Synthesis of Ni/NiAlOx Catalysts for Hydrogenation Saturation of Phenanthrene
The saturation of octahydrophenanthrene was the rate-determining step in the hydrogenation process from phenanthrene to perhydrophenanthrene, which was due to the steric hindrance and competitive adsorption of octahydrophenanthrene. In this work, a series of Ni/NiAlOx catalysts with a uniform electr...
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doaj-02e01f55c47f447f9a0ef787b09a36dc2021-10-08T07:39:06ZengFrontiers Media S.A.Frontiers in Chemistry2296-26462021-10-01910.3389/fchem.2021.757908757908Synthesis of Ni/NiAlOx Catalysts for Hydrogenation Saturation of PhenanthreneDao-Cheng Liu0Dao-Cheng Liu1Yu Chen2Yu Chen3Jie-Ying Jing4Jie-Ying Jing5Antony Rajendran6Antony Rajendran7Hong-Cun Bai8Wen-Ying Li9Wen-Ying Li10State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan, ChinaKey Laboratory of Coal Science and Technology Ministry of Education, Taiyuan University of Technology, Taiyuan, ChinaState Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan, ChinaKey Laboratory of Coal Science and Technology Ministry of Education, Taiyuan University of Technology, Taiyuan, ChinaState Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan, ChinaKey Laboratory of Coal Science and Technology Ministry of Education, Taiyuan University of Technology, Taiyuan, ChinaState Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan, ChinaKey Laboratory of Coal Science and Technology Ministry of Education, Taiyuan University of Technology, Taiyuan, ChinaState Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, Ningxia University, Yinchuan, ChinaState Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan, ChinaKey Laboratory of Coal Science and Technology Ministry of Education, Taiyuan University of Technology, Taiyuan, ChinaThe saturation of octahydrophenanthrene was the rate-determining step in the hydrogenation process from phenanthrene to perhydrophenanthrene, which was due to the steric hindrance and competitive adsorption of octahydrophenanthrene. In this work, a series of Ni/NiAlOx catalysts with a uniform electron-deficient state of Ni derived from the nickel aluminate structure was synthesized to overcome the disadvantage of noble catalyst and the traditional sulfided catalysts in the saturation hydrogenation process of phenanthrene. Results showed that the catalyst calcinated at 650°C possessed more Ni2+ (∼98%) occupying octahedral sites and exhibited the highest robs (1.53 × 10−3 mol kg−1 s−1) and TOF (14.64 × 10−3 s−1) for phenanthrene hydrogenation. Furthermore, its ability to overcome steric hindrance and promote the rate-determining step was proven by octahydrophenanthrene hydrogenation. Comparing the evolution of hydrogenation activity with the change in the electronic structure of surface Ni sites, it was shown that the increase of metallic electron deficiency hindered the π-back bonding between surface Ni and aromatic rings, which was unfavorable for aromatic adsorption. As a result, the phenanthrene hydrogenation saturation performance can be enhanced by stabilizing the electron-deficient state of surface Ni on an optimal degree.https://www.frontiersin.org/articles/10.3389/fchem.2021.757908/fullphenanthrene hydrogenationmetallic electron-deficient statenickel aluminatecalcination temperaturesteric hindrancecompetitive adsorption |
collection |
DOAJ |
language |
English |
format |
Article |
sources |
DOAJ |
author |
Dao-Cheng Liu Dao-Cheng Liu Yu Chen Yu Chen Jie-Ying Jing Jie-Ying Jing Antony Rajendran Antony Rajendran Hong-Cun Bai Wen-Ying Li Wen-Ying Li |
spellingShingle |
Dao-Cheng Liu Dao-Cheng Liu Yu Chen Yu Chen Jie-Ying Jing Jie-Ying Jing Antony Rajendran Antony Rajendran Hong-Cun Bai Wen-Ying Li Wen-Ying Li Synthesis of Ni/NiAlOx Catalysts for Hydrogenation Saturation of Phenanthrene Frontiers in Chemistry phenanthrene hydrogenation metallic electron-deficient state nickel aluminate calcination temperature steric hindrance competitive adsorption |
author_facet |
Dao-Cheng Liu Dao-Cheng Liu Yu Chen Yu Chen Jie-Ying Jing Jie-Ying Jing Antony Rajendran Antony Rajendran Hong-Cun Bai Wen-Ying Li Wen-Ying Li |
author_sort |
Dao-Cheng Liu |
title |
Synthesis of Ni/NiAlOx Catalysts for Hydrogenation Saturation of Phenanthrene |
title_short |
Synthesis of Ni/NiAlOx Catalysts for Hydrogenation Saturation of Phenanthrene |
title_full |
Synthesis of Ni/NiAlOx Catalysts for Hydrogenation Saturation of Phenanthrene |
title_fullStr |
Synthesis of Ni/NiAlOx Catalysts for Hydrogenation Saturation of Phenanthrene |
title_full_unstemmed |
Synthesis of Ni/NiAlOx Catalysts for Hydrogenation Saturation of Phenanthrene |
title_sort |
synthesis of ni/nialox catalysts for hydrogenation saturation of phenanthrene |
publisher |
Frontiers Media S.A. |
series |
Frontiers in Chemistry |
issn |
2296-2646 |
publishDate |
2021-10-01 |
description |
The saturation of octahydrophenanthrene was the rate-determining step in the hydrogenation process from phenanthrene to perhydrophenanthrene, which was due to the steric hindrance and competitive adsorption of octahydrophenanthrene. In this work, a series of Ni/NiAlOx catalysts with a uniform electron-deficient state of Ni derived from the nickel aluminate structure was synthesized to overcome the disadvantage of noble catalyst and the traditional sulfided catalysts in the saturation hydrogenation process of phenanthrene. Results showed that the catalyst calcinated at 650°C possessed more Ni2+ (∼98%) occupying octahedral sites and exhibited the highest robs (1.53 × 10−3 mol kg−1 s−1) and TOF (14.64 × 10−3 s−1) for phenanthrene hydrogenation. Furthermore, its ability to overcome steric hindrance and promote the rate-determining step was proven by octahydrophenanthrene hydrogenation. Comparing the evolution of hydrogenation activity with the change in the electronic structure of surface Ni sites, it was shown that the increase of metallic electron deficiency hindered the π-back bonding between surface Ni and aromatic rings, which was unfavorable for aromatic adsorption. As a result, the phenanthrene hydrogenation saturation performance can be enhanced by stabilizing the electron-deficient state of surface Ni on an optimal degree. |
topic |
phenanthrene hydrogenation metallic electron-deficient state nickel aluminate calcination temperature steric hindrance competitive adsorption |
url |
https://www.frontiersin.org/articles/10.3389/fchem.2021.757908/full |
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