CATALYSIS TODAY
·
2021
·
IF 6.766
Lijie Pei,Jianxin Cao,Fei Liu,Anjie Yang,Mengqin Yao,Tianxiang Zhao,Xiaodan Wang,Sibudjing Kawi
The catalytic properties of bifunctional ZSM-5@t-ZrO 2 catalyst for methanol thiolation were revealed by using methanol and H 2 S as probe molecules. Taking the ZSM-5/t-ZrO 2 physically-blended catalyst, pure ZSM-5 and t-ZrO 2 as control catalysts, we investigated the characteristics of adsorption and transformation of different reaction molecules on or over different catalysts by combination of in-situ diffuse reflectance Fourier transform infrared spectroscopy (Drifts) and a variety of techniques including XRD, XPS, XRF, FT-IR, N 2 adsorption-desorption, CO 2 /NH 3 -TPD, and DSC. The results showed that the synergistic effect of acid sites between ZSM-5 phase and t-ZrO 2 phase in the bifunctional catalyst enhanced the adsorption and dissociation of methanol molecules, while the base sites in t-ZrO 2 phase were mainly responsible for the adsorption and dissociation of H 2 S molecules. Due to the small specific surface area of pure t-ZrO 2 catalyst, precursor species for sulfur deposition and carbon deposition were easily formed. Presulfurization could improve the initial activity of methanol thiolation and shorten the induction period. The dissociation of H 2 S at the base sites was the rate-determining step of the bimolecular reaction, and the appropriate increase of base sites in the bifunctional components could construct the matching formation rate of sulfhydryl and methoxy groups. At the same time, the special composite structure and meso-microporous system of ZSM-5@t-ZrO 2 could effectively reduce the formation rate of carbon and sulfur deposits.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2021
·
IF 8.001
Hui Li,Yongbo Wang,Xiaoling Ma,Min Guo,Yan Li,Guoning Li,Ping Cui,Shoujun Zhou,Mingzhi Yu
Ca 2+ ion leaching and poor pore structure are obstacles of CaO for biodiesel production . To this end, a typical Zr–based metal organic framework, UiO–66(Zr) is adopted to support calcium acetate to prepare CaO/ZrO 2 catalyst. For comparison, catalyst precursor is activated in nitrogen (UCN) and air (UCA) atmosphere, respectively. Preparation factors including calcium acetate addition and activation temperature are evaluated. Moreover, effects of transesterification parameters on oil conversion are investigated and the optimized parameters are further used to examine catalyst reusability . Meanwhile, catalysts are characterized with TG, XRD, XPS , FTIR, Hammett indicator titration, N 2 adsorption and desorption. Results reveal UCN calcined at 650 °C (UCN650) and UCA calcined at 700 °C (UCA700) separately exhibits the best catalytic performance. The maximum conversion of 96.99% is achieved by UCN650 with catalyst amount of 6 wt% and molar ratio of methanol to oil of 9 at 65 °C for 60 min. Even after being used 3 cycles, conversion of 92.76% is still achieved by UCN650. By contrast, UCA700 shows lower conversion of 92.94% at the first cycle with catalyst amount of 8 wt% and molar ratio of methanol to oil of 9 at 65 °C for 60 min.
研究领域:
催化化学
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材料科学
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 17
·7957-7960
·
IF 3.3
Zhicheng Luo,Zhiguo Zhu,Lupeng Han,Rui Xiao,Dawang Chu
WOx/ZrO2 is effective in the hydrogenolysis of cellulose to C3 products but the active sites on the W–Zr interfaces are hardly controlled. Herein, we prepared WOx/ZrO2 catalysts with active WOx species by simply varying the reduction temperatures, which selectively achieved C3 alcohol formation. A series of characterizations showed that increased reduction temperatures (400–600 °C) led to the formation of more dispersed WOx, while higher reduction temperatures (>600 °C) contributed to producing aggregated WO3 and W2C. At 600 °C, the dispersity of WOx peaked with a W5+/∑Wn+ ratio of 19%, providing abundant Lewis acid sites and oxygen vacancies (Vo), which were the active sites for glucose isomerization to fructose and C–C cleavage of fructose. A selectivity of 48% for C3 alcohols was obtained over the optimized WOx/ZrO2(600 °C) + Ru/AC catalyst.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
BIOMASS & BIOENERGY
·
2025
·
IF 5.8
Yunfei Liu,Hewei Yu,Xiuxiu Chen,Zekai Sun,Lizeng Peng,Hongyu Si
This study focused on the optimized preparation of biodiesel over a ZrO 2 -modified CaO catalyst. CaO/ZrO 2 catalysts were synthesized by impregnation, co-precipitation, and sol-gel methods, and analyzed by various characterization methods, including N 2 adsorption-desorption, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), thermally programmed desorption of CO 2 (CO 2 -TPD), and scanning electron microscopy (SEM). The CaO/ZrO 2 catalyst synthesized by the impregnation method had a uniform microstructure, good crystallinity, a uniform spherical particle structure with large pores and slits, and a density of surface alkali sites of 1.898 mmol g - 1 . Using the impregnation method, the best synthesis conditions were determined as a calcination temperature of 700 °C and a Ca/Zr molar ratio of 3:2. Furthermore, the optimal reaction conditions were determined by single-factor experiments as a catalyst dosage of 8 wt%, a molar ratio of methanol to oil of 12, a reaction temperature of 64 °C, and a reaction time of 2 h. Under these reaction conditions, the yield of fatty acid methyl esters (FAME) reached 95.9 %, decreasing only marginally to 77.6 % after four reuses of the catalyst. It is hoped that this study may provide important research guidance for developing solid basic catalysts for preparing FAME by transesterification under mild conditions.
研究领域:
催化化学
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可再生能源
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yilin Zhao,Shenghua Liu,Xiaoqian Feng,Jiaxin Wang,Lijiao Chen,Yonghua Zhao,Huan Wang,Qijian Zhang
Dry reforming of methane (DRM) is a promising pathway to convert greenhouse gas into syngas. However, the commonly used Ni based catalysts suffer deactivation due to severe sintering and coking. In this paper, a series of porous Ni/MgO-ZrO 2 catalysts (5Ni/xM(1-x)Z, x = 0, 20, 40, 60, 80 wt%, respectively) with high specific surface area were synthesized by a facile combustion method followed by incipient impregnation. It is found that the appropriate amount of MgO (40 %) addition in ZrO 2 favors high porosity and high specific area. More MgO enhances the basicity of the catalyst as well as the metal-support interaction (MSI) by the formation of NiO-MgO solid solution, thus improving DRM activity and coking resistance. However, excessive MgO addition leads to over-strong MSI and lower porosity, resulting in lower DRM activity. The catalyst with 40 % MgO addition (5Ni/40M60Z) exhibits the best activity (conversions of CH 4 ∼ 76 %, CO 2 ∼ 83 %) and stability (>50 h) at high GHSV = 96000 ml/g cat ·h and 750 °C. in situ DRIFTS reveals the mechanism that MgO addition improves DRM activity and stability. Compared with ZrO 2 where CO 2 adsorbs as monodentate carbonate, CO 2 tends to adsorb on 40 %MgO-60 %ZrO 2 as bidentate carbonate and then easily transfer to more stable intermediate bidentate formate, thus improving DRM activity and coking resistance. This study provides new insights on the role of Mg addition in Ni/MgO-ZrO 2 DRM catalysts.
研究领域:
催化化学
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材料科学
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能源化学
✓ 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 CATALYSIS A-GENERAL
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2022
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IF 5.723
Meng Zhang,Junfeng Zhang,Qingde Zhang,Yizhuo Han
The surface reactive oxygen species over Y 2 O 3 -ZrO 2 supports were tuned by regulating the interaction between Y and Zr via modulating the zirconium precursors. It was revealed that the content of the surface adsorbed oxygen species (SAOS) over the catalyst with ZrO 2 precursor was the highest, followed by the catalysts with Zr(OH) 4 and ZrO(NO 3 ) 2 ·2H 2 O precursors. The difference of the Y-Zr interaction influenced the reactive oxygen species and the support structure and morphology. However, Ni dispersion was determined by the existence of the isolated Y 2 O 3 due to the enhanced metal-support interaction. High Ni dispersion and abundant surface adsorbed oxygen species were beneficial to promote CH 4 and CO 2 reactivity. Nevertheless, CH 4 dissociation facilitated by the SAOS was more remarkable than CO 2 activation at low temperature. Thus, the improvement of the SAOS on carbon-resistant ability of the catalyst was only achieved at high temperature through balancing the carbon formation and elimination.
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
ChemistrySelect
·
2023
·Vol. 8
·期 28
·e202301088
·
IF 2.1
Hui Zhou,Xiaoliang Sun,Wenming Guo,Tingting Bao,Yi Zhang,Chenxu Guo,Hanning Xiao,Hang Qin,Pengzhao Gao
Graphical [+] These authors contributed equally to this articleDurable CuO/ZnO/CeO 2 /ZrO 2 catalyst on SiC support for methanol steam reforming was prepared by the combination of inverse microemulsion method and precipitation method. The methanol conversion of the catalyst was still reached 98.8 % after 150 h, considerably higher than that of solution combustion method (70 %), without carbon deposition and pronounced sintering after the reaction. Durable CuO/ZnO/CeO 2 /ZrO 2 catalyst on SiC support for methanol steam reforming (MSR) was prepared by the combination of inverse microemulsion method and precipitation method which is termed as inverse microemulsion/precipitation method. The presence of Ce−O−Zr solid solution facilitated the production of oxygen vacancies and Ce 3+ species in the prepared CuO/ZnO/CeO 2 /ZrO 2 catalyst. Owing to the unique tiny reaction pool and the addition of precipitant for inverse microemulsion/precipitation method, the particle size of the prepared catalyst was principally between 2 and 6 nm, with an average size of 3.66 nm. Besides, the small particle size and the highly dispersed of Cu species boosted the reduction performance of the catalyst, enabling the reduction temperature to be only 201 °C. The methanol conversion of the reduced catalyst was still reached 98.8 % after 150 h, considerably higher than that of solution combustion method (70 %), without carbon deposition and pronounced sintering after MSR reaction.
研究领域:
催化化学
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能源材料科学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS SURVEYS FROM ASIA
·
2023
·Vol. 27
·期 4
·406-414
·
IF 3
Han Yujun,Shi Yinteng,Wang Dandan,Zhou Hantao,Chen Jixiang
Ni/ZrO 2 (Ni/Zr) and Ni/WO 3 -ZrO 2 (Ni/ x WZr, x denotes WO 3 /ZrO 2 mass ratios) were prepared by the impregnation-direct reduction method and tested for the aqueous phase hydrogenation of phenol to cyclohexanone in an autoclave reactor. It has been found that the Ni-W alloy forms in Ni/ x WZr, and a charge transfer occurs from Ni to W. The presence of W species promotes the Ni dispersion and increases the amounts of acid sites and spilt-over hydrogen species. This leads to higher hydrogenation and direct deoxygenation activity of Ni/ x WZr than that of Ni/Zr. In addition, the W 6+ and W 4+ species, acted as Lewis acidic sites, may stabilize cyclohexanone and the hydrogenation of cyclohexanone to cyclohexanol is inhibited. Under suitable condition, the phenol conversion and the cyclohexanone selectivity reach 93.1 and 90.6% on Ni/0.8WZr, respectively.
研究领域:
催化
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化学反应工程
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有机化学
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材料科学
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Wubin Yan,Binbin Jin,Jiong Cheng,Xiaoyu Shi,Heng Zhong,Fangming Jin
Direct hydrogenation of CO2 (or HCO3–) into chemicals using organic waste biomass as a hydrogen donor is a promising carbon-negative strategy to alleviate the global warming caused by excessive CO2 emission. However, the reported conversion efficiencies are quite limited. In this work, a facile Ru/ZrO2 catalyst was developed to catalyze the hydrogenation of HCO3– into formate by using biodiesel-waste glycerol as the reductant. It was found that ruthenium can significantly promote the dehydrogenation of glycerol to provide in situ hydrogen for HCO3– hydrogenation according to the in situ Fourier transform infrared spectrometer analysis. Moreover, hydrogen spillover between ruthenium and ZrO2 support was also formed. Consequently, efficient hydrogen transfer could be constructed in the presence of Ru/ZrO2, achieving desirable in situ hydrogenation of HCO3– into formate eventually. The highest yield of formate up to 25.1% was obtained over Ru/ZrO2, while the formate yield was only 4.2% in the case without catalysts.
研究领域:
催化化学
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环境科学
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Yonglong Huang,Zhengkang Duan,Chuan Li,Tian Qiu
The catalytic dehydrogenation of diethanolamine to prepare iminodiacetic acid has attracted considerable research interest. However, the lack of understanding of the structure-activity relationship of the reaction can present a challenge to the control of the catalytic behavior. Concurrently, improving the catalytic performance and reducing the cost have also become urgent issues that require resolution. This work examined the catalytic mechanism of several Cu-Ni X /ZrO 2 catalysts, differing in Cu/Ni ratios, prepared by H 2 reduction, in the context of DEA dehydrogenation to elucidate the structure-activity connection and probable reaction mechanism. Subsequently, a strategy has been put out to generate metal (Ni and Co)-doped copper-zirconium catalysts using the co-precipitation-hydrazine hydrate reduction process. The synergistic effect between metals was combined with the improvement of the surface reaction of the catalyst by hydrazine hydrate through a more efficient preparation method, thereby enhancing the catalyst's overall performance. The representative catalyst Cu-Ni/ZrO 2 required a hydrazine hydrate reduction temperature and time of 40 °C and 30 min, and after 65 min of reaction, it exhibited a high conversion rate (96.3 %) and yield (93.7 %), and after five cycles, both the conversion rate and yield exceeded 85 %. Various characterization techniques have confirmed that Ni doping induced an alloying effect and a size effect. Additionally, the hydrazine hydrate reduction method was discovered to augment the specific surface area, surface hydroxyl groups, hydrophilicity, and optimize the pore size distribution of the catalyst while also regularizing its morphology, thereby significantly enhancing the activity and stability of the metal-doped copper-zirconium catalyst. This paper discussed the correlation between catalyst structure and reaction performance, as well as the catalytic conversion mechanism, which is anticipated to provide a novel reference for the preparation, performance control, and potential applications of dehydrogenation catalysts.
研究领域:
催化化学
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材料科学
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环境工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Guang-Rong Ding,Yao-Feng Wang,Guo-Yi Duan,You-Qian Fan,Bao-Hua Xu
In this study, a tungstated zirconia (WOx/ZrO2) catalyst was developed for the continuous synthesis of adiponitrile (ADN) by gas-phase nitrilation of dimethyl adipate (DMA) with NH3. The highest TOFADN could be reached on WOx/ZrO2 bearing ∼1D WOx species (highly dispersed and discontinuous status) at the surface, which, however, delivered the poorest selectivity toward nitrilation (SADN+MCP). In comparison, both efficient and selective transformation of DMA to ADN was achieved by fabricating WOx/ZrO2 with continuously distributed oligomeric WOx species (∼2D) at the surface, either by varying the dosage of the W-reagent in the preparation of WOx(m)/ZrO2 or by doping a proper amount of the Mn element into WOx(5.0)/ZrO2, bearing WO3 NPs. Furthermore, the in situ diffuse reflectance infrared Fourier transform spectroscopy investigations of both independent and competitive adsorptions of ester functionality and NH3 over W–O–Zr, W–O–W, and Zr–O–Zr boundaries at the surface clarified the synergistic effect of these species in the activation of DMA/NH3 and thereby nitrilation.
研究领域:
催化
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化学工程
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表面科学
✓ 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）