CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Yilong Xu,Shihao Fu,Yuxin Wen,Wenqing Lv,Liangyan Ma,Haoquan Hu,Lijun Jin
Limonene is significant feedstock and how to abundantly acquire or convert into high-value chemicals is crucial. Waste tire pyrolysis oil (TPO) rich in limonene provides an alternative route. To address its difficult separation from other compounds in TPO, especially p -cymene, a new route to convert limonene into α-terpinyl methyl ether (TME) with high boiling point was proposed by alkoxylation over heteropolyacid-modified Hβ zeolite. Strong Brønsted acid centers can attain high efficiency in alkoxylation in limonene- p -cymene binary compounds. 89.24 % conversion was achieved after 5 h at 60 °C while TME yield is the highest (71.70 %) after 3 h with no reaction of p -cymene. Above 80 % limonene is transformed in real fraction of 160–180 °C of TPO and TME yield exceeds 60 %. Initial separation of TME and aromatic was achieved by vacuum distillation. The possible mechanism of limonene alkoxylation was proposed. This work provides a new approach to efficient utilization of limonene.
研究领域:
化学工程
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS COMMUNICATIONS
·
2023
·
IF 3.7
Jiuhu Zhao,Huiying Li,Yungang Wang,Rongshu Zhu,Senlin Sun,Jingwen Zhang,Chaolin Li,Mei Hong
Mesoporous In/Hβ-X series catalysts were prepared by desilication method with tetrapropylammonium hydroxide (TPAOH) and indium incorporation for selective catalytic reduction of NO with methane (CH 4 -SCR). The post desilication treatment conditions for preparing In/Hβ-X were optimized. Etching time is the most important desilication parameter influencing the resulting CH 4 -SCR performance of the catalyst. The In/Hβ-3 sample which was etched for 3 h presents the highest NO x conversion, 22% higher than In/H-Beta counterparts using commercial microporous beta. Obvious analysis reveals that besides generating mesopores, controlled desilication can modulate the proportion of InO + active sites and surface oxygen species, allowing more active sites to be exposed.
研究领域:
催化
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Haoxi Jiang,Zhonghua Liu,Chuanxu Yao,Sheng Wang
The emission of volatile organic compounds (VOCs) causes serious atmospheric environmental problems and catalytic combustion is one of the most promising methods in the treatment of VOCs. In this work, the Pt/Hβ catalyst was fabricated via supercritical fluid deposition (SFD) for the first time and its activity was evaluated for toluene catalytic combustion. The preparation conditions during the SFD process were optimized. Na 2 PtCl 6 was selected as the precursor and 450 °C as the reduction temperature. The catalysts prepared by the SFD and impregnation (IM) were compared. The Pt/Hβ catalyst prepared by SFD had smaller size and higher dispersion and its T90 was 25 °C lower than that prepared by IM, which showed obvious size effect. For the similar activity, the Pt loading on catalyst prepared by SFD is only 50% of that on catalyst prepared by IM, showing obvious reduction effect for noble metal.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2021
·Vol. 152
·期 6
·1844-1853
·
IF 3.186
Li Zihan,Yang Lingbin,Zhu Lijun,Xia Daohong
Novel B-doped NiP/Hβ (Hβ is the hydrogen proton exchanged β molecular sieve) catalysts were prepared and the catalytic performance for n-C 6 (n-hexane) isomerization was studied firstly. It was found that the mole ratio of Ni, P and B in preparing B-doped NiP had important influence on the crystalline structure and catalytic activity of NiPB. When the mole ratio of Ni, P and B was 1:1:1, the prepared NiPB was amorphous and NiPB/Hβ had the best catalytic activity with the conversion rate of n-C 6 , the yield and selectivity of isoparaffins being 79.93%, 78.34% and 98.01% respectively. It was also showed that the preparation conditions of catalyst including NiPB loading on carrier and calcination temperatures were the key factors for the catalytic performance of NiPB/Hβ. In controlled experiments, ammonia poisoned acid sites on the catalyst led to the markedly reducing of catalytic performance and metal sites were essentially for the dehydrogenation-hydrogenation reaction. The isomerization of n-C 6 catalyzed by NiPB/Hβ is a continuous alternating process of acid catalysis and metal catalysis, and the matching of acid sites and metal sites is of importance. Graphic Abstract
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Weipeng Song,Huai Liu,Junhua Zhang,Yong Sun,Lincai Peng
Furfural represents one of the most valuable biomass-derived platform molecules. Its selective production with a smart and tractable catalytic system is highly attractive for technical implementation, yet remains challenging. We herein report a promising protocol involving the mature Hβ zeolites in pure 1,4-dioxane to convert hemicellulose-related sugars into furfural with high rate and impressive selectivity under mild operating conditions. Furfural yields as high as 93.6% (from xylose) and 85.9% (from xylan) were accomplished at 140 °C in 40 min. The solvent 1,4-dioxane served as a shield to maintain the crystal structure and acidic center of Hβ as well as to inhibit the polymerization of furfural. The synergistic action of Hβ with 1,4-dioxane largely promoted the selective conversion of xylose to furfural, as the multiple immobilized acid sites of Hβ in 1,4-dioxane medium accelerated xylose-to-xylulose isomerization. The dehydration process was favorable based on its apparent activation energy of 39.1 kJ mol–1, leading to a high turnover frequency of 53.8 h–1. Density functional theory calculations revealed that the superior catalytic behavior could be ascribed to the higher adsorption of xylose than 1,4-dioxane, allowing xylose molecules to fully access the open Al sites of Hβ and the low Gibbs free energy barrier of xylose isomerization to xylulose in 1,4-dioxane over the Hβ catalyst. Moreover, the heterogeneous zeolite catalyst and the single low-boiling-point solvent 1,4-dioxane (101 °C) were readily recovered from the product with outstanding reusability. This contribution not only opens a high potential avenue for the selective production of furfural but also sheds light on the coordination mechanism of Hβ zeolite and 1,4-dioxane toward developing tailored processes.
研究领域:
化学工程
·
催化
·
生物质转化
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
·
2021
·
IF 6.186
Lin Hu,Xian-Yong Wei,Zhi-Ming Zong
Recently hydrocarbons with high yield from the selective hydrodeoxygenation (HDO) of lignin-derived bio-oil under low temperature still encounters the great challenges. However, metal nanoparticles size and acid site can greatly influence the HDO activity of metal catalyst . Herein, the efficient bifunctional Ru/Hβ catalyst was prepared by modified deposition-precipitation (DP) method for the HDO reaction of guaiacol and catalytic isoproanolysis lignin-derived bio-oil. Notably, compared to the impregnated Ru 3% /Hβ-25 catalyst, Ru 3% /Hβ-25 (DP) catalyst exhibited the higher catalytic activity on the HDO of guaiacol, smaller Ru nanoparticles size, and more acid sites. It was observed that guaiacol can be completely converted to cyclohexane under 180 °C, 3 MPa H 2 , and 2 h in n -hexane. This Ru 3% /Hβ-25 (DP) catalyst proved to be the good recyclability in the HDO reaction of guaiacol, the conversion decreased slightly to 82.3% and the yield of cyclohexane decreased to 71.2 mol% after four recycle times. Furthermore, this high active catalyst was also applied to the upgradation of bio-oil derived from the catalysis isoproanolysis of lignin in the organic phase. As a result, after the upgradation, bio-oil contained high relative content (RC) of hydrocarbons, including 42.99% cycloalkanes and 50.74% arenes, and oxygenated compounds of raw bio-oil were almost removed. Overall, during upgradation of raw lignin-derived bio-oil over Ru 3% /Hβ-25 (DP) catalyst process, not only HDO reaction, but also cleavage of C-O bonds can be achieved in one-pot.
研究领域:
催化化学
·
能源化学
·
生物质转化
✓ 已验证
产品关联
DOI
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2022
·Vol. 48
·期 3
·1095-1109
·
IF 3.134
Deng Renjie,Zeng Manlin,Tian Yao
A novel heterogeneous catalytic system was developed for the preparation of para -nitrobromobenzene ( p -NBr) with nitrogen dioxide (NO 2 ) as nitrating agent in the presence of oxygen (O 2 ). By applying Hβ zeolite as the catalyst, p -NBr can be obtained with high conversion (85.7%) and selectivity (91.7%). In addition, it can be recycled at least five times without a significant decrease in catalytic activity, which demonstrates its high efficiency, good stability and regenerability. Meanwhile, DFT study explained the regioselectivity for the nitronium (NO 2 + ) nitration via electrophilic process, which support the experimental conclusion. Graphical abstract
研究领域:
催化
·
有机化学
·
理论化学
✓ 已验证
DOI
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2025
·
IF 3.5
Yan Jiaqi,Chen Wenkai,Ni Wenjin,Li Lu,Fu Jinfeng,Yang Qian,Yang Zhiyong
N -cyclohexylcyclohexanimine (N-CCA), a by-product of cyclohexylamine (CHA) oxidation to cyclohexanone oxime (CHO), was used as the starting reactant for the efficient conversion to CHO under an oxygen atmosphere, utilizing the constructed surface hydroxyl-rich Ti-based catalysts. Of these, the 20% TiO 2 /Hβ catalyst exhibited unique catalytic activity and stability, achieving 45.9% N-CCA conversion and 82.1% CHO selectivity, with the content of high-boiling by-products not exceeding 1.0%. The superior catalytic performance, as evidenced by characterization results, stems primarily from: (i) the combination of TiO 2 and Hβ, which promotes the formation of a high specific surface area with fine TiO 2 nanoparticles and high-density Ti δ+ active sites, which facilitate the adsorption and activation of N-CCA; (ii) the construction of rich hydroxyl groups, which enhances the Brønsted acid sites, thereby improving the generation of active oxygen species; (iii) the intercrystalline embedding of TiO 2 and Hβ, which forms Ti–O–Si bonds, effectively inhibiting Ti leaching and ensuring excellent catalyst stability. The conversion of N-CCA, the main by-product of CHA oxidation, to the desired CHO using an efficient and robust 20% TiO 2 /Hβ catalyst represents an attractive pathway.
研究领域:
催化
·
材料科学
·
化学反应工程
·
表面化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Jinshe Chen,Zunbin Duan,Zhaoyang Song,Lijun Zhu,Yulu Zhou,Yuzhi Xiang,Daohong Xia
The amorphous NiP nanoparticles were synthesized and a novel amorphous NiP/Hβ catalyst was prepared successfully further. Due to the superior surface property of amorphous NiP/Hβ catalyst, it exhibited good catalytic application for n-hexane isomerization. The catalytic activity of amorphous NiP/Hβ catalyst was close to that of the prepared Pt/Hβ sample, and better than that of commercial catalyst and crystalline Ni 2 P/Hβ catalyst. What's more, the amorphous NiP/Hβ catalyst shows high resistance to different sulfur compounds and water on account of its unique surface property. The effect of loading amounts on surface property and catalytic performance was investigated, and the structure-function relationship among them was studied ulteriorly. The results demonstrate that loading amounts have effect on textural property and surface acid property, which further affect the catalytic performance. The 10 wt.% NiP/Hβ sample has appropriate pore structure and acid property with uniformly dispersed NiP nanoparticles on surface, which is helpful for providing suitable synergistic effect. The effects of reaction conditions on surface reactions and the mechanism for n-hexane isomerization were investigated further. Based on these results, the amorphous NiP/Hβ catalyst with superior surface property probably pavesa way to overcome the drawbacks of traditional noble metal catalyst, which shows good catalytic application prospects.
研究领域:
催化
·
化学工程
·
材料科学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2020
·
IF 5.006
Renjie Deng,Kuiyi You,Wenjin Ni,Fangfang Zhao,Pingle Liu,He’an Luo
In this work, we developed a low-temperature and efficient approach for the highly selective preparation of valuable p -nitrochlorobenzene from the liquid-phase catalytic nitration of chlorobenzene with NO 2 in O 2 -Ac 2 O-Hβ composite system. The results demonstrated that the introduction of molecular oxygen remarkably enhanced the chlorobenzene conversion and the cooperation catalysis of Hβ zeolite and Ac 2 O envidently improved the selectivity to para -nitro product. Under the optimized reaction conditions, 93.6 % of the selectivity to p -nitrochlorobenzene with 84.0 % of chlorobenzene conversion was obtained, and the ratio of p -nitrochlorobenzene to o -nitrochlorobenzene could reach up to 20.3. Furthermore, the selectivity distribution of nitration products was reasonably explained by the density functional theory (DFT) calculation. Finally, the possible nitration reaction pathway of chlorobenzene with NO 2 was suggested in O 2 -Ac 2 O-Hβ composite catalytic system. The present work affords a new and mild nitration approach for highly selective preparation of valuable para -nitro products, and has potential industrial application prospects.
研究领域:
化学工程
·
催化
·
有机化学
✓ 已验证
DOI
高影响因子
Energy Sources Part A-Recovery Utilization and Environmental Effects
·
2019
·
IF 0.894
X. Zhou,X. -Y. Wei,Y. -M. Ma,Z. -M. Zong
An active bifunctional Ni/Hβ was prepared by decomposing Ni(CO)4 to dispersive metallic Ni onto Hβ and applied in hydroconversion of oxydibenzene (ODB), which was used as a model reaction for the catalytic hydroconversion (CHC) of lignin or lignin oligomers to hydrocarbon fuels. The effects of reaction temperature, initial H2 pressure (IHP), and reaction time on the CHC of ODB was studied. Ni/Hβ was found to be effective for converting ODB into cyclohexane at 200°C under higher IHP. The mechanism for the CHC of ODB was discussed and the difference in mechanism under lower and higher IHP can be ascribed to the hydrogen-accepting abilities of unsaturated hydrocarbon products.
✓ 已验证
DOI
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Renjie Deng,Yiming She,Botao Cao,Lele Huang,Junjie Zhu,Huajie Liu,Haishuai Cui,Yao Tian,Fangfang Zhao
Zeolites are used in the field of toluene nitrification reactions, but their intrinsic mechanism is not well explained. In this work, three typical zeolites including HZSM-5, HY, and Hβ are selected as catalysts and used for the nitration of toluene and typical monosubstituted benzenes with NO2, and it explores the intrinsic influences on the nitrification of toluene on various zeolites through experimental and theoretical methods. The acidic properties and pore structures of three different zeolites were investigated through appropriate characterization techniques. Hβ zeolite exhibited the highest catalytic performance among the three zeolites, attributable to its unique pore structure and acidic properties. The theoretical analysis of various zeolites indicates that the Hβ zeolite can effectively reduce the activation energy barrier, thereby significantly enhancing the transfer nitration performance. The theoretical calculations also suggest that the para-nitration product is more readily formed within the pores of Hβ zeolite, resulting in high para-selectivity. This study provides a theoretical basis for the selective catalysis of aromatics on zeolites.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）