Directional Catalytic Hydroconversion of Oxybis (methylene)dibenzene and an Extract from Piliqing Subbituminous Coal over a Magnetic Difunctional Solid Superbase,ChemistrySelect

当前位置： X-MOL 学术 › ChemistrySelect › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Directional Catalytic Hydroconversion of Oxybis (methylene)dibenzene and an Extract from Piliqing Subbituminous Coal over a Magnetic Difunctional Solid Superbase
ChemistrySelect ( IF 1.9 ) Pub Date : 2020-01-20 , DOI: 10.1002/slct.201902388
Mei‐Ling Xu _{1,

2} , Xian‐Yong Wei _{1,

3} , Guang‐Hui Liu ₁ , Feng‐Hai Li ₂ , Yun‐Peng Zhao ₁ , Fang‐Jing Liu ₁ , Sheng Li ₁ , Zhi‐Min Zong ₁ , Xing Fan _{1,

3} , Jing‐Pei Cao ₁ , Wei Zhao ₁ , Feng‐Yun Ma ₃ , Jing‐Mei Liu ₃

Affiliation

An active and novel magnetic difunctional solid superbase catalyst Ni‐Mg₂Si/attapulgite powder (AP) was prepared by thermally decomposing nickel tetracarbonyl onto the as‐synthesized Mg₂Si/AP followed by impregnating Mg₂Si onto AP in CCl₄ and characterized by multiple analyses. It was also successfully used in the catalytic hydroconversion (CHC) of coal‐related model compound oxybis (methylene) dibenzene (OBMDB) and an extract (E) from Piliqing subbituminous coal (PSBC) in n‐hexane. As a result, OBMDB was completely converted to methylcyclohexane by the CHC under 3 MPa of initial hydrogen pressure at 240 °C for 2 h. Ni‐Mg₂Si/AP can activate H₂ to biatomic active hydrogen (H^…H) and split H₂ to immobile H⁺ attached on the Ni‐Mg₂Si/AP surface and relatively mobile H⁻. Then the bridged linkage (BL) in OBMDB can be cleaved by H⁻ attack on a α‐carbon atom in OBMDB, producing toluene and benzyloxy anion, which abstracts H⁺ from the Ni‐Mg₂Si/AP surface to afford phenylmethanol (PM). The α‐carbon in PM is attacked by H^‐ to generate toluene and HO⁻. H^…H transfers to benzene ring in toluene yields methylcyclohexane. The soluble portion (SP) from the CHC (SP_E‐CHC) and non‐CHC (NCHC) (SP_E‐NCHC) of E were analyzed with a gas chromatograph/mass spectrometer and Fourier transform infrared spectrometer. Non‐substituted cycloalkanes (NSCAs) are predominant in the SP_E‐CHC, accounting for 66.9 % of the total group components, and interestingly 65.3 % of NSCAs is cyclohexane, while non‐substituted arenes are the most abundant in the SP_E‐NCHC. The results indicate that the CHC is beneficial to the fracture of COCBB and hydrogenation of ARs to produce more NSCAs.

中文翻译：

磁性双官能固体超碱定向氧化催化氧化双（亚甲基）二苯和P青轻质烟煤的提取物

活性和新颖磁性双官能固体超强碱催化剂Ni-Mg系₂的Si /绿坡缕石粉末（AP）通过热分解四羰基镍制备到如此合成的Mg ₂的Si / AP，随后浸渍的Mg ₂中的CCl的Si到AP ₄和表征通过多次分析。也有人在催化加氢煤相关的模型化合物氧双（亚甲基）二苯（OBMDB）和提取物（的（CHC）成功地用于Ë从皮里青亚烟煤（PSBC））在Ñ正己烷。结果，在240℃的初始氢气压力3 MPa下，CHC将OBMDB在3 MPa的初始氢气压力下完全转化为甲基环己烷。Ni‐Mg ₂ Si / AP可以活化H ₂到biatomic活性氢（H ^... H）和分裂ħ ₂至动ħ ⁺附着在Ni-Mg系上₂的Si / AP表面和相对流动氢^-。然后在OBMDB所述桥接连接（BL）可以由H裂解^-在OBMDB一个α碳原子上的攻击，从而产生甲苯和苄氧基阴离子，其抽象ħ ⁺从Ni-Mg系₂的Si / AP表面，得到苯基甲醇（PM ）。在PM的α碳是由H攻击^-以生成甲苯和HO ^-。H ^… H转移至甲苯中的苯环，生成甲基环己烷。CHC（SP _E_- CHC）中的可溶部分（SP））和非CHC（NCHC）（SP _{Ë -NCHC}的）Ë用气相色谱仪/质谱仪分析和傅里叶变换红外光谱仪。SP _E‐CHC中非取代的环烷烃（NSCAs）占主导地位，占总组份的66.9％，有趣的是NSCAs的65.3％是环己烷，而SPE _‐NCHC中非取代的芳烃含量最高。结果表明，CHC有利于COCBB的断裂和AR的氢化生成更多的NSCA。

更新日期：2020-01-21

点击分享查看原文

点击收藏

阅读更多本刊最新论文本刊介绍/投稿指南11