APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Chunxue Wang,Zhao Li,Junjun Qiu,Xin Sun,Yixing Ma,Chi Wang,Kunlin Li,Ping Ning,Kai Li,Fei Wang
In various industrial processes, particularly iron ore sintering operations, the concurrent use of fossil fuels and selective catalytic reduction by ammonia (NH 3 -SCR) denitrification technology inevitably results in the coexistence of carbon monoxide (CO) and escaped NH 3 in the exhaust gases. While simultaneous catalytic oxidation of CO and NH 3 represents an ideal strategy, it encounters significant challenges due to competition for active centers. Moreover, NH 3 -selective catalytic oxidation (NH 3 -SCO) is potentially inhibited by high CO concentrations. In this investigation, we synthesized a series of Pt/Al-X catalysts (X indicating calcination temperature) that demonstrated inverse activity patterns in independent NH 3 -SCO and CO oxidation reactions. Comprehensive analysis incorporating oxygen activation capacity, reactant adsorption characteristics, reaction kinetics, and in situ diffuse reflection infrared Fourier transform spectrum (DRIFTS) measurements indicated that O 2 activation capacity functioned as the rate-determining factor for NH 3 -SCO, whereas CO adsorption capacity and OH group density predominantly governed CO oxidation. Building on these findings, we engineered a composite catalyst by integrating Pt/Al-600 and Pt/Al-900 catalysts. This novel composite effectively reduced active center competition through strategic combination of functional sites, thereby achieving superior performance in simultaneous CO and NH 3 removal, while maintaining excellent water resistance and operational stability.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Fangxu Shi,Fuxin Liang,Yulin Wei,Junyan Wu,Sai Huang,Honglei Wang,Zhi Wang,Guopu Shi
The hydrogenation-catalyzed synthesis of mirabellone, a drug for the treatment of overactive bladder (OAB), faces the challenge of catalytic efficiency and selectivity regulation of its core intermediate. In this study, we propose an innovative strategy for constructing a Pd/B-Al 2 O 3 composite catalytic system on a foam ceramic substrate using the impregnation method, and systematically investigate the modulation mechanism of different boron doping ratios on the catalyst's performance. Experimental and density functional theory studies demonstrate that the incorporation of boron synergistically enhances surface adsorption of reaction intermediates, facilitates the efficient reduction of PdO, and precisely modulates the distribution of acidic sites, thereby establishing a catalytic environment more favorable for the selective reduction of nitro groups. This catalyst, characterized by its unique three-dimensional pore structure and the interface synergistic effect resulting from boron modification, enables a uniform distribution of catalytically active centers and enhances the efficiency of reaction mass transfer. Through the optimization of process parameters, the yield of the target product was significantly improved, providing an innovative technological path for the preparation of the key intermediate of mirabilon.
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ChemSusChem
·
2024
·
IF 7.5
Tao Xu,Meihui Jiang,Siyu Mo,Xianhui Wang,Tianlin Ren,Zhichen Liu,Zhicheng Wang,Yicheng Qiu,Lingying Gu,Xu Wang,Xuhui Mao
Graphical We designed a carbon-coated aluminum oxide carrier and reinforced it with Mn−Fe bimetal assemblages to prepare a high-performance catalyst Mn−Fe/C-Al 2 O 3 . Mn−Fe/C-Al 2 O 3 catalyst exhibited satisfactory catalytic ozonation activity and stability in the degradation of p -nitrophenol. Experiments and theoretical calculations revealed the internal degradation mechanism of the Mn−Fe/C-Al 2 O 3 catalyst, underscoring the role of the carbon-coated and bimetallic active unit in O 3 activation. Catalysts with high catalytic activity and low production cost are important for industrial application of heterogeneous catalytic ozonation (HCO). In this study, we designed a carbon-coated aluminum oxide carrier (C-Al 2 O 3 ) and reinforced it with Mn−Fe bimetal assemblages to prepare a high-performance catalyst Mn−Fe/C-Al 2 O 3 . The results showed that the carbon embedding significantly improved the abundance of surface oxygen functional groups, conductivity, and adsorption capacity of γ-Al 2 O 3 , while preserving its exceptional mechanical strength as a carrier. The prepared Mn−Fe/C-Al 2 O 3 catalyst exhibited satisfactory catalytic ozonation activity and stability in the degradation of p -nitrophenol (PNP). Electron paramagnetic resonance (EPR) and quenching experiments reveal that radical ( ⋅ OH and ⋅ O 2 ⋅ ) and nonradical oxidation ( 1 O 2 ) dominated the PNP degradation process. Theoretical calculations corroborated that the anchored atomic Fe and Mn sites regulated the local electronic structure of the catalyst. This modulation effectively promoted the activation of O 3 molecules, resulting in the generation of atomic oxygen species (AOS) and reactive oxygen species (ROS). The economic analysis on Mn−Fe/C-Al 2 O 3 revealed that it was a cost-competitive catalyst for HCO. This study not only deepens the understanding on the reaction mechanism of HCO with transition metal/carbon composite catalysts, also provides a high-performance and cost-competitive ozone catalyst for prospective application.
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DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Guiming Xie,Xingyang Bai,Yanrui Niu,Zhangjun Bai,Qingyuan Yang,Jian Liu,Zhou-jun Wang
ZIF-8 was employed as partial Zn source to prepare high-performance Cu/ZnO/Al 2 O 3 catalysts for methanol synthesis via carbon dioxide (CO 2 ) hydrogenation. Among the CuZnAl-x catalysts (x = 1, 0.75, 0.5, 0.25 and 0, denoting molar ratio of ZIF-8/(ZIF-8 + Zn(NO 3 ) 2 ·6H 2 O), the CuZnAl-0.5 catalyst possessed the highest space time yield of methanol ( STY MeOH ), which recorded 416.4 g MeOH kg cat −1 h −1 at 250 °C and 3.0 MPa. Using ZIF-8 as partial Zn source was found to increase the specific surface area, induce oxygen vacancies, intensify metal-oxide interactions and enrich medium basic sites, which may rationalize the excellent methanol synthesis activity of the CuZnAl-0.5 catalyst. Besides, the CuZnAl-0.5 catalyst showed good stability for 30 h of reaction. This work offers a unique route to fabricate catalysts with the aid of MOFs precursors and highlights the significance of oxygen vacancies in methanol synthesis catalysts.
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高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Jiangtao Li,Yunjia Xue,Xueying Zhang,Fan Zhang,Wenhao Hu,Jiachen Liu
The SiC-ZrO 2 coating was prepared on the surface of aluminosilicate ceramic fiber fabric (ASFF) to enhance the radiation heat dissipation. However, the Si-sol in the SiC-ZrO 2 coating caused the fiber to adhere together at high temperatures. The brittle fracture of the ASFF led to a deterioration in its temperature resistance. In this paper, an Al 2 O 3 interface was prepared on the surface of ASFF by spraying alumina precursor. The Al 2 O 3 interface prepared by 3.0 wt% alumina precursor was uniformly covered on the fiber surface. The flexibility of ASFF/Al 2 O 3 /SiC-ZrO 2 was maintained after static oxidation at 1300 °C for 1 h. The tensile strength of ASFF/Al 2 O 3 /SiC-ZrO 2 at 1200 °C were increased from 5 to 7 MPa to 21.35 ± 2.58 MPa. The Al 2 O 3 interface not only limited the direct contact between Si-gel and fiber, but also reacted with Si-gel to produce mullite at high temperature. The problem of fiber adhesion caused by Si-sol in ASFF matrix was solved. Additionally, the SiC-ZrO 2 coating reduced the surface temperature of ASFF rom 1700 °C–1300 °C. Combining the radiation performance of SiC-ZrO 2 coating and the isolation effect of the Al 2 O 3 interface, ASFF/Al 2 O 3 /SiC-ZrO 2 was able to operate continuously for 300 s under the 1700 °C butane-oxygen flame heating condition.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Zhitao Shan,Yuanyuan Kang,Jiayan Zhang,Yanfei Zhang,Qiuju Zheng,Shujiang Liu,Haizheng Tao,Yuanzheng Yue
The hardness ( H v ) and crack initiation resistance ( C R ) of oxide glasses are crucial properties for various applications, such as in vehicles, display devices, and buildings. However, these properties are still limited for many special applications. Here, we studied the evolution of the H v and C R with varying the ratio R = [Al 2 O 3 ]/[CaO] in the low silica (0 and 17 mol% SiO 2 ) aluminate glasses, i.e., so called silico-aluminate glasses, and thereby identified a composition that exhibits the highest C R and H v . The results showed that the H v decreased with increasing R within the peraluminous region. Furthermore, a significant increase in C R value with increasing R was detected in the range of R = 1.0–1.18. In contrast, the glass series containing 50 mol % SiO 2 content exhibited only a slight increase in C R value, but pronounced increases in both T g and H v with increasing R in the peraluminous region. The Raman spectroscopy revealed that [5]Al and oxygen tri-cluster ([3]O) are the controlling factors for C R and H v of the studied glasses. Moreover, the impact of [3]O and [5]Al on H v and C R is highly dependent on the SiO 2 content in the studied glasses.
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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.
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ACS ES&T Water
·
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.
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Li Zhang,Wanlin Wang,Lei Zhang,Jie Zeng,Xu Gao
The dissolution mechanism of Al 2 O 3 inclusions in molten slags was explored by in-situ single hot thermocouple technique combined with X-ray photoelectron spectroscopy. Result shows that it takes 2940 s to completely dissolve Al 2 O 3 inclusions in the molten F-bearing mold flux, which is mainly controlled by boundary layer diffusion. Because the connected [AlO 6 ] octahedra in the Al 2 O 3 inclusion is gradually destroyed by the O 2− ions in the melt. By comparison, the CaO–SiO 2 –B 2 O 3 based F-free mold flux only takes 840 s to completely dissolve Al 2 O 3 inclusions. Because the [AlO 6 ] octahedra is destroyed and further transformed to [AlO 4 ] tetrahedra and produce O 2− ions, which greatly facilitates the dissociation of the Al 2 O 3 particle. However, the formed [AlO 4 ] tetrahedra will promote the precipitation of the dense 2CaO·SiO 2 ·Al 2 O 3 crystals, which tightly encases the Al 2 O 3 particle and causes significant drop in the dissolution rate. Thus, the dissolution rate is controlled by chemical reaction and then by boundary layer diffusion.
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高影响因子
Journal of Physical Chemistry C
·
2021
·
IF 4.126
Feng Shi,Lili Hu,Yun Cui,Jinjun Ren
Glasses in the xLa2O3-yAl2O3-(100 – x – y)NaPO3 system were synthesized by a melt quenching method, where 0 ≤ x ≤ 7.5, y = 0 and x = 5, 5 ≤ y ≤ 15. The structures were characterized by advanced multinuclei solid-state nuclear magnetic resonance spectroscopy (SSNMR) and X-ray photoelectron spectroscopy (XPS). 31P MAS NMR spectroscopy indicates that the glass Q2 structure is depolymerized by La2O3 and Al2O3, forming multiple QxAln and QyLan phosphorus species, where n, x, and y represent the number of P–O–P, P–O–Al, and P–O–La bonds, respectively. The various phosphorus species were identified by the J-coupling effect based one and two-dimensional (1D and 2D) experiments such as 2D J-resolved, 1D refocused INADEQUATE and 1D 31P{27Al} J-coupling heteronuclear multiple quantum coherence (HMQC). La is used as a mimic to simulate the local structure of the luminescent rare earth ions. 139La wideband uniform rate smooth truncation quadrupolar Carr–Purcell–Meiboom–Gill (WURST-QCPMG) spectra show that the coordination number of La is dominantly nine, and some La atoms transfer to lower coordination with the addition of Al2O3. La, Al, and Na atoms exclusively bond to phosphorus tetrahedron PO4, which is evidenced by the 31P/23Na, 31P/27Al double resonance NMR, XPS, and the calculation of charge balance. However, the Al/P and La/P connection methods are much different based on the calculation of charge balance and bond number. Finally, comprehensive and novel local structure models are developed for these rare earth-doped aluminum phosphate glasses.
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高影响因子
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2022
·Vol. 105
·期 11
·6953-6964
·
IF 4.186
Yuchao Qiu,Junjie Shi,Bin Yu,Changle Hou,Jingjing Dong,Song Li,Yumo Zhai,Jianzhong Li,Changsheng Liu
The recycling of titanium from titania-bearing slag is an important part of the circular economy; however, the yield of titania is restricted due to the lack of fundamental thermodynamic data. In the present work, the equilibrium phase relations of MgO–Al 2 O 3 –TiO 2 system in air at 1600°C have been determined using a high-temperature equilibration-quenching technique followed by X-ray photoelectron spectroscopy, scanning electron microscopy-energy-dispersive X-ray spectrometry, and X-ray diffraction. Ti 4+ was confirmed as the stable valence of titanium, and the rutile and spinel solid solution phases were detected to be coexisting with pseudobrookite solid solution phase, respectively. The formation principles of pseudobrookite and spinel solid solutions were confirmed in view of the corresponding crystal structure and the composition substitution relationship of the oxides at 1600°C. However, great discrepancies were found from the comparison of the present experimental results with the thermodynamic calculations and the literature results, and the present equilibrium phase relations are therefore significant for updating the present titania related thermodynamic database for a superior prediction of the thermodynamic behaviors of relevant process.
研究领域:
材料科学
·
冶金工程
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高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2026
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IF 6.7
Dexin Kong,Rui Shan,Shuxiao Wang,Huan Li,Haoran Yuan,Yong Chen
Converting plastic waste into hydrogen provides a promising route to simultaneously address environmental pollution and clean energy production. This study developed a Ni single-atom catalyst stabilized on an Al 2 O 3 /N-C composite support (Ni@Al 2 O 3 /N-C) for H 2 production from polypropylene (PP) via pyrolysis-catalytic reforming. The composite support integrates the high-temperature structural stability of Al 2 O 3 with the strong anchoring capability of N-doped carbon, enabling the formation of stable C-N-Ni active sites and effectively suppressing Ni aggregation under harsh reforming conditions. Under the optimal conditions (catalyst/PP = 1.25:1, water feed = 6 mL h −1 ), the catalyst achieved a gas yield of 127.59 mmol g −1 PP, a hydrogen yield of 84.14 mmol g −1 PP, and a hydrogen selectivity of 65.96%. The catalyst maintained good cyclic performance over 10 consecutive runs, with the H 2 yield decreasing from 84.14 to 69.39 mmol g −1 PP while the H 2 selectivity remained at 64.49% in the 10th cycle. XPS, HAADF-STEM, XRD, Raman, SEM, and TEM analyses confirmed that Ni remained atomically dispersed on the support after reaction, with no obvious nanoparticle agglomeration and only limited carbon nanotube formation. This work provides an effective support-engineering strategy for designing thermally stable single-atom catalysts for plastic reforming and other high-temperature catalytic processes.
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高影响因子
危险品化学品经营许可证（带存储）