Atomistic engineering of active sites with multiple functional motifs has gained significant attention in heterogeneous catalytic science due to their potential synergistic cooperativity. While these catalysts have demonstrated superior performance in various applications, a lack of systematic study hampers the understanding of intricate synergism. In this study, we present a comprehensive investigation into the synergistic cooperativity between a combination of metal sites (M = Fe³⁺ and Cu²⁺) and dominant Brønsted acid sites (BASs, X = B, Ga, and Al) in MFI-type zeolites with delicate control over their quantities and respective distribution. By employing two model catalytic reactions that simultaneously utilize the two active motifs in proximity, we examined the cooperativity required to modulate catalytic reactivity. Combined synchrotron X-ray powder diffraction and theoretical evidence revealed the synergism and the respective contribution of the active pairs of metal-BAS within molecular distances.

中文翻译：

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通过同步加速器X射线粉末衍射研究MFI型沸石中金属-布朗斯台德酸性位点对的协同协同作用


具有多个功能基序的活性位点的原子工程由于其潜在的协同作用而在异质催化科学中获得了极大的关注。虽然这些催化剂在各种应用中表现出优异的性能，但缺乏系统的研究阻碍了对复杂协同作用的理解。在本研究中，我们对 MFI- 中金属位点（M = Fe ³⁺和 Cu ²⁺ ）与占主导地位的布朗斯台德酸位点（BAS、X = B、Ga 和 Al）之间的协同协同性进行了全面研究。类型沸石，对其数量和各自的分布进行精细控制。通过采用同时利用两个邻近活性基序的两个模型催化反应，我们检查了调节催化反应性所需的协同性。同步加速器 X 射线粉末衍射和理论证据相结合揭示了分子距离内金属-BAS 活性对的协同作用和各自的贡献。