APPLIED ORGANOMETALLIC CHEMISTRY
·
2026
·Vol. 40
·期 9
·e70633
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IF 4.3
Wang Ye,Haoyue Xu,Jun Zhang,Xinru Liu,Yingxi Wang,Ling Li
The persistence and environmental hazards of antibiotic residues make the efficient removal of such pollutants from aquatic environments critically important. However, metal–organic framework (MOF) catalysts often face challenges in practical applications, such as poor structural stability and easy leaching of metal ions. In this study, using Co-MOF as a precursor, Co 3 O 4 -based catalysts rich in different concentrations of oxygen vacancies were successfully prepared through pyrolysis combined with sodium borohydride reduction and were employed for the efficient activation of peroxymonosulfate (PMS) to rapidly degrade oxytetracycline (OTC). The catalyst possessed excellent reaction kinetics, enabling rapid PMS activation and efficient OTC degradation. Radical quenching experiments and EPR analysis revealed that the degradation process follows a synergistic radical and nonradical mechanism, in which 1 O 2 and SO 4 • − play dominant roles. Furthermore, possible degradation pathways of OTC were proposed, and the ecotoxicity of its transformation products was evaluated. The results suggest that most intermediates have lower predicted toxicity than the parent compound. The catalyst also demonstrated good degradation performance and applicability in real water samples and for various pollutants. This study provides a new strategy to address the structural instability of MOF powder materials in catalytic applications.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zixian Qin,Yuxiu Sun,Zhengqing Zhang,Chenxu Zhang,Chi Tang,Chenxu Geng,Zhihua Qiao
Oxygen/nitrogen (O 2 /N 2 ) separation is of great importance but faces huge challenges owing to their similar molecular size and close polarity. In this work, we construct a polymer of intrinsic microporosity (PIM-1) based mixed matrix membrane (MMM) for efficient O 2 /N 2 separation by using ZIF-8 as the sieving filler along with surface modification of o-carborane (o-CB) to strengthen selective N 2 adsorption fixation as well as polymer-filler interfaces. Markedly, the o-CB on the outer surface of ZIF-8 not only affords the requisite interfacial compatibility in molecular sieving MMMs, but also increases the diffusion difference between O 2 and N 2 by the preferential adsorption with N 2 molecules. This synergistic effect of molecular sieving and adsorption inhibition achieves efficient O 2 /N 2 diffusion differential separation. As expected, the optimal membrane with o-CB-ZIF-8 loading of 35 wt% exhibits an O 2 permeability of 796.5 Barrer and a mixed O 2 /N 2 selectivity of 8.9 with O 2 /N 2 (20:80, vol.) mixtures, exceeding the latest 2015 upper bound limits. Moreover, the according membrane module with o-CB-ZIF-8 loading of 20 wt% also displays moderate O 2 permeability of 391.7 Barrer and O 2 /N 2 selectivity of 5.5 under pressure of 1 bar. This work may provide a feasible platform for designing high-performance MOF-based membranes in air separations.
研究领域:
材料科学
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分离技术
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CRYSTAL GROWTH & DESIGN
·
2026
·
IF 3.6
Hui Wang,Yuxuan Pan,Huishan Liang,Mingyi Dai,Hao Xiang,Yinbao Tong,Yike Sui,Lei Li,Changcun Han
The development of efficient photocatalytic materials is the key to promoting the advancement and application of photocatalytic technology. Bi2S3, a relatively narrow bandgap semiconductor, can absorb visible light and even near-infrared light. However, the fast recombination rate of photogenerated electron–hole pairs, limited surface active sites, and susceptibility to photocorrosion of pure Bi2S3 severely restrict its photocatalytic efficiency. In this paper, carbon-doped sulfur-rich defective hollow Bi2S3 nanorods were prepared in one step using Bi-MOF as the precursor. The microcrystalline structure and defect structure were regulated by adjusting the hydrothermal reaction time. The ammonia production rate of hollow Bi2S3-2 under full sunlight was approximately 147.78 μmol·h–1·g–1. The superior photocatalytic activity of hollow Bi2S3-2 is mainly attributed to its sulfur defects, which can provide abundant active sites to activate nitrogen molecules. It reveals that the photoexcited electrons generate ammonia through two protonation pathways and weaken the N≡N bond in the photocatalytic nitrogen fixation path. This work provides new insights into photocatalytic nitrogen fixation and achieves efficient N2 photoreduction by synthesizing photocatalysts from MOF derivatives.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122206
·
IF 7.5
Xiaorui Du,Lifei Liu,Pengfei Li,Luyuan Zhang,Yang Deng,Xia An,Xu Wu
The persistence of tetracycline antibiotics in aquatic environments poses significant harm to both ecological systems and public health. In this study, a Cu-MOF-74@TAPT-DHTA-COF hetero-framework was designed by constructing interfacial Cu-N/O coordination bonds, which create efficient electron transfer pathways that enhance charge separation and migration. Mechanistic investigation demonstrated that the molecular oxygen adsorption and activation was enhanced by this interfacial coordination engineering, promoting the selective production of singlet oxygen ( 1 O 2 ) and thus accelerating the photo-oxidation of tetracycline (TC). The hetero-framework achieved 91.5% TC removal within 60 min with apparent value of 0.03325 min⁻¹ . This constant is 2.0 times that of Cu-MOF-74 and 1.9 times that of TAPT-DHTA-COF. Toxicity evaluation confirmed effective reduction of ecological risks, with all final degradation products testing negative for mutagenicity. Furthermore, a photocatalytic membrane reactor based on the hetero-framework demonstrated nearly complete contaminant removal and exceptional stability in continuous-flow wastewater treatment, highlighting its practical applicability. This work elucidates the molecular-level mechanism of 1 O 2 generation boosted by the interfacial coordination engineering and provides novel design principles for advanced photocatalytic water treatment technologies.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Mingxian Duan,Yeshuang Wang,Huiling Fan,Zhelin Su,Chao Yang,Jiawei Kou,Ju Shangguan
Thiophene (C 4 H 4 S) removal from coke oven gas is critical to its subsequent high valuable utilization but remains a challenge. MOF-199 was considered as a promising candidate for C 4 H 4 S adsorption removal owing to its nature of enriched opened Cu sites. However, the presence of mixed valence of Cu(II) and Cu(I) in MOF-199 makes it puzzling to their respective contribution to the removal of C 4 H 4 S. Herein, a series of MOF-199 with different Cu(I) contents were synthesized using different methods, including hydrothermal, solution diffusion, and ultrasonic, and their C 4 H 4 S adsorption performance were investigated. The respective contributions of Cu(II) and Cu(I) to the C 4 H 4 S removal was systematically discussed. The collected results indicated that although the samples prepared with different methods present a remarkable difference in textural characters, the latter was found to have a negligible influence on the C 4 H 4 S removal owing to MOF-199(H) affording an inferior surface area and pore volumes but performing the best C 4 H 4 S removal capacity of 53.7 mg S/g. The co-adsorption results of CH 3 SCH 3 and C 4 H 4 S indicated that the excellent performance of MOF-199(H) mainly attributed to the presence of Cu(I), which provides active sites for C 4 H 4 S adsorption through π complex coordination. Cu(II) species was also found to the C 4 H 4 S adsorption via soft-acid-base coordinated interaction, but its contribution is 8.3 mg S/g, only accounting for 15.5 %. Additionally, the adsorption of C 4 H 4 S on MOF-199(H) was found to follow the intra-particle diffusion model and the Langmuir models. Moreover, MOF-199(H) also exhibited an excellent regeneration performance due to the weak interaction between C 4 H 4 S and their opened Cu sites, the C 4 H 4 S adsorption capacity still reaches 50.6 mg S/g after three regeneration cycles, about 94 % of its initial value. The results collected in this study will provide new insights for the manipulation of performance of C 4 H 4 S adsorption on the MOF-199.
研究领域:
材料科学
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环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Shenghan Ji,Ziheng Li,Yan Dai,Xiaobin Jiang,Xuehua Ruan,Wenji Zheng,Gaohong He
MOF membrane supported on flexible substrates faces the issues of non-selective defects as well as poor mechanical compatibility. Herein, a “rigid and flexible” MOF/COF molecular sieving membrane is acquired by the in-situ polymerization of COFs among the inter-crystalline and interfacial defects in the MOF membrane. Taking advantage of different osmotic pressures on both sides of MOF membrane during the counter-diffusion process, the COFs monomers diffuse from bottom to top to the inter-crystalline and interfacial defects and meet with the catalyst for further polymerization and crystallization, thus repairing non-selective defects of the MOF membrane. In the MOF/COF membrane, COFs exhibit a strong adsorption affinity for CO 2 , which can slow down CO 2 permeation and enhance H 2 /CO 2 selectivity. Meanwhile, the in-situ polymerization of COFs primarily occurs at the inter-crystalline defects of MOF membrane and the interface between MOF membrane and polymer substrate, without forming a resistance layer on MOF membrane surface, which is demonstrated by the SEM and AFM results. Additionally, the counter-diffusion growth of COFs allows for the connection between the organic substrate and the inorganic MOFs layer through COFs, thereby improving the mechanical flexibility of MOF membrane confirmed by the mechanical properties. Besides, through regulating the polymerization process of TpPa-1 including time and monomer concentration, the H 2 /CO 2 separation of ZIF-67/TpPa-1 membrane can be tuned precisely. Therefore, the ZIF-67/TpPa-1–0.90 membrane at a polymerization time of 24 h presents H 2 permeance of 1114 GPU and H 2 /CO 2 selectivity of 17.52, an increase of 178.1 % compared to the pure ZIF-67 membrane, which is far beyond the 2008 upper bound and approaching the up-to-date data line. Together with the additional good mechanical properties, stability and universality, the proposed “rigid and flexible” MOF/COF molecular sieving membrane is promising in H 2 /CO 2 separation.
研究领域:
材料科学
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化学工程
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CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Peng Hu,Mingyuan Jiang,Jialang Hu,Long Li,Gui Shi,Lvming Jin,Yonggang Zhang,Chao Xiong,Hongbing Ji
The efficient separation and purification of natural gas (NG) represents a pivotal industrial procedure. Herein, we rationally designed a hierarchical-discrete MOF (denoted as 1a ) with molecular nanotraps that enable highly efficient C 3 H 8 capture and kinetic separation from light alkane mixtures (CH 4 /C 2 H 6 /C 3 H 8 ). N 2 adsorption analysis and pore visualization reveal hierarchically discrete pore geometries with ultra-submicroporous dimensions of 5.0 × 4.9 Å 2 and 8.3 × 8.2 Å 2 , effectively optimizing the formation of C 3 H 8 -selective molecular nanotraps while improving gas storage and diffusion kinetics through interconnected ultra-submicroporous channels. Significantly, 1a demonstrates exceptional separation performance, with IAST selectivity of equimolar C 3 H 8 /CH 4 and C 2 H 6 /CH 4 for 1a is 575.6 and 34.8 at zero coverage and 298 K, surpassing many well-known MOFs. Dynamic breakthrough experiments confirm the effective separation of ternary CH 4 /C 2 H 6 /C 3 H 8 mixtures and combined density functional theory (DFT) calculations, transient two-dimensional electron-density maps (2D-EDM),etc., reveal the molecular-level host–guest binding mechanisms. This work highlights the importance of multiscale pore cooperation for synergistically enhancing gas storage capacity and diffusion kinetics.
研究领域:
化学工程
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材料科学
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气体分离技术
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纳米多孔材料
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计算化学
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高影响因子
CARBON
·
2025
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IF 11.6
Yinghan Zhang,Jiarui Fan,Meiling Zhu,Xin Wang,Weijie Li,Yuqing Zhang,Jinzhao Shi,Qi Zheng,Guojun Zhang,Lianjun Wang,Wan Jiang
Hierarchical structure engineering and multicomponent design are pivotal for developing high-performance electromagnetic wave (EMW) absorbers, however, conventional synthetic strategies still face significant challenges in simultaneously achieving precise control over multi-component, microstructural construction and size regulation. Herein, an asymmetric hierarchical metal–organic framework (MOF)-derived nanoporous carbon (NPC) composite is fabricated via a polyoxometalate (POM)-mediated coordination competition strategy. Tungsten-based POM (W-POM, Na 3 [PW 12 O 40 ]) acts as a dynamic structural modulator during Cu-MOF assembly. By competitively coordinating with Cu(II) ions against organic ligands, the W-POM precisely regulates Cu(II) ion release kinetics and nucleation, enabling concurrent control over precursor size (100-400 nm), morphology (evolving from octahedra to aggregated polyhedra), and composition. Subsequent pyrolysis transforms these W-POM@Cu-MOF precursors into a hierarchical architecture featuring asymmetrically grown Cu nanosheets on porous carbon matrix, alongside embedded Cu nanoparticles and W-POM-derived Na 2 WO 4 heterostructures (Cu/W/NPC). This unique anisotropic configuration synergistically enhances microwave attenuation, where Cu nanosheets and porous matrix prolong propagation paths and induce multi-scattering, while the uniformly dispersed Na 2 WO 4 and heterogeneous interfaces significantly boost interfacial polarization and dipole polarization. Consequently, the optimized nanocomposite exhibits superior EMW absorption performance, achieving a minimum reflection loss (RL min ) of -61.4 dB and a broad effective absorption bandwidth (EAB) of 6.64 GHz. COMSOL simulations quantitatively confirm the abundant interfaces and porous structures synergize polarization dissipation and multi-reflection mechanisms, optimizing impedance matching. Radar cross-section (RCS) simulations further demonstrate significant attenuation (29.84 dB·m 2 ), highlighting practical stealth utility. This work establishes a versatile POM-mediated coordination competition paradigm for architecturally and compositionally tailored MOF-derived advanced EMW absorbers.
研究领域:
材料科学
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纳米科技
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物理化学
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功能材料
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电磁学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Kuan Wu,Gang Xu,Dengyu Pan,Minghong Wu
Combination of high-capacity and flexibility in electrode materials is crucial for flexible electronics. Recently, red phosphorus (P) has caused increasing focus as a hopeful storage material for lithium storage due to its super-high theoretical capacity and low cost. However, the low conductivity of red P and its large volume change during cycling process lead to reduced electrochemical activity. So far, no effective methods have been developed to construct flexible binder-free electrodes using red P as an active material for high-performance lithium-ion batteries (LIBs). Here, a novel hollow three‐dimensional (3D) internet structure as a flexible high-areal-capacity electrode material was fabricated by confining red P nanoparticles into compact MOF-derived carbon-based composite polyhedrons/carbon nanotube internets. The electrode manifests an excellent lithium storage performance for LIBs with a high discharge capacity of 4.78 mAh cm −2 (1920 mAh g −1 ) at 0.1 mA cm −2 and a good capacity retention of 79.2% at 1 mA cm −2 after 300 cycles (73% and 69% capacity retention at 5 and 10 mA cm −2 after 500 cycles, respectively). The novel flexible anode materials can provide excellent Li + storage performance for flexible electronics applications.
研究领域:
材料科学
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电化学
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纳米材料
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能源存储
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功能材料
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先进电池技术
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高影响因子
JOURNAL OF POWER SOURCES
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2026
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IF 8.4
Xingjia Liu,Ziyang Liu,Kai Zhou,Chenyong Wang,Suyuan Liu,Xue-Zhi Song,Xiaofeng Wang,Zhenquan Tan
The electrochemical nitrate reduction reaction (NO 3 RR) offers a sustainable route for ammonia synthesis and wastewater remediation, yet developing efficient and stable electrocatalysts remains challenging. Herein, we report a high-performance heterostructured electrocatalyst, Cu-Cu 2 O@C-350, derived from controlled pyrolysis of a Cu-BTC metal-organic framework. Calcination at 350 °C transforms the precursor into a three-dimensionally interconnected coral-like carbon architecture embedded with Cu/Cu 2 O heterojunctions, exposing abundant active sites and facilitating mass transport. The optimal catalyst exhibits exceptional NO 3 RR performance, achieving a high ammonia yield of 46.63 mg h −1 mg cat −1 and a Faradaic efficiency of 98.43% at −0.7 V vs. RHE. In situ Raman spectroscopy reveals the synergistic mechanism that metallic Cu sites initiate nitrate reduction to nitrite, while Cu + sites facilitate deep hydrogenation of nitrite to ammonia. Density functional theory calculations demonstrate that the built-in electric field at the Cu-Cu 2 O interface induces directional electron transfer from Cu to Cu 2 O, optimizing intermediate adsorption and lowering the kinetic barrier. Finally, a rechargeable Zn-NO 3 battery with Cu-Cu 2 O@C-350 as the cathode delivers a peak power density of 2.07 mW cm −2 , highlighting its potential for practical energy conversion. This work provides valuable insights into the rational design of MOF-derived heterostructured electrocatalysts for efficient electrocatalytic reactions.
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Advanced Composites and Hybrid Materials
·
2026
·Vol. 9
·期 3
·242
·
IF 15.5
Wang Shuhao,Yang Xing,Peng Yang,Nie Yiyin,Liu Liping,Xu Chunyang
The expanding applications of electromagnetic (EM) wave absorption materials demand broadband absorption coupled with thermal insulation and lightweight properties. Metal-organic framework (MOF)-derived magneto-electric multi-component structures provide a promising platform for designing efficient absorbers. However, precise control over their configuration, composition, and heterogeneous interfaces remains a critical challenge. Herein, a pomegranate-like Ni/C@C microsphere architecture with abundant heterogeneous interfaces is fabricated by the in-situ polymerization and follow-up pyrolysis treatments. This composite material with its rich multicomponent interfaces, unique three-dimensional conductive network, and magnetic-dielectric synergistic system, exhibits a remarkable effective absorption bandwidth (EAB) of 9.28 GHz at a thickness of 2.0 mm. More excitingly, broadband and high absorption performance was achieved after the numerical simulation of periodic metastructures. The EAB of the composite material can be extended to an astonishing 15.14 GHz, with a minimum reflection loss of -55 dB. Furthermore, the excellent thermal insulation property of the hot-pressed composite material makes it suitable for a wider range of applications. This work advances the synthesis and optimization of multifunctional absorbers, accelerating the development of next-generation microwave absorption materials.
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CATALYSIS LETTERS
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2024
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IF 2.3
Yu Lihua,Zhao Yaling,Guo Shuai,Xue Juanqin
Metal–organic frameworks (MOFs) were used as precursors to prepare iron-based heterogeneous Fenton catalysts Fe@C, FeCu@C, and FeCu@N–C via pyrolysis. The catalytic activities were evaluated by measuring the decomposition rate of hydrogen peroxide (H 2 O 2 ). The morphology, structure, and physical properties of the catalysts were analyzed through X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), and nitrogen adsorption. The results showed that at 60 min, the decomposition rates of H 2 O 2 by FeCu@C and FeCu@N–C were 95.4% and 92.5%, respectively, which were 18.5% and 15.6% higher than that by Fe@C, respectively. It was speculated that the iron and copper species present in the bimetallic nanoparticles were available active sites for the Fenton reaction. The synergistic effects between them can promote the activation and decomposition of H 2 O 2 . In addition, the nitrogen-doped catalysts FeCu@N–C had better pH applicability, better reusability, and lower iron leaching than FeCu@C. Nitrogen-doped carbon contributed to the enhanced catalytic performance. This can be attributed to the well dispersibility of Fe and Cu species on the N-doped carbon matrix. The FeCu@N–C was applied to the treatment of enrofloxacin (ENR) antibiotic wastewater. The results indicated that a 90% degradation rate can be achieved in 60 min under the initial concentration of ENR 20 mg/L, catalyst dosage 20 mg/L, H 2 O 2 concentration 1.5 mM, the initial solution pH 3.60, 25 ℃. The rapid degradation of ENR was more relevant to the surface-bound ٠OH rather than free ٠OH and the heterogeneous Fenton reaction played the dominant role. This work provides a potential heterogeneous Fenton catalyst for antibiotics wastewater treatment. Graphical Abstract
研究领域:
环境科学
·
材料科学
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危险品化学品经营许可证（带存储）