INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Xian-Yu Shen,Ya-Nan Wang,Ya-Ting Zheng,Ye Wang,Wen-Wen Dong,Jun Zhao,Dong-Sheng Li
Formaldehyde (HCHO), a crucial industrial chemical, finds extensive applications across diverse sectors, including household products, commercial materials, aviation, and medical supplies. Methane (CH4), as an abundant C1 resource, presents a promising feedstock for HCHO synthesis. However, the direct conversion of CH4 to HCHO remains challenging due to its inherent chemical inertness, characterized by low polarizability and high C–H bond dissociation energy (439 kJ mol–1), coupled with the high reactivity of intermediate products. The development of efficient strategies for selective CH4 oxidation to high-value HCHO under mild conditions is therefore of significant practical importance. In this study, we developed a series of MIL-125-NH2@FeOOH-x heterostructured photocatalysts (FM-x) through the controlled deposition of FeOOH nanoparticles on MIL-125-NH2 surfaces. Comprehensive characterization and photocatalytic evaluations reveal that the optimized FM-1 catalyst facilitates in situ H2O2 generation and subsequent decomposition into hydroxyl radicals (•OH), enabling efficient CH4 photooxidation. Remarkably, the FM-1 catalyst achieves an exceptional HCHO production rate of 197.79 μmol·gcat–1 with >99.99% selectivity in water vapor, significantly outperforming both pristine FeOOH and MIL-125-NH2 components. This work presents a promising photocatalytic system for selective CH4 conversion, offering new insights into the design of efficient catalysts for C1 chemistry.
研究领域:
化学工程
·
材料科学
·
环境科学
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DOI
PubMed
高影响因子
BIOTECHNOLOGY AND BIOPROCESS ENGINEERING
·
2022
·Vol. 27
·期 1
·135-144
·
IF 3.386
Wang Zichen,Liu Yang,Li Jinhong,Meng Guoqing,Zhu Daoyu,Cui Jiandong,Jia Shiru
As a series of metal organic framework (MOFs), materials of institute lavoisier frameworks (MILs) are expected to be excellent supports for enzyme immobilization due to their good water-stability and acid tolerance. However, enzyme loading on MIL-125-NH 2 is very low due to small pore size and few amino groups on the surface of the MIL-125-NH 2 . In this work, catalase (CAT) was immobilized on the MIL-125-NH 2 and amino functionalized MIL-125-NH 2 by adsorption (CAT@MIL-125-NH 2 ) and covalent binding (CAT@Amino MIL-125-NH 2 ), respectively. Compared with the CAT@MIL-125-NH 2 and free CAT, the CAT@Amino MIL-125-NH 2 displayed high activity recovery, good pH stability, stability against denaturants, and thermostability. Furthermore, activity recovery of CAT@Amino MIL-125-NH 2 was 56% higher than CAT@MIL-125-NH 2 . The CAT@Amino MIL-125-NH 2 still retained 50% residual activity for 14 days at room temperature, whereas free CAT lost activity after storage for 1 day at the same storage conditions. Furthermore, the CAT@Amino MIL-125-NH 2 maintained 62% of its initial activity after 4 consecutive uses, showing good reusability. The results showed that the amino functionalized MIL-125-NH 2 is an excellent carrier of enzyme immobilization.
研究领域:
生物化学
·
材料科学
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DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2022
·
IF 8.025
Shichen Wang,Yixuan Liu,Yue Hu,Weibo Shen
Metal-organic frameworks (MOFs) are gradually used since of their huge specific surface area and superior pore structure. However, there are problems such as easy aggregation and difficult separation in water treatment. In this study, we prepared composite microspheres (FMCS-1) by modifying MIL-125-NH 2 with Fe 3 O 4 and chitosan. The structural characterization and performance analysis of the materials showed that the introduction of chitosan effectively prevents the stacking of MOFs. The magnetic test manifested that Fe 3 O 4 solved the problem of the difficult separation of MOFs from water. The removal potential of toxic Cr(VI) was tested by adsorption experiments. The isotherm model indicated that FMCS-1 is a single molecular layer adsorbent with a maximum adsorption capacity of 109.46 mg/g at pH = 2. The adsorption kinetics showed that the adsorption of Cr(VI) by FMCS-1 was chemical adsorption. The acid resistance test demonstrated that FMCS-1 can exist stably in acid solutions. The recycling experiments proved that the adsorbent can be reused and the removal percentage still reaches 50 % after 5 cycles. This work expands the application of MOFs in water treatment and also provides an effective adsorbent for Cr(VI) removal.
研究领域:
环境科学
·
材料科学
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DOI
PubMed
高影响因子
BIOSENSORS & BIOELECTRONICS
·
2024
·
IF 10.7
Yajun Gao,Suhui Xu,Ge Guo,Yajie Li,Wenyuan Zhou,Huaxiang Li,Zhenquan Yang
Herein, novel nanozyme mimics MoO 3 /MIL-125-NH 2 were reported and conjugated with bacteriophages as a new electrochemical probe for high sensitivity and specific electrochemical detection of staphylococcus aureus . The excellent peroxidase-like activity of MoO 3 /MIL-125-NH 2 composites was attributed to the integration of MIL-125-NH 2 with MoO 3 , which can boost the generation of superoxide radicals (O• 2 – ) and thus promote the oxidation of TMB in the presence of H 2 O 2 . In this work, two bacteriophages named SapYZU04 and SapYZU10 were isolated from sewage samples by using staphylococcus aureus YZUsa12 as the host. In comparison, MoO 3 /MIL-125-NH 2 @SapYZU04 was selected as a recognition agent. The DPV current declined linearly with staphylococcus aureus YZUsa12 concentration in the range of 10 1 −10 8 CFU mL −1 , with a low detection limit of 16 CFU mL −1 (S/N = 3). 20 strains including 13 host strains and 7 non-host strains were used to evaluate the selectivity of the proposed sensor. Regardless of the differences in the degrees of lytic performance for phage SapYZU04, all selected host strains can be screened with merely the same DPV current. Host spectrum-oriented bacteriophage sensing is of great importance for the practical application of bacteriophage-based biosensors in the future.
研究领域:
生物传感
·
电化学检测
·
微生物学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xiaran Su,Yuming Dong,Yongfa Zhu,Haifeng Shi
Polyethylene terephthalate plastic is widely used and poses challenges in degradation, highlighting the importance of finding efficient degradation methods. In this study, MIL-125-NH 2 /BNQDs composites were synthesized to degrade polyethylene terephthalate plastic in the peroxymonosulfate-activated persistent photocatalysis system. The results showed that MIL-125-NH 2 /2BNQDs exhibited the best degradation effect on polyethylene terephthalate plastic activated by peroxymonosulfate under light conditions, with a degradation efficiency of 95.71 % achieved by adding 3 mM peroxymonosulfate, which was 3.01 times that of MIL-125-NH 2 alone. Furthermore, all composite samples retained persistent catalytic activity under dark conditions after light irradiation. After visible light irradiation, the polyethylene terephthalate degradation efficiency achieved 90.23 % when MIL-125-NH 2 /2BNQDs activated by peroxymonosulfate were used under dark conditions. The mechanism of action of reactive radicals in the polyethylene terephthalate degradation process was revealed by scavenger experiments. In-situ X-ray photoelectron spectroscopy analysis demonstrated that MIL-125-NH 2 /2BNQDs induce Ti 4+ to Ti 3+ transition through electron transfer, resulting in higher efficiency of peroxymonosulfate activation. The composites achieve improved electron storage capacity and enhanced peroxymonosulfate activation efficiency. Furthermore, the alteration of valence in transition metals (from Ti 4+ to Ti 3+ ) triggers photochromism, which amplifies the ability to absorb light. This study provides new insights for the development of novel photocatalysts for environmentally friendly degradation of polyethylene terephthalate plastics, contributing to the removal of plastic waste and the promotion of resource sustainability.
研究领域:
环境科学
·
材料科学
·
催化化学
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DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2019
·
IF 1.795
Yu Guo,Jie Li,Xuanxuan Yang,Yongbing Lou,Jinxi Chen
Hydrogen production by photocatalysis under visible light irradiation is a pivotal means of obtaining hydrogen. In this study, Zn 0.5 Cd 0.5 S was studied to have optimal hydrogen production performance among different zinc-cadmium ratios of Zn x Cd 1-x S, and a series of Zn 0.5 Cd 0.5 S/MIL-125-NH 2 (Ti) composites with different MIL-125-NH 2 (Ti) contents were prepared by simple ultrasonic method. When the percentage of addition of MIL-125-NH 2 (Ti) was 40%, the optimum hydrogen production rate was 92,498 μmol h −1 g −1 , and the photocatalytic activity was still stable even after 16 h. The mechanism investigations demonstrated that this excellent activity was owing to enhanced visible light absorption intensity, extremely efficient electron transfer and proper conduction band position. This work provides new insights into highly efficient and stable photocatalyst in hydrogen production from water without noble metal doping.
研究领域:
材料科学
·
化学
·
能源
·
纳米技术
·
光催化
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yisha Zheng,Shuoling Lei,Wenjie Guo,Wenlong Xiang,Yanmei Chen,Yanhui Zhang
The high toxicity and persistence of nitroaromatic pollutants pose a serious threat to aquatic ecosystems. In this study, inert SiO 2 was employed as an "inactive enhancer" to construct core-shell MIL-125-NH 2 @ZIF-67/SiO 2 (M@Z/SiO 2 ) heterogeneous MOF catalysts via an epitaxial-wet impregnation method, enabling the efficient reduction of p -nitrophenol ( p -NP) under ambient temperature and pressure. Although SiO 2 itself lacks catalytic activity, the micro-mesoporous network it forms effectively disperses Co active sites and prevents their aggregation. The conversion rate of p -NP increased from 92.5% to 98.4% within 6 min and retained 98% activity after three consecutive cycles. Moreover, the catalyst exhibited excellent stability across a wide pH range (3-11) and in various anionic environments. Mechanistic studies revealed that the interfacial electron transfer between ZIF-67 and MIL-125-NH 2 significantly reduces the activation energy barrier of NaBH 4 . Additionally, the incorporation of SiO 2 not only enhances the mechanical stability of the composite but also optimizes pore structure and substrate mass transfer by modulating surface hydrophilicity. This work provides valuable insights for the precise design of MOF-on-MOF heterostructures and the synergistic engineering of interfacial and surface properties in environmental catalytic materials.
研究领域:
环境科学
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催化
·
材料化学
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纳米技术
·
化学工程
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产品关联
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2023
·
IF 3.3
Jiehong Chen,Yan Li,Gangfeng Liang,Na Ma,Wei Dai
The microcrystalline powders of metal-organic frameworks (MOFs) are usually difficult to be separated and reused, restricting their applications for cadmium ions (Cd(II)) removal from water. Thus, it is imperative to develop the magnetic adsorbents with high adsorption performances and excellent recoverability. Herein, a novel type of magnetic dual MOFs composite for Cd(II) capture has been successfully synthesized with (ZIF-67)-on-(PMA@MIL-125-NH 2 ) as the adsorption mainstay and Fe 3 O 4 nanoparticle as the magnetic component. The advantages of the combination and its synergistic effect are achieved through the self-assembly process. Owing to the associate effect of abundant adsorption sites and high porosity, (ZIF-67)-on-(PMA@MIL-125-NH 2 @Fe 3 O 4 ) exhibits a significant adsorption capacity (152 mg g −1 ) and rapid adsorption rate (20 min) towards Cd(II). The adsorption data are well fitted by the Freundlich and pseudo-second-order kinetic models. The adsorption mechanism involves the critical contributions of π-π interaction, Lewis's acid-base, surface adsorption, electrostatic attraction, etc. Moreover, the adsorbent could be easy obtained from liquid through Fe 3 O 4 magnetism , exhibiting a good reusability. This work provides a new perspective on the synthesis of high-efficiency adsorbents for the Cd(II) capture from water.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
MATERIALS RESEARCH BULLETIN
·
2019
·
IF 3.355
Jianhao Qiu,Lvye Yang,Ming Li,Jianfeng Yao
Metal nanoparticles (NPs) decorated MOFs for photocatalysis has drawn enormous attention in the past decade. Here, a series of M/Ti-MOFs (M = Pt and Au, Ti-MOFs = MIL-125-NH 2 and MIL-125) has been synthesized through a facile post-synthetic method and the metal NPs highly dispersed on surface of MOFs with major sizes of 3–9 nm. Light absorption edges of scaffolds are crucial in the photocatalytic oxidation of benzyl alcohol over M/MIL-125-NH 2 and M/MIL-125. The conversion of benzyl alcohol over Pt/MIL-125-NH 2 is 2.4 times and 1.9 times higher than that of pristine MIL-125-NH 2 and Au/MIL-125-NH 2 , respectively. Besides, Pt/MIL-125-NH 2 photocatalyst also exhibited good activity for Cr(VI) reduction compared to that of MIL-125-NH 2 . The enhanced photocatalytic activity of Pt/MIL-125-NH 2 is contributed to the rapid transfer of photo-induced electrons and decreased recombination of electron-hole pairs, which is verified by measurements of photocurrent and Electrochemical Impedance Spectroscopy. We hope that this study will provide worthy information for designing metal/MOFs or metal/MOFs-NH 2 photocatalysts.
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DOI
高影响因子
Advanced Science
·
2024
·Vol. 11
·期 11
·2308623
·
IF 14.3
Chen-Han Guo,Feng-Fan Lu,Enyu Wu,Jia-Xin Wang,Defa Gu,Bin Li,Guodong Qian
The green water-based adsorption refrigeration is considered as a promising strategy to realize near-zero-carbon cooling applications. Although many metal-organic frameworks (MOFs) have been developed as water adsorbents, their cooling performance are commonly limited by the insufficient water uptakes below P / P 0 = 0.2. Herein, the development of multivariate MOFs (MTV-MOFs) is reported to highly modulate and boost the low-pressure water uptake for improving coefficient of performance (COP) for refrigeration. Through ligand exchange in the pristine MIL-125-NH 2 , a series of MTV-MOFs with bare nitrogen sites are designed and synthesized. The resulting MIL-125-NH 2 /MD-5% exhibits the significantly improved water uptake of 0.39 g g −1 at 298 K and P / P 0 = 0.2, which is three times higher than MIL-125-NH 2 (0.12 g g −1 ) and comparable to some benchmark materials including KMF-1 (0.4 g g −1 ) and MIP-200 (0.36 g g −1 ). Combined with its low-temperature regeneration, fast sorption kinetics and high stability, MIL-125-NH 2 /MD-5% achieves one of the highest COP values (0.8) and working capacities (0.24 g g −1 ) for refrig-2 under an ultralow-driven temperature of 65 °C, which are higher than some best-performing MOFs such as MIP-200 (0.74 and 0.11 g g −1 ) and KMF-2 (0.62 and 0.16 g g −1 ), making it among the best adsorbents for efficient ultralow-temperature-driven refrigeration.
研究领域:
材料科学
·
环境工程
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DOI
PubMed
高影响因子
ACS ES&T Engineering
·
2026
·
IF 6.3
Shen Xiaotie,Li Ruiyi,Chen Baoliang,Zhu Xiaoying
The degradation of perfluorooctanoic acid (PFOA) remained
challenging
due to the extraordinary stability of its carbon–fluorine bonds,
which were resistant to conventional photocatalytic processes. In
this work, a metal–organic framework (MOF), MIL-125-NH 2 , was grown in situ on reduced graphene oxide (rGO) to form
nanocomposites (RMGs), enabling rapid PFOA degradation via an integrated
dual-redox pathway without the addition of sacrificial agents. Under
UV irradiation, the RMG composite achieved an 80.2% degradation of
PFOA (20 mg L –1 ) within 4 h, corresponding to an
apparent rate constant of 0.405 h –1 , and exhibited
competitive degradation productivity among reported photocatalytic
systems operating without external oxidants or sacrificial agents.
PFOA degradation exhibited pronounced pH dependence with the RMG composite
delivering optimal performance at pH 5. Moreover, the RMG catalyst
showed excellent stability and reusability. In natural water matrices,
the RMG composite achieved approximately 70% PFOA degradation within
10 h. The MOF/rGO heterojunction promoted directional charge separation,
enabling photogenerated holes to trigger carbon–carbon bond
cleavage and stepwise shortening of perfluorinated intermediates,
while electrons were efficiently transferred to PFOA to induce hydrogen–fluorine
atom exchange. Overall, this study highlights the pivotal role of
synergistic redox integration in enabling efficient PFOA remediation
in aqueous systems.
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高影响因子
Surfaces and Interfaces
·
2024
·
IF 5.7
Jiaqi Ma,Linkun Fan,Xusheng Wang,Lan Li,Yiming Zhang,Guixia Zhao,Bo Chai,Junkuo Gao
Cr(VI) stands as a profoundly toxic chemical and photocatalysis technology has shown promising potential in photocatalytic reduction of Cr(VI) to Cr(III), where the reduced Cr(III) is less toxic and can be further precipitated in a wide pH range. Metal-organic frameworks (MOFs), as emerging class of porous coordination polymers, is expected to be ideal platform for photocatalysis. In this study, defect engineering on MOFs was applied to promote photoreduction of Cr(VI). The obtained oxygen vacancy-containing MIL-125-NH 2 samples showed modified electron structure, adjusted surface and porous properties, and enriched active sites. Among these oxygen vacancy-containing MIL-125-NH 2 samples, the 300-M (MIL-125-NH 2 heated at 300 °C for 2 h under N 2 atmosphere) displayed the most remarkable performance in terms of photocatalytic Cr(VI) reduction. The pronounced efficacy of 300-M is evident from the achieved removal rate of Cr (VI), reaching an impressive 98 % in just 20 mins (19.6 mg Cr(VI) g −1 cata min −1 ), in stark contrast to MIL-125-NH 2 , which exhibited a modest removal rate of 53 %. Remarkably, the k-value for 300-M is 5.1 times that of MIL-125-NH 2 , further underscoring the superior efficiency of 300-M. The photoreduction mechanism of 300-M was further substantiated through a battery of advanced characterization techniques including transient photocurrent, electrochemical impedance spectroscopy, fluorescence spectroscopy, the Mott-Schottky analysis, and electron spin resonance. Those results disclosed that oxygen vacancies and mesopores introduced via controlled heat treatment play a pivotal role in facilitating the photoreduction of Cr(VI) within the MIL-125-NH 2 structure. More advanced characterizations for the structures of photocatalysts and the photocatalytic mechanisms including charge transfer path need further studied. The systematic exploration of temperature-dependent effects on material properties opens avenues for future research in designing efficient and versatile MOF-based photocatalysts for environmental remediation applications.
研究领域:
材料科学
·
环境科学
·
化学工程
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DOI
高影响因子
危险品化学品经营许可证（带存储）