Journal of Physical Chemistry C
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2024
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IF 3.3
Da Shu,Ruipeng Fan,Songyou Yao,He Jiang,Xiaoyue Zhang,Yue Zheng
Understanding the rotor dynamics within metal–organic frameworks (MOFs) is fundamental to the desired amphidynamic application. However, in-depth investigation has been hindered due to the inadequacy of current characterization tools. In this paper, a technique based on infrared-combined atomic force microscopy (AFM-IR) was developed, in which the infrared spectrum can be obtained under tip bias and tip force with nanometer resolution. The tip bias induced variation in infrared spectra of the Cu2(fbdc)2(dabco) film demonstrates that full width at half-maximum of the vibration–rotation coupling mode is competent for rotor speed characterization. Stalling of dipolar rotor speed in the Cu2(fbdc)2(dabco) film is observed under both tip bias and tip force, which indicates the electrical and mechanical controllability of MOF rotor dynamics. On this basis, the rotor behavior of few-layer MOF films is investigated to reveal the influence of self-assembled molecule stress on rotor dynamics. It is found that the rotor rotation is activated progressively as the film grows and self-assembled molecule stress releases. Our results pave the avenue for direct study of rotor dynamics within MOF films at the nanoscale.
研究领域:
材料科学
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化学
·
物理学
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高影响因子
FUEL
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2023
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IF 7.4
Juan Li,Xiaolei Jiang,Mingyuan Zhu,Bin Dai
Oxidative desulfurization (ODS) is a promising technique for obtaining clean fuel. Designing and researching zirconium-based metal–organic frameworks (Zr-MOFs) with bimetallic catalytic sites are encouraging for its further development. In this study, Cu(Ⅰ)-MOF-808 was successfully synthesized through anchoring Cu + in MOF-808. Pyridine infrared spectrum (Py-IR) and NH 3 temperature programmed desorption (NH 3 -TPD) confirmed that Lewis (L) acid sites existed in the synthesized material. Cu(Ⅰ)-MOF-808 was applied into the ODS reaction, during the reaction process, L acid sites adsorbed sulfide, Cu + sustainably provided electron to H 2 O 2 to formed into •OH, with the synergistic effect of L acid sites and Cu + , 99.9 % of the dibenzothiophene was oxidated to dibenzothiophene sulfone in 120 min. In addition, the cyclic experiment indicated that the ODS performance of Cu(Ⅰ)-MOF-808 was maintained at 99.2 % after 12 times recycling. Powder X-ray diffraction (PXRD) spectra indicated the framework structure of the reused catalyst was stable, inductively coupled plasma optical emission spectrometer (ICP-OES) result displayed no metal ions (Zr, Cu) leaching after the ODS reaction, which also proved the catalytic stability of the Cu(Ⅰ)-MOF-808.
研究领域:
材料科学
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催化化学
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ADVANCED FUNCTIONAL MATERIALS
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2026
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IF 19.9
Junhan Li,Chao Zhou,Shujia Wang,Jingwen Xu,Zhida Gao,Yong Zhang,Yan-Yan Song
Metal–organic frameworks (MOFs) offer unique chemical selectivity for surface-enhanced Raman scattering (SERS), yet their intrinsically weak light–matter coupling fundamentally limits sensitivity and has long hindered their practical deployment as plasmon-free SERS substrates. Here, we report a photonic-crystal strategy that fundamentally amplifies charge-transfer (CT)-mediated SERS in MOFs by exploiting slow photons at the photonic stop-band edge. Using UiO-66(Zr) nanocrystals as the model MOF, the assembled ordered MOF photonic crystals (PhCs) with tunable Bragg reflection are precisely aligned to the excitation wavelength. The resulting slow-light effect dramatically increases photon residence time and local electromagnetic field within the MOF pore domains. This slow-photon confinement synergistically couples with CT processes between MOFs and analyte molecules, resulting in a tenfold enhancement in SERS intensity compared with disordered MOF assemblies and an enhancement factor up to 5.15 × 10 8 without any plasmonic components. By leveraging the intrinsic band-structure tunability of MOFs, selective CT-SERS is further demonstrated across different molecular systems and environments. The optimized MOF-PhCs substrate enables ppb-level detection and multicomponent discrimination of lung-cancer-associated volatile organic compounds, which are digitally encoded into machine-readable Raman barcodes. This work establishes slow-photon-regulated MOF photonic crystals as a versatile platform for plasmon-free, chemically programmable, and functionally integrated SERS sensing.
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Nature Communications
·
2026
·
IF 18.1
Chen Weicheng,Luo Mingyun,Tan Yuxuan,Yan Lintao,Liao TingTing,Liu Weiqi,Liu Fengwen,Chen Zhixuan,Yao Jinze,Liang Xianghui,Fang Yutang,Wang Shuangfeng,Ke Yujie,Suwardi Ady,Yuen Anthony Chun Yin,Tan Swee Ching,Ravi Sai Kishore
Atmospheric water harvesting (AWH) is limited by the high energy demand for sorbent regeneration, while battery thermal management dissipates substantial low-grade heat unused. Here, we propose a thermally symbiotic architecture integrating these systems. Battery discharge waste heat regenerates a MOF-303 sorbent layer via desorption, while the sorption process passively stabilizes battery temperature. The sorbent’s regeneration enthalpy aligns with the battery’s thermal output, triggering desorption under −12 to −20 A discharge. Within 46 min, the MOF exceeds 50 °C, releasing vapor for condensation in a sealed setup. Concurrently, sorption extracts heat from the battery, reducing peak temperatures by ~10 °C. Notably, this integrated system achieves a water production rate of 1.39 g g −1 day −1 , a 117% increase over solar-driven counterparts. Finite-element simulations validate the heat transfer dynamics and identify key thermal efficiency parameters. This work establishes a closed-loop thermal cycle that repurposes energy-storage waste heat to power AWH, enabling sorbent regeneration without solar heating. The strategy offers a pathway to enhance thermal efficiency across various energy and environmental systems through internal heat recovery.
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Analytical Methods
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2025
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IF 2.6
Shaohong Zhang,Ran Zhang,Minzi Li,Hongying Wang,Zhijuan Wang
A metal–organic framework (MOF)-encapsulated nanozyme has been developed to detect L-cysteine (L-Cys) through a facile colorimetric sensing method in this study. This nanozyme was prepared by encapsulating Fmoc-histidine (FH) and hemin within ZIF-8 (FH/hemin@ZIF-8) and exhibited significantly enhanced catalytic activity and great stability because of its unique structure. FH/hemin@ZIF-8 oxidized colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to a distinct blue color with the assistance of H2O2. However, after the addition of L-Cys, this oxidation process was inhibited, resulting in the solution fading from blue to colorless. This change can be observed by the naked eyes and quantitatively analyzed using a UV-vis spectrophotometer. Additionally, this system demonstrated excellent resistance to interference and exceptional selectivity. In addition, this system showed a low detection limit of 23.1 nm (S/N = 3). Consequently, it is believed that the strategy of encapsulating biomimetic nanozymes within MOFs holds significant potential for applications in bioanalysis and the early diagnosis of L-Cys.
研究领域:
生物化学
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分析化学
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材料科学
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PubMed
高影响因子
CATALYSIS TODAY
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2024
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IF 5.2
Guiming Xie,Xingyang Bai,Fei Yu,Qingyuan Yang,Zhou-jun Wang
Three AuCu/ZnO bimetallic catalysts , AuCu/ZnO-BTC, AuCu/ZnO-BDC and AuCu/ZnO-MOF-74, were derived from various MOF precursors using facile hydrothermal methods . Among the resultant catalysts, the AuCu/ZnO-BTC catalyst possessed the best methanol synthesis activity, whose space time yield of methanol ( STY MeOH ) reached 359.0 g MeOH kg cat −1 h −1 at 250 °C under 3 MPa. Structural characterization reveals that in comparison with the AuCu/ZnO-BDC and AuCu/ZnO-MOF-74 catalysts, the AuCu/ZnO-BTC catalyst possessed higher specific surface area ( S BET ), tinier metal particle size, more oxygen vacancies , stronger metal-support interactions and larger amount of medium basic sites. In situ DRIFTS result demonstrates that formate (*HCOO) species were readily generated and bridged-methoxy (*b-OCH 3 ) species were selectively formed on the AuCu/ZnO-BTC catalyst, which may be related with its abundant oxygen vacancies and responsible for its superior methanol synthesis activity. The present work derives high-performance AuCu/ZnO bimetallic catalysts from MOF precursors and provides new insight into structure-activity relationships for CO 2 hydrogenation to methanol.
研究领域:
催化化学
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材料科学
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环境科学
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高影响因子
Journal of Materials Chemistry A
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2016
·Vol. 4
·期 45
·17838-17847
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IF 8.262
Sainan Liu,Jiang Zhou,Zhenyang Cai,Guozhao Fang,Yangsheng Cai,Anqiang Pan,Shuquan Liang
Hybrid supercapacitors (HSCs), which are expected to possess the good characteristics of both lithium batteries and supercapacitors, have become a hot research topic in recent years for catering to the growing market for electric vehicles (EVs) and hybrid electric vehicles (HEVs). Herein, we demonstrate an advanced hybrid material construction by the orthorhombic Nb2O5 quantum dots embedded in nitrogen-doped porous carbon derived from ZIF-8 dodecahedrons, referred to as NQD–NC. Then the applications of this material in LIBs and HSCs are studied in-depth. The LIB test reveals that the novel Nb2O5-based material shows excellent high-rate capability and long-term cyclic stability. Importantly, by assembling a HSC device using a NQD–NC anode and a commercial activated carbon cathode with an organic electrolyte, the HSC shows superior electrochemical performance including ultra-high energy and power density (76.9 W h kg−1 and 11 250 W kg−1, respectively) and superior cyclic stability (capacity retention of ∼85% at 5 A g−1 after 4500 cycles in a voltage range of 0.5–3.0 V). The excellent electrochemical performance of the HSCs indicates combining the advantages of lithium-ion batteries and supercapacitors, which is promising for the next generation of energy storage systems.
研究领域:
材料科学
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能源存储技术
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2023
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IF 8.4
Jie Hu,Xueqing Xiong,Wangwang Guan,Yong Chen,Haizhu Long
In this study, a hierarchical Fe 2 O 3 -Co 3 O 4 heterojunction with abundant oxygen vacancies was fabricated by a MOF-assisted strategy combing with a thermal treatment process. The morphology, nanostructure and other properties of the synthesized samples were comprehensively investigated by related characterizations. The results display that the Co 3 O 4 modified with Fe 2 O 3 nanorod exhibits an admirable mesoporous structure and abundant oxygen vacancies. In addition, the gas sensing devices were constructed by as-prepared samples and demonstrated that the gas sensor based on Fe 2 O 3 -Co 3 O 4 composites shows excellent gas sensitivity of 91.5 towards 100 ppm acetone at a working temperature of 200 °C, with a short response-recovery time of 20/21 s. Meanwhile, the sensor possesses good reproducibility and long-term stability (over 30 days), and outstanding selectivity towards acetone gas. Exploration into a convincing gas sensing mechanism confirms that fabricating of p-n heterojunction architecture, regulating of oxygen vacancies and designing of mesoporous structure synergistically induced the excellent gas sensing performance. Therefore, this work can offer a promising strategy to enhance acetone sensing response of Fe 2 O 3 -Co 3 O 4 in practical applications.
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Small
·
2025
·
IF 12.1
Chang Sun,Zixuan Ma,Wenxuan Fang,Shuyi Huang,Xinrong Guo,Xin Yu,Xishi Tai,Xiangxue Wang,Wen Yao
Conventional strategies for enhancing the performance of metal-organic framework (MOF) adsorbents primarily focus on modifying functional groups, while the critical role of central metal ions remains underexplored. Herein, a definitive structure-activity relationship governing uranyl (U(VI)) elimination by engineering isomorphic HHTP MOFs (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene) with Zn 2+ , Ni 2+ , and Cu 2+ centers is revealed. Advanced characterization confirms that the identity of the metal dictates electronic configurations and binding thermodynamics without altering crystallographic topology. Remarkably, Zn-HHTP achieves a record U(VI) uptake capacity of 458.73 mg·g −1 , surpassing Ni-HHTP (441.27 mg·g −1 ) and Cu-HHTP (317.24 mg·g −1 ), coupled with ultrafast kinetics (80 min) and exceptional selectivity. Mechanistic studies reveal that the optimal electronegativity (χ = 1.65) of Zn 2+ endows it with superior Lewis acidity, facilitating enhanced charge transfer (Δq = 0.065 e − ) via Zn─O─U coordination, as demonstrated by combined XPS analysis and DFT calculations. This lower electronegativity of Zn 2+ promotes greater electron acceptance from U-O, yielding a robust binding energy ( E ads = −35.16 kcal·mol −1 ). This work establishes the modulation of central metal ions as a critical design paradigm for next-generation MOF adsorbents, positioning Zn-HHTP as a transformative material for high-efficiency radioactive wastewater remediation.
研究领域:
环境化学
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材料科学
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放射性废物治理
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配位化学
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理论与计算化学
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Catalysts
·
2020
·Vol. 10
·期 6
·681
·
IF 3.52
Qian Zhang,Yiwen Jiang,Jingheng Gao,Mingli Fu,Sibei Zou,Yanxia Li,Daiqi Ye
A series of CeO2–MnOXcatalysts with different Ce contents was prepared using Mn–BTC MOF as a sacrificial template for toluene oxidation. Interestingly, the performance of CeO2–MnOXincreased rapidly only when the Ce content lower than 5%. The 1%-, 3%- and 10%-Ce-content samples exhibited the T90value of 325 °C, 291 °C and 277 °C, respectively. XRD shows that the catalyst phase changes significantly before (Mn3O4only) and after (Mn2O3, Mn3O4and CeO2) 3% Ce loading. All other results indicated that the Ce–Mn interface properties of different Ce content composite oxides was quite distinguishable in terms of removal and energy efficiency. XRD and XPS results further showed that there a Ce monolayer dispersion threshold existed on the interface of MnOX(3.2 wt%, confirmed by XPS), which caused the difference in performance increment. The dispersed Ce could be divided into a monolayer dispersion state (1–3%) and a crystalline phase state (>3%), according to the existence form, which corresponded to the significant and minor enhancements of toluene conversion rate. Importantly, the Ce in monolayer dispersion state obviously improved the redox properties of catalysts interface, while the Ce in crystal state not. The interfaces with monolayer dispersion Ce result in more abundant metal ion states, oxygen vacancies, better electron transfer performance and catalytic activity.
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
Energy & Environmental Materials
·
2026
·
IF 13.8
Fujuan Wang,Nan Jia,Tianyun Zhang,Xiaoya Kang,Rui Wang,Fen Ran
The performance of hard carbon anodes in sodium-ion batteries is restricted by the inherent trade-off between rate capability and capacity due to uncoordinated ion-electron transport. This research indicates that the microstructure of the carbon host crucially determines the interfacial reconstruction behavior and electrochemical outcome of MOF modification. For porous cellulose-derived carbon, the integration of MOF induces a continuous composite interface, enhancing the Na + diffusion coefficient by an order of magnitude below 0.1 V (reaching 10 −9 cm 2 s −1 ), and yielding a high reversible capacity of 667.2 mAh g −1 with 79% capacity retention. In contrast, on commercial hard carbon with a higher degree of graphitization, MOF forms a discontinuous physical coating that obstructs intrinsic ion pathways, restricting rate performance of hard carbon despite the improvement in its cycling stability. In-situ EIS and distribution of relaxation time analyses disclose lower charge-transfer resistance and optimized SEI evolution in MOF@cellulose-derived carbon, facilitating efficient ion-electron dual transport. The full cell utilizing MOF@cellulose-derived carbon attains a high energy density of 172.8 Wh kg −1 at a power density of 2065 W kg −1 . This work offers mechanistic insights into the correlations among carbon microstructure, interface, and performance, guiding the rational anodes design of high-power and high-energy density sodium-ion batteries.
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Science Advances
·
2024
·Vol. 10
·期 19
·
IF 11.7
Tingting Xu,Bin Wu,Wenmin Li,Yifan Li,Yanran Zhu,Fangmeng Sheng,Qiuhua Li,Liang Ge,Xingya Li,Huanting Wang,Tongwen Xu
Fast transport of monovalent ions is imperative in selective monovalent ion separation based on membranes. Here, we report the in situ growth of crown ether@UiO-66 membranes at a mild condition, where dibenzo-18-crown-6 (DB18C6) or dibenzo-15-crown-5 is perfectly confined in the UiO-66 cavity. Crown ether@UiO-66 membranes exhibit enhanced monovalent ion transport rates and mono-/divalent ion selectivity, due to the combination of size sieving and interaction screening effects toward the complete monovalent ion dehydration. Specifically, the DB18C6@UiO-66 membrane shows a permeation rate (e.g., K+) of 1.2 mol per square meter per hour and a mono-/divalent ion selectivity (e.g., K+/Mg2+) of 57. Theoretical calculations and simulations illustrate that, presumably, ions are completely dehydrated while transporting through the DB18C6@UiO-66 cavity with a lower energy barrier than that of the UiO-66 cavity. This work provides a strategy to develop efficient ion separation membranes via integrating size sieving and interaction screening and to illuminate the effect of ion dehydration on fast ion transport.
研究领域:
材料科学
·
化学工程
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PubMed
高影响因子