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Title: PdMo bimetallene for oxygen reduction catalysis

Journal Article · · Nature (London)
 [1];  [2];  [3];  [3];  [3];  [3];  [3];  [2];  [4];  [3];  [5];  [3];  [4];  [2];  [6]
  1. Peking Univ., Beijing (China). College of Engineering, Dept. of Materials Science and Engineering; Peking Univ., Beijing (China). College of Engineering, BIC-ESAT
  2. California State Univ. (CalState), Long Beach, CA (United States)
  3. Peking Univ., Beijing (China). College of Engineering, Dept. of Materials Science and Engineering
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  5. Chinese Academy of Sciences (CAS), Shanghai (China). Shanghai Synchrotron Radiation Facility, Shanghai Inst. of Applied Physics
  6. Peking Univ., Beijing (China). College of Engineering, Dept. of Materials Science and Engineering; Peking Univ., Beijing (China). College of Engineering, BIC-ESAT; Peking Univ., Beijing (China). Dept. of Energy and Resources Engineering; Peking Univ., Beijing (China). College of Engineering, Key Lab. of Theory and Technology of Advanced Batteries Materials

The efficient interconversion of chemicals and electricity through electrocatalytic processes is central to many renewable-energy initiatives. The sluggish kinetics of the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) has long posed one of the biggest challenges in this field, and electrocatalysts based on expensive platinum-group metals are often required to improve the activity and durability of these reactions. The use of alloyingsurface strain and optimized coordination environments has resulted in platinum-based nanocrystals that enable very high ORR activities in acidic media; however, improving the activity of this reaction in alkaline environments remains challenging because of the difficulty in achieving optimized oxygen binding strength on platinum-group metals in the presence of hydroxide. Here we show that PdMo bimetallene—a palladium–molybdenum alloy in the form of a highly curved and sub-nanometre-thick metal nanosheet—is an efficient and stable electrocatalyst for the ORR and the OER in alkaline electrolytes, and shows promising performance as a cathode in Zn–air and Li–air batteries. The thin-sheet structure of PdMo bimetallene enables a large electrochemically active surface area (138.7 square metres per gram of palladium) as well as high atomic utilization, resulting in a mass activity towards the ORR of 16.37 amperes per milligram of palladium at 0.9 volts versus the reversible hydrogen electrode in alkaline electrolytes. This mass activity is 78 times and 327 times higher than those of commercial Pt/C and Pd/C catalysts, respectively, and shows little decay after 30,000 potential cycles. Density functional theory calculations reveal that the alloying effect, the strain effect due to the curved geometry, and the quantum size effect due to the thinness of the sheets tune the electronic structure of the system for optimized oxygen binding. Finally, given the properties and the structure–activity relationships of PdMo metallene, we suggest that other metallene materials could show great promise in energy electrocatalysis.

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:
1570667
Report Number(s):
BNL-212186-2019-JAAM
Journal Information:
Nature (London), Vol. 574, Issue 7776; ISSN 0028-0836
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 604 works
Citation information provided by
Web of Science

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Precious metal nanocrystals for renewable energy electrocatalysis: structural design and controlled synthesis journal January 2020
Ultrathin Pd-based nanosheets: syntheses, properties and applications journal January 2020
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Ultrahigh Surface Area Three-Dimensional Porous Graphitic Carbon from Conjugated Polymeric Molecular Framework journal May 2015
Carbon Nanomaterials for Energy and Biorelated Catalysis: Recent Advances and Looking Forward journal February 2019
Effect of Intrinsic Properties of Anions on the Electrocatalytic Activity of NiCo2O4 and NiCo2OxS4–x Grown by Chemical Bath Deposition journal August 2018
Facile Synthesis of 3d Transition-Metal-Doped α-Co(OH)2 Nanomaterials in Water–Methanol Mediated with Ammonia for Oxygen Evolution Reaction journal September 2019
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A surface-modified antiperovskite as an electrocatalyst for water oxidation journal June 2018
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Atomically dispersed nickel–nitrogen–sulfur species anchored on porous carbon nanosheets for efficient water oxidation journal March 2019
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Bifunctional hydrous RuO2 nanocluster electrocatalyst embedded in carbon matrix for efficient and durable operation of rechargeable zinc–air batteries journal August 2017
Ultrahigh Oxygen Reduction Reaction Electrocatalytic Activity and Stability over Hierarchical Nanoporous N-doped Carbon journal February 2018
A Facile Approach to Prepare Multiple Heteroatom-Doped Carbon Materials from Imine-Linked Porous Organic Polymers journal March 2018
Porous Carbon Networks Derived From Graphitic Carbon Nitride for Efficient Oxygen Reduction Reaction journal July 2019
Recent developments of nano-structured materials as the catalysts for oxygen reduction reaction journal April 2018
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Nitrogen-Doped Superporous Activated Carbons as Electrocatalysts for the Oxygen Reduction Reaction journal April 2019
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