CHEMICAL ENGINEERING JOURNAL
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2017
·
IF 6.216
Bo Yang,Jianping Deng,Liyan Wei,Yanni Han,Gang Yu,Shubo Deng,Caizhen Zhu,Huabo Duan,Qiongfang Zhuo
2,2′,4,4′-Tetrabromodiphenyl ether (BDE47) is known as a recalcitrant bromated organic pollutant with the significant persistence, toxicity, and bioaccumulation. In this study, a synergistic effect of ball-milled Al particles with vitamin B 12 on the degradation of BDE47 was found according to the coordinated catalytic reduction process. The micro-scale Al particles prepared by ball milling and vitamin B 12 as common pharmaceutical composed a new combination reagent for hydrodebromination with low-cost and high reactivity. The degradation conditions were optimized by the addition of 2.0 g/L BM Al particles and 0.3 mM VB 12 using the solvent of methanol/H 2 O (v:v = 40:60) at pH 4.0. More than 97% of 25 mg/L BDE47 was debrominated into lower-brominated diphenyl ethers in a sequential pattern and finally into diphenyl ethers within a 120-min reaction. UV/Visible spectra showed that vitamin B 12 (Co(III)) was reduced to vitamin B 12s (Co(II)) by the ball-milled Al particles, which possesses super nucleophilic property to associate the carbon atom on C Br bond and then facilitates the hydrodebromination process of brominated diphenyl ethers. The experimental results can provide basic understanding to identify a reaction process of vitamin B 12 /vitamin B 12s for the enhanced reductive debromination of polybrominated diphenyl ethers by ball-milled Al particles, which would be possibly applied to treat soil washing solvent in the field of soil remediation.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
·
IF 3.9
Ketao Shi,Youbing Zhu,Zhen Xu,Nianming Jiao,Hui Wang
The metal coordination state and the corresponding acid property of zeolite closely relate to its catalytic performance. In this study, DBD-plasma (dielectric barrier discharge-plasma), a low-temperature and energy-efficient external activation method, was proposed to activate the NH4+-type ZSM-5 zeolite and to regulate the Al coordination. It was found that DBD treatment could efficiently decompose NH4+ species at 115 °C, far below that required for calcination (550 °C). Characterizations, including X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET), 27Al magic angle spinning nuclear magnetic resonance (27Al MAS NMR), and pyridine-adsorption infrared spectroscopy (Py-IR), revealed that DBD-plasma treatment could inhibit zeolite framework destruction and retain more framework Al and mesoporous structure, thus improving the stability and enhancing the amount of medium-strong Brønsted acid sites. In n-hexane cracking, DBD-activated zeolite exhibited improved conversion and C2–C4 olefin selectivity due to the enhanced monomolecular cracking pathway induced by increased Brønsted acidity, while reducing aromatics and coke formation by suppressing side reactions. This paper presents an alternative method that is more energy-efficient, highly effective, and capable of regulating the metal coordination and acidity of ZSM-5 zeolite.
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Journal of Materials Research and Technology-JMR&T
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2024
·
IF 6.2
Xuewu Li,Chenghu Ma,Tian Shi,Hejie Yang,Chuanwei Zhang,Wei Qi,Chen Li,Rongrong Liu,Weiping He,Yuanhai Liu
Aluminum-Lithium (Al-Li) alloys widely used in aerospace manufacture are highly susceptible to corrosion, which limits their industrial applications. Herein, 1H,1H,2H,2H-perfluorodecyltriethoxysilane (PFDTES) is used as a modifier for low-surface-energy treatment of TiO 2 nanoparticles. The water-based polyurethane (PU) is made as a binder to achieve a tight bonding between modified ceramic particles and Al-Li alloy, thus resulting in the extremely-feasible air-spraying preparation of a superhydrophobic coating with strong abrasion resistance. The water contact angle (CA) of as-prepared coating achieves 160 ± 0.83°, and the rolling angle (SA) is as low as 5.95 ± 0.59°. The surface structure, organization and composition are further characterized using SEM, EDS, XPS and laser confocal microscopy. Meanwhile, the electrochemical impedance and potentiodynamic polarization tests are performed for corrosion characterization. The results show that the corrosion potential of such coating increases by 170 mV compared with substrate, the corrosion current density decreases by two orders of magnitude, and the impedance modulus increases by two orders. The corrosion inhibition rate of the as-prepared coating is 98.8%, indicating that the corrosion resistance has been significantly enhanced. In addition, the mechanical robustness and stability of the coating is evaluated and confirmed using a sandpaper rubbing test. It also possesses great self-cleaning, anti-pollution and thermostable behaviors, thereby allowing them to work in extreme manufactures. Moreover, the as-prepared coating exhibits excellent adaptability to various materials and anti-icing property. This work sheds positive insights in enlarging industrial applications of multifunctional ceramic coatings in aerospace fields.
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ACS Catalysis
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2025
·
IF 13.1
Shuo Cao,Ying Ma,Wei Chu,Bingsen Zhang,Bo Peng,Yuefeng Liu
Molybdenum carbides have received attention for the reverse water gas shift (RWGS) reaction. Normally, MoCx-based catalysts are synthesized via a high-temperature carbonization of 1100 K, leading to the agglomeration of the active phase. In order to minimize the atomic motion leading to single growth, insertion of heteroatoms has been attempted with the usage of components in the catalyst substrate. The current work applied the self-assembling strategy to prepare a Mo–O–Al composite instead of traditional impregnation before carburization. The dynamic structure evolution and detailed coordination environment of the active phase are investigated by in situ X-ray diffraction, quasi in situ X-ray photoelectron spectroscopy, in situ transmission electron microscopy, and temperature-programmed surface reaction techniques. Our findings reveal that Al doping enables carburization at a lower temperature (200 °C) via the topotactic pathway, yielding α-MoCx (fcc); even at a loading as high as 40 wt %, the catalyst maintains an ultrasmall particle size (1 nm). The optimized catalyst exhibits a RWGS reaction rate of 52.1 μmolCO2·gMo–1·s–1 at 400 °C, representing a 2.5-fold enhancement over bulk β-Mo2C. This work provides a possible solution for maintaining high dispersion at high metal loading for catalyst preparation, specially requiring a high temperature during either synthesis or reaction.
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ACS Applied Nano Materials
·
2025
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IF 5.5
Yuhuan Tan,Yiran Yang,Shiyan Li,Zixiong Yao,Shixun Lian,Pengyan Fu,Wenli Zhou
To address issues such as uneven particle size, agglomeration, low luminescence efficiency, and poor stability in the nanosizing of Mn4+-doped fluoride red phosphors, this study combines solid solution engineering and aliovalent charge compensation to prepare high-performance K2LiB1–xB′xF6:Mn4+ (B, B′ = Al, Ga, In) nanoparticles (FNPs). Using an HF-free coprecipitation method for the synthesis of solid-solution matrices, followed by a ligand-assisted reprecipitation step that employs a small amount of HF to dissolve K2MnF6 to rapidly and uniformly incorporate Mn4+ into the matrices, and the particle size is reduced from 33.32 to 16.05 nm with improved dispersibility by adjusting the volume ratio of oleic acid (OA) to oleylamine (OAm) ligands; through the gradual solid solution of Al3+, Ga3+, and In3+, the regulatory mechanism of lattice distortion and local crystal field on luminescence is revealed, with optimal luminescence intensity achieved at specific solid-solution ratios and the emission peak blue-shifted from 636 to 632 nm. Zn2+ codoping for charge compensation enhances the luminescence intensity of the 0.9% Mn4+-doped sample by 120%, with the internal quantum efficiency (IQE) increased to 40.01%, and the fluorescence lifetime extended to 4.11 ms. The FNPs have good thermal stability (56% retention at 150 °C) and moisture resistance (85% retention after 240 h in water). Packaged white light-emitting diode (WLED) exhibits a luminous efficacy of 20.54 lm W–1, and the fluorescent ink enables red–green anticounterfeiting display under UV excitation, providing insights into applications in high-end display and lighting fields, especially micro-LED color conversion layers, WLED packaging, and anticounterfeiting/encryption inks.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 13
·19738-19752
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IF 0
Tian Kun,Pan Jie,Liu Yun,Wang Ping,Zhong Ming,Dong Yuanhua,Wang Meng
Heterogeneous Fenton oxidation using traditional catalysts with H 2 O 2 for the degradation of 1,4-dioxane (1,4-DX) still presents challenge. In this study, we explored the potential of Fe-ZSM-5 zeolites (Fe-zeolite) with three Si/Al ratios (25, 100, 300) as heterogeneous Fenton catalysts for the removal of 1,4-DX from aqueous solution. Fe 2 O 3 or ZSM-5 alone provided ineffective in degrading 1,4-DX when combined with H 2 O 2 . However, the efficient removal of 1,4-DX using H 2 O 2 was observed when Fe 2 O 3 was loaded on ZSM-5. Notably, the Brønsted acid sites of Fe-zeolite played a crucial role during the degradation of 1,4-DX. Fe-zeolites, in combination with H 2 O 2 , effectively removed 1,4-DX via a combination of adsorption and oxidation. Initially, Fe-zeolites demonstrated excellent affinity for 1,4-DX, achieving adsorption equilibrium rapidly in about 10 min, followed by effective catalytic oxidative degradation. Among the Fe-ZSM-5 catalysts, Fe-ZSM-5 (25) exhibited the highest catalytic activity and degraded 1,4-DX the fastest. We identified hydroxyl radicals (·OH) and singlet oxygen ( 1 O 2 ) as the primary reactive oxygen species (ROS) responsible for 1,4-DX degradation, with superoxide anions (HO 2 · /O 2 · − ) mainly converting into 1 O 2 and ·OH. The degradation primarily occurred at the Fe-zeolite interface, with the degradation rate constants proportional to the amount of Brønsted acid sites on the Fe-zeolite. Fe-zeolites were effective over a wide working pH range, with alkaline pH conditions favoring 1,4-DX degradation. Overall, our study provides valuable insights into the selection of suitable catalysts for effective removal of 1,4-DX using a heterogeneous Fenton technology.
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JOURNAL OF CATALYSIS
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2020
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IF 7.888
Jiehua Bao,Yuming Zhou,Yiwei Zhang,Yanyun Wang,Shuang Liang,Zhiwu Guo,Chang Guo,Yi Xue,Tao Zhuang,Yingjie Hu
In this study, we synthesized a series of Ni-based catalysts with different CeO 2 contents (0, 1, 2, 5 and 10 wt%) anchoring on the Al-Mg oxide spheres (AMO) with three-dimensional hollow flower-like structure. The triethoxyoctylsilane (TEOOS) and polyvinylpyrrolidone (PVP) were selected as effective modified reagents to introduce hydrophobic functionality on the surface of AMO and Ni-CeO 2 nanoparticles, respectively, for controllable anchoring Ni-CeO 2 nanoparticles on AMO by hydrophobic interaction driving mechanism. The effects of CeO 2 content on the texture, dispersion of Ni species, the reducibility of Ni 2+ , surface electronic states and acidity were investigated in detail. The Ni-5CeO 2 /AMO was found to achieve the highest 2,2′-bipyridine selectivity of 90.6% and maximum turnover number (TON) of 8611, specifically. Moreover, the Ni-5CeO 2 /AMO exhibits superior stability, maintaining 89% of 2,2′-bipyridine yield after 6 runs, due to the mitigated nickel leaching and promotion of the desorption of 2,2′-bipyridine. Furthermore, with the help of DFT calculations, a possible reaction mechanism was discussed and illustrated.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Dexuan Pei,Ziying Liu,Rui Ma,Shuo Huang,Shuen Hou,Min Liu,Guozhong Cao,Hongyun Jin
Composite polymer electrolytes (CPEs) have shown extraordinary promise for use in all-solid-state lithium metal batteries (LMBs) because of their tunable merits in ionic conductivity and mechanical flexibility. Their practical application is however hindered by the poor interface stability and the uncontrollable Li dendrite formation. Addressing these two issues, we report an in-situ formed Li-Al-O interface layer between CPEs and Li metal anode by introducing Al 2 O 3 nanoparticles in CPEs. X-ray photoelectron spectroscopy results indicated that the CPE-Al 2 O 3 could slowly release Al atoms which react with Li metal to form the current Li-Al-O interface layer. We highlight that the Li-Al-O interface layer can stabilize lithium deposition/stripping over 1400 h in lithium symmetric batteries, and afford an impressive cycle life of 300 cycles in LiFePO 4 -Li batteries with almost no capacity loss. The present findings demonstrate that in-situ constructing a slow-release Li-Al-O interface layer is an easy and effective approach to stabilize the solid electrolyte interface and suppress the Li dendrites growth. Furthermore, the obtained batteries show excellent cycling stability, indicating the strategy with in-situ formed CPEs shed light on improving the processability of fabrication of high-performance electrolytes.
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ACS Applied Materials & Interfaces
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2020
·
IF 8.758
Junxiang Wang,Handong Jiao,Wei-Li Song,Mingyong Wang,Jiguo Tu,Zhongfeng Tang,Hongmin Zhu
Intermediate temperature NaCl–AlCl3-based Al-ion batteries are considered as a promising stationary energy storage system due to their low cost, high safety, etc. However, such a cheap electrolyte has a critical feature, i.e., strong corrosion, which results in the short cycle life of the conventional Al-metal anode and also limits the development of the NaCl–AlCl3-based Al-ion batteries. A noncorrosive electrolyte may be a good choice for addressing the above challenge, while it is difficult to obtain the electrolyte that has advantages of both noncorrosion and low cost. Therefore, here, we report a Ga-metal anode in the affordable NaCl–AlCl3 electrolyte for constructing a long-life stationary Al-ion energy storage system. This featured liquid metal anode shows good alloying and dealloying processes between metallic Ga and Al, as well as renders superior stability of the interface between the electrolyte and the anode (e.g., smoothly running for over 580 h at 2 mA cm–2). No-corrosion and no-pulverization problems appear in this novel liquid/liquid interface. Those advantages demonstrate that the liquid Ga-metal anode has a great promise for the improvement of the NaCl–AlCl3-based Al-ion batteries for large-scale stationary energy storage applications.
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高影响因子
RESOURCES CONSERVATION AND RECYCLING
·
2025
·
IF 10.9
Fei Han,Yaohui Xie,Lin Qu,Zhenzhou Wang,Wei Zhang,Guang Yang,Huiqin Hu,Meiting Huang,Haoxuan Yu,Liming Yang,Xubiao Luo
Deep removal of trace aluminum from lithium extraction slag (LES) is key to recovering high-purity battery-grade iron phosphate (FePO 4 ). Existing methods exhibit low aluminum removal due to the close solubility product constants of Al (III) and Fe (III). In this work, we propose a novel strategy for trace aluminum removal based on fluoride ion-mediated differential coordination of Al (III) and Fe (III). Through precise control of fluoride ion concentration in phosphoric acid solution, iron preferentially precipitates while aluminum predominantly forms soluble fluoride complexes. This distinct behavior enables precise elemental separation through fluoride content optimization. The developed separation technology achieved aluminum removal rate of 98.89 %. It is noteworthy that the aluminum content of precipitated FePO 4 is below 30 ppm, which meets the standard of battery-grade. This work provides a viable technical pathway for the industrialization of Al/Fe separation in the lithium extraction slag leachate and the regeneration of low-Al, high-purity FePO 4 .
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NEW JOURNAL OF CHEMISTRY
·
2017
·Vol. 41
·期 10
·4031-4039
·
IF 3.269
Xiaofei Song,Jianmin Hao,Yijia Bai,Limin Han,Guangfei Yan,Xu Lian,Jiansheng Liu
Al–Cu–Co alloys containing different intermetallic compound phases were fabricated by the arc-melting method and used as heterogeneous catalysts for solvent-free cyclohexane oxidation by oxygen. The element composition and bulk structure were characterized by ICP-OES, XRD, SEM, TEM and XPS. Co species were the major active component and a small amount of Cu dissolved in the Al13Co4 phase of the alloy exhibited a synergetic effect on improving the catalytic activity. Cu dissolved in the Al13Co4 phase, a decagonal quasicrystal approximant with a special atomic arrangement structure, could increase the electrical conductivity and accelerate electron transfer during the catalytic oxidation of cyclohexane, and thus improved the catalytic activity of the alloy. Among all the alloys prepared in the present work, the Al60Cu5Co35 alloy exhibited the best catalytic performance with a cyclohexane conversion of 6.4% and a total selectivity of 95.2% to cyclohexanol and cyclohexanone. No significant change in the catalytic activity of the Al60Cu5Co35 alloy was observed after five cycles.
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ANALYST
·
2014
·Vol. 139
·期 18
·4613-4619
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IF 3.906
Dan Zhang,Ai Gao,Yang Xu,Xue-Bo Yin,Xi-Wen He,Yu-Kui Zhang
Mesoporous silica nanoparticles (MSNs) were co-doped with Gd3+ and Al3+ and then loaded with Ru(bpy)32+ by ion-exchange to prepare Ru/Gd–Al@MSNs. The as-prepared Ru/Gd–Al@MSNs were applied as contrast agents for in vivo fluorescence and magnetic resonance (MR) dual-modality imaging with a mouse as a model. The effects of Al3+ and MSNs on longitudinal relaxivity (r1) and fluorescence were investigated using a series of Gd-containing silica nanoparticles, including Gd@MSNs, Gd–Al@MSNs, and Ru/Gd–Al@nonporous silica nanoparticles. Co-doping with Al3+ improved the loading of Gd3+; the mesoporous structure improved the water exchange rate. The improvement enhanced the MR imaging efficiency of the Ru/Gd–Al@MSN probe. A higher relaxivity (19.2 mM−1 s−1) was observed compared to that from a commercial contrast agent, Gd-diethylene triamine pentaacetic acid (Gd-DTPA). Importantly, the mesoporous structure provided a large specific surface area for the loading of Ru(bpy)32+ by a simple ion-exchange procedure. Intense red fluorescence was observed from Ru/Gd–Al@MSN probes. The versatility of Ru/Gd–Al@MSNs for dual-modality imaging was demonstrated using in vivo fluorescence imaging and T1-weighted MR imaging with a mouse model. The nanoparticles are biocompatible and may be attractive for clinical applications.
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