Ruthenium has been hailed as a competitive alternative for platinum toward hydrogen evolution reaction(HER),a critical process in electrochemical water splitting.In this study,we successfully prepare metallic Ru nanop...Ruthenium has been hailed as a competitive alternative for platinum toward hydrogen evolution reaction(HER),a critical process in electrochemical water splitting.In this study,we successfully prepare metallic Ru nanoparticles supported on carbon paper by utilizing a novel magnetic induction heating(MIH)method.The samples are obtained within seconds,featuring a Cl-enriched surface that is unattainable via conventional thermal annealing.The best sample within the series shows a remarkable HER activity in both acidic and alkaline media with an overpotential of only-23 and-12 mV to reach the current density of 10 mA/cm^(2),highly comparable to that of the Pt/C benchmark.Theoretical studies based on density functional theory show that the excellent electrocatalytic activity is accounted by the surface metal-Cl species that facilitate charge transfer and downshift the d-band center.Results from this study highlight the unique advantages of MIH in rapid sample preparation,where residual anion ligands play a critical role in manipulating the electronic properties of the metal surfaces and the eventual electrocatalytic activity.展开更多
Oxygen reduction reaction(ORR)plays an important role in dictating the performance of various electrochemical energy technologies.As platinum nanoparticles have served as the catalysts of choice towards ORR,minimizing...Oxygen reduction reaction(ORR)plays an important role in dictating the performance of various electrochemical energy technologies.As platinum nanoparticles have served as the catalysts of choice towards ORR,minimizing the cost of the catalysts by diminishing the platinum nanoparticle size has become a critical route to advancing the technological development.Herein,first-principle calculations show that carbon-supported Pt9 clusters represent the threshold domain size,and the ORR activity can be significantly improved by doping of adjacent cobalt atoms.This is confirmed experimentally,where platinum and cobalt are dispersed in nitrogen-doped carbon nanowires in varied forms,single atoms,few-atom clusters,and nanoparticles,depending on the initial feeds.The sample consisting primarily of Pt_(2~7)clusters doped with atomic Co species exhibits the best mass activity among the series,with a current density of 4:16Amg^(-1)_(Pt)at+0.85V vs.RHE that is almost 50 times higher than that of commercial Pt/C.展开更多
Carbon-supported nanocomposites are attracting particular attention as high-performance,low-cost electrocatalysts for electrochemical water splitting.These are mostly prepared by pyrolysis and hydrothermal procedures ...Carbon-supported nanocomposites are attracting particular attention as high-performance,low-cost electrocatalysts for electrochemical water splitting.These are mostly prepared by pyrolysis and hydrothermal procedures that are time-consuming(from hours to days)and typically difficult to produce a nonequilibrium phase.Herein,for the first time ever,we exploit magnetic induction heating-quenching for ultrafast production of carbon-FeNi spinel oxide nanocomposites(within seconds),which exhibit an unprecedentedly high performance towards oxygen evolution reaction(OER),with an ultralow overpotential of only+260 mV to reach the high current density of 100 mA cm^(-2).Experimental and theoretical studies show that the rapid heating and quenching process(ca.10^(3)K s^(-1))impedes the Ni and Fe phase segregation and produces a Cl-rich surface,both contributing to the remarkable catalytic activity.Results from this study highlight the unique advantage of ultrafast heating/quenching in the structural engineering of functional nanocomposites to achieve high electrocatalytic performance towards important electrochemical reactions.展开更多
基金National Science Foundation,Grant/Award Numbers:CHE-1900235,CHE-2003685Office of Science,Office of Basic Energy Sciences,of the U.S.Department of Energy,Grant/Award Number:DE-AC02-05CH11231+3 种基金U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences,Grant/Award Number:DE-AC02-76SF00515NSF MRI program,Grant/Award Number:AST-1828315Grant-in-Aid of Research,Grant/Award Number:G20211001-639National Academy of Sciences,administered by Sigma Xi,The Scientific Research Society。
文摘Ruthenium has been hailed as a competitive alternative for platinum toward hydrogen evolution reaction(HER),a critical process in electrochemical water splitting.In this study,we successfully prepare metallic Ru nanoparticles supported on carbon paper by utilizing a novel magnetic induction heating(MIH)method.The samples are obtained within seconds,featuring a Cl-enriched surface that is unattainable via conventional thermal annealing.The best sample within the series shows a remarkable HER activity in both acidic and alkaline media with an overpotential of only-23 and-12 mV to reach the current density of 10 mA/cm^(2),highly comparable to that of the Pt/C benchmark.Theoretical studies based on density functional theory show that the excellent electrocatalytic activity is accounted by the surface metal-Cl species that facilitate charge transfer and downshift the d-band center.Results from this study highlight the unique advantages of MIH in rapid sample preparation,where residual anion ligands play a critical role in manipulating the electronic properties of the metal surfaces and the eventual electrocatalytic activity.
基金This work was supported in part by the National Science Foundation(CHE-1900235 and CHE-2003685,S.C.)B.L.acknowledges support of a Chancellor’s Dissertation Year Fellowship from University of California,Santa Cruz and a Sigma Xi student grant-in-aid(G201903158663319)+8 种基金Y.P.acknowledges support of the National Science Foundation(DMR-1760260 and CHE-1904547)P.G.acknowledges support of the National Natural Science Foundation of China(51672007 and 11974023)the Key-Area Research and Development Program of Guangdong Province(2018B030327001 and 2018B010109009)This work partially used the Extreme Science and Engineering Discovery Environment(XSEDE)[64]which is supported by National Science Foundation grant number ACI-1548562the lux supercomputer at UC Santa Cruz,funded by NSF MRI grant AST 1828315the Nion U-HERMS200 microscope in the Electron Microscopy Laboratory(EML)of Peking UniversityThis research also used resources of the Advanced Photon Source,an Office of Science User Facility operated for the US Department of Energy(DOE)Office of Science by Argonne National Laboratory,and was supported by the US Department of Energy under contract No.DE-AC02-06CH11357 and the Canadian Light Source(CLS)and its funding partnersThe CLS is supported by the CFI,NSERC,National Research Council Canada,CIHR,the University of Saskatchewan,the Government of Saskatchewan,and Western Economic Diversification Canada.Part of the TEM and XPS work was performed at the Molecular Foundry and National Center for Electron Microscopy,Lawrence Berkeley National Laboratory,which is supported by the US DOE,as part of a user project。
文摘Oxygen reduction reaction(ORR)plays an important role in dictating the performance of various electrochemical energy technologies.As platinum nanoparticles have served as the catalysts of choice towards ORR,minimizing the cost of the catalysts by diminishing the platinum nanoparticle size has become a critical route to advancing the technological development.Herein,first-principle calculations show that carbon-supported Pt9 clusters represent the threshold domain size,and the ORR activity can be significantly improved by doping of adjacent cobalt atoms.This is confirmed experimentally,where platinum and cobalt are dispersed in nitrogen-doped carbon nanowires in varied forms,single atoms,few-atom clusters,and nanoparticles,depending on the initial feeds.The sample consisting primarily of Pt_(2~7)clusters doped with atomic Co species exhibits the best mass activity among the series,with a current density of 4:16Amg^(-1)_(Pt)at+0.85V vs.RHE that is almost 50 times higher than that of commercial Pt/C.
基金This work was supported by grants from the National Science Foundation(CHE-1900235 and CHE-2003685,S.W.C.and CHE-1900401,H.L.X.)Part of the TEM and XPS work was carried out at the National Center for Electron Microscopy and Molecular Foundry,Lawrence Berkeley National Laboratory,which is supported by the Office of Science,Office of Basic Energy Sciences,of U.S.Department of Energy under Contract No.DE-AC02-05CH11231,as part of a user project.The XAS work used resources of the Advanced Photon Source,a User Facility operated for the U.S.Department of Energy(DOE)Office of Science by Argonne National Laboratory and was supported by the DOE under contract No.DE-AC02-06CH11357 and the Canadian Light Source and its funding partners+1 种基金This research also used resources of the Center for Functional Nanomaterials(CFN),which is a U.S.Department of Energy Office of Science User Facility,at Brookhaven National Laboratory under Contract No.DE-SC0012704The authors also thank Mr.Jeremy Barnett for the assistance in sample preparation and data acquisition of X-ray diffraction measurements in the UCSC X-ray Facility which was funded by the National Science Foundation(MRI-1126845).
文摘Carbon-supported nanocomposites are attracting particular attention as high-performance,low-cost electrocatalysts for electrochemical water splitting.These are mostly prepared by pyrolysis and hydrothermal procedures that are time-consuming(from hours to days)and typically difficult to produce a nonequilibrium phase.Herein,for the first time ever,we exploit magnetic induction heating-quenching for ultrafast production of carbon-FeNi spinel oxide nanocomposites(within seconds),which exhibit an unprecedentedly high performance towards oxygen evolution reaction(OER),with an ultralow overpotential of only+260 mV to reach the high current density of 100 mA cm^(-2).Experimental and theoretical studies show that the rapid heating and quenching process(ca.10^(3)K s^(-1))impedes the Ni and Fe phase segregation and produces a Cl-rich surface,both contributing to the remarkable catalytic activity.Results from this study highlight the unique advantage of ultrafast heating/quenching in the structural engineering of functional nanocomposites to achieve high electrocatalytic performance towards important electrochemical reactions.
