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用于丙烷直接脱氢制丙烯的选择性稳定非贵金属金属间化合物催化剂

Selective and Stable Non-Noble-Metal Intermetallic Compound Catalyst for the Direct Dehydrogenation of Propane to Propylene.

作者信息

He Yang, Song Yuanjun, Cullen David A, Laursen Siris

机构信息

Department of Chemical and Biomolecular Engineering , University of Tennessee , Knoxville , Tennessee 37996 , United States.

Materials Science and Technology Division and Center for Nanophase Materials Sciences , Oak Ridge National Laboratory , Oak Ridge , Tennessee 37831 , United States.

出版信息

J Am Chem Soc. 2018 Oct 31;140(43):14010-14014. doi: 10.1021/jacs.8b05060. Epub 2018 Oct 22.

Abstract

A non-noble intermetallic compound catalyst consisting of NiGa nanoparticles supported on AlO that exhibits high selectivity (∼94%), comparable activity (TOF = 4.7 × 10 s), good stability (∼94% to 81% over the 82 h test), and regenerability in the direct dehydrogenation of propane to propylene at 600 °C has been developed. Through synthesis techniques that stabilize the NiGa phase, the surface composition of the catalytic nanoparticles could be tuned by Ni and Ga loading such that improved selectivity toward propylene may be achieved. Comparisons with well-defined silica-supported NiGa and NiGa catalysts and NiGa/AlO with a range of Ni:Ga loading suggested that a specific surface composition range was most promising for propylene production. The presence of Ni at the active particle surface was also found to be critical to drive dehydrogenation and enhance conversion, whereas the presence of Ga was necessary to attenuate the reactivity of the surface to improve selectivity and catalyst stability.

摘要

已开发出一种由负载在AlO上的NiGa纳米颗粒组成的非贵金属金属间化合物催化剂,该催化剂在600℃下丙烷直接脱氢制丙烯反应中表现出高选择性(约94%)、相当的活性(TOF = 4.7×10 s)、良好的稳定性(在82小时测试中从约94%降至81%)和可再生性。通过稳定NiGa相的合成技术,可以通过Ni和Ga负载量调节催化纳米颗粒的表面组成,从而实现对丙烯选择性的提高。与明确的二氧化硅负载的NiGa和NiGa催化剂以及具有一系列Ni:Ga负载量的NiGa/AlO的比较表明,特定的表面组成范围对丙烯生产最有前景。还发现活性颗粒表面存在Ni对于驱动脱氢和提高转化率至关重要,而Ga的存在对于减弱表面反应性以提高选择性和催化剂稳定性是必要的。

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