CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Xiangfei Ding,Youbing Zhu,Ketao Shi,Zhen Xu,Jian Chen,Zengxi Li,Hui Wang
ZSM-5 zeolite is extensively employed for hydrocarbons cracking to generate light olefins, and its acidity is closely related to the activity and product distribution. In this work, Al-Sn bimetallic ZSM-5 was prepared via a “one-pot” route. Characterizations, including XRD, UV–Vis, XPS, revealed that Sn species were mainly embedded into the zeolite framework as tetrahedral Sn (IV). Moreover, the Sn atoms promoted the formation of Lewis acid sites and reduced the Brønsted acid amount, which effectively inhibited occurrence of side reactions ( e.g. , aromatization, hydrogen transfer) and improved the selectivity of light olefins in n-hexane cracking. Light olefins yield over HZ5[100,200] (Si/Al = 100, Si/Sn = 200) reached 33.4 % due to the appropriate acid property, in comparison with only 15.4 % for HZ5[50,∞] (Si/Al = 50, Si/Sn=∞) containing system. Through optimization of reaction conditions, better catalytic performance (n-hexane conversion of 91.6 % and light olefins yield of 37.6 %) was obtained over HZ5[100,200] under 575 °C with WHSV of 2 h −1 .
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CARBOHYDRATE POLYMERS
·
2025
·
IF 12.5
Xin Wang,Pan Jiang,Xinjian Dai,Hao Guan,Xiaoqing Wang
Developing high-performance metal-organic framework (MOF)-based composites with high loading and uniform distribution of MOF nanoparticles is crucial for their adsorption-associated applications but remains challenging due to the lack of ideal carriers. Herein, a novel MOF-based composite was developed by in situ growth of MIL-53(Al) crystals within the carboxylated wood sponge (CWS) derived from natural balsa wood. The conversion of the cellular structure of natural wood into a lamellar structure greatly enhances the accessibility of the wood scaffold, while the introduction of carboxyl groups onto the cellulose skeleton of the wood sponge encourages the selective growth of MIL-53(Al) crystals on the lamellae of CWS. The structural features of the obtained MIL-53(Al)@CWS were investigated with FT-IR, XRD, SEM, and N 2 adsorption/desorption isotherms. The MIL-53(Al) loading can be finely tuned by adjusting the concentration of the MOF precursor solutions, and an appropriate MIL-53(Al) loading of 23 wt% results in the uniform dispersion of MIL-53(Al) crystals within the wood sponge without agglomeration. Benefiting from the high loading of MIL-53(Al) and the unique lamellar channels of CWS, the developed MIL-53(Al)@CWS can effectively adsorb various organic dyes such as rhodamine B (RhB), methylene blue, Congo red, and methyl orange in water, with a high adsorption capacity of 135.82 mg g −1 for RhB. Density functional theory (DFT) calculations reveal the detailed dynamic diffusion pathways and the molecular interactions between RhB and MIL-53(Al). This work demonstrates the advantages and potentials of lamellar wood sponges as a promising host matrix in supporting MOF powders for adsorption-associated applications.
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INTERNATIONAL JOURNAL OF ENVIRONMENTAL ANALYTICAL CHEMISTRY
·
2025
·
IF 2.5
Yuge Liu,Zhiguo Li,Yongmei Jia
The fast detection of environmental contaminants catechol (CC) and hydroquinone (HQ) is of great importance to public health. In this research, a composite was firstly synthesised by a pre-exfoliation method, the components of which were Ni-Al-LDH and reduced graphene (rGO). This material was then utilised in the development of a highly sensitive biosensor for determining CC and HQ. The construction procedure involved modification of glassy carbon electrode (GCE) by the composite and laccase (LAC). Tests conducted by electrochemical methods showed the addition of laccase can greatly improve the response signal of electrochemical measurements on the composite modified GCE to CC and HQ. The electrochemical tests were performed by utilising 0.1 mol/L phosphate-buffer. When separately detected, the detecting linear range for CC by the biosensor was 0.009–0.58 and 0.95–4.4 mmol/L. When it comes to HQ, the range was 0.009–0.57 and 0.95–4.4 mmol/L on the composite/enzyme modified electrode. When the biosensor was used for detecting CC and HQ together, the linear ranges were both 0.019–0.56 and 1.0–4.4 mmol/L. The detection limits calculated for simultaneous detection were 0.75 and 0.47 μmol/L, respectively. The sensor also possessed excellent sensitivity, selectivity and long stability. For applicability of the biosensor, it was used in analysing the two substrates in real water samples, and the recoveries were acceptable.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Ne Ni,Ying Ouyang,Jianqiang Liu,Enhui Xing,Yibin Luo,Xingtian Shu
It was the thermostability and acidity of P precursors that influenced the interaction between P species and framework Al to determine the hydrothermal stability of P modified ZSM-5. With H3PO2 and NH4H2PO2 as P precursors, the P–Al interactions of P modified ZSM-5 samples calcined under different temperatures were systematically investigated by X-ray fluorescence, X-ray photoelectron spectroscopy, 27Al, and 31P MAS NMR spectroscopy, and temperature-programmed desorption of NH3 (NH3-TPD). With H3PO2 as the precursor, lower calcination temperature favored less self-polymerization of P species; however, obvious loss of phosphorus was observed during hydrothermal treatment. Conversely, higher calcination temperature tended to result in excessive interaction between P and framework Al for dealumination. Therefore, moderate interactions between P and framework Al were obtained over H3PO2 modified ZSM-5 calcined at 350 °C, which contributed to weaken the self-polymerization of P species. Compared with H3PO2, neutral NH4H2PO2 generated a relatively weaker P-zeolite interaction, which was less affected by the calcination temperature.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Chi Sun,Yudong Xia,Xue Ye,Wenlin Xu,Hui Shi,Xinhua Gao,Jinghao Yu,Lisheng Guo,Jie Li
The direct dimethyl ether (DME) synthesis reaction via CO2 hydrogenation typically requires a bifunctional catalyst that effectively combines a methanol synthesis catalyst with a methanol dehydration catalyst, but the effect of the relationship between the two catalysts on the catalytic performance has not been as well studied. In this study, we developed a CuZnZr/Al–S(10)-PG bifunctional catalyst physically mixed with Al-modified SBA-15 and the traditional CuZnZr catalyst for the hydrogenation of CO2 to DME. A pivotal discovery is that the modulation of interaction intensity between these two constituents significantly influences the electronic configuration of each component. Through X-ray photoelectron spectroscopy characterization and methanol dehydration experiments, it was confirmed that diminishing the synergistic interplay between CuZnZr and Al-modified SBA-15, which regulated the electronic structure of the Cu–Zn interface and enhanced the Cu–Zn interfacial interaction, played a crucial role in enhancing the catalyst’s performance in CO2 hydrogenation to DME. This finding contests established beliefs about the necessity of strong synergistic interactions in such systems and provides new insights for designing rational bifunctional catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Huibin Liu,Xiao Chen,Wenhao Yang,Weilin Shen,Yan Du,Huamin Wang,Wenjun Zhu,Changhai Liang
The semi‑hydrogenation of alkynes to alkenes remains a challenging topic in the purification of polymer monomers. Achieving selective hydrogenation of alkynes requires careful control of alkene adsorption strength on the catalyst surface while avoiding the production of over‑hydrogenated compounds. The reaction is fundamentally influenced by the electronic structure of the metal active sites on the catalyst surface. In this study, Al 2 O 3 -supported Al Ni intermetallic nanoparticles catalysts are synthesized through in situ reduction-doping methods using LiAlH 4 as Al sources. The coordination environment and electronic structure of the active metal Ni are finely tuned while the Al Ni stoichiometric ratio is adjusted. The turnover frequency of AlNi 3 /Al 2 O 3 (16.7 h -1` ) and AlNi/Al 2 O 3 (9.1 h −1 ) are higher than that of the Ni/Al 2 O 3 catalyst (8.6 h −1 ). The optimal AlNi/Al 2 O 3 catalyst with AlNi intermetallic structure exhibits the high styrene selectivity (>90 %) when the phenylacetylene conversion exceeds 99 %. The metal bond between Al and Ni atoms strengthens electronic coupling, resulting in the hybridization of Al p orbital and s orbital with Ni d orbital. The resulting isolated and electron-rich Ni sites (Ni δ- ) are key to achieving high selectivity for styrene. These sites govern the π-adsorption of styrene molecules. Furthermore, the kinetic selectivity advantage of this unique Ni ensemble (AlNi, an intermetallic compound) has been verified. A lower reaction rate and higher activation energy (Ea = 132 kJ·mol −1 ) for hydrogenation of styrene over AlNi/Al 2 O 3 catalyst are observed. Moreover, the high stability of this catalyst and its broad applicability in the hydrogenation of various alkyne compounds provide valuable insights for selective hydrogenation applications of Al-based intermetallic catalysts, enabling the exploration of their properties and applications.
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ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Hongyang Mao,Shulei Li,Lihui Gao,Si Shen,Yanhong Liu,Keyi Xu
Coal gasification fine slag (CGFS), a typical coal-based solid waste, poses significant environmental challenges with an annual output exceeding 50 million tons in China. The complex distribution of carbon and ash components necessitates the development of a material that can effectively harness both carbon and ash for comprehensive utilization. While layered double hydroxides (LDHs) exhibit catalytic potential, their performance is often limited by severe particle aggregation. Herein, we engineered a robust carbon-anchored Fe-Al-LDH composite (CGFS-LDH) through hydrothermal co-precipitation, demonstrating exceptional efficacy in H 2 O 2 activation for phenol degradation. Remarkably, CGFS-LDH achieved 100 % removal of 200 mg L −1 phenol within 60 min. Advanced characterization (XPS, XRD, EPR, LC-MS, and electrochemical analysis) revealed that CGFS serves dual roles: as a structural scaffold preventing LDH aggregation and as an electron shuttle promoting Fe 2+ /Fe 3+ redox cycling. Although trace amounts of Fe (0.2 wt%) and Al (0.3 wt%) leached due to dynamic precipitation-dissolution equilibrium, the catalyst maintained outstanding stability over multiple cycles, with negligible activity loss. This work introduces an effective strategy for the comprehensive utilization and high-value transformation of CGFS, while also providing novel insights into the development of highly efficient and stable porous nanocomposites catalysts.
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THIN SOLID FILMS
·
2025
·
IF 2
Jinyan Pan,Qiao Huang,Ruotong He,Tiejun Li,Hongyang He,Lingsen Yan,Zhenping Wang,Yan Liu,Jing Li,Yunlong Gao
The resistive properties and mechanisms of devices with different structures were investigated by fabricating TiO 2 and Graphene Oxide (GO) films on Indium Tin Oxides (ITO)conductive glass using spin-coating techniques. The results show that our prepared devices can undergo SET/RESET under different voltages and exhibit unique resistive change characteristics. In addition, we found a complementary resistive switching (CRS) behavior in the Al/TiO 2 /GO/ITO structured devices, similar to the memristor which is reverse-series connection of Al/TiO 2 /ITO and Al/GO/ITO. And its resistive behavior is analogous to neuronal firing processes-depolarizing and polarizing behavior. Furthermore, the resistance is modulated by constant voltage and the stimulus gets gradual resistance increase (long-term depression, LTD), and causes progressive resistance decrease (long-term potentiation, LTP). This study provides a reference for the application of the synergistic combination of CRS behavior and tunable resistance states enables a dual-path approach for implementing neuronal and synaptic functionalities in bio-inspired electronics, offering a reference framework for complementary memristor-based bionic neurons that broadens the application scope of Resistive Random Access Memory.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Yumeng Zhao,Guoshu Gao,Peng Zhu,Haiou Liu,Yu Guo,Xiongfu Zhang
Purification and dehydration of ethyl acetate are important processes in chemical production, and the preparation of stable and efficient pervaporation membrane materials has still been a challenge. In this work, a well-intergrown polycrystalline Al-Fum@CS tubular membrane was successfully prepared by a synergistic strategy involving seeded growth combined with surface remediation and applied for the first time in the separation of a multicomponent mixture containing ethyl acetate by pervaporation. By regulating the synthesis conditions, a continuous Al-Fum membrane with thickness of 1.7 μm was initially grown within the innermost part of a uniform seed layer. Subsequently, a chitosan (CS) layer was introduced onto the membrane to fabricate the Al-Fum@CS membrane. This CS layer significantly modifies the defects existing in the membrane surface. The obtained Al-Fum@CS membrane with the thickness of around 1.8 μm is dense and has strong hydrophilicity. It can preferentially separate water from a ternary azeotropic mixture of water–ethanol–ethyl acetate and displays high pervaporation performance with a permeation flux of 1.88 kg/(m2·h) and a separation factor of ∼6000 at 60 °C. Especially, the Al-Fum@CS membrane can be continuously operated for more than 150 h without any obvious change in separation performance, showing excellent ultrahigh stability. Moreover, the as-prepared membrane has good acid resistance and reusability in complex environments according to the results of multiple mixture pervaporation experiments. Therefore, the Al-Fum@CS tubular membrane has great industrial application potential for the purification of ethyl acetate produced from the esterification reaction.
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Catalysis Science & Technology
·
2024
·Vol. 14
·期 3
·735-745
·
IF 4.4
Xueting Song,Haifeng Yang,Chenghua Zhang,Guizhi Zhang,Hong Wu,Youzhou He,Min Fu,Xingyan Liu,Siqi Li,Siping Wei
Synergistically modulating electron distribution between metal nodes in metal–organic frameworks (MOFs) is an effective strategy to improve the electrocatalytic performance of MOFs. Herein, a special bimetallic MOF composite (Al0.35/Ru0.15-TCPP-CNTs) was constructed by introducing highly dispersed Ru and Al co-existing in the MOF metal clusters and combining them with conductive carboxylic multi-walled carbon nanotubes (CNTs). Notably, the catalyst exhibited excellent hydrogen evolution reaction (HER) performance, with an overpotential of as low as 32 mV at a current density of 10 mA cm−2 in acidic media, comparable to commercial Pt/C. Experimental results and density functional theory (DFT) calculations proved that a reasonable proportion of Al/Ru bimetallic clusters in MOFs and the loaded CNTs induced charge redistribution and cooperative electronic coupling, which not only optimized the adsorption energy of H intermediates (ΔGH*) and produced a possible hydrogen spillover effect, but also increased the specific surface area and facilitated electron/mass transfer. This work may provide an improved method and research idea for the study of MOF electrocatalysts at the atomic level.
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AICHE JOURNAL
·
2024
·
IF 3.5
Yanru Zhu,Zhen Zhang,Yunfei Zou,Jian Zhang,Zhe An,Xin Shu,Hongyan Song,Jing He
Catalytic conversion of biomass-derived 5-(hydroxymethyl)furfural (5-HMF) into carbon-increased hydrocarbons as drop-in energy-rich biofuels has received a great deal of concern for the development of sustainable chemical industry. Here, we demonstrate a one-pot conversion of 5-HMF into C 9 -alkanes on one single catalyst, acidic–basic layered double oxides (Mg(Al)(Zr)O) supported CuCo alloy. The well-defined multifunctional catalytic sites with harmonious combination carry out cascade catalysis, affording C 9 -alkanes (including 30% of more value-added branched-cycloalkanes) in 83% yield. The basic–acidic sites on Mg(Al)(Zr)O show high activity for aldol condensation of 5-HMF and acetone, producing 4-[5-(hydroxymethyl)-2-furanyl]-3-buten-2-one (HAc) in a yield of >99%. The engineered Co–Cu–Co linkages on supported CuCo perform efficient hydrodeoxygenation, affording C 9 -alkanes in a selectivity of 96% from HAc. C 9 -cycloalkanes are generated from the cyclization of the corresponding monohydric alcohol intermediates by the synergy of acidic and CuCo sites in the hydrodeoxygenation reaction.
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Nanomaterials
·
2020
·Vol. 10
·期 5
·955
·
IF 4.324
Xiaogang Guo,Qi Sun,Taotao Liang,A. S. Giwa
Film-forming techniques and the control of heat release in micro-energetic chips or devices create challenges and bottlenecks for the utilization of energy. In this study, promising nano-Al/MoO3metastable intermolecular composite (MIC) chips with an uniform distribution of particles were firstly designed via a convenient and high-efficiency electrophoretic deposition (EPD) technique at room temperature and under ambient pressure conditions. The mixture of isopropanol, polyethyleneimine, and benzoic acid proved to be an optimized dispersing agent for EPD. The kinetics of EPD for oxidants (Al) and reductants (MoO3) were systematically investigated, which contributed to adjusting the equivalence ratio of targeted energetic chips after changing the EPD dynamic behaviors of Al and MoO3in suspension. In addition, the obtained nano-Al/MoO3MIC energetic chips showed excellent heat-release performance with a high heat release of ca. 3340 J/g, and were successfully ignited with a dazzling flame recorded by a high-speed camera. Moreover, the fabrication method here is fully compatible with a micro-electromechanical system (MEMS), which suggests promising potential in designing and developing other MIC energetic chips or devices for micro-ignition/propulsion applications.Keywords:nano-Al/MoO3MIC;stable suspension;electrophoretic deposition;kinetics;micro initiator
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