JOURNAL OF SOLID STATE CHEMISTRY
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2025
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IF 3.5
Tongxin Xiao,Kangyue Qiao,Guodong Hao,Songyao Du,Yue Wang,Chao Sui
This study employed a solvothermal method to prepare an NH 2 -MIL-101(Fe, Co) bimetallic organic framework composite catalyst aimed at enhancing the photocatalytic reduction performance of Cr(VI). The experimental results show that introducing Co into the single-metal NH 2 -MIL-101(Fe) does not alter the material's octahedral structure. However, the bimetallic synergistic effect shifts the light absorption range to the red end of the spectrum, reduces the bandgap, and significantly improves carrier separation efficiency. Under visible light irradiation, the NH 2 -MIL-101(Fe, 0.15Co) catalyst exhibited outstanding photocatalytic performance, achieving a reduction efficiency of 94.7% for Cr(VI) within 40 minutes and 100% within 50 minutes, with a reaction rate constant 4.7 times that of the single-metal NH 2 -MIL-101(Fe). Free radical capture experiments further revealed that ·O 2 - is the key active species in the Cr(VI) reduction process, while photo-generated holes in the valence band can oxidise OH - to ·OH, synergistically participating in the reaction. Additionally, cyclic stability experiments showed that the catalyst maintained 85.8% reduction efficiency after five cycles, demonstrating excellent stability and practical application potential.
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INORGANIC CHEMISTRY
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2024
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IF 4.3
Huijiao Wang,Gening Du,Jinzhi Jia,Junfeng Huang,Mudong Tu,Jinhua Zhang,Yong Peng,Hua Li,Cailing Xu
The Electrochemical reduction of nitrate to ammonia (NH3) is a process of great significance to energy utilization and environmental protection. However, it suffers from sluggish multielectron/proton-involved steps involving coupling reactions between different reaction intermediates and active hydrogen species (Hads) produced by water decomposition. In this study, a Ru-doped NiFe-MIL-53 (NiFeRu-MIL-53) supported on Ni foam (NF) has been designed for the nitrate reduction reaction (NO3RR). The NiFeRu-MIL-53 exhibits excellent NO3RR activity with a maximum Faradaic efficiency (FE) of 100% at −0.4 V vs. RHE for NH3 and a maximum NH3 yield of 62.39 mg h–1 cm–2 at −0.7 V vs. RHE in alkaline media. This excellent performance for the NO3RR is attributed to a strong synergistic effect between Ru and reconstructed NiFe(OH)2. Additionally, the doped Ru facilitates water dissociation, leading to an appropriate supply of Hads required for N species hydrogenation during NO3RR, thereby further enhancing its performance. Furthermore, in situ Raman analysis reveals that incorporating Ru facilitates the reconstruction of MOFs and promotes the formation of hydroxide active species during the NO3RR process. This work provides a valuable strategy for designing electrocatalysts to improve the efficiency of the reduction of electrochemical nitrate to ammonia.
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RSC Advances
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2024
·Vol. 14
·期 8
·5142-5148
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IF 3.9
Chunhong Jin,Jingchao Liu,Yilin Yin,Zenghe Li
In wastewater containing heavy metals, Cr(VI) is a potentially toxic metal, mainly derived from production and processing processes such as textile printing, dyeing, ore mining, battery applications, metal cleaning and electroplating. WO3 is widely used in photocatalytic degradation and reduction, and its utilization rate of visible light is high. However, the rapid recombination of photogenerated electron–hole pairs of WO3 limits its use. In this work, the composite material (WxMy) of WO3 and MIL-125 (Ti) was prepared by the ball milling method, and the catalyst was used to photocatalytically reduce Cr(VI). After using W90M10 as a photocatalyst for 50 min, the reduction rate of Cr(VI) can reach 99.2%, and the reduction rate is 2.3 times that of WO3. After 5 cycles of use, the reduction rate can still reach 91.3%. It is mainly due to the formation of a II-type heterojunction between WO3 and MIL-125 (Ti), which promotes the separation of photogenerated electron–hole pairs, thus improving the efficiency of photocatalytic reduction of Cr(VI).
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yong Tang,Jianhao Qiu,Dingliang Dai,Guanglu Xia,Biyao Fang,Yixin Li,Jianfeng Yao
Defect engineering is used in the development of photocatalysts and has received widespread attention for achieving efficient photocatalysis. Here, ZnIn 2 S 4 with rich sulfur vacancies (V S -ZnIn 2 S 4 ) was integrated with MIL-53-NH 2 for photocatalytic H 2 O 2 production from O 2 reduction under visible light. The sulfur vacancy could effectively promote charge separation and O 2 capture, and the heterostructure between ZnIn 2 S 4 and MIL-53-NH 2 further inhibits charge recombination, which promises highly boosted photocatalytic activities. In ambient air and pure water, V S -ZnIn 2 S 4 /MIL-53-NH 2 heterostructures exhibit superior photocatalytic H 2 O 2 production performance (705 μmol·L −1 ) relative to those of monomeric Znln 2 S 4 (78 μmol·L −1 ), V S -Znln 2 S 4 (210 μmol·L −1 ), MIL-53-NH 2 (38 μmol·L −1 ), as well as ZnIn 2 S 4 /MIL-53-NH 2 (395 μmol·L −1 ). Mechanistic studies have confirmed that the main pathway for H 2 O 2 formation on V S -ZnIn 2 S 4 /MIL-53-NH 2 is ⋅O 2 – -triggered O 2 reduction, and sulfur vacancy can adsorb and activate O 2 to facilitate the production of ⋅O 2 – . This study provides new insights into catalyst design and green synthesis of H 2 O 2 .
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Carbon Energy
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2025
·
IF 24.2
Ze Liu,Kaiyong Feng,Fengjun Deng,Xiaochen Zhang,Jiangchang Chen,Yingjian Yu
Silicon–air (Si–air) batteries have received significant attention owing to their high theoretical energy density and safety profile. However, the actual energy density of the Si–air battery remains significantly lower than the theoretical value, primarily due to corrosion issues and passivation. This study used various metal–organic framework (MOF) materials, such as MIL-53(Al), MIL-88(Fe), and MIL-101(Cr), to modify Si anodes. The MOFs were fabricated to have different morphologies, particle sizes, and pore sizes by altering their central metal nodes and ligands. This approach aimed to modulate the adsorption behavior of H 2 O, SiO 2 , and OH − , thereby mitigating corrosion and passivation reactions. Under a constant current of 150 μA, Si–air batteries with MIL-53(Al)@Si, MIL-88(Fe)@Si, and MIL-101(Cr)@Si as anodes demonstrated lifetimes of 293, 412, and 336 h, respectively, surpassing the 276 h observed with pristine silicon anodes. Among these composite anodes, MIL-88(Fe)@Si displayed the best performance due to its superior hydrophobicity and optimal pore size, which enhance OH − migration. This study offers a promising strategy for enhancing Si–air battery performance by developing an anodic protective layer with selective screening properties.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2025
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IF 4.7
Jian Luo,Yonghui Lin,Yanfeng Liu,Siliang Wang,Yiduo Chen,Xudong Tian,Weiting Yang,Zhongmin Su
Roxarsone (3-nitro-4-hydroxyphenylarsenic acid, ROX) is easily converted into highly toxic inorganic arsenic compounds, therefore, the development of highly efficient adsorbents for the removal of ROX from wastewater is necessary but remains challenging. In this study, NH 2 -MIL-101 (Fe) was synthesised and modified with TPA-CHO (4-(N, N-diphenylamine) benzaldehyde) to obtain TPA-MIL-101(Fe) with triphenylamine functionalised groups. The modified TPA-MIL-101(Fe) exhibits the very high adsorption capacity (728.2 mg g −1 ) and fast adsorption equilibrium (2 h). The TPA-MIL-101(Fe) showed excellent selectivity, and the adsorption efficiency hardly decreased in the presence of competing ions (Cl − , NO 3 − , SO 4 2− ). The TPA-MIL-101(Fe) showed good adsorption performance for ROX at pH 3–13, with the best performance at pH = 9. In addition, TPA-MIL-101(Fe) was able to remove trace amounts of ROX from actual water samples (<5 mg L −1 ) with an efficiency of 99.46 %, and the remaining ROX content meets the international drinking water standards of the World Health Organization (29 μg L −1 ). The mechanism studies have shown that the Fe-O-As coordination and the π-π stacking interaction between TPA-MIL-101(Fe) and ROX greatly enhance its adsorption performance. In conclusion, this work provides a promising material for effective removal of ROX from the environmental water.
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LANGMUIR
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2025
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IF 3.9
Mingyang Xiong,Yao Zeng,Ruisi Qiu,Hongxing He,Yi Zhang,Zhifeng Nie,Bing Wang
Bisphenol A (BPA) is extensively utilized as an industrial chemical in the production of certain plastics and epoxy resins. They are frequently found in environmental water and have the potential to cause risks to both the environment and human health. To efficiently remove the endocrine disruptor BPA from aqueous solutions, sea urchin-like magnetic material Fe3O4@PDA@NH2-MIL-101 (Fe) was synthesized via hydrothermal methods. Fe3O4@PDA@NH2-MIL-101 (Fe) has excellent adsorption performance, with a theoretical maximum adsorption capacity of 300.47 mg/g for BPA. The adsorption kinetics of BPA by Fe3O4@PDA@NH2-MIL-101 (Fe) followed the pseudo-second-order kinetic model and Liu’s isotherm model. Magnetic separation experiments reveal a high recovery efficiency, maintaining 94.82% of its initial adsorption capacity after five cycles. The primary adsorption mechanisms of Fe3O4@PDA@NH2-MIL-101 (Fe) on BPA included pore filling, hydrogen bonding, π–π interaction, and Lewis acid–base interaction. Additionally, the material showed excellent removal performance of BPA, with a maximum adsorbed amount of 135.27 mg/g for total organic carbon (TOC) in the shale gas fracturing flowback fluid. These findings suggest that Fe3O4@PDA@NH2-MIL-101 (Fe) holds significant potential as an adsorbent for BPA removal from actual wastewater, offering promising prospects for practical applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
IF 9
Xin-Ru Chen,Heng Mao,Qiu-Ying Zhang,Wei-Min Liu,Shen-Hui Li,Qian-Qian Li,Li-Hao Xu,Yan-Mei Zhang,Xin-Yue Zhang,Jun-Jie Liu,Ao Kou,Zhi-Ping Zhao
Interfacial engineering in mixed matrix membranes (MMMs) is essential to attain superior separation performance and ensure long-term operational stability. In this research, a range of novel MMMs were designed and fabricated for pervaporation (PV) separation of n-butanol/water solution by introducing the MIL-53(Al) particles and three variants (i.e., MIL-53(Al)–NH 2 , MIL-53(Al)–NO 2 , MIL-53(Al)–OH) into PEBA polymer matrix. These four MIL-53(Al) counterparts were synthesized via a microwave-assisted solvothermal method by selectively functionalizing the terephthalic acid linkers with different chemical groups. The functional MIL-53(Al) variants were employed to explore the relationship between membrane microstructures and PV performance by manipulating the interfacial interactions with PEBA matrix. The findings reveal that incorporating MIL-53(Al) variants not only displayed excellent interfacial compatibility and uniform dispersion within PEBA matrix, but also constructed the preferential transport pathways for n-butanol over water molecules. Impressively, in a 1 wt% n-butanol aqueous solution at 40 °C, the resultant membrane attained a permeation flux of 1483.3 g·m -2 ·h -1 and a separation factor of 18.1. Compared to the PEBA/PVDF membrane, the total flux was enhanced by 17.1 %, and the separation factor was improved by 46.4 %. Moreover, the embedding MIL-53(Al) variants boosted thermal and mechanical properties of the membrane, endowing it with considerable potential for practical applications.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
·
IF 5.4
Zhicong Yuan,Xuelian Chen,Xiqiang Pan,Guojuan Hai
The development of efficient electrocatalysts through heterostructure engineering is crucial for boosting the oxygen evolution reaction (OER) kinetics. Herein, we demonstrate a hierarchical MIL-53/NiCu-LDH(12) heterostructure in-situ grown on nickel foam (NF), where the MIL-53 component is controllably constructed on NiCu-LDH/NF to establish robust interfacial contact and electronic coupling. This multi-level architecture synergistically endows the catalyst with enlarged electrochemical active surface area, abundant accessible active sites, accelerated electron transfer kinetics, and reduced band gap. Remarkably, operando characterization reveals that the heterojunction undergoes partial structural reconstruction during OER to generate γ-FeOOH/γ-NiOOH active phases. The formed Fe-O-Ni bridging bonds facilitate interfacial charge redistribution, which effectively modulates the electronic configuration and optimizes reaction intermediates adsorption. Benefiting from these merits, the MIL-53/NiCu-LDH(12)/NF electrode delivers exceptional alkaline OER performance, requiring ultralow overpotentials of 160 and 226 mV to achieve current densities of 10 and 100 mA cm −2 , respectively, along with a small Tafel slope of 42 mV dec −1 . This work proposes an innovative strategy integrating hierarchical architecture design with interfacial electronic modulation for developing advanced transition metal-based OER electrocatalysts.
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JOURNAL OF MOLECULAR STRUCTURE
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2025
·
IF 4.7
Zhaobo Wang,Tao Yu,Xiaomao Liu,Jinsheng Li,Xuanwen Liu,Rui Guo
To improve the performance of MIL-100(Fe) in the photo-peroxydisulfate (photo -PDS) degradation system, this study introduced the amino-containing bidentate ligand 5-aminoisophthalic acid (AIA) to simultaneously engineer structural defects and photosensitive sites, thereby synergistically enhancing both photocatalytic activity and metal-mediated catalytic capability. This study synthesized MIL-100(Fe) materials with varying AIA incorporation levels (denoted as M-x %NH₂) and systematically investigated the effects of AIA integration on the catalyst. Degradation experiments were performed in the photo-PDS system using rhodamine B (RhB) as a model pollutant. The results demonstrate that the introduction of AIA induced multiple advantageous effects in the photo-PDS process:1.It enhanced the visible-light absorption capacity;2.Improved the separation efficiency of photogenerated charge carriers;3.Generated defects to increase metal active sites, thereby accelerating PDS activation. Among the samples, M-30 % NH₂ exhibited the optimal performance, achieving nearly complete degradation of RhB within 50 min. The pseudo-first-order rate constant (k) was three times higher than that of unmodified MIL-100(Fe). The catalyst retained approximately 90 % degradation efficiency after five consecutive cycles and demonstrated robust performance across pH 3–9, along with the capability to degrade diverse organic pollutants. Quenching experiments confirmed sulfate radicals (·SO 4 ⁻) and hydroxyl radicals (·OH) as the main active species, and the degradation pathways were elucidated. This study provides foundational insights for modifying MIL-100(Fe) and developing high-efficiency PDS catalysts.
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CARBON
·
2025
·
IF 11.6
Qin Guo,Hankun Wang,Xianhan Shao,Yingzan Zhuang,Yuhu Zhai,Xiaohan Sun,Guobin Shao,Hao Zhang,Tingxi Li,Yong Ma
The growing demands from sectors such as advanced electronic packaging and defense have made the creation of high-performance electromagnetic wave (EMW) absorbers a research and development priority. In this study, α-Fe 2 O 3 @PPy (FOP1) and Fe 3 O 4 @PPy (FCP1) composites were synthesized via controlled thermal treatment of MIL-88A under varying conditions, followed by in-situ oxidative polymerization. This synthetic strategy allows precise tuning of the composition and microstructure of the composites, thereby facilitating systematic investigation of the synergistic electromagnetic effects on microwave absorption performance. The absorption properties of FOP1 are characterized by a minimum reflection loss (RL min ) of −21.96 dB at 6.14 mm. Furthermore, a thickness of 3.19 mm yields an effective absorption bandwidth (EAB) of 2.96 GHz. The FCP1 composite exhibits markedly superior performance, achieving an RL min of −56.03 dB at 3.64 mm and an ultra-wide EAB of 6.2 GHz at a mere 2.41 mm thickness. This performance enhancement is attributed to its enhanced magnetic loss capability and significantly improved impedance matching. A substantial radar cross-section (RCS) reduction of 33.21 dB m 2 was observed in the specular reflection direction (0°), as confirmed by simulations. This result corroborates the excellent electromagnetic wave absorption performance of the material. The remarkable microwave absorption is driven by the effective integration of multiple loss mechanisms, including interfacial polarization, conductive loss, dipole polarization, and magnetic loss. The material's performance stems from the concurrent enhancement of attenuation efficiency and impedance matching enabled by this integration. This work offers valuable insights into the design of high-performance microwave absorbers through tailored electromagnetic synergy.
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RSC Advances
·
2017
·Vol. 7
·期 80
·50829-50837
·
IF 3.108
Juntao Tang,Jianlong Wang
A MIL-100(Fe)/graphene oxide (GO) composite was prepared by a one-step hydrothermal method and utilized as a heterogeneous Fenton-like catalyst for methyl orange (MO) degradation. The obtained catalyst was characterized by X-ray diffraction (XRD), field-emission scanning electron microscopy (FESEM), nitrogen adsorption–desorption isotherms, thermogravimetric (TG) analysis, X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectroscopy (FTIR). The effects of H2O2 dosage, initial pH and catalyst dosage on the degradation of MO were investigated. The MIL-100(Fe)/GO presented high catalytic activity for the degradation of MO, achieving almost complete decomposition of MO after 240 min with reaction conditions of 8 mM H2O2, pH of 3.0 and 0.5 g L−1 catalyst. Kinetics analysis showed that MO removal followed a pseudo-first-order kinetic model. The catalyst showed stable catalytic activity and reusability after three successive runs. The possible catalytic mechanism of MIL-100(Fe)/GO was also proposed.
研究领域:
环境科学
·
材料科学
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