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 · 06 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. ^[4]; Nair, Aruna N. ^[4]; Chava, Venkata N. ^[4]; Fernandez‐Delgado, Olivia ^[4]; Allam, Nageh K. ^[3]; Stevenson, Steven ^[2]; Sreenivasan, Sreeprasad T. ^[4];

^[4]

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

A new isolation protocol was recently reported for highly purified metallic Fullertubes D_5h-C₉₀, D_3d-C₉₆, and D_5d-C₁₀₀, which exhibit unique electronic features. Here, we report the oxygen reduction electrocatalytic behavior of C₆₀, C₇₀ (spheroidal fullerenes), and C₉₀, C₉₆, and C₁₀₀ (tubular fullerenes) using a combination of experimental and theoretical approaches. C₉₆ (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. Here we achieved an excellent power density of 0.75 W cm⁻² using C₉₆ 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 C₉₆.

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Research Organization:: University 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)

Grant/Contract Number:: FE0031908

OSTI ID:: 1976278

Alternate ID(s):: OSTI ID: 1856284

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 21 Vol. 61; 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)

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