Grain-Boundary-Dependent CO2 Electroreduction Activity
Grain-Boundary-Dependent CO2 Electroreduction Activity
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DOI：
10.1021/ja5130513
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发表时间：
2015-04-15
影响因子：
15
通讯作者：
Kanan, Matthew W.
中科院分区：
文献类型：
--
作者：
Feng, Xiaofeng;Jiang, Kaili;Kanan, Matthew W.
揭示金属纳米颗粒（NP）电催化剂的新结构-活性关系对于推进许多能量转换技术至关重要。晶界（GBs）可以用来稳定独特的活性表面，但GBs和催化活性之间的定量相关性尚未建立。在这里，我们使用气相沉积制备碳纳米管上的Au NPs（Au/CNT）。在沉积时，Au NP具有相对高的密度，其易于通过透射电子显微镜（TEM）成像;热退火以受控的方式降低密度。我们发现，二氧化碳还原的表面积归一化活性与GB表面密度在Au/CNT上线性相关，表明GB工程是提高金属纳米颗粒催化活性的有力途径。
Uncovering new structure-activity relationships for metal nanoparticle (NP) electrocatalysts is crucial for advancing many energy conversion technologies. Grain boundaries (GBs) could be used to stabilize unique active surfaces, but a quantitative correlation between GBs and catalytic activity has not been established. Here we use vapor deposition to prepare Au NPs on carbon nanotubes (Au/CNT). As deposited, the Au NPs have a relatively high density of GBs that are readily imaged by transmission electron microscopy (TEM); thermal annealing lowers the density in a controlled manner. We show that the surface-area-normalized activity for CO2 reduction is linearly correlated with GB surface density on Au/CNT, demonstrating that GB engineering is a powerful approach to improving the catalytic activity of metal NPs.