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Ru-loaded pyrrolic-N-doped extensively graphitized porous carbon for high performance electrochemical hydrogen evolution

Title
Ru-loaded pyrrolic-N-doped extensively graphitized porous carbon for high performance electrochemical hydrogen evolution
Author(s)
Shin, Cheol-HwanYu, Ted H.Lee, Ha-YoungLee, Byong-JuneKwon, SoonhoGoddard, William A.Yu, Jong-Sung
Issued Date
2023-10
Citation
Applied Catalysis B: Environmental, v.334
Type
Article
Author Keywords
Graphitized carbonMg reductionPyrrolic-NHydrogen evolutionElectrochemical water splittingQuantum mechanics calculation
Keywords
RUTHENIUM-BASED CATALYSTMESOPOROUS MATERIALSNITROGENELECTROCATALYSTSEFFICIENTDESIGNELECTRODENITRIDESULFUR
ISSN
0926-3373
Abstract
Herein, we report a novel methodology for preparation of new N-doped extensively graphitized porous carbon (N-GPC) as a new catalyst support for Ru nanoparticles (NPs) with dramatically improved hydrogen evolution reaction (HER) activity. Our method is remarkably simple: pyrolyzing g-C3N4 in the presence of Mg metal. Here, we show that Mg plays marvelous dual roles as a reducing agent to graphitize the g-C3N4 precursor at low temperature and as a precursor for Mg3N2, which generates network-structured porous carbon as a new porogen. This offers highly robust graphitized carbon with high electrical conductivity, network-structured high porosity, and proper N content, most desired as a catalyst support. As-prepared Ru/N-GPC catalyst shows a remarkably low overpotential of 9.6 mV (vs. RHE) at 10 mA/cm2, which is near ideal, providing 12 times faster hydrogen production rate than state-of-the-art Pt/C. We explain the atomistic basis for this low overpotential and superb stability via Grand canonical quantum mechanics calculations. These calculations show that pyrrolic-N in the support strengthens the coupling to the Ru NP while weakening the binding of H to Ru NP to accelerate the Tafel step. © 2023 Elsevier B.V.
URI
http://hdl.handle.net/20.500.11750/46079
DOI
10.1016/j.apcatb.2023.122829
Publisher
Elsevier B.V.
Related Researcher
  • 유종성 Yu, Jong-Sung 에너지공학과
  • Research Interests Materials chemistry; nanomaterials; electrochemistry; carbon and porous materials; fuel cell; battery; supercapacitor; sensor and photochemical catalyst
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Appears in Collections:
Department of Energy Science and Engineering Light, Salts and Water Research Group 1. Journal Articles

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