Catalysis Science & Technology
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2022
·Vol. 13
·期 2
·468-478
·
IF 6.177
Xinyu Lu,Xiaoli Gu
The chemical demand for alkyl phenols (mainly extracted from fossil-derived resources) has been increasingly growing, which has accelerated global energy shortages. Due to the inherent aromaticity of lignin, its effective conversion into alkyl phenols is central to its adoption as a sustainable precursor to produce biochemicals. In this study, catalytic transfer hydrogenation (CTH) of alkali lignin was carried out in a mixed medium (isopropanol/formic acid) at 240 °C for 8 h over a series of bimetallic Ni based catalysts. The acidity and reducibility of the as-prepared catalysts are enhanced via WO3 introduction (to form a WO3–Al2O3 mixed support) and a bimetallic synergistic effect, respectively, leading to improved catalytic activity and selectivity towards alkyl phenols. Different kinds of phenolic compounds (e.g., those with substitutions of methoxyl, alkyl, alkenyl, carbonyl, carboxyl, or hydroxyl groups) were generated over these bimetallic Ni based catalysts with various combinations of Ni + Fe/Zn/Co/Mo/Cu, which was due to their own catalytic promotion of certain reactions (e.g., hydrogenation, deoxygenation, and/or hydrogenolysis). Reaction mechanisms of lignin depolymerization were proposed according to the distribution of phenolic compounds. This work provides a comprehensive investigation on yielding alkyl phenols from lignin CTH over a series of inexpensive bimetallic Ni based catalysts (Ni/(Fe/Zn/Co/Mo/Cu)–WO3/Al2O3), and undertook a catalytic evaluation of the bimetallic synergistic effects on improving the chemical selectivity towards alky phenols, which is beneficial for lignin valorization.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Xin Ning,Heming Wang,Ganghua Zhou,Longyun Zhang,Yanju Yang,Jingya Sun,Xiaozhi Wang
Ni catalysts decorated with trace Rh supported on γ-Al2O3 were prepared by the co-impregnation method. To obtain the Ni–Rh nanoparticles with different nanostructures and chemical compositions, bimetallic catalysts with varied Ni/Rh molar ratios were prepared. For comparison, monometallic Ni/γ-Al2O3 and Rh/γ-Al2O3 catalysts were also prepared by the impregnation method. The selective gas phase catalytic hydrodechlorination of 1,2-dichloroethane to ethylene was used to evaluate catalytic performances of the catalysts. The catalysts were characterized by X-ray diffraction, N2 adsorption, X-ray photoelectron spectroscopy, H2 temperature-programmed reduction, transmission electron microscopy–energy-dispersive X-ray, and CO chemisorption. It was found that the introduction of Rh to Ni catalyst facilitated the generation of spillover hydrogen which could enhance the ability of the Ni catalyst for H2 activation. In bimetallic catalysts, there was an intimate interaction between Ni and Rh, and isolated Rh sites were formed due to the dilution effect of Ni. Accordingly, compared with the monometallic Ni catalyst for gas phase catalytic hydrodechlorination of 1,2-dichloroethane, the bimetallic Ni–Rh(800)/γ-Al2O3 catalyst exhibited markedly higher 1,2-dichloroethane conversion (37%) and comparable selectivity to ethylene (95%). The findings in this study indicate that Ni–Rh/γ-Al2O3 with trace Rh can be used as a promising catalyst for highly effective and selective catalytic hydrodechlorination of chlorinated hydrocarbons.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2023
·
IF 5.7
Wenxin Du,Kailei Lu,Bing He,Xiaolan Zhou,Xu Huang,Jianqi Qi,Tiecheng Lu
In this work, transparent aluminate oxynitride (AlON) ceramic wafers were successfully fabricated by the direct non-aqueous tape casting of Al 2 O 3 /AlN slurry and the one-step reaction sintering for the first time. The reaction sintered AlON ceramic wafer exhibits high transmittance of 73.2 % at the wavelength of 1600 nm. This fabricating route realizes smooth and flexible tape without cracks or pinholes in Al 2 O 3 /AlN system and efficiently shortens the preparation cycle of transparent AlON wafers, which is a feasible way to prepare high-quality transparent AlON ceramics with large lateral sizes and thin thicknesses by reaction sintering, might also promote the application of transparent AlON ceramic wafers.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Yong Liu,Xinghua Zhang,Lungang Chen,Jianguo Liu,Qi Zhang,Longlong Ma
This study explores the efficacy of a cost-effective Cu-ZnO-Al 2 O 3 catalyst for one-pot hydrodeoxygenation of guaiacol into hydrocarbons. Notably, complete conversion of guaiacol was achieved, yielding a 99.6% hydrocarbon over the robust Cu(6)Zn(3)Al(1) catalyst under the conditions of 4 MPa H 2 , 300 °C, and 8 h with a catalyst/guaiacol ratio of 0.5 g/1.0 g. In-depth catalyst characterizations unveiled the presence of oxygen vacancies within the ZnO surface layer, acting as pivotal active sites that facilitated the hydrodeoxygenation of guaiacol. Furthermore, Density Functional Theory (DFT) calculations were employed to evaluate several potential active sites, revealing that the oxygen vacancy of ZnO on the Cu surface played a crucial role. This vacancy enhanced the adsorption of intermediate cyclohexanol and markedly reduced the energy barrier for the rate-limiting step. This comprehensive investigation sheds light on the catalytic pathway and offers insights into designing efficient and sustainable biofuel production processes.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 53
·80399-80410
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IF 5.19
Shu Xinpeng,Bi Huaqi,Wang Jun,Yang Jiaxin,Wang Jue,Liu Guangqing,Su Bensheng
Catalytic ozonation with supported metal oxides is a promising strategy for addressing refractory pollutants in wastewater. In this study, γ-Al 2 O 3 supported MnO x -CeO x catalysts (MC 1 , MC 2 , and MC 3 ) obtained at different calcination temperatures (400 °C, 550 °C, and 700 °C) were applied as effective catalysts for ozonation and explored the feasibility of the treatment of oxytetracycline (OTC) wastewater. Comparatively, the MC 2 possessed the highest molar ratios of Mn 3+ /Mn 4+ (1.60) and Ce 3+ /Ce 4+ (0.96), the largest surface area (273.8 m 2 g −1 ) with a petal-shaped structure, and most abundant surface hydroxyls (3.78 mmol g −1 ). These physicochemical characteristics benefited the surface reaction and resulted in the acceleration of ozone decomposition, electron transfer, and •OH generation, thereby improving the catalyst’s adsorption ability and catalytic activity. The combination with MC 2 increased the OTC and COD removal of the ozonation process from 59.1% and 29.0% to 94.7% and 83.3% in 25 min, respectively. By employing electron paramagnetic resonance (EPR) and radical quenching experiments, it was verified that •OH species generation promoted the mineralization of OTC. The possible degradation pathways of OTC were investigated through mass spectrometry, and the route consisted of dehydration, deamination, and demethylation. Moreover, during a 12-day continuous experiment, MC 2 catalyst exhibited excellent reusability and catalytic stability, with COD removal efficiencies above 80%.
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PubMed
高影响因子
Virtual and Physical Prototyping
·
2022
·
IF 10.962
Xueqin Zhang,Keqiang Zhang,Bin Zhang,Ying Li,Rujie He
Ceramic lattice structures (CLSs) are promising candidates for structural applications used in conventional and extreme environments because of their extraordinary properties. Herein, CLSs with different structural configurations, including body-centred cubic (BCC), Octet, and modified body-centred cubic (MBCC), were designed and fabricated by digital light processing (DLP)-based additive manufacturing technology to explore their quasi-static and dynamic compressive behaviours. It was demonstrated that when relative density was a constant, quasi-static compressive strength (QS), quasi-static Young’s modulus (QY), and quasi-static energy absorption (QE) of CLSs with an MBCC structural configuration were the best, Octet ranked secondly, BCC was the poorest. The same thing happened on dynamic mechanical properties of CLSs. Increasing the relative density from 20% to 40% dramatically improved the QS, QY, and QE of CLSs. Furthermore, it was revealed by experiment and simulation that the quasi-static failure mode of CLSs changed from partially fracture along a specific plane to integrally fracture at most nodes as relative density increased. Furthermore, the dynamical mechanical properties of CLSs were significantly outstanding than quasi-static mechanical properties due to the strain-rate effect. This study provides a new basis for further study on tailoring the mechanical properties of CLSs.
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INTERNATIONAL JOURNAL OF ENERGY RESEARCH
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2022
·Vol. 46
·期 11
·15709-15721
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IF 4.672
Qiuwan Shen,Zicheng Shao,Zhongwen Cai,Min Yan,Guogang Yang,Shian Li
Summary Methanol steam reforming (MSR) is a promising method for hydrogen production from renewable energy. The effect of λ-Al 2 O 3 support derived from metal-organic frameworks (MOFs) aluminum fumarate (A520) on the performance and stability of LaNi 0.4 Al 0.6 O 3-δ for MSR is investigated. Results demonstrate that compared with LaNi 0.4 Al 0.6 O 3-δ , LaNi 0.4 Al 0.6 O 3-δ /λ-Al 2 O 3 can achieve complete conversion of methanol and excellent thermal stability due to the higher S BET and strong interaction between the metal components and λ-Al 2 O 3 . Characterization results indicate that the LaNi 0.4 Al 0.6 O 3-δ /λ-Al 2 O 3 catalyst, which was not successfully reduced due to its robust structure, still has active sites for the MSR reaction. This characteristic of the catalyst has the potential to be applied for onboard in-situ hydrogen production, because it can shorten the time of hydrogen reduction process. Furthermore, the effects of catalytic temperature, feed water-methanol ratio, and liquid hourly space velocity on performance of LaNi 0.4 Al 0.6 O 3-δ /λ-Al 2 O 3 are studied in detail and the optimal conditions are determined and applied for stability tests.
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JOURNAL OF MOLECULAR LIQUIDS
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2022
·
IF 6.633
Ling Ding,Ting Xiong,Zhibo Zhao,Jun Liao,Yong Zhang
In this study, Al 2 O 3 -TiO 2 nanocomposite was in-situ fabricated using cross-linking-freeze-drying technology for the separation of U(VI). Al 2 O 3 -TiO 2 nanocomposite exhibited an excellent removal property for U(VI) with a removal efficiency of 97.5% and a maximum adsorption capacity of 586.7 mg g −1 , which exceeded those of other TiO 2 -based adsorption materials. After five cycles, the removal percentage for U(VI) on Al 2 O 3 -TiO 2 nanocomposite still maintained more than 90.0%. The study of isotherm and kinetic demonstrated that the removal behavior of Al 2 O 3 -TiO 2 nanocomposite for U(VI) was monolayer chemisorption . Furthermore, the results of pH zpc , BET, SEM, FTIR and XPS analysis manifested that the interactions between Al 2 O 3 -TiO 2 nanocomposite and U(VI) included electrostatic interaction, surface complexation, oxygen vacancy chemistry and redox reactions . In one word, Al 2 O 3 -TiO 2 nanocomposite was a potential candidate as adsorbent in U(VI)-bearing wastewater remediation owing to its simple preparation method and the excellent removal properties.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Shuisen He,Tingting Huang,Yu Fan
Novel alumina-supported Ni-Mo hydrodesulfurization (HDS) catalysts were prepared via assembly of Mo and Al precursors induced by tetradecylamine (TDA). Compared with conventional impregnation, this assembly method improves Mo dispersion, weakens metal-support interactions, enhances Ni modification at MoS 2 edge sites, and produces more NiMoS phases on Al 2 O 3 . The optimal NiMoS microstructure was obtained by modulating the TDA/Mo ratio in the assembly. A microstructure-activity correlation indicated that the S vacancies at the NiMoS corner sites favored σ-adsorption and direct desulfurization of 4,6-dimethylbenzothiophene (4,6-DMDBT), and those at the NiMoS edge sites promoted C-S breaking in hydrogenated derivatives of 4,6-DMDBT. Among these catalysts, NiTMo-2.0/Al 2 O 3 , which had the most corner and edge S vacancies, exhibited the highest reaction rate constant of 5.89 × 10 −7 mol·g −1 ·s −1 and the highest desulfurization ratio of 99.5% in HDS of 4,6-DMDBT.
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ChemCatChem
·
2022
·Vol. 14
·期 7
·e202101728
·
IF 5.497
Shiqing Wang,Xiaocheng Lan,Boyang Liu,Babar Ali,Tiefeng Wang
Graphical Octylamine synthesis : Ni x Fe 1 /Al 2 O 3 was used as catalyst for 1-octanol amination and provided the highest yield among the reported nonprecious metal catalysts. The generation of Ni−FeO x interactions provided sufficient Fe 2+ /Fe 3+ −O 2− sites for the activation of 1-octanol. Meanwhile, the cooperation between Ni site and Lewis acid-base pairs significantly enhanced the amination of 1-octanol to 1-octylamine. The synthesis of 1-octylamine, a primary platform molecule, remained a great challenge in catalysis. In this work, Ni x Fe 1 /Al 2 O 3 was used for direct amination of 1-octanol to 1-octylamine. Catalyst evaluation indicated that the promotion effect of Fe/Ni ratio on the catalytic amination activity followed a volcano curve while the selectivity to 1-octylamine was positively correlated with the Fe loading. Compared with the Ni/Al 2 O 3 catalyst, the amination activity was increased by 2.8 times by optimizing the Fe/Ni ratio to 0.33, and the selectivity to 1-octylamine was increased from 84.0 % to 96.3 % when increasing the Fe/Ni ratio from 0 to 1. Based on catalyst characterizations, the good performance of Ni x Fe 1 /Al 2 O 3 was ascribed to the combined modification effect of the NiFe alloy and Ni−FeO x interface. The FeO x species enriched on the Ni particle surface provided sufficient Fe 2+ /Fe 3+ −O 2− sites for the activation of 1-octanol, and the cooperation between Ni sites and Lewis acid-base pairs enhanced the amination of 1-octanol to 1-octylamine. This work sheds new light on the design of Ni-based catalysts without using a noble metal for primary amine preparation.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Zhihao Zhou,Soomro Sarmad,Chao Huang,Guoshu Deng,Zhenkun Sun,Lunbo Duan
Ni-based catalysts supported on ordered mesoporous Al 2 O 3 with 2-D hexagonal and 3-D cubic pore structures are synthesized via evaporation-induced self-assembly for catalyzing dry CH 4 reforming to produce syngas . The Ni–Al 2 O 3 catalysts with 3-D pore structure exhibit higher activity in terms of CH 4 and CO 2 conversions than those with 2-D pore symmetry, due to the better mass transfer of the 3-D interconnected pore structure for the accessibility of Ni 0 active sites. And a higher Ni content slightly promotes catalytic activity , owing to more exposed active sites. However, a higher Ni content causes more severe carbon deposition during long-term reaction. During the long-term stability tests, the catalysts with 2.5 wt% Ni maintain the highest stability regardless of the pore structure, and the catalyst with 3-D pore structure is more advantageous to both activity and stability. Meanwhile, the catalyst with 2.5 wt% Ni and 3-D pore structure shows the lowest carbon deposition.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Weizhen Zhang,Wenqian He,Qian Yan,Lele Zhang,Nan Ni,Shaorui Song,Shuhua Tu,Jie Feng
Surfactant-free interfacial synthesis of hollow Al 2 O 3 via kinetic modulation • Chelation enables precursor transition from hydrophobic to amphiphilic states. • Simple room-temperature strategy bypasses harsh energy-intensive methods. • PDRC coatings deliver 97.6% solar reflectance and 0.976 mid-IR emissivity. • The scalable coatings realize a remarkable sub-ambient cooling of 9.66 °C. Hollow γ-Al 2 O 3 architectures are highly attractive for passive daytime radiative cooling (PDRC) owing to their low density and unique optical characteristics. However, their fabrication typically relies on sacrificial templates, hydrothermal treatments, or high-temperature processing, while the intrinsically ultrafast hydrolysis of aluminum alkoxides has long prevented their use in hollow-structure engineering. Here, we report a surfactant-free, chelation-enabled interfacial synthesis strategy that overcomes this limitation through kinetic regulation of aluminum sec-butoxide. The coordination process gradually transforms the precursor from hydrophobic to amphiphilic, enabling spontaneous self-emulsification and controlled interfacial assembly. As a result, hierarchical hollow γ-AlO(OH) microspheres are obtained at room temperature and subsequently converted into hollow γ-Al 2 O 3 microspheres by calcination. The resulting hollow γ-Al 2 O 3 microspheres exhibit tunable diameters (3.3–15.8 μm), uniform nanoscale shells (162 ± 60 nm), and an ultralow density of 0.083 g·cm −3 . The process is readily scalable using an industrial homogenizer. When incorporated into coatings, the hollow microspheres provide abundant dielectric interfaces that enhance solar reflection and thermal emission, delivering a solar reflectance of 97.6%, an atmospheric window emissivity of 0.976, and a sub-ambient cooling of 9.66 °C under a solar irradiance of 454.5 W·m −2 . This work provides a scalable and energy-efficient manufacturing strategy for hollow γ-Al 2 O 3 architectures, offering significant potential for large-area radiative cooling coatings and thermal management applications. Download: Download high-res image (108KB) Download: Download full-size image
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危险品化学品经营许可证（带存储）