Cylindrical C96 Fullertubes: A Highly Active Metal-Free O2-Reduction Electrocatalyst

Sanad, Mohamed Fathi; Franklin, Hannah M.; Ali, Basant A.; Puente Santiago, Alain R.; Nair, Aruna N.; Chava, Venkata N.; Fernandez‐Delgado, Olivia; Allam, Nageh K.; Stevenson, Steven; Sreenivasan, Sreeprasad T.; Echegoyen, Luis

doi:10.1002/anie.202116727

Title: Cylindrical C₉₆ Fullertubes: A Highly Active Metal-Free O₂-Reduction Electrocatalyst

Journal Article · 07 March 2022 · Angewandte Chemie (International Edition)

DOI: https://doi.org/10.1002/anie.202116727 · OSTI ID:1976278

Sanad, Mohamed Fathi ^[1]; Franklin, Hannah M. ^[2]; Ali, Basant A. ^[3]; Puente Santiago, Alain R. ^[1]; Nair, Aruna N. ^[1]; Chava, Venkata N. ^[1]; Fernandez‐Delgado, Olivia ^[1]; Allam, Nageh K. ^[3]; Stevenson, Steven ^[2]; Sreenivasan, Sreeprasad T. ^[1];

^[1]

University of Texas at El Paso, TX (United States)
Purdue University, West Lafayette, IN (United States)
American University in Cairo, New Cairo (Egypt)

Abstract A new isolation protocol was recently reported for highly purified metallic Fullertubes D _5h ‐C ₉₀ , D _3d ‐C ₉₆ , and D _5d ‐C _100, which exhibit unique electronic features. Here, we report the oxygen reduction electrocatalytic behavior of C ₆₀ , C ₇₀ (spheroidal fullerenes), and C ₉₀ , C ₉₆ , and C ₁₀₀ (tubular fullerenes) using a combination of experimental and theoretical approaches. C ₉₆ (a metal‐free catalyst) displayed remarkable oxygen reduction reaction (ORR) activity, with an onset potential of 0.85 V and a halfway potential of 0.75 V, which are close to the state‐of‐the‐art Pt/C benchmark catalyst values. We achieved an excellent power density of 0.75 W cm ⁻² using C ₉₆ as a modified cathode in a proton‐exchange membrane fuel cell, comparable to other recently reported efficient metal‐free catalysts. Combined band structure (experimentally calculated) and free‐energy (DFT) investigations show that both favorable energy‐level alignment active catalytic sites on the carbon cage are responsible for the superior activity of C ₉₆ .

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Research Organization:: Univ. of Texas at El Paso, TX (United States)

Sponsoring Organization:: USDOE Office of Fossil Energy (FE); National Science Foundation (NSF); Robert A. Welch Foundation; Nanotechnology Collaborative Infrastructure (NCI); Arab-German Young Academy of Sciences and Humanities (AGYA); USDOE

Grant/Contract Number:: FE0031908; CHE-1801317; AH-0033; RUI-1856461

OSTI ID:: 1976278

Alternate ID(s):: OSTI ID: 1856284

Journal Information:: Angewandte Chemie (International Edition), Vol. 61, Issue 21; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
electrocatalysis
fullerene
ORR
band alignment
C96
molecular catalysis

Title: Cylindrical C96 Fullertubes: A Highly Active Metal-Free O2-Reduction Electrocatalyst

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References (27)

Figures / Tables (3)

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Related Subjects

Title: Cylindrical C₉₆ Fullertubes: A Highly Active Metal-Free O₂-Reduction Electrocatalyst