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Pt/Pd Single-Atom Alloys as Highly Active Electrochemical Catalysts and the Origin of Enhanced Activity
ACS Catalysis ( IF 11.3 ) Pub Date : 2019-09-18 , DOI: 10.1021/acscatal.9b01677 Lei Zhang 1 , Hanshuo Liu 2 , Sihang Liu 3 , Mohammad Norouzi Banis 1 , Zhongxin Song 1 , Junjie Li 1 , Lijun Yang 4 , Matthew Markiewicz 4 , Yang Zhao 1 , Ruying Li 1 , Matthew Zheng 1 , Siyu Ye 4 , Zhi-Jian Zhao 3 , Gianluigi A. Botton 2 , Xueliang Sun 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2019-09-18 , DOI: 10.1021/acscatal.9b01677 Lei Zhang 1 , Hanshuo Liu 2 , Sihang Liu 3 , Mohammad Norouzi Banis 1 , Zhongxin Song 1 , Junjie Li 1 , Lijun Yang 4 , Matthew Markiewicz 4 , Yang Zhao 1 , Ruying Li 1 , Matthew Zheng 1 , Siyu Ye 4 , Zhi-Jian Zhao 3 , Gianluigi A. Botton 2 , Xueliang Sun 1
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Pt single-atom catalysts are receiving more and more attention due to their different properties compared with nanostructures. As one typical kind of single-atom catalysts, Pt-based single-atom alloys (SAAs) have generated significant interest due to their application in several heterogeneous catalytic reactions. However, almost all of the reported Pt-based SAAs are on Cu surface. In addition, it is still great challenge to apply Pt single-atom alloys in electrocatalytic reactions. Herein, we demonstrated a fabrication of Pt/Pd SAA catalysts on nitrogen-doped carbon nanotubes by atomic layer deposition. The as-prepared octahedral Pt/Pd SAA catalysts exhibited greatly improved activity compared to commercial Pt/C catalysts for electrochemical catalytic reactions. According to the X-ray adsorption spectrum, the Pt atoms in Pt/Pd SAA catalysts exhibited higher unoccupied 5d character density of states and a lower Pt–Pt coordination number, compared to those in core–shell structures. In addition, we used density functional theory calculation results to explain the enhanced mechanism of Pt/Pd SAA catalysts for electrochemical reactions. This study opens up an avenue of developing different types of Pt-based catalysts for electrocatalytic reactions and brings insight understanding about catalytic performances of SAA catalysts.
中文翻译：
Pt / Pd单原子合金作为高活性电化学催化剂和增强活性的起源
铂单原子催化剂由于其与纳米结构相比的不同性能而受到越来越多的关注。基于Pt的单原子合金（SAA）作为一种典型的单原子催化剂，由于其在几种异相催化反应中的应用而引起了人们的极大兴趣。但是，几乎所有已报道的基于Pt的SAA都位于Cu表面。另外，将Pt单原子合金应用于电催化反应中仍然是巨大的挑战。在这里，我们证明了通过原子层沉积在氮掺杂碳纳米管上制备Pt / Pd SAA催化剂。与用于电化学催化反应的商业Pt / C催化剂相比，所制备的八面体Pt / Pd SAA催化剂表现出大大改善的活性。根据X射线吸收光谱，与核-壳结构相比，Pt / Pd SAA催化剂中的Pt原子表现出较高的空位5d特征密度和较低的Pt-Pt配位数。此外，我们使用密度泛函理论计算结果来解释Pt / Pd SAA催化剂用于电化学反应的增强机理。这项研究为开发用于电催化反应的不同类型的Pt基催化剂开辟了一条途径，并带来了对SAA催化剂催化性能的深刻理解。
更新日期：2019-09-18
中文翻译：
Pt / Pd单原子合金作为高活性电化学催化剂和增强活性的起源
铂单原子催化剂由于其与纳米结构相比的不同性能而受到越来越多的关注。基于Pt的单原子合金（SAA）作为一种典型的单原子催化剂，由于其在几种异相催化反应中的应用而引起了人们的极大兴趣。但是，几乎所有已报道的基于Pt的SAA都位于Cu表面。另外，将Pt单原子合金应用于电催化反应中仍然是巨大的挑战。在这里，我们证明了通过原子层沉积在氮掺杂碳纳米管上制备Pt / Pd SAA催化剂。与用于电化学催化反应的商业Pt / C催化剂相比，所制备的八面体Pt / Pd SAA催化剂表现出大大改善的活性。根据X射线吸收光谱，与核-壳结构相比，Pt / Pd SAA催化剂中的Pt原子表现出较高的空位5d特征密度和较低的Pt-Pt配位数。此外，我们使用密度泛函理论计算结果来解释Pt / Pd SAA催化剂用于电化学反应的增强机理。这项研究为开发用于电催化反应的不同类型的Pt基催化剂开辟了一条途径，并带来了对SAA催化剂催化性能的深刻理解。
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