TY - JOUR
T1 - Two-Dimensional Conductive Ni-HAB as a Catalyst for the Electrochemical Oxygen Reduction Reaction
AU - Park, Jihye
AU - Chen, Zhihua
AU - Flores, Raul A.
AU - Wallnerström, Gustaf
AU - Kulkarni, Ambarish
AU - Nørskov, Jens K.
AU - Jaramillo, Thomas F.
AU - Bao, Zhenan
PY - 2020
Y1 - 2020
N2 - Catalytic systems whose properties can be systematically tuned via changes in synthesis conditions are highly desirable for the next-generation catalyst design and optimization. Herein, we present a two-dimensional (2D) conductive metal-organic framework consisting of M-N4 units (M = Ni, Cu) and a hexaaminobenzene (HAB) linker as a catalyst for the oxygen reduction reaction. By varying synthetic conditions, we prepared two Ni-HAB catalysts with different crystallinities, resulting in catalytic systems with different electric conductivities, electrochemical activity, and stability. We show that crystallinity has a positive impact on conductivity and demonstrate that this improved crystallinity/conductivity improves the catalytic performance of our model system. Additionally, density functional theory simulations were performed to probe the origin of M-HAB's catalytic activity, and they suggest that M-HAB's organic linker acts as the active site with the role of the metal being to modulate the linker sites' binding strength.
AB - Catalytic systems whose properties can be systematically tuned via changes in synthesis conditions are highly desirable for the next-generation catalyst design and optimization. Herein, we present a two-dimensional (2D) conductive metal-organic framework consisting of M-N4 units (M = Ni, Cu) and a hexaaminobenzene (HAB) linker as a catalyst for the oxygen reduction reaction. By varying synthetic conditions, we prepared two Ni-HAB catalysts with different crystallinities, resulting in catalytic systems with different electric conductivities, electrochemical activity, and stability. We show that crystallinity has a positive impact on conductivity and demonstrate that this improved crystallinity/conductivity improves the catalytic performance of our model system. Additionally, density functional theory simulations were performed to probe the origin of M-HAB's catalytic activity, and they suggest that M-HAB's organic linker acts as the active site with the role of the metal being to modulate the linker sites' binding strength.
KW - Metal−organic frameworks
KW - Electrical conductivity
KW - Electrocatalysis
KW - Active sites
KW - Oxygen reduction reactions
KW - Density functional theory
U2 - 10.1021/acsami.0c09323
DO - 10.1021/acsami.0c09323
M3 - Journal article
C2 - 32805928
SN - 1944-8244
VL - 12
SP - 39074
EP - 39081
JO - A C S Applied Materials and Interfaces
JF - A C S Applied Materials and Interfaces
IS - 35
ER -