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负载于MgBO微晶上的自演化硼氧化物用于丙烷的高效氧化脱氢反应

Self-evolved BO anchored on MgBO crystallites for high-performance oxidative dehydrogenation of propane.

作者信息

Zhang Dake, Wang Shenghua, Lu Xingyu, Zhang Chengcheng, Feng Kai, He Le, Zhang Hui, Sun Wei, Yang Deren

机构信息

State Key Laboratory of Silicon Materials and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, Zhejiang 310027, People's Republic of China.

Key Laboratory of Precise Synthesis of Functional Molecules of Zhejiang Province, Instrumentation and Service Center for Molecular Sciences, Westlake University, 18 Shilongshan Road, Hangzhou 310024, Zhejiang Province, China.

出版信息

iScience. 2023 Oct 6;26(11):108135. doi: 10.1016/j.isci.2023.108135. eCollection 2023 Nov 17.

DOI:10.1016/j.isci.2023.108135
PMID:37876808
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10590969/
Abstract

Oxidative dehydrogenation of propane (ODHP) is a promising process for producing propene. Recently, some boron-based catalysts have exhibited excellent olefin selectivity in ODHP. However, their complex synthetic routes and poor stability under high-temperature reaction conditions have hindered their practical application. Herein, we report a self-evolution method rather than conventional assembly approaches to acquire structures with excellent stability under a high propane conversion, from a single precursor-MgB. The catalyst feasibly prepared and optimized exhibited a striking performance: 60% propane conversion with a 43.2% olefin yield at 535°C. The BO corona pinned by the strong interaction with the borate enabled zero loss of the high conversion (around 40%) and olefins selectivity (above 80%) for over 100 h at 520°C. This all-in-one strategy of deriving all the necessary components from just one raw chemical provides a new way to synthesize effective and economic catalysts for potential industrial implementation.

摘要

丙烷氧化脱氢(ODHP)是一种很有前景的生产丙烯的工艺。最近,一些硼基催化剂在ODHP中表现出优异的烯烃选择性。然而,它们复杂的合成路线以及在高温反应条件下较差的稳定性阻碍了其实际应用。在此,我们报道了一种自我演化方法,而非传统的组装方法,从单一前驱体MgB中获得在高丙烷转化率下具有优异稳定性的结构。通过可行的制备和优化得到的催化剂展现出了显著的性能:在535°C时丙烷转化率为60%,烯烃产率为43.2%。与硼酸盐的强相互作用固定的BO冠层使得在520°C下超过100小时内高转化率(约40%)和烯烃选择性(高于80%)零损失。这种仅从一种原料化学品中衍生出所有必要组分的一体化策略为潜在工业应用合成有效且经济的催化剂提供了一种新方法。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a0c4/10590969/a3781877e962/gr6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a0c4/10590969/f4ff52cfff9b/fx1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a0c4/10590969/7d615ebd1692/gr1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a0c4/10590969/358335bda41c/gr2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a0c4/10590969/947970833bb4/gr3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a0c4/10590969/f87a334c7be5/gr4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a0c4/10590969/3e95bc3c2d0f/gr5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a0c4/10590969/a3781877e962/gr6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a0c4/10590969/f4ff52cfff9b/fx1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a0c4/10590969/7d615ebd1692/gr1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a0c4/10590969/358335bda41c/gr2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a0c4/10590969/947970833bb4/gr3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a0c4/10590969/f87a334c7be5/gr4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a0c4/10590969/3e95bc3c2d0f/gr5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a0c4/10590969/a3781877e962/gr6.jpg

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本文引用的文献

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2
Illustrating new understanding of adsorbed water on silica for inducing tetrahedral cobalt(II) for propane dehydrogenation.阐明了关于硅胶吸附水诱导四面体钴(II)进行丙烷脱氢的新认识。
Nat Commun. 2023 Jan 6;14(1):100. doi: 10.1038/s41467-022-35698-0.
3
Engineering O-O Species in Boron Nitrous Nanotubes Increases Olefins for Propane Oxidative Dehydrogenation.
在氮化硼纳米管中设计氧-氧物种可提高用于丙烷氧化脱氢的烯烃产量。
J Am Chem Soc. 2022 Apr 6;144(13):5930-5936. doi: 10.1021/jacs.1c13563. Epub 2022 Mar 22.
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In situ formation of ZnO species for efficient propane dehydrogenation.原位形成 ZnO 物种以实现高效丙烷脱氢。
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Plasma Tuning Local Environment of Hexagonal Boron Nitride for Oxidative Dehydrogenation of Propane.用于丙烷氧化脱氢的等离子体调节六方氮化硼的局部环境
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