Ultralow Content of Chromium Species in Zeolite for Efficient Catalytic Propane Dehydrogenation

IF 15.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Hang Zhou, Guodong Qi, Yueying Chu, Liang Wang*, Yu Hui, Zhangyi Yao, Feng Ryan Wang, Shengqi Chu, Yucai Qin, Lijuan Song, Lu Liu, Xuedi Qin, Jun Xu*, Feng Deng and Feng-Shou Xiao*, 
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Abstract

Supported chromia catalysts have been commercially used in propane dehydrogenation, which relies on Cr loading at weight fractions of up to 20 wt %. This leads to problems in managing spent catalysts with a high content of toxic chromium species. These catalysts also rapidly deactivate within 10–15 min, requiring frequent regeneration in each cycle. To overcome these problems, we developed a siliceous MFI zeolite with an ultralow Cr content (e.g., 0.09 wt %) that exhibits high activity and durability for propane dehydrogenation. A mechanism study revealed that the chromic hydroxyl species readily dissociated the C–H bonds, accelerating the rapid desorption of propylene products and resulting in a slow deactivation rate. Therefore, the catalyst lifetime can be prolonged to more than 30 days under mild operating conditions (525 °C).

Abstract Image

Abstract Image

高效催化丙烷脱氢的超低铬沸石
负载型铬催化剂已经在丙烷脱氢中得到了商业应用,这依赖于Cr在重量分数高达20%的情况下的负载。这导致了管理含有高含量有毒铬的废催化剂的问题。这些催化剂在10-15分钟内迅速失活,在每个循环中需要频繁的再生。为了克服这些问题,我们开发了一种硅质MFI沸石,其Cr含量极低(例如0.09 wt %),对丙烷脱氢具有高活性和耐久性。机理研究表明,铬羟基易于解离C-H键,加速丙烯产品的快速脱附,使其失活速率减慢。因此,在温和的操作条件下(525℃),催化剂寿命可延长至30天以上。
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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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