FUEL
·
2021
·
IF 6.609
Pengcheng Wang,Jun Liu,Guo Liu,Peiwen Xu,Xinzhen Feng,Weijie Ji,Yulan Gao,Chak-Tong Au
In this work, we studied how the oxidic CoMoO x /Al 2 O 3 and sulphurated CoMoS x /Al 2 O 3 interfacial structures determine catalytic efficiency in selective hydrodesulfurization (HDS) of dibenzothiophene (DBT). To achieve this goal, we first synthesized the γ-Al 2 O 3 materials of unique morphologies through the ionic liquid-assisted hydrothermal process under different conditions. The resulting γ-Al 2 O 3 hexagonal plates (HP) and stacked hexagonal plates (SHP) are single crystallites with the dominant (1 1 0) and (1 1 1)/(1 0 0) facet structures, respectively; whereas the Al 2 O 3 rods show polycrystalline feature. Through impregnation of Mo/Co salts of different loadings, the various CoMoO x precursors were generated on the different Al 2 O 3 facets owing to the distinct interaction: mostly the two-dimensional (2D) poly-/mono-meric MoO x species together with the three-dimensional (3D) MoO 3 on the Al 2 O 3 (1 1 0) facet vs. the quasi 2D polymeric MoO x species on the Al 2 O 3 polycrystalline facet. Such structural difference further affected the sulfidation of the MoCoO x as well as the quantity of active MoCoS x entities on different γ-Al 2 O 3 supports: 10Mo3CoS x /Al 2 O 3 -HP had the highest level of MoCoO x sulfidation thus a much higher fraction of MoS 2 plus Co 9 S 8 /CoMoS species whereas less quantity of partially sulphurated CoMoO x S 2 /CoO x together with SO x 2- species. All the distinct interfacial domains of the sulphurated catalysts reasonably account for significantly different efficiency in HDS of DBT. Surface MoS 2 /CoMoS/Co 9 S 8 species of the highest content over the Al 2 O 3 (1 1 0) facet correspond to the highest DBT areal conversion rate and TOF value, owing to the enhanced MoS 2 -Co 9 S 8 and MoS 2 -CoMoS conjunction and synergism.
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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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2025
·
IF 9.2
Chuanya Li,Qianfeng Zhou,Changhu Leng,Yongchao Wang,Chenyang Ma,Junlei Zhang,Zhijun Li
Polyolefin plastics, though highly resistant to degradation due to their thermodynamic stability and chemical inertness, can be catalytically depolymerized into liquid fuels, offering a promising route to mitigate white pollution and fossil fuel dependency. Here, a sustainable catalytic route for closed-loop polyolefin upcycling is achieved using a bifunctional Sn1W9/γ-Al2O3 catalyst that integrates redox and acidic functionalities within a self-regenerative hydrogen relay cycle. The optimized interface between Sn and W species promotes simultaneous C-H dehydrogenation and C-C metathesis via dynamic Sn-H ↔ W-OH coupling, enabling quantitative conversion of polypropylene at 250 o C within 1 hour and selective production of C5-C22 liquid hydrocarbons (95.0%). Structural, spectroscopic, and kinetic analyses identify hydroxylated W 5+ -OH sites as the principal active centers, stabilized by Sn-mediated hydrogen spillover. The catalyst achieves exceptional stability and reusability across multiple degradation cycles and diverse commercial plastics. Life cycle and techno-economic assessments reveal 16-fold enhanced thermal efficiency, > 85% solvent recyclability, and a carbon footprint of 7.3 kg CO2 e•kg⁻¹surpassing benchmark catalysts in both sustainability and energy utilization. This self-sustaining redox-hydroxyl loop establishes a scalable, low-carbon paradigm for circular plastic valorization. Under mild conditions, the system delivers excellent degradation performance and stability, demonstrating scalability for kilogram-scale recovery.
研究领域:
催化化学
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可持续化学
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高分子科学
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化学工程
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环境科学
·
能源与燃料
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Xinglin Wen,Ye Zhu,Yong Pan,Yonglu Yang,Xiaoyue Wan,Ahmed Mebarki,Juncheng Jiang
The direct hydrogenation of 2,4-dinitrotoluene (2,4-DNT) to 1-methyl-2,4-cyclohexanediamine (2,4-MCHD) represents a significant yet non-industrialized green process for synthesizing methylcyclohexane diisocyanate (HTDI), known for its excellent properties. This process faces considerable challenges due to the hydrogenation of the benzene ring, the reduction of two nitro groups, and the need to avoid deamination reactions. In this study, an alkali-free heterogeneous catalytic system was developed for the direct hydrogenation of 2,4-DNT to 2,4-MCHD using Ru nanoclusters supported on γ-Al 2 O 3 . Side reactions such as deamination were effectively inhibited, resulting in a 2,4-MCHD selectivity exceeding 95% and a 2,4-DNT conversion greater than 99%. Kinetic studies indicated that the hydrogenation of 2,4-DNT in this system operates as a tandem reaction, with the hydrogenation of the benzene ring serving as the rate-determining step. Structure-activity relationship studies demonstrated that the valence state of Ru nanoclusters, the acidity and basicity of the catalyst, and the synergistic effect between Ru and the support significantly influence catalytic performance. This work represents the first example of the direct hydrogenation of dinitroaromatic compounds to aliphatic diamines in a system that does not require the addition of alkali elements, thereby establishing a solid foundation for the further exploration of such reaction systems.
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产品关联
DOI
高影响因子
Surfaces and Interfaces
·
2026
·
IF 6
Weijie Lin,Hong Deng,Yishun Wang,Jiaxin Lv,Xucun Ye
Typically, the high-temperature calcination of secondary aluminum dross (SAD) following pyrometallurgical or hydrometallurgical treatments yields α -Al 2 O 3 as the primary product. However, the inherent lack of catalytic activity in this material restricts its application as a high-value-added catalyst. Herein, we propose a targeted "waste-to-catalyst" upcycling strategy that achieves the phase transformation of SAD into γ -Al 2 O 3 nanorods for peroxymonosulfate (PMS) activation and ciprofloxacin (CIP) degradation. Aluminum was first extracted via a Na 2 CO 3 -assisted roasting-leaching process, achieving an aluminum recovery efficiency of 85.1% and a final purity exceeding 98.5%, providing a high-quality precursor. The recovered material was subsequently engineered into a specific nanorod morphology through a geometry-controlled hydrothermal treatment followed by low-temperature calcination. The optimized catalyst (B-400) exhibited superior catalytic performance, removing over 98.5% of CIP within 1.5 h. Notably, the reaction rate constant increased to 2.53 h –1 , which is significantly higher than the 1.34 h –1 observed for unmodified alumina. Mechanistic investigations and theoretical calculations revealed that the enhanced activity originates from the combined effect of the unique nanorod structure and low crystallinity, which collectively preserve abundant coordinatively unsaturated Al 3+ sites and oxygen vacancies. These active sites facilitate PMS activation to generate singlet oxygen ( 1 O 2 ) as the dominant reactive species responsible for pollutant degradation. This work establishes a practical pathway not only for mitigating the environmental risk posed by SAD but also for its directional conversion into high-performance, functional catalytic materials, thereby contributing to a circular economy.
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Shu-Xiang Xiang,Jin-Peng Wang,Su Gao,Zhan-Kuo Guo,Hui-Lin Jiang,Bao-Xia Dong,Yun-Lei Teng
The CH 4 yield over dual functional materials (DFMs) remains low and requires further improvement. In this work, we first examined the influence of Mn on the performance of the Ni-CaO/γ-Al 2 O 3 DFM for CO 2 capture and in situ methanation. Our results showed that the MnNi-DFM-3 (MnNi-CaO/γ-Al 2 O 3 DFM) exhibited the best performance at 350 °C, with a CH 4 yield of 0.56 mmol/g which is 4 times higher than that of the Ni-DFM-1 (Ni-CaO/γ-Al 2 O 3 DFM) (0.14 mmol/g). Nanoscale characterization revealed that highly scattered Mn 3 O 4 acted as a barrier preventing the agglomeration of Ni-based catalysts. Furthermore, our density functional theory (DFT) analysis demonstrated that the introduction of Mn enhanced the activation of CO 2 , promoted the dissociation of H 2 and intermediates, and reduced the activation energy needed to produce carboxylic acid intermediates on the Ni catalyst. The prepared MnNi-DFM is promising to be a cheap efficient material for CO 2 capture and in situ methanation. This work opens up a new pathway for enhancing the performance of DFMs using inexpensive transition metals.
研究领域:
化学工程
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS ES&T Water
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2021
·
IF 0
Qiang Cao,Fengyan Lou,Na Liu,Jisong Zhang,Lidong Wu
Today, the Al2O3-supported catalyst in the heterogeneous catalytic ozonation system attracts attention due to its stable structure and relatively high surface activity. Herein, Mn and Cu oxides loaded on γ-Al2O3 pellets were prepared using an impregnation method to improve the removal efficiency in a micropacked bed reactor (μPBR). The effects of the initial pH, the ratio of O3 to chemical oxygen demand (COD), and HO• scavenger on the catalytic performance were investigated. Experimental results showed that the MnO2/γ-Al2O3 and CuO/γ-Al2O3 catalysts exhibited excellent catalytic performance. The COD removal efficiencies were 86.3% for CuO/Al2O3, 76.9% for MnO2/Al2O3, 71.6% for Al2O3, and 35.8% for ozone alone within 71 s. Compared with those of batch reactors, the apparent degradation rate constant of COD with prepared catalysts in a μPBR increased by 2–3 orders of magnitude. In addition, the CuO/γ-Al2O3 catalyst maintained a relatively stable activity in the continuous flow test for a long time (100 h). Finally, some typical antibiotics were treated by catalytic ozonation in a μPBR. The removal efficiencies of these antibiotics and COD reached approximately 100.0% and 62.9–87.8% within 71 s, respectively. Thus, the continuous catalytic ozonation system with the CuO/γ-Al2O3 catalyst based on μPBRs could be a promising pathway for the treatment of industrial wastewater with antibiotics.
研究领域:
环境工程
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化工工程
·
水处理
✓ 已验证
DOI
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2018
·Vol. 43
·期 16
·7973-7981
·
IF 4.229
Shaowei Yang,Hui Xie,Hongwei Zhu,Lijuan Zhang,Yunshan Zhou,Huixian Zhang,Zipeng Zhao
In this work, metal-organic framework compound CPL-1 of a formula {[Cu 2 (pzdc) 2 (pyz)]⋅2H 2 O} n (pzdc = pyrazine-2,3-dicarboxylate, pyz = pyrazine) possessing kinetic quantum sieving effect on H 2 /D 2 separation was selected to prepare two new chromatography stationary phase materials CPL-1@γ-Al 2 O 3 and MnCl 2 @CPL-1@γ-Al 2 O 3 by loading CPL-1 on γ-Al 2 O 3 particles with size 80–100 mesh through repeating in situ crystallization process , and afterwards by loading MnCl 2 on CPL-1@γ-Al 2 O 3 via impregnation approach. The two optimized materials were thoroughly characterized by IR, XRD , SEM, EDS and TG/DTA method. The experimental results showed that, under liquid nitrogen temperature by using just 1-m chromatographic column and cheap He gas as carrier gas, the MnCl 2 @CPL-1@γ-Al 2 O 3 can solve the problem of long separation time and trailing phenomenon existing in the CPL-1@γ-Al 2 O 3 column, can realize highly effective hydrogen isotope H 2 /D 2 separation with good separation resolution (R = 1.62) and approximate Gauss distribution of chromatographic peak, can be used for both qualitative and quantitative analysis of hydrogen isotope H 2 /D 2 with short separation time of 6.5 min.
研究领域:
分离科学
·
材料化学
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物理化学
·
核化学
·
色谱学
✓ 已验证
DOI
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2024
·
IF 6.9
Shupo Liu,Zixiang He,Xiaobin Liao,Xinyue Liu,Menglan Gao,Huayu Zhang,Jing Zou,Zhenming Zhou,Baoling Yuan,Zhimin Yang
Antibiotics and ammonia are generally co-existed in aquaculture tailwater; moreover, ammonia would also be produced from during ozonation, and should be simultaneously removed before discharge or reuse. In this study, catalyst Cu-Co/γ-Al 2 O 3 was screened from a variety of metal oxides and applied in catalytic ozonation of three kinds of antibiotics and NH + 4 -N. Factors that affected their removal, including catalyst dosages, O 3 concentration, initial pH as well as co-existing ions, were investigated. Moreover, the mechanisms were probed by exploring free radicals’ role as well as intermediates identification; and the characteristics of catalysts before and after use were evaluated using SEM, EDS, XRD, XPS, and BET. Results demonstrated that Cu-Co/γ-Al 2 O 3 could significantly stimulate the degradation of the selected antibiotics and NH + 4 -N during ozonation. The degradation efficiencies of ciprofloxacin (CIP), tetracycline (TC), sulfamethoxazole (SMX) and NH + 4 -N can reach up to 95.0 %, 100.0 %, 96.2 %, and 75.7 %, respectively. Plenty of oxygen vacancy (O vs ) and sufficient alkaline sites on the surface of catalyst facilitated the adsorption of pollutants. Furthermore, the transformation of metal ions Cu + /Cu 2+ and Co 2+ /Co 3+ enhanced the electron transfer capacity and favored the formation of reactive oxygen species (ROS) during catalytic ozonation reaction, and their roles in catalytic ozonation has also been verified. The radical quenching experiments demonstrated that ·OH was the main contributor for enhancing pollutants removal. The results of Gaussian calculation coincided with those intermediates detected by UPLC-Q-TOF-MS, the pollutants’ removal mechanisms by catalytic ozonation were proposed basing on them. The overall toxicities were compared for ozone only/catalytic ozonation by zebrafish embryo experiment. The results of this study would provide new a feasible way for treating antibiotics and NH + 4 -N simultaneously in aquaculture wastewater.
研究领域:
环境科学
·
水处理技术
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Zhichao Sun,Songyin Yu,Yuhang Gong,Changhai Liang,Chuang Li
Different from the dehydration of ethanol, the catalytic dehydration of long-chain fatty alcohols to linear α-olefins with the low selectivity arises from a complex reaction network, particularly the secondary isomerization to internal olefins. This study aimed to elucidate the fundamental mechanisms governing selectivity in the catalytic dehydration of n-octanol to 1-octene over conventional γ-Al 2 O 3 catalysts. The combination of kinetic analysis, in situ infrared spectroscopy, and density functional theory (DFT) calculations, we demonstrated that the reaction primarily proceeded via a dioctyl ether intermediate, which rapidly decomposed into olefin and alcohol. In contrast, the isomerization of 1-octene followed a water-assisted re-adsorption and hydration pathway: 1-octene re-adsorbed onto surface acid sites, hydrated to form 2-octanol, and subsequently underwent secondary dehydration, preferentially yielding internal olefins in accordance with Saytzeff's rule. Based on these mechanistic insights, an integrated reaction-separation process was designed using Aspen Plus simulation. Employing a dual-column distillation scheme with heat integration, the process achieved a 1-octene product purity exceeding 98% with ~5.9% lower overall energy consumption. This work provided systematic insights and a feasible strategy, that bridges molecular-scale mechanisms with process engineering, facilitating the highly selective production of α-olefins from biomass-derived long-chain alcohols.
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2015
·
IF 2.711
Shan Huang,Zhichun Si,Duan Weng
Highly stable Ag:AgBr/γ-Al 2 O 3 photo-catalyst was obtained by dispersing AgBr sol on hollow γ-Al 2 O 3 microsphere. Metallic Ag nanoparticles were in situ generated on AgBr crystals by a photo-reduction method. The activity of catalyst was characterized by MO and phenol decomposition. The light irradiation response, the life times of the photo-induced charges, and the charge separation and transition were determined by the UV–vis diffuse reflection spectra, open circuit voltage decay spectra and transient photocurrent responses. The as-prepared Ag:AgBr/γ-Al 2 O 3 catalyst can response to visible light irradiation. Charge separation was clarified to correlate with electrons transferring from Ag to AgBr surface and the consequent reaction with ads-O 2 to generate O 2 − species. It was found that the O 2 − rather than OH played a dominant role in the photocatalytic oxidation of MO and phenol in water. However, the electrons trended to transfer from AgBr to Ag intrinsically without light irradiation. Therefore, the electron transfer between Ag and AgBr reaching the dynamic equilibrium was the key factor for obtaining a high stable Ag/AgBr catalyst which can be obtained by optimizing the Ag:AgBr ratio. Loading amount of Ag:AgBr on γ-Al 2 O 3 was optimized to 30 wt.% and the metallic Ag content was stabilized at 9 wt.% of Ag:AgBr catalyst.
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zifan Wu,Lu Chen,Yacong Deng,Fengyu Tian,Guangzheng Sun,Yuting Qiu,Yichuan Li,Yuan Pan,Bin Liu,Bin Dong,Yongming Chai
Lignin-derived phenols, with their high energy density and rich aromatic structure, are potentially high-quality feedstocks for the production of aviation fuel-range cycloalkanes. Herein, we fabricated a Ni Mo alloy catalyst anchored on graphitic carbon nitride (g-C 3 N 4 ) coated γ-Al 2 O 3 (10Ni-5Mo/CN@γ-Al 2 O 3 ), which could completely hydrodeoxygenate various lignin-derived phenols into cycloalkanes under mild conditions. 10Ni-5Mo/CN@γ-Al 2 O 3 significantly catalyzed the hydrodeoxygenation of lignin oil at 240 °C under 3 MPa H 2 for 8 h, achieving a deoxygenation degree of 96.5 % and a high propylcyclohexane selectivity (41.8 %), and the resulting products met the requirements for aviation fuels. The study results showed that electron transfer within Ni Mo alloys and the strong interaction between g-C 3 N 4 and surface anchored Ni Mo alloys in 10Ni-5Mo/CN@γ-Al 2 O 3 facilitated the dissociation of H 2 into active hydrogen to hydrogenate the aromatic rings. Meanwhile, the formation of oxygen vacancies enhanced the adsorption and activation ability of the catalyst for oxygen-containing substrates, which was beneficial for the demethoxylation and dehydroxylation reactions. This work provides a new strategy for constructing supported non-noble metal catalysts for the hydrodeoxygenation of lignin oil into aviation fuels.
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产品关联
DOI
高影响因子
Catalysts
·
2020
·Vol. 10
·期 9
·1068
·
IF 3.52
Jing Zhao,Xiaorui Yang,Wei Wang,Jinhua Liang,Yasin Orooji,Chaowen Dai,Xiaomin Fu,Yunsong Yang,Wenlong Xu,Jianliang Zhu
In this work, a core-shell-like sphere ruthenium catalyst, named as 5%Ru/γ-Al2O3@ASMA, has been successfully synthesized through impregnating the ruthenium nanoparticles (NPs) on the surface of the amino poly (styrene-co-maleic) polymer (ASMA) encapsulating γ-Al2O3pellet support. The interaction between the Ru cations and the electro-donating polymer shell rich in hydroxyl and amino groups through the coordination bond would guarantee that the Ru NPs can be highly dispersed and firmly embedded on the surface of the support. In addition, the solid sphere γ-Al2O3pellet could serve as the core to support the resulted catalysts applied in the flow process in a trickle bed reactor to promote the productivity. The resulted catalyst 5%Ru/γ-Al2O3@ASMA can be applied efficiently in the glucose hydrogenation and presents a steadfast sorbitol yield of almost 90% both in batch reactor and the trickle bed reactor, indicating the potential feasibility of the core-shell-like catalyst in the efficient production of sorbitol.Keywords:core-shell;organic-inorganic hybrid;ruthenium catalyst;hydrogenation;d-glucose;targeting effect
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
危险品化学品经营许可证（带存储）