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首页> 外文期刊>Journal of Catalysis >Highly-active nickel phosphide hydrotreating catalysts prepared in situ using nickel hypophosphite precursors
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Highly-active nickel phosphide hydrotreating catalysts prepared in situ using nickel hypophosphite precursors

机译：使用次磷酸镍前体原位制备的高活性磷化镍加氢处理催化剂

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摘要

An in situ method for the preparation of nickel phosphide (Ni2P) on silica, alumina, and amorphous silica alumina (ASA) supports is described. The synthesis avoids the use of nickel and phosphorus salts by employing the reaction between nickel hydroxide (Ni(OH)(2)) and hypophosphorus acid (H3PO2), allowing the impregnation of nickel hypophosphite (Ni(H2PO2)(2)) onto the oxide supports in the absence of salt by-products. Temperature-programmed reduction (TPR) in flowing hydrogen at 573-773 K yields phase pure Ni2P on the supports with small average particle sizes (3-4 nm) as measured using transmission electron microscopy. The conversion of Ni(H2PO2)(2) to Ni2P and related reactions were probed using TPR with on-line mass spectral analysis of the gas effluent. Unsupported Ni(H2PO2)(2) reacts in flowing hydrogen to produce PH3 and H2O at 468 and 482 K, respectively; the reaction is shifted to increasingly higher temperatures for Ni(H2PO2)(2) supported on SiO2, Al2O3 and ASA. The hydrodenitrogenation (HDN) and hydrodesulfurization (HDS) properties of the Ni2P catalysts were probed using a mixed feed containing carbazole and benzothiophene. While Ni2P/SiO2 catalysts prepared by the different methods exhibited similar HDN and HDS activities, the in situ prepared Ni2P/Al2O3 and Ni2P/ASA catalysts were substantially more active than their ex situ counterparts prepared from hypophosphite- and phosphate-based precursors. (C) 2015 Elsevier Inc. All rights reserved.
机译：描述了在二氧化硅，氧化铝和无定形二氧化硅氧化铝（ASA）载体上制备磷化镍（Ni2P）的原位方法。该合成通过利用氢氧化镍（Ni（OH）（2））和次磷酸（H3PO2）之间的反应避免使用镍盐和磷盐，从而将次磷酸镍（Ni（H2PO2）（2））浸渍到不含盐副产物的氧化物载体。使用透射电子显微镜测量，在573-773 K下流动的氢气中的程序升温还原（TPR）可在载体上产生纯的Ni2P相，平均粒径小（3-4 nm）。使用TPR对废气进行在线质谱分析，探讨了Ni（H2PO2）（2）向Ni2P的转化以及相关的反应。无载体的Ni（H2PO2）（2）在流动的氢气中反应，分别在468 K和482 K时产生PH3和H2O。对于负载在SiO2，Al2O3和ASA上的Ni（H2PO2）（2），反应转移到越来越高的温度。使用含有咔唑和苯并噻吩的混合进料对Ni2P催化剂的加氢脱氮（HDN）和加氢脱硫（HDS）性能进行了研究。尽管通过不同方法制备的Ni2P / SiO2催化剂表现出相似的HDN和HDS活性，但原位制备的Ni2P / Al2O3和Ni2P / ASA催化剂的活性远高于由次磷酸盐和磷酸盐前体制备的原位催化剂。 （C）2015 Elsevier Inc.保留所有权利。

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