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Bismuth Oxyhydroxide-Pt Inverse Interface for Enhanced Methanol Electrooxidation Performance.
Nano Letters ( IF 9.6 ) Pub Date : 2020-09-22 , DOI: 10.1021/acs.nanolett.0c03340 Xuchun Wang 1, 2 , Miao Xie 1 , Fenglei Lyu 1 , Yun-Mui Yiu 2 , Zhiqiang Wang 2 , Jiatang Chen 2 , Lo-Yueh Chang 1 , Yujian Xia 1 , Qixuan Zhong 1 , Mingyu Chu 1 , Hao Yang 1 , Tao Cheng 1 , Tsun-Kong Sham 2 , Qiao Zhang 1
Nano Letters ( IF 9.6 ) Pub Date : 2020-09-22 , DOI: 10.1021/acs.nanolett.0c03340 Xuchun Wang 1, 2 , Miao Xie 1 , Fenglei Lyu 1 , Yun-Mui Yiu 2 , Zhiqiang Wang 2 , Jiatang Chen 2 , Lo-Yueh Chang 1 , Yujian Xia 1 , Qixuan Zhong 1 , Mingyu Chu 1 , Hao Yang 1 , Tao Cheng 1 , Tsun-Kong Sham 2 , Qiao Zhang 1
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Developing efficient Pt-based electrocatalysts for the methanol oxidation reaction (MOR) is of pivotal importance for large-scale application of direct methanol fuel cells (DMFCs), but Pt suffers from severe deactivation brought by the carbonaceous intermediates such as CO. Here, we demonstrate the formation of a bismuth oxyhydroxide (BiOx(OH)y)-Pt inverse interface via electrochemical reconstruction for enhanced methanol oxidation. By combining density functional theory calculations, X-ray absorption spectroscopy, ambient pressure X-ray photoelectron spectroscopy, and electrochemical characterizations, we reveal that the BiOx(OH)y-Pt inverse interface can induce the electron deficiency of neighboring Pt; this would result in weakened CO adsorption and strengthened OH adsorption, thereby facilitating the removal of the poisonous intermediates and ensuring the high activity and good stability of Pt2Bi sample. This work provides a comprehensive understanding of the inverse interface structure and deep insight into the active sites for MOR, offering great opportunities for rational fabrication of efficient electrocatalysts for DMFCs.
中文翻译：
羟基氧化铋-Pt反向界面可增强甲醇的电氧化性能。
开发用于甲醇氧化反应（MOR）的高效基于Pt的电催化剂对于直接应用甲醇燃料电池（DMFC）的大规模应用至关重要，但是Pt受到碳质中间体（如CO）带来的严重失活的影响。证明了通过电化学重建以增强甲醇氧化形成羟基氧化铋（BiO x（OH）y）-Pt反向界面。通过结合密度泛函理论计算，X射线吸收光谱，环境压力X射线光电子能谱和电化学表征，我们揭示了BiO x（OH）y-Pt逆界面可引起邻近Pt的电子缺乏；这将导致减弱的CO吸附和增强的OH吸附，从而促进有毒中间体的去除，并确保Pt 2 Bi样品的高活性和良好的稳定性。这项工作提供了对逆界面结构的全面理解，并深入了解了MOR的活性位点，为合理制造DMFC的高效电催化剂提供了巨大的机会。
更新日期：2020-10-15
中文翻译：
羟基氧化铋-Pt反向界面可增强甲醇的电氧化性能。
开发用于甲醇氧化反应（MOR）的高效基于Pt的电催化剂对于直接应用甲醇燃料电池（DMFC）的大规模应用至关重要，但是Pt受到碳质中间体（如CO）带来的严重失活的影响。证明了通过电化学重建以增强甲醇氧化形成羟基氧化铋（BiO x（OH）y）-Pt反向界面。通过结合密度泛函理论计算，X射线吸收光谱，环境压力X射线光电子能谱和电化学表征，我们揭示了BiO x（OH）y-Pt逆界面可引起邻近Pt的电子缺乏；这将导致减弱的CO吸附和增强的OH吸附，从而促进有毒中间体的去除，并确保Pt 2 Bi样品的高活性和良好的稳定性。这项工作提供了对逆界面结构的全面理解，并深入了解了MOR的活性位点，为合理制造DMFC的高效电催化剂提供了巨大的机会。
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