Surfaces
·
2025
·Vol. 8
·期 4
·69
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IF 2.9
Huajie Zhang,Yunhan Pu,Yanjun Li,Mingli Fu
The selective oxidation of methane to methanol under mild conditions remains a significant challenge due to its stable C-H bond and the propensity for overoxidation of products. Herein, we investigated the Fe- and Cu-modified ZSM-5 catalysts using H2O2as an oxidant for the selective oxidation of methane. It was found that the Fe/Cu ratio had a great impact on methanol yield. The Fe3Cu1displayed the highest methanol yield of 29.7 mmol gcat−1h−1with a selectivity of 80.9% at 70 °C. Further analysis revealed that Fe3Cu1showed the highest Fe3+and Cu+contents. The optimal dual valence cycle not only facilitates the efficient utilization of H2O2, promoting the activation of methane to •CH3at the Fe site, but also suppresses the deep oxidation caused by the Fenton-like effect of Fe/H2O2, thus maintaining the high yield and high selectivity of methanol.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Minghao Shi,Jihui Yang,Mingjia Zhang,Shule Zhang,Qin Zhong
The Ce-based catalysts show promising activity in the selective reduction of NO x with NH 3 (NH 3 -SCR) at medium and low temperatures, yet their limited sulfur tolerance hinders broader application. We have developed a catalyst by confining CeO 2 within the mesopores of ZSM-5 zeolite (CeO 2 @ZSM-5), resulting in uniform dispersion and ultra-small CeO 2 nanoparticles (<10 nm). This distinctive structure enhances the interaction between the carrier and active species, reducing the catalyst's surface basicity and its affinity for acidic SO 2 gas. Additionally, the small CeO 2 particle size leads to an increased Ce 3+ concentration, which inhibits the reaction between Ce active sites and SO 2 . Employing a dual strategy of reducing adsorption and inhibiting reactions, we significantly minimized the impact of SO 2 on NH 3 -SCR. Impressively, common Ce-based catalysts become deactivated due to the formation of corresponding sulfates through reaction with SO 2 , however, CeO 2 @ZSM-5 achieves NO x conversion above 98% and N 2 selectivity of 100% within the temperature range of 250 °C to 450 °C. The addition of 100 ppm SO 2 does not significantly affect NH 3 -SCR activity. This study provides an effective approach to mitigate SO 2 adsorption and reactions, offering a valuable strategy for the development of highly efficient sulfur-resistant catalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Xin Meng,Yaochun Yan,Zeyu Chen,Mengting Xu,Zhaoyang Fei,Ming Xia,Xian Chen,Hui Shi,Xu Qiao,Qing Liu
Catalytic oxidation is a promising technology for the deep cracking of chlorinated organic compounds (COCs) in pharmaceutical waste salts. The critical challenge lies in the development of catalysts that can synergistically activate C Cl bonds and promote highly efficient oxidation. Herein, this study employed a B-site doping strategy to develop a series of perovskite-type catalysts that successfully achieved the synergy of acidic and redox sites. Among them, the LaMn 0.8 Cr 0.2 O 3 /ZSM-5(25) catalyst exhibited the optimal performance in the catalytic cracking-oxidation of the model pollutant 1-chloro-3-phenylpropane. It achieved a T 90 of 260 °C, representing a significant reduction of 48 °C compared to the undoped catalyst. Moreover, it retained around 90% conversion over 60 h. In-depth mechanism study indicated that the pronounced electron transfer between Cr and Mn ions (3Cr 2+ +3Mn 4+ → 2Cr 3+ +Cr 6+ +3Mn 2+ ) not only increased the oxygen vacancy concentration but also significantly enhanced the activity of both chemisorbed oxygen (0.37 mmol·g cat −1 ) and lattice oxygen (0.23 mmol·g cat −1 ). Concurrently, the metal doping effectively exposed the inherent Si-OH-Al acidic sites in the ZSM-5 framework without altering their intrinsic nature. This synergistic mechanism drives the efficient cracking-oxidation of COCs by accelerating the steps of C Cl bond cleavage and deep oxidation of intermediates, rather than altering the reaction pathway. This work provides a solid theoretical basis and profound insights for designing multi-site synergistic catalysts for the purification of COCs.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2022
·
IF 7.926
Qingxiang Shu,Zhenhua Sun,Ganyu Zhu,Chenye Wang,Huiquan Li,Fang Qi,Qikun Zhang,Shaopeng Li
The increased production of coal gasification coarse slag (CGCS) has placed a significant environmental load on the environment. In this research, one-step microwave synthesis employing coal gasification coarse slag desilication solution as the major source of Si and Na increased the nucleation and crystallization rate of ZSM-5 zeolite . The optimum synthesis conditions were 180 °C, 4 h, Na 2 O/SiO 2 molar ratio of 0.2, and SiO 2 /Al 2 O 3 molar ratio of 200, which led to a relative crystallinity of ZSM-5 zeolite higher than 100 % and a specific surface area of 344.27 m 2 •g −1 . The resulting high-purity ZSM-5 zeolite not only has high SiO 2 /Al 2 O 3 molar ratio, good specific surface area, and regular hexagonal prism structure, but also has high crystallinity, smooth crystal surface and great grain homogeneity because of the microwave process. Its static adsorption capacities toward p -xylene and butyl acetate were 106.84 and 115.47 mg•g −1 , respectively, and the dynamic adsorption capacities were 81.44 and 176.14 mg•g −1 , respectively. The preparation method of ZSM-5 zeolite with high efficiency and low cost proposed in this paper not only contributes to the high-value utilization of CGCS, but also provides an effective method and practical guidance for the removal of volatile organic compounds (VOCs).
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Guohao Xu,Jiaqi Liu,Xin Gao,Xuedong Zhu
Hollow b-oriented ZSM-5 with a thickness of approximately 80 nm was synthesized for methane co-aromatization with propane (MCP) through the desilication–recrystallization of b-oriented ZSM-5 using tetrapropylammonium hydroxide (TPAOH) as a template. A hollow structure was introduced into b-oriented ZSM-5 via desilication with OH− and a thin intact shell was formed during recrystallization of leached Si species under TPA+ template application. By regulating the recrystallization time, shell thicknesses could be controlled from 120 nm to 60 nm. Under a recrystallization time of 24 h, the hollow b-oriented ZSM-5 possessed suitable acidity as well as the largest SBET and daver. When the hollow b-oriented ZSM-5 zeolite was used as the support for a zinc-based catalyst, aromatic selectivity and the conversion of methane and propane were improved. A maximum aromatic selectivity of 87.5% was achieved, with methane and propane conversion of 10.7% and 77.9%, respectively.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Bowen Zhao,Jianyi Lu,Qing Xu,Fei Zheng,Zhiyong Zhou
Owing to its strong chemical inertness, sulfur hexafluoride (SF 6 ) is intrinsically resistant to degradation. Accordingly, a composite material was developed by coupling sulfidated nanoscale zero-valent iron (S-nZVI) with fly ash-derived zeolite ZSM-5, forming a multi-level heterostructure for efficient SF 6 degradation. Experimental results confirmed that the composite exhibited exceptional low-temperature degradation performance, achieving complete removal of 2 vol% SF 6 at 600 °C with a specific degradation amount of 206.1 mL/g. Remarkably, effective degradation was still maintained at 300 °C, surpassing the previously reported minimum temperature limit (∼450 °C) for SF 6 degradation. Kinetic analysis revealed a near-zero-order reaction behavior with an apparent activation energy of only 27.61 kJ/mol, indicating that the initial stage was dominated by adsorption, diffusion, or interfacial electron transfer rather than S F bond cleavage. Comprehensive characterization showed that the composite possessed Fe 0 /FeS and FeS/ZSM-5 dual heterointerfaces, serving simultaneously as adsorption carriers, electron donors and acceptors. Specifically, the microporous framework of ZSM-5 physically confines nonpolar SF 6 molecules through van der Waals and confinement effects, enriching their local concentration and forming a favorable adsorption-activation interface. Electrons released by Fe 0 migrate directionally to these enrichment sites under the drive of the multi-level heterostructure, enabling concurrent adsorption and electron-induced activation of SF 6 , and thereby facilitating S F bond cleavage. The resulting fluoride ions initially react with Fe 0 to generate FeF 3 , which subsequently interacts with the silicate framework to produce SiF 4 , establishing a mediated fluorine migration pathway from SF 6 to SiF 4 and enabling deep degradation with sustained reactivity.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Jie Yang,Liyuan Huai,Jiang Gan,Hualei Hu,Shenghu Zhou,Jian Zhang
The 5,5′(oxy-bis(methylene))bis-2-furfural (OBMF) formation from the 5-hydroxymethylfurfural (HMF) self-etherification over zeolites is an important reaction for the synthesis of value-added chemicals from biomass resources. However, there is still a lack of knowledge about the reaction mechanism and the roles of different acid sites that impedes the exploitation of zeolite catalysts for efficient OBMF production. In the present study, the ZSM-5 (HPZ) catalysts of four hierarchically micromesopores were successfully synthesized in different Si/Al ratios by adjusting the amount of Al in the solvent evaporation with the assistance of a dry gel conversion method. The kinetics of OBMF formation from HMF self-etherification was investigated. The apparent activation energy and the conversion reaction order were calculated to be 104.6 kJ/mol and 0.65, respectively. The intrinsic activity comparison of four catalysts and density functional theory (DFT) calculations showed that HMF adsorption and etherification benefit from Brønsted-acid sites. Besides, the DFT results suggested that the etherification proceeds via a concerted step, instead of the sequential pathways, thus leading to the high selectivity of OBMF on hierarchically micromesoporous ZSM-5 (HPZ) catalysts.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2025
·
IF 3.7
Mengkun Luan,Wenli Su,Huijuan Guo,Yu Fan
ZSM-5 molecular sieves are potential catalysts for the catalytic pyrolysis of light naphtha. Nevertheless, traditional ZSM-5 is constrained by its low yield of light olefins and poor stability, limiting its use as a pyrolysis catalyst. In this work, a method involving quaternary ammonium salt (QAS)-assisted acid hydrolysis of silicon sources was developed to construct hierarchical and highly crystalline ZSM-5 molecular sieves for the efficient catalytic pyrolysis of n- pentane. The mesoporous sizes in hierarchical ZSM-5 were controlled by varying the alkyl chain length of the QASs. Diffusional measurements revealed that the diffusion time constant of n- pentane increased with increasing mesoporous size in ZSM-5. The n- pentane pyrolysis tests revealed that a suitable mesoporous size (10.8 nm) facilitated the n- pentane monomolecular cracking pathway while the hydrogen transfer reactions were inhibited. Among the series of ZSM-5 molecular sieves, the D-ZH5 catalyst synthesized by dodecyl trimethyl ammonium bromide (DTAB)-assisted acid hydrolysis of ethyl orthosilicate (TEOS) achieved the highest yields of light olefins (41.69% (mass) for ethylene and propylene) and the lowest deactivation rate (0.13%·h –1 ).
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2024
·
IF 4.8
Mengkun Luan,Xiangjie Lei,Yu Fan
To increase the yield of light olefins during the catalytic pyrolysis of alkanes, a novel hierarchical Fe-incorporated ZSM-5 molecular sieve (FeM-Z5) was synthesized using an Fe-based metal-organic framework (Fe-MOF) as a mesoporogen and iron source through the dry gel conversion (DGC) method. In contrast to the conventional method of incorporating Fe species into ZSM-5 via impregnation, the DGC method incorporates Fe species into the framework of ZSM-5, decreasing the amount of Brønsted (B) acid sites and thereby inhibiting the side reactions of hydrogen transfer during the catalytic pyrolysis of alkanes. Compared with the FeN-Z5 catalyst prepared by the DGC method with Fe(NO 3 ) 3 as an iron source, FeM-Z5 had a larger amount of strong B acid sites and more mesopores with a size range of 10–40 nm originating from the decomposition of Fe-MOF; these aspects improved n-pentane pyrolysis and ethylene and propylene diffusion. As a result, the optimal FeM-Z5 catalyst exhibited the highest yield of ethylene and propylene (33.4 wt%) and the lowest deactivation rate (0.07 %/h) among the prepared catalysts during the catalytic pyrolysis of n-pentane.
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ACS Catalysis
·
2025
·
IF 13.1
Yufeng Li,Jinbiao Yuan,Yunxuan Ji,Siyang Yan,Jiaxu Liu,Bing Liu,Xiaohao Liu
Developing efficient and stable catalysts to convert CO2 to desirable C1 products is of great importance for carbon resource utilization. Cobalt-based catalysts usually show high activity in methanation but poor selectivity to CO from the reverse water-gas shift (RWGS) reaction. Herein, we synthesized In-doped CeO2-supported cobalt catalysts for RWGS reaction, which achieved almost reverse 100% selectivity toward CO with a near-equilibrium CO2 conversion of about 49% at 500 °C and 1 MPa. Results showed that catalyst reduction could result in In species migration onto Co particles to form an InCo alloy, thereby modulating the cobalt electronic structure. It thus strengthened Co–H* bonding but weakened CO adsorption and activation, in turn inhibiting CH4 formation via HCOO* and CO hydrogenation. Interestingly, the reaction temperature-dependent deactivation was observed over 10Co/CeO2, owing to cobalt oxidation determined by the O atom chemical potential (μO). Theoretical investigations demonstrate that μO is related to the free energy of H2O and H2 (μO = GH2O‐GH2), where the reaction temperature exhibits different degrees of effect on GH2OandGH2. Based on the deactivation behavior study, we successfully developed a simple strategy to suppress oxidation deactivation by mixing with hydrophilic H-ZSM-5 zeolite to drive H2O desorption away from the cobalt surface during the CO2 methanation reaction with much more H2O molecules produced.
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CHEMOSPHERE
·
2023
·
IF 8.8
Jida Gao,Qianji Lin,Tingzhi Yang,Yong chao Bao,Juan Liu
Coal gangue is a kind of solid waste produced in the process of coal mining and washing. Its silicon aluminum silicon aluminum oxide content is high, respectively, which are suitable for resource utilization as raw materials for Si–Al molecular sieving. In this paper, a novel, simple, low-cost, and environmentally friendly process was carried out to prepare ZSM-5 zeolite by solvent free method after calcination, acid leaching, and alkali melting. The obtained samples were characterized by Energy Dispersive Spectrometer (EDS), Inductively Coupled Plasma (ICP), Thermo-gravimetry Analysis (TG), X-ray Photoelectron Spectroscopy (XPS), Fourier Transform Infrared Spectrometer (FTIR) X-Ray Diffraction (XRD), Scanning Electron Microscope (SEM) and N 2 adsorption isotherm. The characteristics of the raw materials and the adsorption mechanism of the prepared samples were characterized. Through a series of pretreatment such as calcined acid leaching and alkali melting of the raw materials, the silicon-aluminum ratio of the sample reaches 1.749, and the maximum specific surface area of the sample can reach 252.59 m 2 /g. The obtained samples were used to adsorb heavy metal ions and methylene blue solution, and the removal rate of lead ions and methylene blue solution was more than 95%. The theoretical maximum adsorption capacity of Pb ion, methylene blue solution and copper ion can reach 232.56 mg/g and 118.34 mg/g. The adsorption process is mainly chemical adsorption. The product could be suitable for removing both heavy metal ions and cationic dyes from the wastewater and had broad application prospects.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Run Cai,Likun Wen,Yihua Cao,Yindan Wu,Yichen Song,Xinyu Wang,Hanyang Zhou,Yurui Zhang,Xiaoping Dai,Xin Zhang
The benzene-methanol alkylation offers a strategic route to valorize methanol surplus and meets the growing demand for high-purity aromatics. For industrially viable shaped catalysts, achieving a balance between sufficient acidity and optimal diffusion capacity remains critical. Traditional shaping methods using binders inadvertently compromise mass transfer efficiency within zeolite crystals while introducing strong acid sites that disrupt the tailored weak-acid properties. To overcome these limitations, we developed a dual-approach strategy employing 1) B-Mg-co- substitution in ZSM-5 frameworks to effectively suppress ethylbenzene generation while enhancing catalytic durability, and 2) recrystallization-driven structural engineering to create binder-free architectures featuring cheese-like macropore. Intelligent gravimetric analysis (IGA) and fluorescence probe diffusion mapping further reveals three-dimensionally interconnected micro-meso-macroporous networks that facilitate enhanced molecular transport for both small and bulky aromatic species. The optimized catalyst demonstrates remarkable stability during extended operation (1008 h) under 460 °C, 0.4 MPa and 2.5 h −1 , achieving 45–50 % benzene conversion (X B ) with toluene selectivity (S T ) ~50 %, C 8 selectivity (S C8 ) ~37 %, C 9+ selectivity (C 9+ ) ~ 14.0 %, and yield of EB in C 8 (Y EBinC8 ) <9 %. This work establishes a morphology-directed synthesis protocol for isomorphously substituted zeolites, offering a scale-up manufacturing route for acid site-engineered catalysts that combine hierarchical porosity with optimized Brønsted-Lewis acid synergy.
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