CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2021
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IF 3.171
Xiao Zhao,Xuan Shi,Zhongshun Chen,Long Xu,Chengyi Dai,Yazhou Zhang,Xinwen Guo,Dongyuan Yang,Xiaoxun Ma
A series of ZnO-ZrO 2 solid solutions with different Zn contents were synthesized by the urea co-precipitation method, which were coupled with H-ZSM-5 zeolite to form bifunctional catalysts. As a new benzene alkylation reagent, syngas was used instead of methanol to realize the efficient conversion of syngas and benzene into toluene and xylene. A suitable ratio of ZnO-ZrO 2 led to the significant improvement in the catalytic performance, and a suitable amount of acid helped to increase the selectivity of toluene/xylene and reduce the selectivity of the by-products ethylbenzene and C 9 + aromatics. The highest benzene conversion of 89.2% and toluene/xylene selectivity of 88.7% were achieved over 10% ZnO-ZrO 2 &H-ZSM-5 (Si/Al = 23) at a pressure of 3 MPa and a temperature of 450 °C. In addition, the effect of the zeolite framework structure on product distribution was examined. Similar to the molecular dynamics of aromatic hydrocarbons , H-ZSM-5 zeolites comprise 10-membered-ring pores, which are beneficial to the activation of benzene; hence, the conversion of benzene is higher. H-ZSM-35 and H-MOR zeolites exhibited small eight-membered-ring channels, which were not conducive to the passage of benzene; hence, the by-product ethylbenzene exhibits a higher selectivity. The distance between the active centers of the bifunctional catalysts was the main factor affecting the catalytic performance, and the powder mixing method was more conducive to the conversion of syngas and benzene.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2020
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IF 2.627
Jiyuan Li,Mifen Cui,Zhuxiu Zhang,Xian Chen,Qing Liu,Zhaoyang Fei,Jihai Tang,Xu Qiao
Isooctane attracts great interest in recent years because of its promising potential as friendly-environmental gasoline, which is obtained by dimerization of isobutene with a hydrogenation step. Herein, a solid acid catalyst sulfated zirconia modified by ZnO was prepared. The oligomerization of isobutene had been investigated over ZrO 2 -SO 4 and ZnO( X )/ZrO 2 -SO 4 catalyst in order to find efficient catalysts for the production of isobutene oligomers . The presence of ZnO obviously enhanced the dimerization of isobutene and ZnO( X )/ZrO 2 -SO 4 exhibited the highest di-isobutene yield of 60%. Kinetic studies showed the higher trimerization-to-dimerization activation energy ratios of ZnO( X )/ZrO 2 -SO 4 than those of ZrO 2 -SO 4 from 353 to 393 K. In addition, reaction rate of dimerization was higher than trimerization over ZnO( X )/ZrO 2 -SO 4 . The high L/B ratio manifested the capability to enhance the selectivity of C 8 in isobutene dimerization. Furthermore, ZnO( X )/ZrO 2 -SO 4 exhibited stable conversion for the dimerization of isobutene.
研究领域:
化学工程
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催化
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石油化学
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2022
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IF 12.92
Zhaopeng Liu,Youming Ni,Zhongpan Hu,Yi Fu,Xudong Fang,Qike Jiang,Zhiyang Chen,Wenliang Zhu,Zhongmin Liu
The utilization of metal oxide-zeolite catalysts in the syngas-to-olefin reaction is a promising strategy for producing C 2 –C 4 olefins from non-petroleum resources. However, the effect of the crystal phase of metal oxides on the catalytic activity of these oxides is still ambiguous. Herein, typical metal oxides (ZnO/ZrO 2 ) with different crystal phases (monoclinic ( m -ZrO 2 ) and tetragonal ( t -ZrO 2 )) were employed for syngas conversion. The (ZnO/ m -ZrO 2 +SAPO-34) composite catalyst exhibited 80.5% selectivity for C 2 –C 4 olefins at a CO conversion of 27.9%, where the results are superior to those (CO conversion of 16.4% and C 2 –C 4 olefin selectivity of 76.1%) obtained over (ZnO/ t -ZrO 2 +SAPO-34). The distinct differences are ascribed to the larger number of hydroxyl groups, Lewis acid sites, and oxygen defects in ZnO/ m -ZrO 2 compared to ZnO/ t -ZrO 2 . These features result in the formation of more formate and methoxy intermediate species on the ZnO/ m -ZrO 2 oxides during syngas conversion, followed by the formation of more light olefins over SAPO-34. The present findings provide useful information for the design of highly efficient ZrO 2 -based catalysts for syngas conversion.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
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IF 4.9
Yueming Wang,Yong Men,Lini Liao,Lijie Fu,Zaiwei Lu,Shuyi Xu,Jinguo Wang,Zhenrong Yan,Xuelong Miao
The ZnO/ZrO 2 binary catalyst system has been an emerging and promising catalyst for efficient production of H 2 through methanol steam reforming (MSR). Herein, ZrO 2 supports with different crystalline phases were prepared by the oxygen vacancy engineering strategy of Li doping, and then ZnO/ZrO 2 catalysts were prepared by the isovolumic impregnation method. The different quantities of doped Li have been found to have a significant impact on dominant crystal phase of ZrO 2 supports, which dictates the interaction between ZnO and ZrO 2 and the number of oxygen vacancies. In comparison with ZnO/ZrO 2 -20Li and ZnO/ZrO 2 -40Li catalysts with predominate tetragonal and monoclinic crystal phase, ZnO/ZrO 2 -3Li with a mixed crystalline phase exhibits higher catalytic activity for methanol conversion ( X CH 3 OH ) and CO selectivity (S CO ). Complete methanol conversion of the best performing ZnO/ZrO 2 -3Li catalyst was observed at a very low CO selectivity of 3.1 % at 375 ℃. The XRD, UV, and XPS characterization results indicate that the strong interaction between ZrO 2 and ZnO leads to the appearance of large amount of oxygen vacancies at the ZnO/ZrO 2 interface, which greatly improves the performance of the catalyst. ZnO/ZrO 2 catalyst showed remarkable stability without obvious deactivation after 32 hours of continuous testing. This work highlights the effectiveness of oxygen vacancy engineering of the ZnO/ZrO 2 catalysts for applications in methanol steam reforming and other heterogeneous catalytic systems.
研究领域:
化学工程
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催化科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Sustainability
·
2025
·
IF 7.9
Pengyuan Guan,Yongjie Zhao,Yihui Wu,Weixian Li,Xiao Zhang,Xiang Gao,Xiaoxia Ou,Wai Siong Chai,Yinfeng He,Hao Nan Li
CuO–ZnO–ZrO 2 catalyst attracted significant attention for CO 2 hydrogenation to methanol. Gyroid-based triply period minimal surface lattice structures feature highly ordered porous networks, which could be used to enhance catalytic performance and efficiency. This paper presents a formulating and one-step calcination strategy that united the removal of polymer resin and calcination of catalyst precursor at one temperature. This enabled 3D printing gyroid-structured CuO–ZnO–ZrO 2 catalyst for CO 2 hydrogenation while minimizing the impact of overheating on the catalyst performance. A photocurable formulation loaded with CuO–ZnO–ZrO 2 precursor was developed. Using the optimized formulation, gyroid structures with varying pore sizes were successfully printed and calcined. The optimal lattice wall thickness that balances porosity and structural stability was identified. The results indicate that the resin used for 3D printing was successfully removed at a lower temperature and the catalytic activity of the 3D-printed structured catalyst was retained through the one-step calcination process while the gyroid lattice geometry can enhance catalytic efficiency than cylindrical structure.
研究领域:
材料科学
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催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Fuyuan Han,Xue Ye,Xinhua Gao,Jinghao Yu,Lisheng Guo,Jie Li
ZnO/ZrO 2 solid solution was introduced as the catalyst for synthesizing dimethyl carbonate (DMC) from propylene carbonate (PC) and methanol. Homogeneous catalysts with strong alkaline nature are the current main catalysts for this reaction. Therefore, to supplant the former with a more applicable multiphase one, it is necessary to construct stable and efficient alkaline active centers on the surface of solid catalysts. The ZnO/ZrO 2 solid solution created defective structures of coordinative unsaturation in the form of oxygen vacancies (O V ) by substituting Zn atoms for Zr atoms in ZrO 2 crystals. Characterizations showed that electrons were transferred to the surrounding Zn atoms upon the formation of these O V , leading to a local enrichment of electrons and the formation of basic active centers. The number of oxygen defects and the alkalinity were effectively regulated by changing the ratio of the two metal atoms in the solid solution. Experiments demonstrated that the catalyst had the best DMC selectivity (92.2%) and the highest DMC yield (57.2%) at a 1:1 ratio of Zn to Zr, at 160 °C and 4 h. This superior performance not only establishes the feasibility of solid solution catalysts in synthesizing DMC but also provides a new perspective on the essential understanding of the active centers of such catalysts.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
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IF 5.518
Dandan Tian,Yong Men,Shuang Liu,Jinguo Wang,Zhuping Li,Keye Qin,Tianle Shi,Wei An
Advances in design concept of oxide-zeolite (OX-ZEO) bifunctional tandem catalysts have demonstrated its potential for highly enhanced selectivity and yield in CO 2 conversion by assigning CO 2 activation and C-C coupling to specific oxide and zeolite , respectively. However, the crystalline structural effects of oxides have not been thoroughly investigated. Here, ZnO/ZrO 2 with different ZrO 2 crystalline phases modulated by Li doping has been used as an oxide catalyst to combine with SAPO-34 as a bifunctional composite catalyst for CO 2 hydrogenation to light olefins . With the transformation of the support ZrO 2 crystalline phase from tetragonal phase to mixed crystalline phase in the catalyst, the CO 2 conversion and yield of target product light olefins were significantly improved. The best-performing ZnO/5Li-ZrO 2 catalyst exhibited a CO 2 conversion of 28.56%, light olefins selectivity of 82.00% with a yield of 8.77% along with good stability under the reaction conditions of 380 °C, 3 MPa, and 6000 mL/g/h. The characterization results by XRD , Raman, HRTEM , XPS and CO 2 -TPD confirmed that the highly enhanced catalytic performance was attributed to the strong interaction between the mixed crystal phase 5Li-ZrO 2 and ZnO, which generated a large number of oxygen vacancies for CO 2 activation. The results indicate that controlling the crystal phase of the oxide support is of prime importance in designing more active and selective oxide-zeolite bifunctional catalysts for high-efficiency CO 2 to light olefins conversion.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Hao Huang,Wei Na,Xiangying Wang,Zhenhui Huang,Zhao Ai,Wengui Gao,Hua Wang
A detailed understanding of the role of Y in Cu/ZnO/ZrO 2 catalysts for methanol synthesis was studied by XRD, HRTEM, TPR, TPD, N 2 O titration and XPS techniques in this work. The addition of Y enhances the interaction between Cu and ZnO. With the increase of Y content, the crystal size of Cu and ZnO decreased and Cu 0 surface area increased, CO 2 /H 2 -TPD exhibited the larger CO 2 and H 2 desorption peak at relative high temperature, XPS confirmed the reduction degree of ZnO to Zn 0 on the catalyst surface also increased, and forming more Cu-ZnO x active sites. However, excess Y content leads to a much stronger interaction between Cu and ZnO, which is not beneficial for migration and stabilization of the formed ZnO x species during the reaction atmosphere, and thus generating less Cu-ZnO x sites for methanol synthesis. This work enlightens the migratable and metastabe of the formed ZnO x species on Cu surface by regulation of promoter and offers a perspective for exploring Cu-ZnO interactions in modified Cu/ZnO/ZrO 2 catalysts.
研究领域:
催化化学
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能源化学
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材料化学
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工业催化
·
碳资源利用
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Xinbao Zhang,Guanghui Zhang,Xiangkun Zhou,Zhiqun Wang,Yi Liu,Jie Zhu,Chunshan Song,Xinwen Guo
Interest in identifying the structure of the catalysts in the reaction atmosphere has grown, but it remains challenging, especially when the changes only occur on the surface. Herein, we track the reaction-induced structural changes of ZnO/ZrO2 and their consequent effects on the activity and selectivity of CO2 hydrogenation. Utilizing a combination of in situ infrared and controlled experiments, we meticulously investigate the dynamic changes of the catalyst’s surface structure with time on stream. The reaction-driven growth of ZnOx clusters is correlated with the enhanced CO2 hydrogenation activity of ZnO/ZrO2. Furthermore, in situ infrared results show that the aggregation of ZnOx clusters promotes hydrogen activation, thereby facilitating the synthesis of methanol. The modification of the interfacial sites confirms the significance of the ZnO–ZrO2 interface as the main site for CO formation, while the surface of ZnOx clusters predominantly contributes to methanol synthesis at low zinc loading. These findings advance our comprehension of the structure–activity relationship of zinc-based catalysts for CO2 hydrogenation.
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Yi Xiang,Zidan Mei,Lulu Zhou,Yue Li,Yongdong Chen
The hydrogenation of CO2 to light olefins is a promising method for CO2 resource utilization. Tandem catalysts composed of metal oxides and zeolites have been widely studied for the hydrogenation of CO2 to light olefins, but there are bottleneck problems in terms of CO2 conversion and light olefins yield. ZnO-ZrO2 catalyst is extensively employed in CO2 hydrogenation because of its excellent stability at high temperatures, but there is still a "seesaw" problem between the CO2 conversion and light olefins selectivity. In addition, the synergetic effect between Zn and Zr sites on the reaction process remains unclear. In this work, a series of ZnO-ZrO2 catalytic materials with various Zn: Zr ratios were synthesized by co-precipitation, and the interaction between Zn and Zr could be regulated by altering the Zn: Zr ratio. XRD and TEM results confirmed the successful synthesis of ZnO-ZrO2 composite oxide and the existence of a certain interaction between Zn and Zr. CO2-TPD, H2-TPR and XPS results indicated that the interaction between Zn and Zr could improve the hydrogenation capacity of the catalyst and also induce the generation of abundant oxygen vacancies to effectively promote the adsorption and activation of CO2. Catalytic performance results showed that ZnO-ZrO2(1:4)/SAPO-34 exhibits the best CO2 to light olefins activity with a CO2 conversion rate of 26.4% and a C2=-C4=selectivity of 72.6%. This work provides a feasible strategy for rational designing and optimizing of CO2 hydrogenation catalyst.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Xing Yan,Dongren Cai,Meihong Lin,Zhijie Wu,Yegang Xia,Yanmei Cai,Sajid Ali,Kok Bing Tan,Andriambinintsoa Ranaivoson Tojonirina,Hao Sun,Guowu Zhan
The selective hydrogenation of CO 2 to methanol demands precise control of both catalyst architecture and reaction pathways. Here, we design an atomic layer deposition (ALD)-engineered Pd/ZnO/ZrO 2 ternary catalyst with atomic-scale ZnO interlayers to decouple and reconfigure active sites at dual interfaces (Pd-ZnO and ZnO-ZrO 2 ). This interfacial engineering drives a 7-fold enhancement in methanol space–time yield (0.584 vs. 0.084 g MeOH g cat −1 h −1 ) and switches the dominant reaction pathway from CO-mediated to formate-driven selectivity (methanol selectivity remarkably surges from 6 % to 64 %). Multimodal characterization and theoretical calculations reveal that ZnO interlayers orchestrate bifunctional cooperation: activating CO 2 /CO adsorption while suppressing CO/CH 4 formation through electronic effects. Long-term stability study uncovers a dynamic restructuring mechanism, where Pd-ZnO interfaces gradually evolve into PdZn β alloy phases under the reaction conditions. This work establishes ALD-mediated interface design as a generalizable strategy to manipulate reaction networks and methanol selectivity in catalytic CO 2 hydrogenation systems.
研究领域:
催化化学
·
材料科学
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化学工程
·
可持续能源
·
表面科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）