Selective Formation of Acetic Acid and Methanol by Direct Methane Oxidation Using Rhodium Single-Atom Catalysts,Journal of the American Chemical Society

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Selective Formation of Acetic Acid and Methanol by Direct Methane Oxidation Using Rhodium Single-Atom Catalysts
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-05-12 , DOI: 10.1021/jacs.3c03113
Haoyi Li ₁ , Chuanye Xiong ₂ , Muchun Fei ₁ , Lu Ma ₃ , Hongna Zhang ₁ , Xingxu Yan _{4,

5} , Peter Tieu ₆ , Yucheng Yuan ₁ , Yuhan Zhang ₁ , James Nyakuchena ₇ , Jier Huang ₇ , Xiaoqing Pan _{4,

5,

8} , Matthias M Waegele ₁ , De-En Jiang ₂ , Dunwei Wang ₁

Affiliation

Atomically dispersed catalysts such as single-atom catalysts have been shown to be effective in selectively oxidizing methane, promising a direct synthetic route to value-added oxygenates such as acetic acid or methanol. However, an important challenge of this approach has been that the loading of active sites by single-atom catalysts is low, leading to a low overall yield of the products. Here, we report an approach that can address this issue. It utilizes a metal–organic framework built with porphyrin as the linker, which provides high concentrations of binding sites to support atomically dispersed rhodium. It is shown that up to 5 wt% rhodium loading can be achieved with excellent dispersity. When used for acetic acid synthesis by methane oxidation, a new benchmark performance of 23.62 mmol·g_cat^–1·h^–1 was measured. Furthermore, the catalyst exhibits a unique sensitivity to light, producing acetic acid (under illumination, up to 66.4% selectivity) or methanol (in the dark, up to 65.0% selectivity) under otherwise identical reaction conditions.

中文翻译：

铑单原子催化剂直接氧化甲烷选择性生成乙酸和甲醇

原子分散的催化剂如单原子催化剂已被证明可有效地选择性氧化甲烷，有望为乙酸或甲醇等增值含氧化合物提供直接合成途径。然而，这种方法的一个重要挑战是单原子催化剂的活性位点负载量低，导致产品的总收率低。在这里，我们报告了一种可以解决此问题的方法。它利用以卟啉作为连接体构建的金属有机框架，提供高浓度的结合位点以支持原子分散的铑。结果表明，可以实现高达 5 wt% 的铑载量并具有出色的分散性。用于甲烷氧化合成乙酸时，新基准性能为23.62 mmol·g _cat^–1·h ^–1被测量。此外，该催化剂对光表现出独特的敏感性，在其他相同的反应条件下产生乙酸（在光照下，选择性高达 66.4%）或甲醇（在黑暗中，选择性高达 65.0%）。

更新日期：2023-05-12

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