A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction.
Conversion of the greenhouse gas carbon dioxide (CO2) to value-added products is an important challenge for sustainable energy research, and nanomaterials offer a broad class of heterogeneous catalysts for such transformations. Here we report a molecular surface functionalization approach to tuning gold nanoparticle (Au NP) electrocatalysts for reduction of CO2 to CO. The N-heterocyclic (NHC) carbene-functionalized Au NP catalyst exhibits improved faradaic efficiency (FE = 83%) for reduction of CO2 to CO in water at neutral pH at an overpotential of 0.46 V with a 7.6-fold increase in current density compared to that of the parent Au NP (FE = 53%). Tafel plots of the NHC carbene-functionalized Au NP (72 mV/decade) vs parent Au NP (138 mV/decade) systems further show that the molecular ligand influences mechanistic pathways for CO2 reduction. The results establish molecular surface functionalization as a complementary approach to size, shape, composition, and defect control for nanoparticle catalyst design.
Zhi
Z
Cao
Dohyung
D
Kim
Dachao
D
Hong
Yi
Y
Yu
Jun
J
Xu
Song
S
Lin
Institute of Coal Chemistry, Chinese Academy of Sciences , Taiyuan, Shanxi 030001, China.|Synfuels China , Beijing 100195, China.
Xiaodong
X
Wen
Eva M
EM
Nichols
Keunhong
K
Jeong
Jeffrey A
JA
Reimer
Kavli Energy Nanosciences Institute , Berkeley, California 94720, United States.
Peidong
P
Yang
Christopher J
CJ
Chang