INORGANIC CHEMISTRY COMMUNICATIONS
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2025
·
IF 5.4
Biao Li,Yuqi Liu,Baizhuang Li,Yusi He,Yufeng Zhang,Xinying Wang,Yuebin Feng,Wei Li
Tetracycline (TC) antibiotics in aquatic environments pose severe ecological and health risks due to their difficult biodegradability and environmental accumulation. Persulfate-based advanced oxidation process (PS-AOP) has been proven to be a promising method for TC degradation in wastewater treatment but requires efficient, stable catalysts. Herein, three melamine-modified POM@MOF composites WCo@C-1, WCo@C-5 and WCo@C-10 (WCo-PMOFs and melamine in mass ratios of 1:1, 1:5, and1:10, respectively) were synthesized by calcining a mixture of WCo-PMOFs and melamine, which were used as catalysts for peroxymonosulfate (PMS) activation to degrade TC efficiently. The results demonstrated that the TC degradation rate by WCo @ C-10 activated persulfate (PMS) reached 95.83 % within 2 h superior to that of WCo@C-1 and WCo@C-5 under the same experimental conditions. Notably, the WCo@C-10/PMS system exhibited exceptional cycling stability, maintaining a degradation efficiency of 83.51 % even after four consecutive cycles. The X-ray photoelectron spectroscopy (XPS) and electrochemical impedance spectroscopy (EIS) characterization results indicate that the WCo@C-10 composite material exhibits outstanding catalytic performance. This characteristic is mainly attributed to the significant improvement in the material's dispersion and its having the smallest impedance arc radius among a series of materials, which reflects a lower charge transfer resistance and excellent electrical conductivity. These characteristics synergistically promote the efficient conversion of Co(III) to Co(II). The quenching experiment combined with electron paramagnetic resonance (EPR) analysis confirmed that superoxide radicals (O 2 ·- ) and singlet oxygen ( 1 O₂) are the main reactive oxygen species in this system. This study provides a new idea for designing efficient PMS-based advanced oxidation systems.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Xin-Ran Shi,Sai-Nan Guo,Ruoxi Zhang,Biao Yang,Hua Zou,Jie-Xin Wang
Metal–organic frameworks (MOFs) have emerged as pivotal materials for the photocatalytic reduction of CO2 to CO due to their exceptionally high surface areas and abundant active sites. However, most of the currently reported MOFs are confined to micropores (<2 nm), which limits adsorption/desorption and substance transport during photocatalytic CO2 reduction reactions. Herein, hierarchically porous MOFs (HP-MOF-74) were synthesized based on the assembly of MOF-74-Ni nanoparticles with different particle sizes (21, 42, and 85 nm) using spray-drying technology. The simultaneous enhancement of CO2 adsorption performance and photoelectroactivity was achieved in HP-MOF-74 due to the additional mesoporous structure formed by the nanoparticle stacking. The HP-MOF-74 exhibits 1.14–1.38 times improvement in the CO2 adsorption capacity compared to the corresponding initial MOF-74 nanoparticles (N-MOF-74). Meanwhile, the hierarchical architecture enhances photon utilization through improved light reflections and accelerates electronic transmission via additional mesopore pathways. These synergistic advantages collectively contribute to a 1.2–2.1 times enhancement in the CO generation rates of HP-MOF-74 compared with N-MOF-74 counterparts. Particularly, HP-MOF-74–42 nm demonstrated the highest CO production rate of 6.65 μmol h–1, outperforming most reported MOF-based photocatalysts. The construction of hierarchically porous MOFs provides a new idea for the design of highly efficient CO2 reduction photocatalysts.
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GREEN CHEMISTRY
·
2025
·
IF 9.2
Mengran Lou,Ruiying Wang,Luxiang Wang,Yang Wang,Mei Wu,Shengjiao Wen,Xia Kong,Taotao Lv,Bo Ma
Hydrogen has emerged as a promising clean energy source, driving extensive research into efficient electrocatalysts for the hydrogen evolution reaction (HER). This work reports the synthesis of a self-supported Co₂P/nitrogen-doped coal-based carbon fiber catalyst (Co₂P/N-C-CFs(S-ZIF-67)) with cobalt (Co) vacancies via pyrolysis of a nanoscale metal-organic framework (NMOF) precursor. Compared to conventional ZIF-67, NMOF of S-ZIF-67 (40 nm) derives smaller Co2P (7.3 nm), simultaneously generating hierarchical porosity with increased specific surface area. More importantly, the pyrolysis of S-ZIF-67 generates Co vacancies that optimize the electronic structure and increase the active site density of catalyst. Density functional theory (DFT) calculations confirm that these Co vacancies lower the d-band center and promote electron transfer within the catalyst. Furthermore, the N-C-CFs as supporter provides both structural flexibility and tunable hydrogen adsorption Gibbs free energy (ΔGH*). Consequently, Co₂P/N-C-CFs(ZIF-67) exhibits exceptional HER performance in 0.5 M H₂SO₄, requiring only 66 mV overpotential to reach 10 mA cm⁻² current density, and demonstrates remarkable stability for 120 h at 20 mA cm⁻². Notably, it surpasses both Co₂P/N-C-CFs(ZIF-67) and commercial 20% Pt/C under high current densities. This study establishes an effective strategy for designing advanced HER catalysts through precise control of NMOF size and vacancy engineering.
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MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 10
·1-10
·
IF 5.3
Shen Yang,Chen Rou,Wang Yun,Qiu Yanjun,Zhang Yuting,Wang Xiaoli,Zhou Nandi
Hydrogen a metal–organic framework (MOF)-based ratiometric fluorescent biosensor (Uio-66-N 3 @Cy3) was developed for the determination of hydrogen sulfide (H 2 S). The sensor combines the high specificity of the H 2 S-azide reaction with the inherent self-calibration capability of MOF-based dual-emission signals for efficient detection. The biosensor operates via H 2 S-selective azide-to-amine conversion, which suppresses photoinduced electron transfer to simultaneously restore the MOF's intrinsic fluorescence while maintaining Cy3's stable fluorescence, enabling ratiometric detection. The biosensor exhibits a dual-linear response across 0.5–100 nM and 0.5–4.0 μM, with detection limits as low as 36 pM and 27 nM, respectively. Furthermore, the biosensor shows exceptional selectivity against 18 potential interferents and long-term stability (RSD < 3.5% over 14 days). Importantly, the ratiometric mechanism enables robust performance in complex food samples (beer and milk), yielding 99.74–103.00% recoveries with minimal variance. Unlike intensity-based probes, this system provides intrinsic calibration through simultaneous dual-channel detection, making it ideal for real-world applications. Our work not only delivers a superior H 2 S sensor but also establishes a generalizable platform for ratiometric detection of diverse contaminants in food systems. Graphical
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ACS Applied Polymer Materials
·
2024
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IF 4.4
Linlin Yu,Jiawei Ji,Ruoyu Chen,Qian Jia
Frequent oil spill incidents and increasing amounts of industrial wastewater pose a serious threat to the environment. The use of superhydrophobic materials to separate oil/water mixtures has attracted widespread attention. In this work, a superhydrophobic sponge based on MOF-5 was prepared to achieve efficient continuous oil–water separation and emulsion purification. HDTMS-MOF-5@PDA@MS (H-MOF-5@PDA@MS) not only exhibited superhydrophobic property (WCA = 153.8°, SA = 6.5°) but also exhibited excellent saturated adsorption capacity, with an oil adsorption capacity of 66 (petroleum ether)-168 (chloroform) g/g and oil–water separation efficiency of 99.2%. It also demonstrated efficient performance in various emulsion purification processes. Furthermore, it maintained a stable superhydrophobicity in some extreme environments. H-MOF-5@PDA@MS is expected to have wide application perspective in the fields of environmental pollution control and wastewater treatment due to its low cost, simple process, excellent oil–water separation efficiency, reusability, and environmental friendliness.
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Journal of Water Process Engineering
·
2024
·
IF 6.3
Zahira Bano,Muhammad Akram,Naveed Zafar Ali,Muhammad Usman Khan,Fengyun Wang,Linrui Li,Mingzhu Xia
In this research, a novel composite of maleic acid derived 3D porous graphene and zeolatic imidazolate framework (ZIF-67) was developed by using one step in-situ preparation method. The synergistic impact of ZIF-67 embedded on 3D porous graphene network enhances the adsorption capacity of the organic dyes (Congo Red and Methylene Blue). The obtained structured composite material possesses macroporous and mesoporous channels up to 14.42 nm with enhanced morphological stability. The resultant 3DPGZF composite exhibits the maximum adsorption capacity towards the CR (589.46 mg g −1 ) and MB (350.79 mg g −1 ), with a removal rate of 100 % within 50 min. The kinetic study and isothermal analysis showed that pseudo second-order-kinetic model and non-linear form of the Freundlich isotherm model were more fitted with adsorption data. The adsorption of CR and MB occurred spontaneously and exhibited an endothermic nature. The DFT studies and characterization after utilization of the composite demonstrated that electrostatic attractions, pi-pi interaction, pore filling and surface binding reactions were the primary forces of the sorption process. The after adsorption XPS, FTIR, TEM and XRD results revealed that the prepared composite 3DPGZF is highly stable and was successfully regenerated multiple times without deforming its internal structure and morphology.
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Nano Materials Science
·
2024
·
IF 12.6
Mirza Abdullah Rehan,Honghua Liang,Guiqiang Li
The construction of a well-defined and efficient Z-scheme heterostructure with enhanced photogenerated charge carriers and their rapid transfer is vital for realizing efficient photocatalytic hydrogen production, to achieve carbon neutrality. Herein, we study the H 2 evolution reaction by rationally constructing a hybrid Au-anchored UiO-66-NH 2 with localized surface plasmon resonance (LSPR) properties, embedded with ZnIn 2 S 4 /MoS 2 nanosheets. Interestingly, the synergistic effect of excellent heterojunction, tunes additional catalytic active sites, provides effective separation of photogenerated charges at the junction interface and establishes a dedicated microenvironment for the boosted electron transfer. Notably, the optimized hybrid photocatalyst (Au 6 @U6N) 15 /ZIS/MS 5 exhibits highly efficient H 2 generation of 58.2 mmol g −1 h −1 , which is almost 16 and 1.5 folds of the pristine ZIS and MS/U6N/ZIS, correspondingly. It has an apparent quantum efficiency of 19.6% at a wavelength of 420 nm, surpassing several reported MOF-based ZnIn 2 S 4 photocatalytic H 2 evolution activities. Significantly, this research provides insights into the design of interface-engineered plasmonic MOF with layered encapsulated heterostructures that elucidate the role of plasmonic LSPR effect and efficiently regulate the charge transfer with enhanced microchannels, hence boosting the visible-light-driven photocatalytic activity for realizing efficient green energy conversion.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2025
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IF 4.6
Yaqiong Zhang,Junping Lv,Qin Zhou,Kaile Chu,Min Li,Yayuan Li,Jie An,Zhifang Wu,Sijin Li
Ratiometric fluorescent (RF) sensors, leveraging their inherent calibration mechanism, can greatly reduce the interference of irrelevant factors and exhibits superior detection sensitivity and more attractive visual detection effects in the process of quantitative analysis. Up to now, there are few probes that can detect fluorine by the proportional fluorescence signal. Herein, we constructed a RF probe for determination of fluorine by confining self-synthesized red emitting organic small molecules 10-(diethylamino)-3-hydroxy-5,6-dihydrobenzo[ c ]xanthen-12-ium (HTD) into the microchannels and cavity structures of UiO-66-NH 2 , exhibiting two emission maxima at 428 nm and 616 nm, respectively. After introducing fluoride into the system of probe, a drastic fluorescence enhancement at 428 nm was emerged, whereas the emission peak at 616 nm underwent minor fluctuations. The probe that has been developed enables the sensitive and selective detection of fluoride ions, exhibiting excellent linear relationships in the range of 0–100 μM. The detection limit value was estimated to be 6.93 μM. This unique ratiometric luminescence behavior of probe toward fluoride resulted from the creation of hydrogen bonds between fluoride and amino groups in HTD@UiO-66-NH 2 . Notably, the probe could utilize as an effective tool for detecting fluoride in cells with high-quality results, which could have important implications for research in biology, toxicology, and related fields. Simultaneously, its corresponding portable online test strips can be easily acquired and employed for fluoride detection through visual colorimetric analysis. The proposed method offers an alternative technology for quantifying fluoride levels in real-life water samples.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Guoshu Gao,Yumeng Zhao,Peng Zhu,Haiou Liu,Xiongfu Zhang,Yu Guo,Guohui Yang
The Co-gallate MOF membrane exhibits great potential for separating MeOH/MTBE mixtures due to its regular pore size, exceptional stability, and high hydrophilicity. Nevertheless, the rapid nucleation and growth rate of the Co-gallate crystals in the synthesis solution cause poor nucleation on the substrate surface, which presents a significant challenge for the preparation of continuous Co-gallate membranes. In this study, we presented a cobalt carbonate hydroxide nanowire array (Co-NWA)-induced strategy that enabled the rapid and defect-free synthesis of tubular Co-gallate membranes within just 1 h. The presynthesized Co-NWAs on the substrate played as nucleation centers and anchoring sites, facilitating robust membrane formation. The effects of various synthesis parameters on the crystal morphology and membrane compactness were systematically examined. The optimized Co-gallate membrane demonstrated excellent pervaporation performance, with a permeation flux of 2.03 kg m–2 h–1 and a separation factor of 6711 for a 14.3/85.7 wt % MeOH/MTBE mixture, maintaining high performance for over 100 h, indicative of its remarkable long-term stability. This Co-NWA-induced synthesis strategy presents a promising approach for the industrial-scale application of Co-gallate MOF membranes and the design of other MOF membranes, thereby advancing their utility in requisite liquid separation processes.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Li Long,Xuechun Wang,Heyun Fu,Xiaolei Qu,Shourong Zheng,Zhaoyi Xu
Iron-based materials are effective for the reductive removal of the disinfection byproduct bromate in water, while the construction of highly stable and active Fe-based materials with wide pH adaptability remains greatly challenging. In this study, highly dispersed iron phosphide-decorated porous carbon (Fe2P(x)@P(z)NC-y) was prepared via the thermal hydrolysis of Fe@ZIF-8, followed by phosphorus doping (P-doping) and pyrolysis. The reduction performances of Fe2P(x)@P(z)NC-y for bromate reduction were evaluated. Characterization results showed that the Fe, P, and N elements were homogeneously distributed in the carbonaceous matrix. P-doping regulated the coordination environment of Fe atoms and enhanced the conductivity, porosity, and wettability of the carbonaceous matrix. As a result, Fe2P(x)@P(1.0)NC-950 exhibited enhanced reactivity and stability with an intrinsic reduction kinetic constant (kint) 1.53–1.85 times higher than Fe(x)@NC-950 without P-doping. Furthermore, Fe2P(0.125)@P(1.0)NC-950 displayed superior reduction efficiency and prominent stability with very low Fe leaching (4.53–22.98 μg L–1) in a wide pH range of 4.0–10.0. The used Fe2P(0.125)@P(1.0)NC-950 could be regenerated by phosphating, and the regenerated Fe2P(0.125)@P(1.0)NC-950 maintained 85% of its primary reduction activity after five reuse cycles. The study clearly demonstrates that Fe2P-decorated porous carbon can be applied as a robust and stable Fe-based material in aqueous bromate reduction.
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DESALINATION
·
2024
·
IF 8.3
Junhua Li,Zhipeng Xu,Junbin Liao,Edison Huixiang Ang,Xuanhua Chen,Junjie Mu,Jiangnan Shen
Ion selective separations play crucial roles in the fields of energy storage, pollution management, and industrial processes, etc. Ion exchange membranes (IEMs) offer promise for these separations but often lacking the required selectivity . In this work, we have developed a kind of IEM based on metal-organic frameworks (MOFs) to enhance membrane separation performance for electrodialysis (ED). Specifically, for poly(arylene ether sulfone)-based anion exchange membranes (AEMs), we introduced the modified MOFs through doping to create a transport pathway for target ions, leveraging their precise size-based separation effects. This approach significantly improves ion selectivity. Remarkably, at a current density of 2.5 mA·cm −2 , the monovalent ion selectivity (Cl − /SO 4 2− ) of PAES-UIO-66-Pyr could reach 54.26, while the monovalent ion selectivity (NO 3 − /SO 4 2− ) could reach 55.90. These enhancements may stem from the incorporation of MOF particles, which facilitate the formation of fixed-size channel structures within membrane matrix. These fixed-size channels, coupled with the hydrophobic differences between the original poly(arylene ether sulfone) polymer, created a composite channel system that significantly improved the separation performance for monovalent ions, including Cl − /SO 4 2− and NO 3 − /SO 4 2− .
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 17
·7964-7971
·
IF 2.7
Xuanhua Zhang,Chao Wang,Chao Luan,Mengyin Liao,Wenyuan Xu
Direct methanol fuel cells (DMFC) are a promising new energy source. However, the lack of high-performance and low-cost methanol oxidation electrocatalysts hinders their commercial application. Firstly, we successfully prepared NENU-5-derived molybdenum carbide material (Cu-MoC) via a co-precipitation and high-temperature carbonization method using a material composed of a copper-based metal–organic skeleton and a molybdenum-based carbide as the main body. Secondly, PtCu nano-alloy catalysts (Pt/Cu-MoC) were prepared using a unique, spontaneous single replacement reaction after metal–organic skeleton (MOF) carbonization. Through the synergistic effect between Pt and Cu and the strong interaction between Mo2C and PtCu, the electronic structure of the Pt is modified, the energy of the d-band center is reduced, electron exchange is accelerated, and catalytic activity is enhanced. Compared with a commercial Pt/C catalyst in alkaline environments, the Pt0.10/Cu-MoC catalyst has a better MOR catalytic activity (563.25 mA mgPt−1), which is 1.5 times higher than that of commercial Pt/C (376.67 mA mgPt−1). The Pt0.10/Cu-MoC catalyst has an onset potential for CO oxidation that is 16 mV lower than that of commercial Pt/C, indicating better resistance to CO poisoning. Exploring carbon materials derived from MOFs with excellent junction support and using them as carriers to prepare Pt-based catalysts is a practical and feasible approach. It provides a way to develop new Pt-based catalysts that perform efficient MOR.
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