Pseudo-Pt Monolayer for Robust Hydrogen Oxidation.

Heteroepitaxial core-shell structure is conducive to combining the advantages of the epilayer and the substrate, creating a novel multifunctionality for catalysis application. Herein, we report a pseudomorphic-Pt atomic layer (PmPt) epitaxially growing on an IrPd-core matrix (PmPt@IrPd/C) as an efficient and stable catalyst for alkaline hydrogen oxidation reaction that exhibits ∼29.2 times more mass activity enhancement than that of benchmark Pt/C. The PmPt@IrPd/C catalyst also gives rise to ∼25.0 times more enhancement than Pt/C during a 50,000-cycle accelerated stability test. This robust stability originates from the resistance to carbon corrosion owing to the stronger H2O interaction instead of carbon oxide (COx) poison species, and the modulated hydroxyl (OH*) adsorption could inhibit the OH* species from shuffling the surface Pt atoms away from the substrate. Moreover, the anion-exchange membrane fuel cells assembled by PmPt@IrPd/C with an ultralow Pt loading of 0.009 mgPt cm-2 in the anode can deliver a power density of 1.27 W cm-2.

[1]  M. Zachman,et al.  Atomically dispersed iron sites with a nitrogen–carbon coating as highly active and durable oxygen reduction catalysts for fuel cells , 2022, Nature Energy.

[2]  Dingsheng Wang,et al.  Understanding the structure-performance relationship of active sites at atomic scale , 2022, Nano Research.

[3]  Jeremy L. Hitt,et al.  Electrocatalysis in Alkaline Media and Alkaline Membrane-Based Energy Technologies. , 2022, Chemical reviews.

[4]  Zhenxing Feng,et al.  Improving Pd–N–C fuel cell electrocatalysts through fluorination-driven rearrangements of local coordination environment , 2021, Nature Energy.

[5]  Licheng Sun,et al.  Engineering lattice oxygen activation of iridium clusters stabilized on amorphous bimetal borides array for oxygen evolution reaction. , 2021, Angewandte Chemie.

[6]  Dingsheng Wang,et al.  Design concept for electrocatalysts , 2021, Nano Research.

[7]  Xueping Qin,et al.  The role of ruthenium in improving the kinetics of hydrogen oxidation and evolution reactions of platinum , 2021, Nature Catalysis.

[8]  Lun Pan,et al.  Pt/Fe2O3 with Pt–Fe pair sites as a catalyst for oxygen reduction with ultralow Pt loading , 2021, Nature Energy.

[9]  Jaewook Shin,et al.  Boosting the Role of Ir in Mitigating Corrosion of Carbon Support by Alloying with Pt , 2020 .

[10]  Dario R. Dekel,et al.  Improved Hydrogen Oxidation Reaction Activity and Stability of Buried Metal-Oxide Electrocatalyst Interfaces , 2020, Chemistry of Materials.

[11]  M. Chatenet,et al.  Recent Advances in the Understanding of Nickel-Based Catalysts for the Oxidation of Hydrogen-Containing Fuels in Alkaline Media , 2020, ACS Catalysis.

[12]  D. Papageorgopoulos,et al.  Perspective—The Next Decade of AEMFCs: Near-Term Targets to Accelerate Applied R&D , 2020 .

[13]  Zidong Wei,et al.  Lattice-confined Ru clusters with high CO tolerance and activity for the hydrogen oxidation reaction , 2020, Nature Catalysis.

[14]  Hao Ming Chen,et al.  Efficient hydrogen oxidation catalyzed by strain-engineered nickel nanoparticles. , 2020, Angewandte Chemie.

[15]  W. Mustain,et al.  Catalytic Advantages, Challenges, and Priorities in Alkaline Membrane Fuel Cells , 2020 .

[16]  Yushan Yan,et al.  Understanding the pH Dependence of Underpotential Deposited Hydrogen on Platinum. , 2019, Angewandte Chemie.

[17]  S. Mukerjee,et al.  Alkaline Anion-Exchange Membrane Fuel Cells: Challenges in Electrocatalysis and Interfacial Charge Transfer. , 2019, Chemical reviews.

[18]  Shengli Chen,et al.  Boosting Hydrogen Oxidation Activity of Ni in Alkaline Media through Oxygen‐Vacancy‐Rich CeO 2 /Ni Heterostructures , 2019, Angewandte Chemie.

[19]  M. Zhang,et al.  Enhanced electrocatalytic hydrogen oxidation on Ni/NiO/C derived from a Ni-based MOF. , 2019, Angewandte Chemie.

[20]  F. Maillard,et al.  Degradation of Carbon-Supported Platinum-Group-Metal Electrocatalysts in Alkaline Media Studied by in Situ Fourier Transform Infrared Spectroscopy and Identical-Location Transmission Electron Microscopy , 2019, ACS Catalysis.

[21]  Pengcheng Zhao,et al.  Hydrogen Evolution and Oxidation: Mechanistic Studies and Material Advances , 2019, Advanced materials.

[22]  L. Zhuang,et al.  The Comparability of Pt to Pt-Ru in Catalyzing the Hydrogen Oxidation Reaction for Alkaline Polymer Electrolyte Fuel Cells Operated at 80 °C. , 2019, Angewandte Chemie.

[23]  Wei Li,et al.  Interfacing nickel nitride and nickel boosts both electrocatalytic hydrogen evolution and oxidation reactions , 2018, Nature Communications.

[24]  Dario R. Dekel,et al.  Electrocatalysts for Hydrogen Oxidation Reaction in Alkaline Electrolytes , 2018, ACS Catalysis.

[25]  Dario R. Dekel,et al.  Anion exchange membrane fuel cells: Current status and remaining challenges , 2018 .

[26]  Dario R. Dekel.  Review of cell performance in anion exchange membrane fuel cells , 2018 .

[27]  Dario R. Dekel,et al.  Accelerated Stress Test of Pt/C Nanoparticles in an Interface with an Anion-Exchange Membrane—An Identical-Location Transmission Electron Microscopy Study , 2018 .

[28]  H. Abruña,et al.  IrPdRu/C as H2 Oxidation Catalysts for Alkaline Fuel Cells. , 2017, Journal of the American Chemical Society.

[29]  Siqi Lu,et al.  Investigating the Influences of the Adsorbed Species on Catalytic Activity for Hydrogen Oxidation Reaction in Alkaline Electrolyte. , 2017, Journal of the American Chemical Society.

[30]  Colin F. Dickens,et al.  Combining theory and experiment in electrocatalysis: Insights into materials design , 2017, Science.

[31]  Brian P. Setzler,et al.  Activity targets for nanostructured platinum-group-metal-free catalysts in hydroxide exchange membrane fuel cells. , 2016, Nature nanotechnology.

[32]  Dario R. Dekel,et al.  A Pd/C-CeO2 Anode Catalyst for High-Performance Platinum-Free Anion Exchange Membrane Fuel Cells. , 2016, Angewandte Chemie.

[33]  Yushan Yan,et al.  Universal dependence of hydrogen oxidation and evolution reaction activity of platinum-group metals on pH and hydrogen binding energy , 2016, Science Advances.

[34]  Dionisios G. Vlachos,et al.  Nickel supported on nitrogen-doped carbon nanotubes as hydrogen oxidation reaction catalyst in alkaline electrolyte , 2016, Nature Communications.

[35]  R. Hennig,et al.  Implicit self-consistent electrolyte model in plane-wave density-functional theory. , 2016, The Journal of chemical physics.

[36]  P. Atanassov,et al.  Instability Of Commercial Pt/C And Pd/C Electrocatalysts In Alkaline Media , 2015 .

[37]  N. Sergent,et al.  Huge Instability of Pt/C Catalysts in Alkaline Medium , 2015 .

[38]  Jingguang G. Chen,et al.  Correlating hydrogen oxidation and evolution activity on platinum at different pH with measured hydrogen binding energy , 2015, Nature Communications.

[39]  Kendra Letchworth-Weaver,et al.  Implicit solvation model for density-functional study of nanocrystal surfaces and reaction pathways. , 2013, The Journal of chemical physics.

[40]  Bryan S. Pivovar,et al.  Platinum-coated copper nanowires with high activity for hydrogen oxidation reaction in base. , 2013, Journal of the American Chemical Society.

[41]  Yuta Yamamoto,et al.  Size specifically high activity of Ru nanoparticles for hydrogen oxidation reaction in alkaline electrolyte. , 2013, Journal of the American Chemical Society.

[42]  Hansung Kim,et al.  Effect of water electrolysis catalysts on carbon corrosion in polymer electrolyte membrane fuel cells. , 2010, Journal of the American Chemical Society.

[43]  G. Kresse,et al.  Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set , 1996 .

[44]  I. Zenyuk,et al.  Hot topics in alkaline exchange membrane fuel cells , 2018 .