We present a straightforward physical approach for synthesizing multiwalled carbon nanotubes(CNTs)-Pd Au/Pt trimetallic nanoparticles(NPs), which allows predesign and control of the metal compositional ratio by simply...We present a straightforward physical approach for synthesizing multiwalled carbon nanotubes(CNTs)-Pd Au/Pt trimetallic nanoparticles(NPs), which allows predesign and control of the metal compositional ratio by simply adjusting the sputtering targets and conditions. The small-sized CNTs-Pd Au/Pt NPs(~3 nm, Pd/Au/Pt ratio of 3:1:2) act as nanocatalysts for the methanol oxidationreaction(MOR), showing excellent performance with electrocatalytic peak current of 4.4 A mg^(-1) Pt and high stability over 7000 s. The electrocatalytic activity and stability of the Pd Au/Pt trimetallic NPs are much superior to those of the corresponding Pd/Pt and Au/Pt bimetallic NPs,as well as a commercial Pt/C catalyst. Systematic investigation of the microscopic, crystalline, and electronic structure of the Pd Au/Pt NPs reveals alloying and charge redistribution in the Pd Au/Pt NPs, which are responsible for the promotion of the electrocatalytic performance.展开更多
Nafion-stabilized Pt nanoparticle colloidal solution is synthesized through ethylene glycol reduction.Pt/Nafion added with carbon black as electric conduction material（labeled Pt/Nafion-XC72） shows excellent electro...Nafion-stabilized Pt nanoparticle colloidal solution is synthesized through ethylene glycol reduction.Pt/Nafion added with carbon black as electric conduction material（labeled Pt/Nafion-XC72） shows excellent electrochemical property compared with Pt/C.After a 300-cycle discharging durability test,the cell performance of membrane electrode assembly（MEA） with the Pt/Nafion-XC72 and Pt/C catalysts indicates a 29.9% and 92.2% decrease,respectively.The charge transfer resistances of Pt/Nafion-XC72 and Pt/C increase by 27.2% and 101.9%,respectively.The remaining electrochemically active surface area of Pt is about 61.7% in Pt/Nafion-XC72 and about 38.1% in Pt/C after the durability test.The particle size of Pt/C increases from about 5.1 nm to about 10.8 nm but only from 3.6 nm to 5.8 nm in the case of Pt/Nafion-XC72.These data suggest that Pt/Nafion-XC72 as a catalyst can enhance the durability of PEMFCs compared with Pt/C.展开更多
Fine and well dispersed Pt-Cu bimetallic nanoparticles stabilized by polyvinyl pyrrolidone （PVP） were synthesized by alkaline polyol method. The molar ratio of Pt to Cu was 1 ： 1. Further, the Pt-Cu bimetallic nano...Fine and well dispersed Pt-Cu bimetallic nanoparticles stabilized by polyvinyl pyrrolidone （PVP） were synthesized by alkaline polyol method. The molar ratio of Pt to Cu was 1 ： 1. Further, the Pt-Cu bimetallic nanoparticles were supported on alumina and their catalytic behavior in methane combustion was investigated. The as-prepared as well as the supported Pt-Cu nanoparticles were characterized by transmission elec- tron microscopy （TEM）, X-ray photoelectron spectroscopy （XPS）, fractal analysis and X-ray diffraction （XRD）. The dependence of methane combustion on the morphology and surface composition of Pt-Cu nanoparticles was analyzed based on the experimental results.展开更多
This work demonstrates the outstanding performance of alloyed Au1 Pt1 nanoparticles on hydrogen oxidation reaction(HOR)in alkaline solution.Due to the weakened hydrogen binding energy caused by uniform incorporation o...This work demonstrates the outstanding performance of alloyed Au1 Pt1 nanoparticles on hydrogen oxidation reaction(HOR)in alkaline solution.Due to the weakened hydrogen binding energy caused by uniform incorporation of Au,the alloyed Au1Pt1/C nanoparticles exhibit superior HOR activity than commercial PtRu/C.On the contrary,the catalytic performance of the phase-segregated Au2Pt1/C and Au1Pt1/C bimetallic nanoparticles in HOR is significantly worse.Moreover,Au1Pt1/C shows a remarkable durability with activity dropping only 4% after 3000 CV cycles,while performance attenuation of commercial PtRu/C is high up to 15% under the same condition.Our results indicate that the alloyed Au1Pt1/C is a promising candidate to substitute commercial PtRu/C for hydrogen oxidation reaction in alkaline electrolyte.展开更多
It is reported that the highly dispersed Pt nanoparticles on carbon nanotubes can be synthesized under mild conditions by in situ plasma treatment.The carbon nanotube was pretreated by O_2 plasma to transform into oxi...It is reported that the highly dispersed Pt nanoparticles on carbon nanotubes can be synthesized under mild conditions by in situ plasma treatment.The carbon nanotube was pretreated by O_2 plasma to transform into oxide carbon nanotubes（O-CNTs）,and then it was mixed with the precursors（the mixture of H_2 PtCl_6and PdCl_6）.After that,the O-CNTs and the precursors were simultaneously treated by H_2 plasma.The precursors were transformed into Pt-Pd nanoparticles（NPs）and the O-CNTs transformed into CNT.The synthesized CNT-based Pt-Pd nanoparticles were characterized by scanning electron microscopy,transmission electron microscopy,X-ray diffraction and X-ray photoelectron spectroscopy.All the analysis showed that the Pt-Pd nanoparticles were deposited on CNT as a form of face-centered cubical structure.展开更多
ABSTRACT Rationally designing broad-spectrum photocatalysts to harvest whole visible-light region photons and enhance solar energy conversion is a“holy grail”for researchers,but is still a challenging issue.Herein,b...ABSTRACT Rationally designing broad-spectrum photocatalysts to harvest whole visible-light region photons and enhance solar energy conversion is a“holy grail”for researchers,but is still a challenging issue.Herein,based on the common polymeric carbon nitride(PCN),a hybrid co-catalysts system comprising plasmonic Au nanoparticles(NPs)and atomically dispersed Pt single atoms(PtSAs)with different functions was constructed to address this challenge.For the dual co-catalysts decorated PCN(PtSAs–Au_(2.5)/PCN),the PCN is photoexcited to generate electrons under UV and short-wavelength visible light,and the synergetic Au NPs and PtSAs not only accelerate charge separation and transfer though Schottky junctions and metal-support bond but also act as the co-catalysts for H_(2) evolution.Furthermore,the Au NPs absorb long-wavelength visible light owing to its localized surface plasmon resonance,and the adjacent PtSAs trap the plasmonic hot-electrons for H_(2) evolution via direct electron transfer effect.Consequently,the PtSAs–Au_(2.5)/PCN exhibits excellent broad-spectrum photocatalytic H_(2) evolution activity with the H_(2) evolution rate of 8.8 mmol g^(−1) h^(−1) at 420 nm and 264μmol g^(−1) h^(−1) at 550 nm,much higher than that of Au_(2.5)/PCN and PtSAs–PCN,respectively.This work provides a new strategy to design broad-spectrum photocatalysts for energy conversion reaction.展开更多
Nanocollision electrochemistry is employed to evaluate the ORR’s activity of one single Pt nanoparticle,the effect of the size and ligand is investigated.The size-normalized activity of the Pt nanoparticle of 4 nm is...Nanocollision electrochemistry is employed to evaluate the ORR’s activity of one single Pt nanoparticle,the effect of the size and ligand is investigated.The size-normalized activity of the Pt nanoparticle of 4 nm is two times higher than that of 25 nm,confirming that the intrinsic activity does depend on the size of the nanoparticles.It is further found that the adsorbed ligand does yield effect on electrocatalysis,and the adsorption strength follows the order of PVP>CTAB>citrate.This work is of significance to understand the nature of the ORR’s electrocatalysis at the level of an individual entity,which makes the structure-activity correlation in a more reliable way.展开更多
In the electrochemical process,Pt nanoparticles(NPs)in Pt-based catalysts usually agglomerate due to Oswald ripening or lack of restraint,ultimately resulting in reduction of the active sites and catalytic efficiency....In the electrochemical process,Pt nanoparticles(NPs)in Pt-based catalysts usually agglomerate due to Oswald ripening or lack of restraint,ultimately resulting in reduction of the active sites and catalytic efficiency.How to uniformly disperse and firmly fix Pt NPs on carbon matrix with suitable particle size for catalysis is still a big challenge.Herein,to prevent the agglomeration and shedding of Pt NPs,Ni species is introduced and are evenly dispersed in the surface of carbon matrix in the form of Ni-N-C active sites(Ni ZIF-NC).The Ni sites can be used to anchor Pt NPs,and then effectively limit the further growth and agglomeration of Pt NPs during the reaction process.Compared with commercial Pt/C catalyst,Pt@Ni ZIF-NC,with ultralow Pt loading(7 wt%)and ideal particle size(2.3 nm),not only increases the active center,but also promotes the catalysis kinetics,greatly improving the ORR and HER catalytic activity.Under acidic conditions,its half-wave potential(0.902 V)is superior to commercial Pt/C(0.861 V),and the mass activity(0.38 A per mg Pt)at 0.9 V is 4.7 times that of Pt/C(0.08 A per mg Pt).Besides,it also shows outstanding HER performance.At 20 and 30 mV,its mass activity is even 2 and 6 times that of Pt/C,respectively.Whether it is under ORR or HER conditions,it still shows excellent durability.These undoubtedly indicate the realization of dual-functional catalysts with low-Pt and high-efficiency properties.展开更多
To obtain the electrocatalyst with an improved electrocatalytic performance towards formic acid electrooxidation(FAEO), a simple impregnation method is used to prepare Pt3Ni nanoparticles loaded on carbon black, assis...To obtain the electrocatalyst with an improved electrocatalytic performance towards formic acid electrooxidation(FAEO), a simple impregnation method is used to prepare Pt3Ni nanoparticles loaded on carbon black, assisted with electrochemically dealloying process. The X-ray powder diffraction(XRD) results as well as transmission electron microscopy(TEM) analysis of as-synthesized electrocatalyst demonstrates that the reduction temperature has a great influence on the FAEO activity of the dealloyed Pt3Ni nanoparticles. X-ray photoelectron spectroscopy(XPS) analyses confirm the variation in the electronic structure of platinum by incorporation of nickel atoms which reduces chemisorption of toxic carbon monoxide and promotes the dehydrogenation pathway of FAEO. The size of the dealloyed Pt3Ni nanoparticles remains within the range of about 2.7 nm. All electrochemical results illustrate that the performance of the asobtained electrocatalyst towards the FAEO is significantly enhanced. Moreover, the carbon black content,incorporation of Ni atoms, and reduction temperature conditions have been proven to be the key factors for modification of the crystal structure and morphology which leads to enhanced catalytic performance.展开更多
As a rapid uniform and efficient heating method, microwave irradiation has been widely used in chemical reaction and preparing nanomaterials. Here Pt/carbon nanotube(CNT) catalysts with w(Pt)=18.1% and 9.4 % were rapi...As a rapid uniform and efficient heating method, microwave irradiation has been widely used in chemical reaction and preparing nanomaterials. Here Pt/carbon nanotube(CNT) catalysts with w(Pt)=18.1% and 9.4 % were rapidly synthesized by microwave irradiation heating polyol process and employing the ethylene glycol solution of H 2PtCl 6 as the precursors in the presence of CNT support. TEM imaging showed that microwave-prepared Pt nanoparticles were very uniform in size, with an average size of 3.1 nm, and uniformly dispersed on the CNT surface. Electrochemical experiments demonstrated that microwave-synthesized Pt/CNT catalysts exhibited a higher catalytic activity for electrooxidation of liquid methanol than E-TEK Pt/C. The significant improvement in catalyst performance derives from that microwave-synthesized Pt nanoparticles have a uniform small particle size and uniforml dispersion on the CNT surface.展开更多
基金supported by the National Natural Science Foundation of China (Nos. 61675143, 11661131002)the Natural Science Foundation of Jiangsu Province (No. BK20160277)+2 种基金the Soochow University-Western University Joint Centre for Synchrotron Radiation Researchthe Collaborative Innovation Center of Suzhou Nano Science & Technologythe Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
文摘We present a straightforward physical approach for synthesizing multiwalled carbon nanotubes(CNTs)-Pd Au/Pt trimetallic nanoparticles(NPs), which allows predesign and control of the metal compositional ratio by simply adjusting the sputtering targets and conditions. The small-sized CNTs-Pd Au/Pt NPs(~3 nm, Pd/Au/Pt ratio of 3:1:2) act as nanocatalysts for the methanol oxidationreaction(MOR), showing excellent performance with electrocatalytic peak current of 4.4 A mg^(-1) Pt and high stability over 7000 s. The electrocatalytic activity and stability of the Pd Au/Pt trimetallic NPs are much superior to those of the corresponding Pd/Pt and Au/Pt bimetallic NPs,as well as a commercial Pt/C catalyst. Systematic investigation of the microscopic, crystalline, and electronic structure of the Pd Au/Pt NPs reveals alloying and charge redistribution in the Pd Au/Pt NPs, which are responsible for the promotion of the electrocatalytic performance.
基金supported by the National Basic Research Program of China(973 Program,Grant No.2012CB215500the National High-Tech Research and Development Program of China(863 Plan)(No.2012AA052002)the National Natural Science Foundation of China(No.21406024)
文摘Nafion-stabilized Pt nanoparticle colloidal solution is synthesized through ethylene glycol reduction.Pt/Nafion added with carbon black as electric conduction material（labeled Pt/Nafion-XC72） shows excellent electrochemical property compared with Pt/C.After a 300-cycle discharging durability test,the cell performance of membrane electrode assembly（MEA） with the Pt/Nafion-XC72 and Pt/C catalysts indicates a 29.9% and 92.2% decrease,respectively.The charge transfer resistances of Pt/Nafion-XC72 and Pt/C increase by 27.2% and 101.9%,respectively.The remaining electrochemically active surface area of Pt is about 61.7% in Pt/Nafion-XC72 and about 38.1% in Pt/C after the durability test.The particle size of Pt/C increases from about 5.1 nm to about 10.8 nm but only from 3.6 nm to 5.8 nm in the case of Pt/Nafion-XC72.These data suggest that Pt/Nafion-XC72 as a catalyst can enhance the durability of PEMFCs compared with Pt/C.
文摘Fine and well dispersed Pt-Cu bimetallic nanoparticles stabilized by polyvinyl pyrrolidone （PVP） were synthesized by alkaline polyol method. The molar ratio of Pt to Cu was 1 ： 1. Further, the Pt-Cu bimetallic nanoparticles were supported on alumina and their catalytic behavior in methane combustion was investigated. The as-prepared as well as the supported Pt-Cu nanoparticles were characterized by transmission elec- tron microscopy （TEM）, X-ray photoelectron spectroscopy （XPS）, fractal analysis and X-ray diffraction （XRD）. The dependence of methane combustion on the morphology and surface composition of Pt-Cu nanoparticles was analyzed based on the experimental results.
基金financially supported by the National Natural Science Foundation of China (Grants no. 21376283, 21436003 and 21576032)
文摘This work demonstrates the outstanding performance of alloyed Au1 Pt1 nanoparticles on hydrogen oxidation reaction(HOR)in alkaline solution.Due to the weakened hydrogen binding energy caused by uniform incorporation of Au,the alloyed Au1Pt1/C nanoparticles exhibit superior HOR activity than commercial PtRu/C.On the contrary,the catalytic performance of the phase-segregated Au2Pt1/C and Au1Pt1/C bimetallic nanoparticles in HOR is significantly worse.Moreover,Au1Pt1/C shows a remarkable durability with activity dropping only 4% after 3000 CV cycles,while performance attenuation of commercial PtRu/C is high up to 15% under the same condition.Our results indicate that the alloyed Au1Pt1/C is a promising candidate to substitute commercial PtRu/C for hydrogen oxidation reaction in alkaline electrolyte.
基金supported by National Natural Science Foundation of China(Nos.11305218,11575253)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2015262)+1 种基金the CASHIPS Director’s Fund(No.YZJJ201505)Anhui Provincial Natural Science Foundation for Distinguished Young Scholars of China(No.1608085J03)
文摘It is reported that the highly dispersed Pt nanoparticles on carbon nanotubes can be synthesized under mild conditions by in situ plasma treatment.The carbon nanotube was pretreated by O_2 plasma to transform into oxide carbon nanotubes（O-CNTs）,and then it was mixed with the precursors（the mixture of H_2 PtCl_6and PdCl_6）.After that,the O-CNTs and the precursors were simultaneously treated by H_2 plasma.The precursors were transformed into Pt-Pd nanoparticles（NPs）and the O-CNTs transformed into CNT.The synthesized CNT-based Pt-Pd nanoparticles were characterized by scanning electron microscopy,transmission electron microscopy,X-ray diffraction and X-ray photoelectron spectroscopy.All the analysis showed that the Pt-Pd nanoparticles were deposited on CNT as a form of face-centered cubical structure.
基金supported by the National Natural Science Foundation of China(Grant No.51871078 and 52071119)Interdisciplinary Research Foundation of HIT(Grant No.IR2021208)+1 种基金State Key Laboratory of Urban Water Resource and Environment(Harbin Institute of Technology)(No.2022TS38)Heilongjiang Science Foundation(No.LH2020B006).
文摘ABSTRACT Rationally designing broad-spectrum photocatalysts to harvest whole visible-light region photons and enhance solar energy conversion is a“holy grail”for researchers,but is still a challenging issue.Herein,based on the common polymeric carbon nitride(PCN),a hybrid co-catalysts system comprising plasmonic Au nanoparticles(NPs)and atomically dispersed Pt single atoms(PtSAs)with different functions was constructed to address this challenge.For the dual co-catalysts decorated PCN(PtSAs–Au_(2.5)/PCN),the PCN is photoexcited to generate electrons under UV and short-wavelength visible light,and the synergetic Au NPs and PtSAs not only accelerate charge separation and transfer though Schottky junctions and metal-support bond but also act as the co-catalysts for H_(2) evolution.Furthermore,the Au NPs absorb long-wavelength visible light owing to its localized surface plasmon resonance,and the adjacent PtSAs trap the plasmonic hot-electrons for H_(2) evolution via direct electron transfer effect.Consequently,the PtSAs–Au_(2.5)/PCN exhibits excellent broad-spectrum photocatalytic H_(2) evolution activity with the H_(2) evolution rate of 8.8 mmol g^(−1) h^(−1) at 420 nm and 264μmol g^(−1) h^(−1) at 550 nm,much higher than that of Au_(2.5)/PCN and PtSAs–PCN,respectively.This work provides a new strategy to design broad-spectrum photocatalysts for energy conversion reaction.
基金jointly supported by the National Natural Science Foundation of China(Nos.21903026,21975081,21975079,21676106)Science and Technology Program of Guangdong Province(2017A050506015)+2 种基金Science and Technology Program of Guangzhou(201704030065)China Postdoctoral Science Foundation(2019M652877)the Fundamental Research Funds for the Central Universities。
文摘Nanocollision electrochemistry is employed to evaluate the ORR’s activity of one single Pt nanoparticle,the effect of the size and ligand is investigated.The size-normalized activity of the Pt nanoparticle of 4 nm is two times higher than that of 25 nm,confirming that the intrinsic activity does depend on the size of the nanoparticles.It is further found that the adsorbed ligand does yield effect on electrocatalysis,and the adsorption strength follows the order of PVP>CTAB>citrate.This work is of significance to understand the nature of the ORR’s electrocatalysis at the level of an individual entity,which makes the structure-activity correlation in a more reliable way.
基金supported by the National Natural Science Foundation of China(22075223,51701146)the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing(Wuhan University of Technology)(2021-ZD-4)。
文摘In the electrochemical process,Pt nanoparticles(NPs)in Pt-based catalysts usually agglomerate due to Oswald ripening or lack of restraint,ultimately resulting in reduction of the active sites and catalytic efficiency.How to uniformly disperse and firmly fix Pt NPs on carbon matrix with suitable particle size for catalysis is still a big challenge.Herein,to prevent the agglomeration and shedding of Pt NPs,Ni species is introduced and are evenly dispersed in the surface of carbon matrix in the form of Ni-N-C active sites(Ni ZIF-NC).The Ni sites can be used to anchor Pt NPs,and then effectively limit the further growth and agglomeration of Pt NPs during the reaction process.Compared with commercial Pt/C catalyst,Pt@Ni ZIF-NC,with ultralow Pt loading(7 wt%)and ideal particle size(2.3 nm),not only increases the active center,but also promotes the catalysis kinetics,greatly improving the ORR and HER catalytic activity.Under acidic conditions,its half-wave potential(0.902 V)is superior to commercial Pt/C(0.861 V),and the mass activity(0.38 A per mg Pt)at 0.9 V is 4.7 times that of Pt/C(0.08 A per mg Pt).Besides,it also shows outstanding HER performance.At 20 and 30 mV,its mass activity is even 2 and 6 times that of Pt/C,respectively.Whether it is under ORR or HER conditions,it still shows excellent durability.These undoubtedly indicate the realization of dual-functional catalysts with low-Pt and high-efficiency properties.
基金supported by the National Natural Science Foundation of China(No.51602209)the Provincial Nature Science Foundation of Sichuan(No.2016GZ0423,2017CC0017,2018FZ0105)the Fundamental Research Funds supported by Ministry of Education of the People’s Republic of China(No.YJ201746,2018SCUH0025)
文摘To obtain the electrocatalyst with an improved electrocatalytic performance towards formic acid electrooxidation(FAEO), a simple impregnation method is used to prepare Pt3Ni nanoparticles loaded on carbon black, assisted with electrochemically dealloying process. The X-ray powder diffraction(XRD) results as well as transmission electron microscopy(TEM) analysis of as-synthesized electrocatalyst demonstrates that the reduction temperature has a great influence on the FAEO activity of the dealloyed Pt3Ni nanoparticles. X-ray photoelectron spectroscopy(XPS) analyses confirm the variation in the electronic structure of platinum by incorporation of nickel atoms which reduces chemisorption of toxic carbon monoxide and promotes the dehydrogenation pathway of FAEO. The size of the dealloyed Pt3Ni nanoparticles remains within the range of about 2.7 nm. All electrochemical results illustrate that the performance of the asobtained electrocatalyst towards the FAEO is significantly enhanced. Moreover, the carbon black content,incorporation of Ni atoms, and reduction temperature conditions have been proven to be the key factors for modification of the crystal structure and morphology which leads to enhanced catalytic performance.
文摘As a rapid uniform and efficient heating method, microwave irradiation has been widely used in chemical reaction and preparing nanomaterials. Here Pt/carbon nanotube(CNT) catalysts with w(Pt)=18.1% and 9.4 % were rapidly synthesized by microwave irradiation heating polyol process and employing the ethylene glycol solution of H 2PtCl 6 as the precursors in the presence of CNT support. TEM imaging showed that microwave-prepared Pt nanoparticles were very uniform in size, with an average size of 3.1 nm, and uniformly dispersed on the CNT surface. Electrochemical experiments demonstrated that microwave-synthesized Pt/CNT catalysts exhibited a higher catalytic activity for electrooxidation of liquid methanol than E-TEK Pt/C. The significant improvement in catalyst performance derives from that microwave-synthesized Pt nanoparticles have a uniform small particle size and uniforml dispersion on the CNT surface.
基金supported by the Program for Changjiang Scholars and Innovative Research Team in University,China(PCSIRT)Hunan Provincial Natural Science Foundation,China(12JJ2010)+1 种基金Young Teachers Growth Plan(2012)Specialized Research Fund for the Doctoral Program of Higher Education,China(20110161110009)~~
