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Title: Core-Shell Structuring of Pure Metallic Aerogels towards Highly Efficient Platinum Utilization for the Oxygen Reduction Reaction

Journal Article · · Angewandte Chemie (International Edition)
 [1];  [2];  [3];  [4];  [3];  [4];  [3];  [5];  [3]; ORCiD logo [4]
  1. Technische Univ. Dresden (Germany); Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Helmholtz-Zentrum Dresden-Rossendorf, (Germany)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Technische Univ. Dresden (Germany)
  5. Leibniz Inst. for Solid State and Materials Research (IFW), Dresden (Germany)

Abstract The development of core–shell structures remains a fundamental challenge for pure metallic aerogels. Here we report the synthesis of Pd x Au‐Pt core–shell aerogels composed of an ultrathin Pt shell and a composition‐tunable Pd x Au alloy core. The universality of this strategy ensures the extension of core compositions to Pd transition‐metal alloys. The core–shell aerogels exhibited largely improved Pt utilization efficiencies for the oxygen reduction reaction and their activities show a volcano‐type relationship as a function of the lattice parameter of the core substrate. The maximum mass and specific activities are 5.25 A mg Pt −1 and 2.53 mA cm −2 , which are 18.7 and 4.1 times higher than those of Pt/C, respectively, demonstrating the superiority of the core–shell metallic aerogels. The proposed core‐based activity descriptor provides a new possible strategy for the design of future core–shell electrocatalysts.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012704
OSTI ID:
1425037
Alternate ID(s):
OSTI ID: 1419897
Report Number(s):
BNL-200018-2018-JAAM
Journal Information:
Angewandte Chemie (International Edition), Vol. 57, Issue 11; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 118 works
Citation information provided by
Web of Science

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Emerging Hierarchical Aerogels: Self-Assembly of Metal and Semiconductor Nanocrystals journal June 2018
Promoting Electrocatalysis upon Aerogels journal December 2018
Engineering Self‐Supported Noble Metal Foams Toward Electrocatalysis and Beyond journal August 2019
Oxygen Reduction Reactions on Single‐ or Few‐Atom Discrete Active Sites for Heterogeneous Catalysis journal September 2019
Engineering Multimetallic Aerogels for pH‐Universal HER and ORR Electrocatalysis journal March 2020
Promoting the Electrocatalytic Performance of Noble Metal Aerogels by Ligand‐Directed Modulation journal January 2020
Promoting the Electrocatalytic Performance of Noble Metal Aerogels by Ligand‐Directed Modulation journal January 2020
Mechanism on The Disproportionating Synthesis of Dichlorodimethyl‐ silane by ZSM‐5(5 T)@γ‐Al 2 O 3 Series Core‐Shell Catalysts journal December 2019
Design of Noble Metal Electrocatalysts on an Atomic Level journal October 2018
Surface Atomic Regulation of Core–Shell Noble Metal Catalysts journal January 2019
Atomically Dispersed Pt on Screw‐like Pd/Au Core‐shell Nanowires for Enhanced Electrocatalysis journal October 2019
Pt Islands on 3 D Nut-like PtAg Nanocrystals for Efficient Formic Acid Oxidation Electrocatalysis journal February 2018
Versatile Aerogels for Sensors journal September 2019
Modulating the Electronic Structure of Single‐Atom Catalysts on 2D Nanomaterials for Enhanced Electrocatalytic Performance journal March 2019
Preparation of an ultrathin Pt electrocatalyst via a galvanic replacement reaction of electrodeposited CuCl for the oxidation of methanol in an alkaline medium journal January 2018
Au@ h -Al 2 O 3 analogic yolk–shell nanocatalyst for highly selective synthesis of biomass-derived d -xylonic acid via regulation of structure effects journal January 2018
pH-Dependent growth of atomic Pd layers on trisoctahedral gold nanoparticles to realize enhanced performance in electrocatalysis and chemical catalysis journal January 2018
Facile synthesis of monodispersed yolk-shelled molybdenum disulfide microspheres with enhanced photocatalytic properties journal January 2018
Ternary PtRuCu aerogels for enhanced methanol electrooxidation journal January 2019
Versatile route to core–shell reinforced network nanostructures journal January 2019
Leaching- and sintering-resistant hollow or structurally ordered intermetallic PtFe alloy catalysts for oxygen reduction reactions journal January 2019
Single iron atoms stabilized by microporous defects of biomass-derived carbon aerogels as high-performance cathode electrocatalysts for aluminum–air batteries journal January 2019
Fabrication of Au aerogels with {110}-rich facets by size-dependent surface reconstruction for enzyme-free glucose detection journal January 2019
Galvanic replacement induced electromotive force to propel Janus micromotors journal April 2019
Platinum as an electrocatalyst: effect of morphological aspects of Pt/Pt-based materials journal July 2018
Specific ion effects directed noble metal aerogels: Versatile manipulation for electrocatalysis and beyond journal May 2019
Fast Cryomediated Dynamic Equilibrium Hydrolysates towards Grain Boundary-Enriched Platinum Scaffolds for Efficient Methanol Oxidation journal October 2019
Versatile route to core-shell reinforced network nanostructures other January 2019