A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction

详细信息    查看全文

• 作者：Zhi Cao ; Dohyung Kim ; Dachao Hong ; Yi Yu ; Jun Xu ; Song Lin ; Xiaodong Wen ; Eva M. Nichols ; Keunhong Jeong ; Jeffrey A. Reimer ; Peidong Yang ; Christopher J. Chang
• 刊名：Journal of the American Chemical Society
• 出版年：2016
• 出版时间：July 6, 2016
• 年：2016
• 卷：138
• 期：26
• 页码：8120-8125
• 全文大小：397K
• 年卷期：0
• ISSN：1520-5126

文摘

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.