近日,中国科学院苏州纳米技术与纳米仿生研究所徐勇团队研究了超耐用再生丙烷脱氢催化剂的氟化约束与定位。2025年10月13日出版的《美国化学会志》发表了这项成果。
在化学工业中,丙烷脱氢催化剂的精心设计应具有丙烷转化率高、丙烯选择性强、耐烧结、耐积炭、易于再生等特点。
研究组报道了一种用于PDH的氟化硅化MFI沸石包裹的PtSn的独特设计,其中氟化诱导在全硅分子筛中形成“孔”和超小型PtSn纳米微米的位置,这是因其高活性、选择性,特别是在PDH超过5000小时的烧结过程中具有显著的耐烧结性。目前的催化剂在本国相关条件下分别显示出接近热力学极限的丙烷转化率和94%的丙烯选择性纯丙烷。
令人印象深刻的是,焦化催化剂可在相同温度下通过H2处理简单地再生PDH,避免了传统再生方法中复杂、有毒、腐蚀性强的氧化氯化过程,这将有助于原位PDH工艺的广泛应用。详细的研究表明,氟改性的PtSn纳米柱与MFI沸石之间的强协同作用可以促进PDH对丙烯的选择性,并稳定PtSn纳米柱的烧结和积炭性能。催化剂的独特设计和性能提升将为解决目前工业PDH工艺中的难题提供一个可行的策略。
附:英文原文
Title: Ultradurable Regenerative Propane Dehydrogenation Catalyst by Fluorination-Induced Confining and Positioning
Author: Yuting He, Shiyun Xiong, Zhongliang Huang, Guodong Qi, Xiaoqing Li, Xiaozhi Liu, Jun Xu, Dong Su, Zhiwei Hu, Wei-Hsiang Huang, Chih-Wen Pao, Shuangli Yang, Mingshu Chen, Yong Xu, Xiaoqing Huang
Issue&Volume: October 13, 2025
Abstract: In the chemical industry, an elaborated design of catalysts for propane dehydrogenation (PDH) should be capable of high propane conversion and propylene selectivity, strong resistance to sintering and coke deposition, and easy regeneration. Here, we report a unique design of fluorinated siliceous MFI zeolite-clothed PtSn for PDH, where the fluorination induces the formation of “holes” in all-silica molecular sieves and the position of ultrasmall PtSn nanoclusters as a result of high activity, selectivity, and especially remarkable resistance to sintering during PDH over 5000 h. The present catalyst displays a near-thermodynamic-limited propane conversion and 94% propylene selectivity in pure propane, respectively, under industrially relevant conditions. Impressively, the coked catalyst can be simply regenerated by H2 treatment at the same temperature for PDH, avoiding the complicated, poisonous, and corrosive oxychlorination process in the conventional method for regeneration, which will contribute to the extensive application of the industrial PDH process. Detailed investigations demonstrate that the strong synergy between F-modified PtSn nanoclusters and MFI zeolite can promote the selective PDH to propylene and stabilize PtSn nanoclusters against sintering and coke deposition. The unique design of the catalyst and the enhanced performance will provide a feasible strategy to solve the current difficulties in the industrial PDH process.
DOI: 10.1021/jacs.5c11524
Source: https://pubs.acs.org/doi/abs/10.1021/jacs.5c11524
JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:16.383
官方网址:https://pubs.acs.org/journal/jacsat
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