·cm^(–2)at 0.65 V under H_(2)-air conditions,along with 74%mass activity retention after the accelerated stress test.
基金National Key Research and Development Program of China(2017YFA0700704)China Postdoctoral Science Foundation(2023M733570)+1 种基金Excellent Youth Foundation of Liaoning Province(2021-YQ-02)Science Center for Gas Turbine Project(P2021-A-Ⅳ-002-002)。
文摘The influence of applied temperatures on the creep rupture life of the third-generation low-cost single crystal(SX)superalloy with Pt-Al coating was evaluated.The creep damage was observed under the conditions of 1100℃/137 MPa,1120℃/137 MPa,and 1140℃/137 MPa.Results show that the properties of bare superalloy outperform those of coated superalloy under all test conditions.The most significant reduction in creep life reaches 50%when the test condition is 1100℃/137 MPa.At higher temperatures(1120 and 1140℃),the crack propagation rate in Pt-Al coatings to SX superalloy substrate decreases,thereby reducing the degradation degree of mechanical properties.Instead of the penetration into SX substrate,tip oxidation and Al diffusion of the coating cracks cause the formation of oxides,therefore leading to the slow degradation in microstructures of the substrate beneath the coating.At 1100℃,however,the microstructure of coating/SX superalloy substrate degrades due to the Al internal diffusion.This diffusion mechanism promotes the formation of harmful topologically close packed phases around 1100℃.At 1120 and 1140℃,the dislocation of SX superalloy substrate beneath the coating is relatively unchanged,compared to that in the inner superalloy.In contrast,the dislocation network of the substrate beneath the coating becomes sparse,and the number of superdislocations cutting intoγ′phases increases at 1100℃.
