Size-dependent electrocatalytic reduction of CO2 over Pd nanoparticles

Journal of the American Chemical Society
Dunfeng GaoXinhe Bao

Abstract

Size effect has been regularly utilized to tune the catalytic activity and selectivity of metal nanoparticles (NPs). Yet, there is a lack of understanding of the size effect in the electrocatalytic reduction of CO2, an important reaction that couples with intermittent renewable energy storage and carbon cycle utilization. We report here a prominent size-dependent activity/selectivity in the electrocatalytic reduction of CO2 over differently sized Pd NPs, ranging from 2.4 to 10.3 nm. The Faradaic efficiency for CO production varies from 5.8% at -0.89 V (vs reversible hydrogen electrode) over 10.3 nm NPs to 91.2% over 3.7 nm NPs, along with an 18.4-fold increase in current density. Based on the Gibbs free energy diagrams from density functional theory calculations, the adsorption of CO2 and the formation of key reaction intermediate COOH* are much easier on edge and corner sites than on terrace sites of Pd NPs. In contrast, the formation of H* for competitive hydrogen evolution reaction is similar on all three sites. A volcano-like curve of the turnover frequency for CO production within the size range suggests that CO2 adsorption, COOH* formation, and CO* removal during CO2 reduction can be tuned by varying the size of Pd NPs du...Continue Reading

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Citations

Sep 25, 2015·Chemical Reviews·Aicheng Chen, Cassandra Ostrom
Oct 8, 2015·Chemical Reviews·James L WhiteAndrew B Bocarsly
Oct 9, 2015·Journal of the American Chemical Society·Cheonghee KimYun Jeong Hwang
Jan 2, 2016·The Journal of Physical Chemistry Letters·Ruud KortleverMarc T M Koper
Jun 21, 2016·Journal of the American Chemical Society·Zhi CaoChristopher J Chang
Oct 29, 2015·Journal of the American Chemical Society·Nikolay KornienkoPeidong Yang
Feb 6, 2017·Journal of the American Chemical Society·Subiao LiuJing-Li Luo
Mar 18, 2017·Chemical Reviews·Tao ChenNing Fang
Apr 11, 2017·Journal of the American Chemical Society·Dunfeng GaoXinhe Bao
Mar 22, 2016·Advanced Materials·Dong Dong ZhuShi Zhang Qiao
Jul 28, 2016·Chemistry : a European Journal·Jaecheol ChoiDavid L Officer
Mar 16, 2017·Journal of the American Chemical Society·Qing LiShouheng Sun
Sep 5, 2015·Physical Chemistry Chemical Physics : PCCP·Hu ZhouJianguo Wang
Jul 5, 2016·Chemical Communications : Chem Comm·R KortleverM T M Koper
Jul 29, 2016·Physical Chemistry Chemical Physics : PCCP·Tao ChenWeilin Xu
Dec 5, 2017·Advanced Science·Jinghua WuYanguang Li
Aug 2, 2017·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Yulin WangPeng Kang
Sep 15, 2017·Small·Yuhang WangGengfeng Zheng
May 3, 2016·Angewandte Chemie·Munir Ullah KhanJie Zeng

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