Skip to main content
OSTI.GOVU.S. Department of Energy Office of Scientific and Technical Information
U.S. Department of Energy
Office of Scientific and Technical Information
 

Single-atom Rh/N-doped carbon electrocatalyst for formic acid oxidation

Journal Article · · Nature Nanotechnology
 [1];  [2];  [3];  [4];  [4];  [5];  [4];  [6];  [6];  [7];  [8];  [9];  [10];  [11];  [8];  [9];  [12];  [12];  [4];  [4] more »;  [3];  [4];  [4] « less
  1. Tsinghua Univ., Beijing (China); Central South Univ., Changsha (China)
  2. Chinese Academy of Sciences (CAS), Beijing (China). Inst. of High Energy Physics, Beijing Synchrotron Radiation Facility
  3. Xi’an Jiaotong Univ. (China)
  4. Tsinghua Univ., Beijing (China)
  5. Chinese Academy of Science (CAS), Shanghai (China). Shanghai Inst. of Applied Physics, Shanghai Synchrotron Radiation Facilities
  6. Chinese Academy of Sciences, Changchun (China). Changchun Inst. of Applied Chemistry; Jilin Province Key Lab. of Low Carbon Chemical Power Sources, Changchun (China)
  7. Beijing Univ. of Chemical Technology (China)
  8. Xiamen Univ. (China)
  9. Wuhan Univ. (China)
  10. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  11. Chinese Academy of Sciences (CAS), Beijing (China). Beijing National Lab. for Condensed Matter Physics,
  12. Central South Univ., Changsha (China)
+ Show Author Affiliations
To meet the requirements of potential applications, it is of great importance to explore new catalysts for formic acid oxidation that have both ultra-high mass activity and CO resistance. In this work, we successfully synthesize atomically dispersed Rh on N-doped carbon (SA-Rh/CN) and discover that SA-Rh/CN exhibits promising electrocatalytic properties for formic acid oxidation. The mass activity shows 28- and 67-fold enhancements compared with state-of-the-art Pd/C and Pt/C, respectively, despite the low activity of Rh/C. Interestingly, SA-Rh/CN exhibits greatly enhanced tolerance to CO poisoning, and Rh atoms in SA-Rh/CN resist sintering after long-term testing, resulting in excellent catalytic stability. Density functional theory calculations suggest that the formate route is more favourable on SA-Rh/CN. According to calculations, the high barrier to produce CO, together with the relatively unfavourable binding with CO, contribute to its CO tolerance.
Research Organization:
SLAC National Accelerator Laboratory, Menlo Park, CA (United States)
Sponsoring Organization:
China Postdoctoral Science Foundation; Jilin Province Science and Technology Development Program; National Key R&D Program of China; National Natural Science Foundation of China (NSFC); USDOE; USDOE Laboratory Directed Research and Development (LDRD) Program; Youth Innovation Promotion Association CAS
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1616956
Journal Information:
Nature Nanotechnology, Journal Name: Nature Nanotechnology Journal Issue: 5 Vol. 15; ISSN 1748-3387
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (64)

“Raisin Bun”-Like Nanocomposites of Palladium Clusters and Porphyrin for Superior Formic Acid Oxidation journal April 2013
Towards More Active and Stable Electrocatalysts for Formic Acid Electrooxidation: Antimony-Decorated Octahedral Platinum Nanoparticles journal November 2012
Shape-Controlled Synthesis of Surface-Clean Ultrathin Palladium Nanosheets by Simply Mixing a Dinuclear Pd I Carbonyl Chloride Complex with H 2 O journal June 2013
An Effective Pd-Ni 2 P/C Anode Catalyst for Direct Formic Acid Fuel Cells journal November 2013
Size-Controlled Synthesis of Platinum-Copper Hierarchical Trigonal Bipyramid Nanoframes journal October 2014
Spatially Resolved Quantification of the Surface Reactivity of Solid Catalysts journal April 2016
Single-Site Active Cobalt-Based Photocatalyst with a Long Carrier Lifetime for Spontaneous Overall Water Splitting journal June 2017
Atomic-Level Insight into Optimizing the Hydrogen Evolution Pathway over a Co 1 -N 4 Single-Site Photocatalyst journal August 2017
Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces journal March 2011
Pd-Ag alloy hollow nanostructures with interatomic charge polarization for enhanced electrocatalytic formic acid oxidation journal March 2016
A stepwise-designed Rh-Au-Si nanocomposite that surpasses Pt/C hydrogen evolution activity at high overpotentials journal February 2017
A mixed-solvent route to unique PtAuCu ternary nanotubes templated from Cu nanowires as efficient dual electrocatalysts journal February 2016
The adsorption of bisulfate and sulfate anions over a Pt(111) electrode: A first principle study of adsorption configurations, vibrational frequencies and linear sweep voltammogram simulations journal March 2013
High selectivity PtRh/RGO catalysts for ethanol electro-oxidation at low potentials: Enhancing the efficiency of CO2 from alcoholic groups journal December 2018
Oxygen reduction reaction mechanism on nitrogen-doped graphene: A density functional theory study journal August 2011
Catalytic activities of Pt thin films electrodeposited onto Bi coated glassy carbon substrate toward formic acid electrooxidation journal December 2014
Single-Atom Catalysts: Synthetic Strategies and Electrochemical Applications journal July 2018
Ultra-uniform PdBi nanodots with high activity towards formic acid oxidation journal July 2017
Catalysis by Supported Single Metal Atoms journal November 2016
Role of Heteronuclear Interactions in Selective H 2 Formation from HCOOH Decomposition on Bimetallic Pd/M (M = Late Transition FCC Metal) Catalysts journal March 2017
Single-Atom Catalysts: A New Frontier in Heterogeneous Catalysis journal April 2013
Trends in Formic Acid Decomposition on Model Transition Metal Surfaces: A Density Functional Theory study journal November 2014
XAS and DFT Investigation of Mononuclear Cobalt(III) Peroxo Complexes: Electronic Control of the Geometric Structure in CoO 2 versus NiO 2 Systems journal January 2011
Ultrathin and Ultralong Single-Crystal Platinum Nanowire Assemblies with Highly Stable Electrocatalytic Activity journal June 2013
Surfactant-Directed Synthesis of Mesoporous Pd Films with Perpendicular Mesochannels as Efficient Electrocatalysts journal September 2015
Single Atom (Pd/Pt) Supported on Graphitic Carbon Nitride as an Efficient Photocatalyst for Visible-Light Reduction of Carbon Dioxide journal May 2016
Mechanistic Studies of Single-Step Styrene Production Using a Rhodium(I) Catalyst journal January 2017
Deprotonation of Solvated Formic Acid:  Car−Parrinello and Metadynamics Simulations journal February 2006
Bridge-Bonded Formate:  Active Intermediate or Spectator Species in Formic Acid Oxidation on a Pt Film Electrode? † journal December 2006
Nanocrystalline intermetallics on mesoporous carbon for direct formic acid fuel cell anodes journal February 2010
Atomic-level insights in optimizing reaction paths for hydroformylation reaction over Rh/CoO single-atom catalyst journal December 2016
Nanostructured materials for advanced energy conversion and storage devices journal May 2005
Identification of catalytic sites for oxygen reduction in iron- and nitrogen-doped graphene materials journal August 2015
Freestanding palladium nanosheets with plasmonic and catalytic properties journal December 2010
Identification of catalytic sites in cobalt-nitrogen-carbon materials for the oxygen reduction reaction journal October 2017
Inflating hollow nanocrystals through a repeated Kirkendall cavitation process journal November 2017
Dendritic defect-rich palladium–copper–cobalt nanoalloys as robust multifunctional non-platinum electrocatalysts for fuel cells journal September 2018
Direct observation of noble metal nanoparticles transforming to thermally stable single atoms journal July 2018
General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities journal January 2018
Pentamethylcyclopentadienyl rhodium(III)–chiral disulfonate hybrid catalysis for enantioselective C–H bond functionalization journal July 2018
One-Pot Synthesis of Graphene-Supported Monodisperse Pd Nanoparticles as Catalyst for Formic Acid Electro-oxidation journal March 2014
A first principles comparison of the mechanism and site requirements for the electrocatalytic oxidation of methanol and formic acid over Pt journal January 2009
The facile synthesis of single crystalline palladium arrow-headed tripods and their application in formic acid electro-oxidation journal January 2015
Concave and duck web-like platinum nanopentagons with enhanced electrocatalytic properties for formic acid oxidation journal January 2016
Highly doped and exposed Cu( i )–N active sites within graphene towards efficient oxygen reduction for zinc–air batteries journal January 2016
Single-atom dispersed Co–N–C catalyst: structure identification and performance for hydrogenative coupling of nitroarenes journal January 2016
Multimetallic nanosheets: synthesis and applications in fuel cells journal January 2018
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu journal April 2010
A unified formulation of the constant temperature molecular dynamics methods journal July 1984
A dimer method for finding saddle points on high dimensional potential surfaces using only first derivatives journal October 1999
Implicit solvation model for density-functional study of nanocrystal surfaces and reaction pathways journal February 2014
Self-consistent aspects of x-ray absorption calculations journal August 2009
Canonical dynamics: Equilibrium phase-space distributions journal March 1985
Special points for Brillouin-zone integrations journal June 1976
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium journal May 1994
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
From ultrasoft pseudopotentials to the projector augmented-wave method journal January 1999
Wavelet analysis of extended x-ray absorption fine structure data journal March 2005
Generalized Gradient Approximation Made Simple journal October 1996
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT journal June 2005
Direct, Nonoxidative Conversion of Methane to Ethylene, Aromatics, and Hydrogen journal May 2014
Photochemical route for synthesizing atomically dispersed palladium catalysts journal May 2016
Thermally stable single-atom platinum-on-ceria catalysts via atom trapping journal July 2016
An ab Initio Molecular Dynamics Study on the Solvation of Formate ion and Formic acid in Water journal October 2012

Similar Records

Facile synthesis of PtAu alloy nanoparticles with high activity for formic acid oxidation
Journal Article · Sun Feb 14 23:00:00 EST 2010 · Journal of Power Sources, 195(4):1103-1106 · OSTI ID:972531
Platinum and Palladium Monolayer Electrocatalysts for Formic Acid Oxidation
Journal Article · Tue Apr 21 20:00:00 EDT 2020 · Topics in Catalysis · OSTI ID:1646577
Localized Pd Overgrowth on Cubic Pt Nanocrystals for Enhanced Electrocatalytic Oxidation of Formic Acid
Journal Article · Thu Mar 20 00:00:00 EDT 2008 · JACS · OSTI ID:953767

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Electrocatalysis
Materials science