JOURNAL OF THE BRAZILIAN CHEMICAL SOCIETY
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2023
·Vol. 34
·期 7
·987-991
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IF 1.4
Su Xiao-Ping,Zhao Le,Wang Xiang-Tong,Wang Zhao,Wang Zhi-Chao,Shen Tao,Zhang Ping
Different Al2O3 carriers were synthesized by co-precipitation and sol-gel method. From them, 4%NiO-20%MoO3/Al2O3 catalysts were prepared by incipient wetness impregnation. The catalysts were characterized by X-ray diffraction analysis (XRD), N2 adsorption-desorption, NH3 temperature programmed desorption (TPD) and H2-temperature programmed reduction (TPR) and subsequently used for selective hydrogenation of naphthalene to high-value tetralin. The results showed that Ni-Mo/so-ge Al2O3 (900) exhibited better catalytic performance than Ni Mo/commercial Al2O3, achieving 99.56% naphthalene conversion and 99.43% tetralin selectivity.
研究领域:
催化化学
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材料科学
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Pengxin Zeng,Chuanwen Zhao,Xinmei Wang,Xinzheng Wei,Jian Sun,Ruiling Wang,Yafei Guo
The desirable CO 2 adsorption capacity and mechanical property are both important for the large-scale industrial applications of K 2 CO 3 -based CO 2 adsorbents. In this work, graphite-casted, Al 2 O 3 -supported, K 2 CO 3 -based pellets were prepared for CO 2 adsorption. The prepared K 2 CO 3 -based pellets containing 30 wt% of K 2 CO 3 calcinated at 900 °C exhibit CO 2 adsorption capacity of 1.4 mmol/g, which is over 2.5 times that of the pellets calcinated at 300 °C. It is mainly attributed to the residual graphite coating on the surface of the K 2 CO 3 -based pellets calcinated at 300 °C, which inhibits the diffusion of H 2 O due to the hydrophobicity of graphite and further causes the poor carbonation performance. Moreover, the addition of 40 wt% of microcrystalline cellulose can further enhance the adsorption capacity of the graphite-casted K 2 CO 3 -based pellets to ∼1.95 mmol/g due to the improved pore structure. However, excessive addition of microcrystalline cellulose (50–60 wt%) will lead to poor CO 2 adsorption performance (1.07–1.16 mmol/g) because of the active sites within the pellets being covered by molten K 2 CO 3 . Additionally, the structurally improved K 2 CO 3 -based pellets also exhibit desirable mechanical property with a compression strength of 69.45 MPa. Comprehensively considering the simple and easily scaled-up preparation route of graphite-casting method, the structurally improved, graphite-casted, Al 2 O 3 -supported, K 2 CO 3 -based pellets possess potential practical application prospect.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
CATALYSIS TODAY
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2020
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IF 5.825
Hongqin Ma,Yanan Guan,Wenyao Chen,Zhijun Sui,Gang Qian,De Chen,Xinggui Zhou,Xuezhi Duan
In this work, the support effects on vapor-phase aldol condensation of methyl acetate (MeOAc) with formaldehyde (HCHO) over cesium catalysts are understood by the employment of Al 2 O 3 with different morphologies and crystal phases. The structural and electronic properties of these supported Cs catalysts are characterized by multiple techniques, such as XRD, HAADF-STEM, EDS-mapping, XPS, NH 3 -TPD and CO 2 -TPD. The Cs species are found to be highly dispersed on the Al 2 O 3 surfaces, and their compositions vary with the identity of Al 2 O 3 . A combined catalyst characterization and testing results indicates a balance between acidic and basic sites, i.e., an acid-base synergy, for the production of MA: the excess acidic sites lead to the lower MA selectivity due to the promoted further condensation, while the excess basic sites with the lower MeOAc conversion due to the insufficient activated HCHO species. These insights could be valuable for the design and optimization of catalysts for this reaction.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2024
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IF 4.7
Wenqin Zhao,Zonghao Zhang,Bo Wang,Yang Lv,Lei Huang,Pingle Liu
Catalytic hydrodeoxygenation is a plausible route to upgrade the quality of biomass energy sources. Herein, a series of Ru-Co alloy catalysts (Ru-Co/TiO 2 -Al 2 O 3 ) were prepared and applied in guaiacol hydrodeoxygenation to cyclohexanol. It was found that Ru-Co nanoparticles with average size of about 8.67 nm were uniformly dispersed on TiO 2 -Al 2 O 3 support. It was verified that Co doping led to the formation of electron-rich Ru and hence promoted the desorption of active hydrogen, while the constructed TiO 2 -Al 2 O 3 support possessed abundant oxygen vacancies and acidic sites, which facilitated adsorption and hydrogenolysis of −OCH 3 functional group. 5Ru-5Co/TiO 2 -Al 2 O 3 catalyst gives the best catalytic performance of >99% guaiacol conversion and 94% selectivity to cyclohexanol. In addition, the strong interactions between Ru-Co nanoparticles and TiO 2 -Al 2 O 3 could significantly inhibit aggregation and leaching of Ru-Co nanoparticles during the reaction. The research results will provide reference to design highly efficient and stable bimetallic catalysts in converting lignin-derived bio-oils.
研究领域:
催化化学
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生物质能
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高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2024
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IF 2.8
Boyun Gao,Huijiang Huang,Mooeez Ur Rehman,Bin Ren,Yuruo Liu,Weipeng Fan,Pengfei Li,Lizhi Zhang,Yan Xu,Yujun Zhao
BACKGROUND The synthesis of fatty amines via fatty alcohol amination offers a promising avenue for environmentally friendly production, particularly when compared with the methods employing hydrocyanic acid which often involve significant emissions. RESULT This study explores the synthesis of n-hexylamine through one-step amination of n-hexanol utilizing a series of Ru-doped Ni catalysts supported over γ-Al 2 O 3 , achieving 61% n-hexanol yield, 35% dihylamine yield and 3.5% trihylamine yield at the n-hexanol conversion of 99%. CONCLUSION The characterization results of the catalysts revealed a significant interaction between ruthenium and nickel in the bimetallic catalysts, leading to the enhanced reducibility of Ni species and improved metal dispersion. Moreover, ruthenium species were found to play an important role in the dissociation of NH 3 into NH x (x = 1, 2), thereby significantly improving the dehydrogenation process of n-hexanol at Ni sites. The synergistic effect between the two kinds of metal sites emerges as crucial factor for the boosted alcohols amination process. © 2024 Society of Chemical Industry (SCI).
研究领域:
催化化学
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环境科学
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DOI
高影响因子
AICHE JOURNAL
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2022
·Vol. 69
·期 3
·e17895
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IF 4.167
Xuyu Wang,Fu Yang,Jianjian Yi,Jiejing Kong,Juanjuan Gong,Aihua Yuan,Zebao Rui,Hongbing Ji
Rational engineering of noble metal/transition metal bimetallic catalysts is considered as an effective way to constructing synergistic effect between adsorbed oxygen and hydroxyl for enhanced catalytic formaldehyde oxidation. Herein, we developed a Pt–Ni bimetallic catalysts loading on γ-Al 2 O 3 support for room-temperature formaldehyde oxidation. Catalytic experiment results showed that the conversion rate was >97% with a >100 h stability. Several noble metals (Pd, Au, and Ag) were compared to identify the activity effect in formaldehyde oxidation. The activity and stability test in different atmospheres and in situ infrared test suggested that the PtNi/γ-Al 2 O 3 has the best activity and stability. At a meantime, the results also demonstrated that Pt sites motivate more surface adsorbed oxygen through activating ambient oxygen molecules, while the neighboring Ni atoms contribute to adsorbed hydroxyl, thereby offering sustainable activity. The high efficiency and stability of PtNi/γ-Al 2 O 3 catalysts for formaldehyde oxidation could be a promising candidate for air purification.
研究领域:
催化化学
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环境科学
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材料科学
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2025
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IF 4.8
Yuan Ma,Baining Lin,Chaojun Guo,Yang Yang,Chuli Shi,Shuobin Fu,Yonghua Zhou
Non-metallic materials have attracted continuous interest in the direct dehydrogenation (DDH) of ethylbenzene due to their coke resistance and environmental friendliness. However, the catalytic activity was limited by the exposed density of active sites in non-metal catalysts. Herein, we report an atmosphere-pretreatment strategy using H 2 or O 2 at 350 ℃ to improve the exposure of active sites in Al 2 O 3 -supported phosphorus oxynitride (PNO) catalysts, thereby enhancing their catalytic performance in DDH of ethylbenzene. XPS, FTIR, and in situ DRIFTS analyses demonstrated that H 2 or O 2 pretreatment partially cleaved P–N bonds in the P 3 N 5 framework, inducing structural reorganization and exposing the inner N 2 P = O groups, thereby increasing the active site density. Among them, the H 2 -pretreated PNO/Al 2 O 3 catalyst (PNO/Al 2 O 3 -H) exhibited the highest N 2 P = O content (a 74.2 % increase compared with PNO/Al 2 O 3 ), which resulted in the highest catalytic activity ( X EB =58.5 %) under high-concentration ethylbenzene feed (12.2 vol%). This work demonstrates, for the first time, the application of atmosphere pretreatment to phosphorus-nitrogen catalysts and proposes a novel strategy for regulating the active site in dehydrogenation catalysis.
研究领域:
催化
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材料科学
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化学反应工程
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表面化学
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Qiu Xu,Chungang Wang,Zongling Shang,Chao Zhang,Xinchao Wang,Qiang Liu,Lingling Dang,Yanchun Liu,Fengyu Zhao
The activation and ring opening reaction of lactone bond is of great significance in biomass utilization. Cu-based catalysts are widely used in the biomass hydrogenation processes, in which the effect of oxide promoters on Cu catalysts is one of the most attractive research topics. Herein, the transformation of lactones to diols over Cu/Al 2 O 3 and CuLa x /Al 2 O 3 catalysts was studied and the promoting role of LaO x has been discussed. The CuLa 0.25 /Al 2 O 3 catalyst showed outstanding catalytic performance with high 1,4-butanediol yield of > 90 %, and it also showed high efficiency for the hydrogenation of series of five- and six-membered lactones (γ-butyrolactone, γ-valerolactone, δ -hexalactone, etc) to diols. Based on the comprehensive analysis of the XRD, TEM, TPR, XPS, low temperature CO-DRIFT results, the crucial contribution of LaO x species in promoting the selectivity and stability of catalysts were investigated in detail. The presence of LaO x species not only results in the formation of Cu + -LaO x interfacial active sites, which facilitate the adsorption and activation of lactones, but also promotes the stability of catalyst.
研究领域:
化学工程
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催化科学
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
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IF 4.2
Hua Yang,Zhang Zhang,Yongsheng He,Peng Wang,Zhuangzhuang Ren,Lizhi Wu,Yu Tang,Li Tan
Ni-based catalysts have been widely investigated in the partial oxidation of methane (POM). However, sintering and carbon deposition are severe problems for Ni-based catalysts in the POM reaction. Here, Ni/Al2O3 catalysts with Al2O3 supports prepared by different synthesis methods are used to investigate the effect of strong metal–support interaction (SMSI) and their relationships to the catalytic performance. As a result, the different strengths of SMSI between Ni species and various Al2O3 supports contribute to generating different contents of the reduced metallic Ni0 sites in the catalysts, which affects the catalytic activity in the POM reaction obviously. The surface unsaturated pentahedral coordination Al3+ centers supply SMSI in the Ni/Al2O3-H catalyst to prevent the catalyst from sintering and coking in the POM reaction, which results in better catalytic activity and catalyst stability. A new view is provided to solve the design of stable metal oxide catalysts by utilizing their SMSI effect.
研究领域:
催化
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化学工程
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材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Lin Ai,Yanping Chen,Fang Lu,Jiaxu Liu,Xiao-Feng Wu,Shengjun Huang
The fundamental challenge in the gas-phase selective hydrogenation of α,β-unsaturated aldehydes to α,β-unsaturated alcohols lies in the construction of microscopic environment for the preferential hydrogenation of C = O bond along with the preservation of C = C bond under the reductive atmosphere. Herein, we proposed a structure-matching strategy for the catalyst design, in which In component in metallic form and oxide form are interplayed with metallic Ni and Al 2 O 3 support, respectively. The fabrication of In-Ni intermetallic compound stokes up the desirable electropositive-electronegative environment (In δ+ -Ni δ- ) for the adsorption of polar carbonyl group. The In species in the In-oxo form are engaged in the network of Al 2 O 3 support in the formation of In-O-Al-O entities, which stabilizes the heterolytically dissociated H species to match the preferential saturation of polar C = O bond. Therefore, the resulting In-Ni-Al 2 O 3 catalyst achieves a selectivity of 77.2 % to methallyl alcohol with a conversion of 53.8 % in the gas-phase hydrogenation process, which present a striking contrast to the outcomes upon the counterpart Ni-Al 2 O 3 (non-selectivity to methallyl alcohol). Such structure-matching strategy enriches the fundamental understandings and basis for the rational design of catalysts for the selective hydrogenation of unsaturated aldehydes.
研究领域:
催化
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化学工程
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材料科学
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高影响因子
JOURNAL OF CATALYSIS
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2025
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IF 6.5
Ziyang Xu,Liang Chen,Chunbo Wang
Reaching high activity over Ni-based catalysts for CO 2 methanation at lower temperature remains a critical challenge. Herein, a surface hydroxylation strategy was developed to enhance the catalytic performance of Ni catalysts under mild conditions. By treating γ-Al 2 O 3 with H 2 O 2 solutions of varying concentrations, the surface hydroxyl (–OH) group density was effectively tuned. Catalytic evaluations revealed that hydroxylation of the support significantly enhances CO 2 methanation performance. Among the series, Ni/A-OH-6 exhibited the highest activity, achieving a turnover frequency (TOF) of 2.129 h −1 at 240 °C, approximately eight times higher than that of the unmodified Ni/A catalyst (0.266 h −1 ), thereby demonstrating a remarkable enhancement in intrinsic activity. Comprehensive characterizations demonstrated that surface –OH significantly enhanced CO 2 adsorption via the formation of HCO 3 * species. In situ DRIFTS studies further confirmed that hydroxyl-induced HCO 3 * species convert more readily to HCOO*, facilitating the hydrogenation pathway and thus contributing to the improved low-temperature activity. This work highlights surface hydroxyl engineering as a simple yet effective approach to boost catalytic efficiency, delivering guidance for the rational development of high-efficiency CO 2 utilization catalysts.
研究领域:
催化
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材料科学
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环境化学
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表面工程
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高影响因子
ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Yusheng Qiu,Shuzhuang Sun
The activity and selectivity of catalytic reactions are profoundly influenced by metal–support interactions. The strong metal–support interaction (SMSI) plays a critical role in selectively driving the conversion of CO2 toward CO instead of CH4 in Ni-based catalytic systems. Moreover, the dispersion of active species governs the population of accessible reaction sites, thereby enhancing catalytic activity. In this work, highly efficient SMSI was successfully constructed via steam aging post-treatment over CeO2–Al2O3 nanocrystalline loaded Ni catalysts (NiCeAl). Remarkably, the NiCeAl–H2O catalyst achieves ∼50% CO2 conversion with 90% CO selectivity at 600 °C, representing a dramatic improvement over the untreated NiCeAl catalyst (23% CO2 conversion with ∼92% CO selectivity). Furthermore, the steam-treated catalyst demonstrates superior stability in prolonged CO2 hydrogenation tests, maintaining its performance with only a ∼4% conversion decrease over 10 h of continuous operation. In situ diffuse reflectance infrared Fourier transform spectroscopy analysis revealed that CO2 chemisorbs on the catalyst surface to form bidentate carbonates, which undergo sequential hydrogenation to form formate intermediates. These formate species subsequently decompose catalytically to produce CO, with the enhanced MSI in NiCeAl–H2O facilitating optimal CO desorption kinetics, thereby promoting superior reverse water–gas shift activity.
研究领域:
催化
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材料科学
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化学工程
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环境化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）