Pure Siliceous Zeolite-Supported Ru Single-Atom Active Sites for Ammonia Synthesis
Pure Siliceous Zeolite-Supported Ru Single-Atom Active Sites for Ammonia Synthesis
复制标题
纯硅质沸石负载Ru单原子合成氨活性位点
DOI：
10.1021/acs.chemmater.9b03099
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发表时间：
2019-10
影响因子：
8.6
通讯作者：
Jiuxing Jiang
中科院分区：
文献类型：
--
作者：
Jiang-Zhen Qiu;Jibo Hu;Jinggang Lan;Long-Fei Wang;Guangying Fu;Rujian Xiao;Binghui Ge;Jiuxing Jiang
单原子催化剂（SAC）作为最活跃的新领域，集多相和均相催化剂的优点于一身，将对氨合成研究的百年历史产生重大影响。在这里，Ru SAC已被证明是活性和有效的氨合成。为此，设计了一种理想的模型催化剂，即纯硅质沸石负载的Ru SAC（Ru SAs/S-1），与传统的Ru催化剂相比，它显示出令人惊讶的催化氨合成活性。原子分辨率扫描透射电子显微镜，X-射线吸收光谱分析，并在原位漫反射红外傅里叶变换光谱确定的Ru SA/S-1的反应前后的单Ru原子的性质。进一步的DFT计算表明，该反应机理不同于传统的反应机理.因此，本文提供了一种替代SAC策略来设计高性能的氨合成钌催化剂。
As the most active new frontier, a single-atom catalyst (SAC) combining the merits of heterogeneous and homogeneous catalysts would have a significant effect on the 100 year history of ammonia synthesis research. Here, the Ru SAC has been demonstrated to be active and efficient for ammonia synthesis. To this end, an ideal model catalyst, pure siliceous zeolite-supported Ru SAC (Ru SAs/S-1), which shows surprising catalytic ammonia synthesis activity compared to that of a conventional Ru catalyst, was designed. Both atomic-resolution scanning transmission electron microscopy, X-ray absorption spectrometric analysis, and in situ diffuse reflectance infrared Fourier transform spectroscopy identify the single-Ru-atom nature of Ru SAs/S-1 before and after the reaction. Further DFT calculations reveal that the reaction mechanism is different from traditional mechanisms. Therefore, this paper provides an alternative SAC strategy to design high-performance Ru catalysts for ammonia synthesis.
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通讯作者：
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