Pt/Pt 4+-TiO2 photocatalyst prepared by a modified sol-gel process was investigated by X-ray diffraction, UV-Vis diffuse reflectance spectra, X-ray photoelectron spectroscopy, time-resolved photoconductivity and terep...Pt/Pt 4+-TiO2 photocatalyst prepared by a modified sol-gel process was investigated by X-ray diffraction, UV-Vis diffuse reflectance spectra, X-ray photoelectron spectroscopy, time-resolved photoconductivity and terephthalic acid fluorescence probing. The photocatalytic activities of catalysts were evaluated by using ethylene oxidation studies under visible light irradiation（λ>450 nm） from 40 to 62 ℃. It is found that the platinum doping in titania caused significant absorption shift to the visible region and the surface recombination of photogenerated carriers was inhibited. The results show that ethylene was not converted on conventional TiO2 while the conversion was 90% and the complete mineralization was achieved over Pt-Pt 4+/TiO2 at 62 ℃ in our experiment. Besides the exponential increase of thermalcatalytic activity, pure photocatalytic activity of the planitized sample enhanced linearly with the increase of temperature.展开更多
A support(denoted AM) was prepared using pseudo-boehmite and mordenite.Ni-B and NiPtB amorphous catalysts were prepared on the support by the impregnation method followed by chemical reduction with a KBH4 solution.And...A support(denoted AM) was prepared using pseudo-boehmite and mordenite.Ni-B and NiPtB amorphous catalysts were prepared on the support by the impregnation method followed by chemical reduction with a KBH4 solution.And the catalysts were characterized by X-ray diffraction(XRD),environment scanning electron microscope(ESEM),inductively coupled plasma(ICP),H2-temperature programmed reduction(H2-TPR),differential thermal analysis(DTA),and BET.Benzene hydrogenation was used as a probe reaction to evaluate the effect of addition of small quantities of Pt on the NiB/AM catalyst.The results show that Pt can promote the reduction of NiO and the formation of active sites,leading to smaller catalyst particles and better dispersion of active metal particles on the support.The catalytic activity,sulfur resistance and thermal stability were remarkably improved by Pt doping of the NiB/AM catalyst.展开更多
Catalytic oxidation of formaldehyde (HCHO) is the most efficient way to purify indoor air of HCHO pollutant. This work investigated rare earth La‐doped Pt/TiO2 for low concentration HCHO oxidation at room temperature...Catalytic oxidation of formaldehyde (HCHO) is the most efficient way to purify indoor air of HCHO pollutant. This work investigated rare earth La‐doped Pt/TiO2 for low concentration HCHO oxidation at room temperature. La‐doped Pt/TiO2 had a dramatically promoted catalytic performance for HCHO oxidation. The reasons for the La promotion effect were investigated by N2 adsorption, X‐raydiffraction, CO chemisorption, X‐ray photoelectron spectroscopy, transmission electron microscopy(TEM) and high‐angle annular dark field scanning TEM. The Pt nanoparticle size was reduced to 1.7nm from 2.2 nm after modification by La, which led to higher Pt dispersion, more exposed activesites and enhanced metal‐support interaction. Thus a superior activity for indoor low concentrationHCHO oxidation was obtained. Moreover, the La‐doped TiO2 can be wash‐coated on a cordieritemonolith so that very low amounts of Pt (0.01 wt%) can be used. The catalyst was evaluated in asimulated indoor HCHO elimination environment and displayed high purifying efficiency and stability.It can be potentially used as a commercial catalyst for indoor HCHO elimination.展开更多
Hierarchical nitrogen-doped carbon nanocages （hNCNC） with large specific surface areas were used as a catalyst support to immobilize Pt nanoparticles by a microwave-assisted polyol method. The Pt/hNCNC catalyst with...Hierarchical nitrogen-doped carbon nanocages （hNCNC） with large specific surface areas were used as a catalyst support to immobilize Pt nanoparticles by a microwave-assisted polyol method. The Pt/hNCNC catalyst with 20 wt% loading has a homogeneous dispersion of Pt nanoparticles with the average size of 3.3 nm, which is smaller than 4.3 and 4.9 nm for the control catalysts with the same loading supported on hierarchical carbon nanocages （hCNC） and commercial Vulcan XC-72, respec- tively. Accordingly, Pt/hNCNC has a larger electrochemical surface area than Pt/hCNC and Pt/XC-72. The Pt/hNCNC catalyst exhibited excellent electrocatalytic activity and stability for methanol oxidation, which was better than the control catalysts. This was attributed to the en- hanced interaction between Pt and hNCNC due to nitrogen participation in the anchoring function. By making use of the unique advantages of the hNCNC support, a heavy Pt loading up to 60 wt% was prepared without serious agglomeration, which gave a high peak-current density per unit mass of catalyst of 95.6 mA/mg for achieving a high power density. These results showed the potential of the Pt/hNCNC catalyst for methanol oxidation and of the new hNCNC support for wide applications.展开更多
A Pt/CNTs catalyst coated with N‐doped carbon（xNC‐Pt/CNTs） is synthesized by atomic layer dep‐osition（ALD） and applied in methanol electrooxidation reaction. Pt nanoparticles and polyimide（PI） are sequentiall...A Pt/CNTs catalyst coated with N‐doped carbon（xNC‐Pt/CNTs） is synthesized by atomic layer dep‐osition（ALD） and applied in methanol electrooxidation reaction. Pt nanoparticles and polyimide（PI） are sequentially deposited on carbon nanotubes（CNTs） by ALD. After annealing at 600 °C in H2 atmosphere, the PI is carbonized to produce porous N‐doped carbon. Upon coating with a moder‐ately thick layer of N‐doped carbon, the optimized 50 NC‐Pt/CNTs show higher activity, better long‐term stability, and improved CO resistance towards methanol electrooxidation compared with Pt/CNTs and commercial Pt/C（20 wt%）. X‐ray photoelectron spectroscopy characterization result indicates that the Pt–CO bond is weakened after N‐doped carbon coating and CO adsorption on the Pt surface is weakened, leading to superior electrocatalytic performance.展开更多
A series of Sn‐incorporated SBA‐15materials with high specific surface areas and highly orderedmesoporous structures were synthesized by a facile one‐pot method and used as catalyst supports.A reference sample was ...A series of Sn‐incorporated SBA‐15materials with high specific surface areas and highly orderedmesoporous structures were synthesized by a facile one‐pot method and used as catalyst supports.A reference sample was also prepared using a conventional impregnation method.The catalystswere characterized using various methods,and their activities in propane dehydrogenation wereinvestigated.The incorporation of Sn into the SBA‐15matrix led to strong interactions between Snspecies and the support,and these helped to maintain the oxidation states of Sn species during thereaction.Substitution with Sn changed the interfacial properties of the Pt species and improved thefunction and effect of the Sn promoter.The catalytic activities and stabilities of the Pt catalysts supportedon Sn‐incorporated SBA‐15were better than those of the impregnated sample.However,thecatalytic performance deteriorated when an excessive amount of Sn was introduced and the interactionsamong Pt,Sn species,and the support became weaker.The Pt/0.5Sn‐SBA‐15catalyst gavethe best propene selectivity,i.e.,98.5%,with a corresponding propane conversion of about43.8%.展开更多
The emergency of superconductivity at the edge of charge density wave （CDW） state by pressure or chemical doping in 1T transi- tion metal dichalcogenides （TMDs） has attracted much attention in past decade [1, 2]. ...The emergency of superconductivity at the edge of charge density wave （CDW） state by pressure or chemical doping in 1T transi- tion metal dichalcogenides （TMDs） has attracted much attention in past decade [1, 2]. The interplay of CDW and superconduc- tivity has triggered the hot debate： why does superconductivity arise after suppressing the CDW and what＇s the driving force of the charge modulation？ For the 5d transition metal ditelluride IrTe2, a layered compound with trigonal symmetry, previous studies have shown an ordered superstructure below ～ 280 K, and a superconducting state when doped or intercalated with Pd or Pt [3, 4]. In IrTe2, the Fermi surface nesting has been excluded as the impetus of superstructure; instead, splitting of Te orbitals by the crystal field [5] or destabilization of polymeric Te-Te networks was proposed [6], evident from the visualized periodic dimer- ization of Te atoms by scanning tunneling microscopy （STM） [7]. Meanwhile, a charge disproportionated CDW by covalent bond- ing Ir dimers was also presented [8]. However, though the origin of the superstructure formation becomes more and more clear, the underlying mechanism of the appearance of superconductivity by doping Pd or Pt is still obscure.展开更多
A facile strategy is established for constructing composite nanostructure with ultrasmall Pt nanoparticles(NPs) of ~2 nm in diameter being homogeneously embedded in N-doped carbon nanosheets. The strong coordination b...A facile strategy is established for constructing composite nanostructure with ultrasmall Pt nanoparticles(NPs) of ~2 nm in diameter being homogeneously embedded in N-doped carbon nanosheets. The strong coordination between Pt atoms in cisplatin and N atoms in pyrrole contributes to the robust embedding of Pt NP into the N-doped carbon nanosheets after annealing. Such a unique partially-embedding structure facilitates the active site exposure while stabilizing the ultrasmall Pt NPs, leading to the comparable electrochemical activities for hydrogen evolution and oxygen reduction reactions, and substantially improves durability performance compared to that of the state-of-the-art Pt/C(20 wt%).展开更多
The IrTe2 transition metal dichalcogenide un- dergoes a series of structural and electronic phase transi- tions when doped with Pt. The nature of each phase and the mechanism of the phase transitions have attracted mu...The IrTe2 transition metal dichalcogenide un- dergoes a series of structural and electronic phase transi- tions when doped with Pt. The nature of each phase and the mechanism of the phase transitions have attracted much attention. In this paper, we report scanning tunneling mi- croscopy and spectroscopy studies of Pt-doped IrTe2 with varied Pt contents. In pure IrTe2, we find that the ground state has a 1/6 superstructure, and the electronic structure is inconsistent with Fermi surface nesting-induced charge density wave order. Upon Pt doping, the crystal structure changes to a 1/5 superstructure and then to a quasi-periodic hexagonal phase. First-principles calculations show that the superstructures and electronic structures are determined by the global chemical strain and local impurity states that can be tuned systematically by Pt doping.展开更多
Developing efficient platinum(Pt)-based electrocatalysts is enormously significant for fuel cells.Herein,we report an integrated electrocatalyst of ultralow-Pt alloy encapsulated into nitrogen-doped nanocarbon archite...Developing efficient platinum(Pt)-based electrocatalysts is enormously significant for fuel cells.Herein,we report an integrated electrocatalyst of ultralow-Pt alloy encapsulated into nitrogen-doped nanocarbon architecture for efficient oxygen reduction reaction.This hybrid Pt-based catalyst achieves a mass activity of 3.46 A mg^(-1)_(pt)the potential of 0.9 V vs.RHE with a negligible stability decay after 10,000 cycles.More importantly,this half-cell activity can be expressed at full cell level with a high Pt utilization of 10.22 W mg^(-1)_(Pt cathode)and remarkable durability after 30,000 cycles in single-cell.Experimental and theoretical investigations reveal that a highly strained Pt structure with an optimal Pt-0 binding energy is induced by the incorporation of Co/Ni into Pt lattice,which would account for the improved reaction kinetics.The synergistic catalysis due to nitrogen-doped nanocarbon architecture and active Pt component is responsible for the enhanced catalytic activity.Meanwhile,the strong metal-support interaction and optimized hydrophilic properties of nanocarbon matrix facilitate efficient mass transport and water management.This work may provide significant insights in designing the low-Pt integrated electrocatalysts for fuel cells and beyond.展开更多
文摘Pt/Pt 4+-TiO2 photocatalyst prepared by a modified sol-gel process was investigated by X-ray diffraction, UV-Vis diffuse reflectance spectra, X-ray photoelectron spectroscopy, time-resolved photoconductivity and terephthalic acid fluorescence probing. The photocatalytic activities of catalysts were evaluated by using ethylene oxidation studies under visible light irradiation（λ>450 nm） from 40 to 62 ℃. It is found that the platinum doping in titania caused significant absorption shift to the visible region and the surface recombination of photogenerated carriers was inhibited. The results show that ethylene was not converted on conventional TiO2 while the conversion was 90% and the complete mineralization was achieved over Pt-Pt 4+/TiO2 at 62 ℃ in our experiment. Besides the exponential increase of thermalcatalytic activity, pure photocatalytic activity of the planitized sample enhanced linearly with the increase of temperature.
基金Supported by the Overseas Scholars of Heilongjiang Province of China (1151hq006)
文摘A support(denoted AM) was prepared using pseudo-boehmite and mordenite.Ni-B and NiPtB amorphous catalysts were prepared on the support by the impregnation method followed by chemical reduction with a KBH4 solution.And the catalysts were characterized by X-ray diffraction(XRD),environment scanning electron microscope(ESEM),inductively coupled plasma(ICP),H2-temperature programmed reduction(H2-TPR),differential thermal analysis(DTA),and BET.Benzene hydrogenation was used as a probe reaction to evaluate the effect of addition of small quantities of Pt on the NiB/AM catalyst.The results show that Pt can promote the reduction of NiO and the formation of active sites,leading to smaller catalyst particles and better dispersion of active metal particles on the support.The catalytic activity,sulfur resistance and thermal stability were remarkably improved by Pt doping of the NiB/AM catalyst.
基金supported by the National Key Research and Development Program (2016YFC0205900)the National Natural Science Foundation of China (21503106, 21567016)+1 种基金the Education Department of Jiangxi Province (KJLD14005)the Natural Science Foundation of Jiangxi Province (20142BAB213013 and 20151BBE50006)~~
文摘Catalytic oxidation of formaldehyde (HCHO) is the most efficient way to purify indoor air of HCHO pollutant. This work investigated rare earth La‐doped Pt/TiO2 for low concentration HCHO oxidation at room temperature. La‐doped Pt/TiO2 had a dramatically promoted catalytic performance for HCHO oxidation. The reasons for the La promotion effect were investigated by N2 adsorption, X‐raydiffraction, CO chemisorption, X‐ray photoelectron spectroscopy, transmission electron microscopy(TEM) and high‐angle annular dark field scanning TEM. The Pt nanoparticle size was reduced to 1.7nm from 2.2 nm after modification by La, which led to higher Pt dispersion, more exposed activesites and enhanced metal‐support interaction. Thus a superior activity for indoor low concentrationHCHO oxidation was obtained. Moreover, the La‐doped TiO2 can be wash‐coated on a cordieritemonolith so that very low amounts of Pt (0.01 wt%) can be used. The catalyst was evaluated in asimulated indoor HCHO elimination environment and displayed high purifying efficiency and stability.It can be potentially used as a commercial catalyst for indoor HCHO elimination.
基金supported by the National Natural Science Foundation of China(21473089,51232003,21373108,51571110,21573107)the Nation-al Basic Research Program of China(973 Program,2013CB932902)+2 种基金Suzhou Science and Technology Projects(ZXG2013025)Changzhou Science and Technology Projects(CE20130032)supported by a Project Funded by the Technology Support Priority Academic Program Development of Jiangsu Higher Education Institutions
文摘Hierarchical nitrogen-doped carbon nanocages （hNCNC） with large specific surface areas were used as a catalyst support to immobilize Pt nanoparticles by a microwave-assisted polyol method. The Pt/hNCNC catalyst with 20 wt% loading has a homogeneous dispersion of Pt nanoparticles with the average size of 3.3 nm, which is smaller than 4.3 and 4.9 nm for the control catalysts with the same loading supported on hierarchical carbon nanocages （hCNC） and commercial Vulcan XC-72, respec- tively. Accordingly, Pt/hNCNC has a larger electrochemical surface area than Pt/hCNC and Pt/XC-72. The Pt/hNCNC catalyst exhibited excellent electrocatalytic activity and stability for methanol oxidation, which was better than the control catalysts. This was attributed to the en- hanced interaction between Pt and hNCNC due to nitrogen participation in the anchoring function. By making use of the unique advantages of the hNCNC support, a heavy Pt loading up to 60 wt% was prepared without serious agglomeration, which gave a high peak-current density per unit mass of catalyst of 95.6 mA/mg for achieving a high power density. These results showed the potential of the Pt/hNCNC catalyst for methanol oxidation and of the new hNCNC support for wide applications.
基金supported by the National Natural Science Foundation of China (21403272, 21673269)the Natural Science Foundation of Shanxi Province (2015021046)~~
文摘A Pt/CNTs catalyst coated with N‐doped carbon（xNC‐Pt/CNTs） is synthesized by atomic layer dep‐osition（ALD） and applied in methanol electrooxidation reaction. Pt nanoparticles and polyimide（PI） are sequentially deposited on carbon nanotubes（CNTs） by ALD. After annealing at 600 °C in H2 atmosphere, the PI is carbonized to produce porous N‐doped carbon. Upon coating with a moder‐ately thick layer of N‐doped carbon, the optimized 50 NC‐Pt/CNTs show higher activity, better long‐term stability, and improved CO resistance towards methanol electrooxidation compared with Pt/CNTs and commercial Pt/C（20 wt%）. X‐ray photoelectron spectroscopy characterization result indicates that the Pt–CO bond is weakened after N‐doped carbon coating and CO adsorption on the Pt surface is weakened, leading to superior electrocatalytic performance.
基金supported by the Science & Technology Support Plan Projects of Sichuan Province (2016GZ0371)National Natural Science Foun-dation of China (NNSFC,21476145,21506111)~~
文摘A series of Sn‐incorporated SBA‐15materials with high specific surface areas and highly orderedmesoporous structures were synthesized by a facile one‐pot method and used as catalyst supports.A reference sample was also prepared using a conventional impregnation method.The catalystswere characterized using various methods,and their activities in propane dehydrogenation wereinvestigated.The incorporation of Sn into the SBA‐15matrix led to strong interactions between Snspecies and the support,and these helped to maintain the oxidation states of Sn species during thereaction.Substitution with Sn changed the interfacial properties of the Pt species and improved thefunction and effect of the Sn promoter.The catalytic activities and stabilities of the Pt catalysts supportedon Sn‐incorporated SBA‐15were better than those of the impregnated sample.However,thecatalytic performance deteriorated when an excessive amount of Sn was introduced and the interactionsamong Pt,Sn species,and the support became weaker.The Pt/0.5Sn‐SBA‐15catalyst gavethe best propene selectivity,i.e.,98.5%,with a corresponding propane conversion of about43.8%.
文摘The emergency of superconductivity at the edge of charge density wave （CDW） state by pressure or chemical doping in 1T transi- tion metal dichalcogenides （TMDs） has attracted much attention in past decade [1, 2]. The interplay of CDW and superconduc- tivity has triggered the hot debate： why does superconductivity arise after suppressing the CDW and what＇s the driving force of the charge modulation？ For the 5d transition metal ditelluride IrTe2, a layered compound with trigonal symmetry, previous studies have shown an ordered superstructure below ～ 280 K, and a superconducting state when doped or intercalated with Pd or Pt [3, 4]. In IrTe2, the Fermi surface nesting has been excluded as the impetus of superstructure; instead, splitting of Te orbitals by the crystal field [5] or destabilization of polymeric Te-Te networks was proposed [6], evident from the visualized periodic dimer- ization of Te atoms by scanning tunneling microscopy （STM） [7]. Meanwhile, a charge disproportionated CDW by covalent bond- ing Ir dimers was also presented [8]. However, though the origin of the superstructure formation becomes more and more clear, the underlying mechanism of the appearance of superconductivity by doping Pd or Pt is still obscure.
基金supported by the National Key Basic Research Program of China(2013CB933200)the Natural Science Foundation of Shanghai(16ZR1440600)+1 种基金the State key laboratory of heavy oil processing(SKLOP201402003)the National Natural Science Foundation of China(U1510107)
文摘A facile strategy is established for constructing composite nanostructure with ultrasmall Pt nanoparticles(NPs) of ~2 nm in diameter being homogeneously embedded in N-doped carbon nanosheets. The strong coordination between Pt atoms in cisplatin and N atoms in pyrrole contributes to the robust embedding of Pt NP into the N-doped carbon nanosheets after annealing. Such a unique partially-embedding structure facilitates the active site exposure while stabilizing the ultrasmall Pt NPs, leading to the comparable electrochemical activities for hydrogen evolution and oxygen reduction reactions, and substantially improves durability performance compared to that of the state-of-the-art Pt/C(20 wt%).
基金supported by the National Natural Science Foundation and Ministry of Science and Technology of China(2011CB921901,2011CB921701,2012CB821403,and 2015CB921000)
文摘The IrTe2 transition metal dichalcogenide un- dergoes a series of structural and electronic phase transi- tions when doped with Pt. The nature of each phase and the mechanism of the phase transitions have attracted much attention. In this paper, we report scanning tunneling mi- croscopy and spectroscopy studies of Pt-doped IrTe2 with varied Pt contents. In pure IrTe2, we find that the ground state has a 1/6 superstructure, and the electronic structure is inconsistent with Fermi surface nesting-induced charge density wave order. Upon Pt doping, the crystal structure changes to a 1/5 superstructure and then to a quasi-periodic hexagonal phase. First-principles calculations show that the superstructures and electronic structures are determined by the global chemical strain and local impurity states that can be tuned systematically by Pt doping.
基金the National Natural Science Foundation of China(22075092 and 21805104)the Program for Huazhong University of Science and Technology(HUST)Academic Frontier Youth Team(2018QYTD15)The Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)。
文摘Developing efficient platinum(Pt)-based electrocatalysts is enormously significant for fuel cells.Herein,we report an integrated electrocatalyst of ultralow-Pt alloy encapsulated into nitrogen-doped nanocarbon architecture for efficient oxygen reduction reaction.This hybrid Pt-based catalyst achieves a mass activity of 3.46 A mg^(-1)_(pt)the potential of 0.9 V vs.RHE with a negligible stability decay after 10,000 cycles.More importantly,this half-cell activity can be expressed at full cell level with a high Pt utilization of 10.22 W mg^(-1)_(Pt cathode)and remarkable durability after 30,000 cycles in single-cell.Experimental and theoretical investigations reveal that a highly strained Pt structure with an optimal Pt-0 binding energy is induced by the incorporation of Co/Ni into Pt lattice,which would account for the improved reaction kinetics.The synergistic catalysis due to nitrogen-doped nanocarbon architecture and active Pt component is responsible for the enhanced catalytic activity.Meanwhile,the strong metal-support interaction and optimized hydrophilic properties of nanocarbon matrix facilitate efficient mass transport and water management.This work may provide significant insights in designing the low-Pt integrated electrocatalysts for fuel cells and beyond.
