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Mastering the surface strain of platinum catalysts for efficient electrocatalysis

机译：掌握铂催化剂的表面菌株，以高效电催化

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摘要

Platinum (Pt) has found wide use as an electrocatalyst for sustainable energy conversion systems(1-3). The activity of Pt is controlled by its electronic structure (typically, the d-band centre), which depends sensitively on lattice strain(4,5). This dependence can be exploited for catalyst design(4,6-8), and the use of core-shell structures and elastic substrates has resulted in strain-engineered Pt catalysts with drastically improved electrocatalytic performances(7,9-13). However, it is challenging to map in detail the strain-activity correlations in Pt-catalysed conversions, which can involve a number of distinct processes, and to identify the optimal strain modification for specific reactions. Here we show that when ultrathin Pt shells are deposited on palladium-based nanocubes, expansion and shrinkage of the nanocubes through phosphorization and dephosphorization induces strain in the Pt(100) lattice that can be adjusted from -5.1 per cent to 5.9 per cent. We use this strain control to tune the electrocatalytic activity of the Pt shells over a wide range, finding that the strain-activity correlation for the methanol oxidation reaction and hydrogen evolution reaction follows an M-shaped curve and a volcano-shaped curve, respectively. We anticipate that our approach can be used to screen out lattice strain that will optimize the performance of Pt catalysts-and potentially other metal catalysts-for a wide range of reactions.
机译：铂（PT）已根据可持续能量转换系统（1-3）广泛用作电催化剂。 PT的活性由其电子结构（通常是D波段中心）控制，这取决于晶格菌株（4,5）的敏感性。可以利用这种依赖性用于催化剂设计（4,6-8），并且使用核 - 壳结构和弹性衬底的使用导致具有急剧改善的电催化性能（7,9-13）的应变工程化Pt催化剂。然而，将详细绘制在Pt催化转化中的应变活性相关性具有挑战性，这可以涉及许多不同的过程，并鉴定特定反应的最佳应变改性。在这里，我们表明，当超薄Pt壳沉积在基于钯的纳米尺寸上，通过磷化铝化合物的膨胀和收缩率，脱磷诱导Pt（100）晶格中的菌株从-5.1％到5.9％调节。我们使用该应变控制在宽范围内调整Pt壳的电催化活性，发现甲醇氧化反应和氢进化反应的应变活性相关性分别遵循M形曲线和火山形曲线。我们预期我们的方法可用于筛选出晶格菌株，其将优化Pt催化剂的性能 - 以及潜在的其他金属催化剂 - 用于广泛的反应。

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  • 来源
    《Nature》 |2021年第7879期|76-81|共6页
  • 作者

    He Tianou; Wang Weicong; Shi Fenglei; Yang Xiaolong; Li Xiang; Wu Jianbo; Yin Yadong; Jin Mingshang;

  • 作者单位

    Xi An Jiao Tong Univ State Key Lab Multiphase Flow Power Engn Xian Peoples R China|Xi An Jiao Tong Univ Frontier Inst Sci & Technol Xian Peoples R China;

    Xi An Jiao Tong Univ State Key Lab Multiphase Flow Power Engn Xian Peoples R China|Xi An Jiao Tong Univ Frontier Inst Sci & Technol Xian Peoples R China;

    Shanghai Jiao Tong Univ Sch Mat Sci & Engn State Key Lab Met Matrix Composites Shanghai Peoples R China;

    Chongqing Univ Coll Phys Chongqing Peoples R China|Chongqing Univ Ctr Quantum Mat & Devices Chongqing Peoples R China;

    Xian Technol Univ Sch Mat & Chem Engn Xian Peoples R China;

    Shanghai Jiao Tong Univ Sch Mat Sci & Engn State Key Lab Met Matrix Composites Shanghai Peoples R China|Shanghai Jiao Tong Univ Ctr Hydrogen Sci Shanghai Peoples R China|Shanghai Jiao Tong Univ Mat Genome Initiat Ctr Shanghai Peoples R China;

    Univ Calif Riverside Dept Chem Riverside CA 92521 USA;

    Xi An Jiao Tong Univ State Key Lab Multiphase Flow Power Engn Xian Peoples R China|Xi An Jiao Tong Univ Frontier Inst Sci & Technol Xian Peoples R China;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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