Coking-resistant iron catalyst in ethane dehydrogenation achieved through siliceous zeolite modulation,Journal of the American Chemical Society

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Coking-resistant iron catalyst in ethane dehydrogenation achieved through siliceous zeolite modulation
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-08-29 , DOI: 10.1021/jacs.0c07792
Zhiyuan Yang _{1,

2} , Huan Li ₃ , Hang Zhou ₁ , Liang Wang ₁ , Lingxiang Wang ₂ , Qiuyan Zhu ₂ , Jianping Xiao ₃ , Xiangju Meng ₂ , Junxiang Chen ₄ , Feng-Shou Xiao _{1,

2}

Affiliation

Non-oxidative dehydrogenation is promising for production of light olefins from shale gas, but current technology relies on pre-cious Pt or toxic Cr catalysts and suffers from thermodynamically oriented coke formation. To solve these issues, the earth-abundant iron catalyst is employed, where Fe species are effectively modulated by siliceous zeolite, which is realized by the syn-thesis of Fe-containing MFI siliceous zeolite in the presence of ethylenediaminetetraacetic sodium (FeS-1-EDTA). Catalytic tests in ethane dehydrogenation show that this catalyst has a superior coke resistance in a 200-hour run without any deactivation with extremely high activity and selectivity (e.g. 26.3% conversion and over 97.5% selectivity to ethene in at 873 K, close to the thermodynamic equilibrium limitation). Multiple characterizations demonstrate that the catalyst has uniformly and stably isolated Fe sites, which improves ethane dehydrogenation to facilitate the fast desorption of hydrogen and olefin products in the zeolite micropores, and hinders the coke formation, as also identified by density functional calculations.

中文翻译：

通过硅质沸石调制实现乙烷脱氢抗焦化铁催化剂

非氧化脱氢有望从页岩气生产轻质烯烃，但目前的技术依赖于贵重的 Pt 或有毒的 Cr 催化剂，并且存在热力学取向的焦炭形成问题。为了解决这些问题，采用地球上丰富的铁催化剂，其中 Fe 物种被硅质沸石有效调节，这是通过在乙二胺四乙酸钠 (FeS-1-) 存在下合成含 Fe 的 MFI 硅质沸石来实现的。乙二胺四乙酸）。乙烷脱氢的催化试验表明，该催化剂在 200 小时的运行中具有优异的抗焦炭性，且没有任何失活，具有极高的活性和选择性（例如，在 873 K 时转化率为 26.3%，乙烯选择性超过 97.5%，接近热力学平衡限制）。

更新日期：2020-08-29

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