TY - JOUR
T1 - Promotion of Ternary Pt-Sn-Ag Catalysts toward Ethanol Oxidation Reaction
T2 - Revealing Electronic and Structural Effects of Additive Metals
AU - Dai, Sheng
AU - Huang, Tzu Hsi
AU - Yan, Xingxu
AU - Yang, Chao Yu
AU - Chen, Tsan Yao
AU - Wang, Jeng Han
AU - Pan, Xiaoqing
AU - Wang, Kuan Wen
N1 - Funding Information:
This work was supported by UC Irvine’s Office of Research, the National Science Foundation (Grant Number DMR-1506535), and the Ministry of Science and Technology, R.O.C. (MOST 104-2628-E-008-005-MY3 and 106-2113-M-003-003). CPU time at Taiwan’s National Center for High-performance Computing (NCHC) is greatly appreciated. The authors would like to thank the National Synchrotron Radiation Research Center (NSRRC) for providing the beam time. Additional support was provided by the Irvine Materials Research Institute (IMRI) through the use of TEM facilities.
Publisher Copyright:
© Copyright 2018 American Chemical Society.
PY - 2018/10/12
Y1 - 2018/10/12
N2 - The use of a computation-guided method and the discovered structure-property relationship would establish a rational strategy to aid the development of ethanol oxidation reaction (EOR) catalysts for possible commercialization of direct ethanol fuel cells. Here, we investigate the promotion roles of additive metals in ternary Pt-Sn-Ag catalysts toward EOR via a combination of density functional theory calculation and experimental evidence. By calculating the EOR energetics, the promotion roles of Sn and Ag were revealed from the viewpoints of electronic and structural effects, respectively: (1) The addition of Sn and Ag on Pt essentially reduce the reaction energy and activation barrier of the second two-electron transfer process of EOR, facilitating the oxidation of acetaldehyde to acetic acid; (2) a homogeneous Pt-Sn-Ag surface configuration strengthens the adsorption energy of ethanol, thus improving the activity for ethanol oxidizing to acetaldehyde. Experimentally, various Pt-Sn-Ag nanorod catalysts with different surface configurations were synthesized, and their electrochemical performances demonstrate the two EOR promotion effects as predicted. Notably, our extended Pt6-Sn-Ag nanorod catalyst shows remarkably enhanced EOR activity and stability, highlighting a homogeneous Pt-Sn-Ag surface configuration as an optimal structure for EOR catalysts.
AB - The use of a computation-guided method and the discovered structure-property relationship would establish a rational strategy to aid the development of ethanol oxidation reaction (EOR) catalysts for possible commercialization of direct ethanol fuel cells. Here, we investigate the promotion roles of additive metals in ternary Pt-Sn-Ag catalysts toward EOR via a combination of density functional theory calculation and experimental evidence. By calculating the EOR energetics, the promotion roles of Sn and Ag were revealed from the viewpoints of electronic and structural effects, respectively: (1) The addition of Sn and Ag on Pt essentially reduce the reaction energy and activation barrier of the second two-electron transfer process of EOR, facilitating the oxidation of acetaldehyde to acetic acid; (2) a homogeneous Pt-Sn-Ag surface configuration strengthens the adsorption energy of ethanol, thus improving the activity for ethanol oxidizing to acetaldehyde. Experimentally, various Pt-Sn-Ag nanorod catalysts with different surface configurations were synthesized, and their electrochemical performances demonstrate the two EOR promotion effects as predicted. Notably, our extended Pt6-Sn-Ag nanorod catalyst shows remarkably enhanced EOR activity and stability, highlighting a homogeneous Pt-Sn-Ag surface configuration as an optimal structure for EOR catalysts.
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U2 - 10.1021/acsenergylett.8b01632
DO - 10.1021/acsenergylett.8b01632
M3 - Article
AN - SCOPUS:85054408588
SN - 2380-8195
VL - 3
SP - 2550
EP - 2557
JO - ACS Energy Letters
JF - ACS Energy Letters
IS - 10
ER -
