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Low-Temperature Acetylene Semi-Hydrogenation over the Pd1–Cu1 Dual-Atom Catalyst
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2022-09-26 , DOI: 10.1021/jacs.2c07208
Fei Huang 1 , Mi Peng 2 , Yunlei Chen 3 , Xiangbin Cai 4 , Xuetao Qin 2 , Ning Wang 4 , Dequan Xiao 5 , Li Jin 6 , Guoqing Wang 6 , Xiao-Dong Wen 3 , Hongyang Liu 1 , Ding Ma 2
Affiliation  

The atomically dispersed metal catalyst or single-atom catalyst (SAC) with the utmost metal utilization efficiency shows excellent selectivity toward ethylene compared to the metal nanoparticles catalyst in the acetylene semi-hydrogenation reaction. However, these catalysts normally work at relatively high temperatures. Achieving low-temperature reactivity while preserving high selectivity remains a challenge. To improve the intrinsic reactivity of SACs, rationally tailoring the coordination environments of the first metal atom by coordinating it with a second neighboring metal atom affords an opportunity. Here, we report the fabrication of a dual-atom catalyst (DAC) that features a bonded Pd1–Cu1 atomic pair anchoring on nanodiamond graphene (ND@G). Compared to the single-atom Pd or Cu catalyst, it exhibits increased reactivity at a lower temperature, with 100% acetylene conversion and 92% ethylene selectivity at 110 °C. This work provides a strategy for designing DACs for low-temperature hydrogenation by manipulating the coordination environment of catalytic sites at the atomic level.

中文翻译:

Pd1-Cu1双原子催化剂上的低温乙炔半加氢反应

在乙炔半加氢反应中,与金属纳米颗粒催化剂相比,具有最高金属利用效率的原子分散金属催化剂或单原子催化剂(SAC)对乙烯表现出优异的选择性。然而,这些催化剂通常在相对较高的温度下工作。在保持高选择性的同时实现低温反应仍然是一个挑战。为了提高 SAC 的固有反应性,通过与第二个相邻金属原子配位来合理地调整第一个金属原子的配位环境提供了机会。在这里,我们报告了具有键合 Pd 1 –Cu 1的双原子催化剂 (DAC) 的制造。锚定在纳米金刚石石墨烯(ND@G)上的原子对。与单原子 Pd 或 Cu 催化剂相比,它在较低温度下表现出更高的反应性,在 110 °C 时乙炔转化率为 100%,乙烯选择性为 92%。这项工作提供了一种通过在原子水平上操纵催化位点的配位环境来设计用于低温加氢的 DAC 的策略。
更新日期:2022-09-26
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