Accurately decoding the three-dimensional atomic structure of surface active sites is essential yet challenging for a rational catalyst design. Here, we used comprehensive techniques combining the pair distribution function and reverse Monte Carlo simulation to reveal the surficial distribution of Pd active sites and adjacent coordination environment in palladium–copper nanoalloys. After the fine-tuning of the atomic arrangement, excellent catalytic performance with 98% ethylene selectivity at complete acetylene conversion was obtained in the Pd₃₄Cu₆₆ nanocatalysts, outperforming most of the reported advanced catalysts. The quantitative deciphering shows a large number of active sites with a Pd–Pd coordination number of 3 distributed on the surface of Pd₃₄Cu₆₆ nanoalloys, which play a decisive role in highly efficient semihydrogenation. This finding not only opens the way for guiding the precise design of bimetal nanocatalysts from atomic-level insight but also provides a method to resolve the spatial structure of active sites.

中文翻译：

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解码钯-铜纳米合金中乙炔高效半氢化的活性位点


准确解码表面活性位点的三维原子结构对于合理的催化剂设计至关重要但又具有挑战性。在这里，我们使用配对分布函数和反向蒙特卡罗模拟相结合的综合技术来揭示钯-铜纳米合金中Pd活性位点的表面分布和相邻的配位环境。经过原子排列的微调，Pd ₃₄ Cu ₆₆ 纳米催化剂在乙炔完全转化时获得了优异的催化性能，乙烯选择性为 98%，优于大多数已报道的先进催化剂。催化剂。定量破译显示Pd ₃₄ Cu ₆₆ 纳米合金表面分布有大量Pd-Pd配位数为3的活性位点，这些活性位点对高效能起决定性作用。半氢化。这一发现不仅为从原子水平洞察指导双金属纳米催化剂的精确设计开辟了道路，而且提供了一种解析活性位点空间结构的方法。