JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2023
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IF 5.7
Yuzhu Shen,Wei Sun,Yonglong Xu,Qingbo Wen,Hongbo Zhang,Xiang Xiong
In this study, to overcome the difficulties associated with the preparation of PyC-ceramic interface and controllable deposition of the structure, we initially used a two-step molten salt infiltration method to prepare a C/C-Me-Zr-Hf (Me = Ta, Si) composite with excellent oxyacetylene ablation performance. The microstructure and the behavior of ablative were addressed by scanning electron microscopy (SEM) and transmission electron microscopy (TEM) as well as by X-ray diffraction（XRD）. The results reveals that C/C-ZrHfC-SiC composite prepared by two-step molten salt infiltration method have a controllable ultra-high temperature ceramic structure and better ablation resistance.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Qunfeng Chen,Daobin Tang,Qi Zhang,Zhiyuan Tang,Longlong Ma,Xinghua Zhang
Electron-metal support interactions (EMSI), which can tailor the microenvironment through electron transfer and coordination structure design, are an effective strategy to augment the intrinsic catalytic activity of catalysts. However, it remains challenging to establish the interfacial structure and interfacial electron configuration of catalysts to precisely regulate and enhance EMSI. In this work, the spatially defective sites and specific electronic states of Pd-UiO-66 were modified by in-situ constructing a W-O-Zr interface to strengthen the EMSI between Pd nanoparticles (Pd NPs) and UiO-66 support via implanting W into the defective Pd-UiO-66, realizing the effective hydrodeoxygenation (HDO) of vanillin (VAN) at room temperature (RT). The as-prepared catalyst Pd-UiO-66–0.24 W achieved > 99 % conversion of VAN and > 99 % yield of 2-methoxy-4-methylphenol (MMP) within 12 h, which surpassed the previous reports. The DFT analysis revealed that the narrow band-gap energy between Pd-UiO-66–0.24 W and H 2 molecule, along with the σ or π coordination adsorption between p and d orbitals of the implanted W and O in C=O, facilitated the activation of the H 2 molecules and reactant molecules. In addition, the constructed electron-deficient W-O-Zr interfacial sites provided more acidic sites that favor the cleavage of C-O bonds, promoting the HDO process of VAN. This work provides important insights into the modulation of EMSI, structural defects and acidic sites of metal–organic frameworks (MOFs)-based catalysts for efficient HDO of lignin-derived oxygenated compounds.
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Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 22
·13473-13482
·
IF 10.733
Kailun Zou,Yu Dan,Yuxi Yu,Ying Zhang,Qingfeng Zhang,Yinmei Lu,Haitao Huang,Xin Zhang,Yunbin He
Dielectric nanocomposites composed of a polymer matrix with high electric breakdown strength and inorganic ferroelectric nanofillers with large maximum electric displacement (Dmax) have recently attracted much attention due to their high power density, superior flexibility, and good fatigue endurance. However, their discharge energy density and energy efficiency are limited because of the high remnant displacement (Dr) and small Dmax − Dr values of the ferroelectric fillers. Compared with ferroelectrics, antiferroelectrics exhibit much lower Dr (near zero) and far larger Dmax − Dr values, and thus if they are used as the fillers of the dielectric composite, a larger discharge energy density and higher energy efficiency may be obtained simultaneously. Based on this, in this work, Pb0.97La0.02(Zr0.50Sn0.45Ti0.05)O3 (PLZST) antiferroelectric nanoparticles (∼200 nm in diameter) coated with a dense and robust dopamine layer are prepared in order to develop dopamine-modified PLZST filler/poly(vinylidene fluoride-co-hexafluoropropylene) (P(VDF-HFP)) polymer nanocomposites with superior energy storage properties. The experimental results indicate that optimizing the filler content leads to a small Dr (0.61 μC cm−2), large Dmax − Dr value (6.14 μC cm−2), and high electric breakdown strength (3136 kV cm−1), as a result of which, the PLZST/P(VDF-HFP) nanocomposites filled with 5 wt% dopamine-modified PLZST nanoparticles simultaneously exhibit a large discharge energy density of 9.39 J cm−3 and high energy efficiency of 82%. These energy storage properties are superior to those of most ferroelectric filler (including nanowires and nanofibers prepared by complicated methods)/polymer nanocomposites with a single-layer structure. Our work not only proves that, antiferroelectric nanoparticles are excellent fillers that can be comparable to, or even better than, ferroelectric nanowires and nanofibers prepared by very complicated methods, for energy-storage inorganic/polymer dielectric composites, but also provides a convenient and effective way to prepare and design flexible dielectric capacitors with superior energy storage capacity.
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ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Xu Pan,Junhong Wang,Ye Chen,Qing Wen,Cunguo Lin,Haiping Gao,Zhenghui Qiu,Liuqingying Yang
Microbial fuel cells (MFCs) represent a green and sustainable energy technology capable of generating electricity through biomass conversion. However, their widespread application is hindered by the relatively low energy conversion efficiency and electricity generation activity of biofilms. The selection of appropriate bioelectrocatalysts emerges as a promising strategy to enhance extracellular electron transfer (EET) efficiency and substrate utilization rates. This study introduces a novel biofunctional anode material composed of Zr3S4/FeS heterogeneous nanostructures embedded in hierarchical porous N-doped carbon spheres (HPNC/Zr3S4/FeS), designed to optimize EET efficiency and interfacial charge transfer kinetics. Compared to HPNC/ZrO2 MFC, the maximum power density of HPNC/Zr3S4/FeS MFC increased by 51.11% (from 4.05 to 6.12 W/m2) and the Coulombic efficiency improved from 24.33% to 30.76%. The bioelectrocatalytic activity of the HPNC/Zr3S4/FeS bioanode was significantly enhanced, as evidenced by increased exchange current density (from 0.76 to 1.74 mA/cm2) and reduced charge transfer resistance (from 3.16 to 1.24 Ω). Fourier-Transformed alternating current voltammetry (FTACV) and distribution of relaxation time (DRT) analyses jointly confirmed that the Zr3S4/FeS heterogeneous interface mediates and promotes the c-type cytochrome-mediated direct EET process, enhancing charge transfer rates at the biofilm-electrode interface. Density Functional Theory (DFT) calculations indicated that the Zr3S4/FeS interface facilitates the adsorption of c-type cytochrome proteins with heme prosthetic groups. High-throughput sequencing demonstrated that HPNC/Zr3S4/FeS selectively enriches electrogenic bacteria (Desulfurivibrio and Geoalkalibacter), a process that further enhances the electrogenic functional traits of the biofilm. This study not only validates the superior bioelectrocatalytic activity of HPNC/Zr3S4/FeS but also highlights the mechanistic role of heterogeneous structures in regulating the sustainable energy conversion efficiency.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2026
·Vol. 40
·期 4
·e70546
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IF 4.3
Hangyu Zhang,Shuang Yao,Zhiwen Jiang,Lei Xie,Zixia Lin,Guoliang Dai,Juanhong Li,Xin Liu,Feng Liu
In Fenton-like reactions, the catalysts generally have an inherent drawback: Their active centers are prone to being lost from the catalyst supports, leading to a continuous decline in catalytic efficiency and causing secondary pollution. To address this issue, two catalysts, including Fe 3 O 4 @UiO-66(Zr) and Fe 3 O 4 @UiO-66(Zr)-COOH, were prepared in this study by confining Fe 3 O 4 active centers within the pores of UiO-66(Zr) and grafting -COOH groups to enhance metal coordination interactions. The Fe 3 O 4 @UiO-66(Zr)-COOH achieved 99% removal efficiency of carbamazepine within 5 min under the conditions of pH = 3.0, 40 mM H 2 O 2 , 20 mg·L −1 carbamazepine, and 2 g·L −1 catalyst. This efficiency far exceeded that of Fe 3 O 4 @UiO-66(Zr) (61.5%) and was 3.96 times higher than that of the Fenton-like system. The rapid degradation of CBZ was realized through stabilized active centers and enhanced metal coordination. In this work, the iron-based material was found to enhance the coordination between Fe and Zr. As confirmed by quenching experiments, electron spin resonance, electrochemical tests, and density functional theory calculations, ·OH and 1 O 2 were identified as the dominant active species. The -COOH, acting as electron bridges, enhanced electrical conductivity and reduced electron transfer barriers, thereby facilitating faster charge transfer processes. In addition, it was demonstrated by six cycles of experiments that Fe 3 O 4 @UiO-66(Zr)-COOH possessed excellent stability. It was also shown by the characterization of the catalyst after the cycles that both the performance and morphology of the composite material could be maintained unchanged.
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Journal of Materials Chemistry A
·
2026
·
IF 9.5
Ziyao Wang,Sijia Huo,Meichen Pan,Yihan Qiu,Ying Tian,Ying Zhou,Wei Yan,Wen Wang,Yu Zhou,Xiaoming Duan
Lithium metal is considered an ideal anode material owing to its high specific capacity, low density, and low redox potential, but its practical use in liquid systems is hindered by dendrite growth and interfacial instability. Solid-state electrolytes (SSEs) offer high thermal stability and mechanical strength, with Li 7 La 3 Zr 2 O 12 (LLZO) particularly attractive for its high ionic conductivity and wide electrochemical window. Semi-solid-state electrolytes (SSSEs), integrating the advantages of SSEs and liquid electrolytes (LEs), can be further enhanced by introducing porous solid frameworks. Such structures improve wettability and transport while providing mechanical support that suppresses dendrites, thereby achieving both high conductivity and structural safety. In this work, a two-dimensional porous solid-state skeleton model was established to investigate the influence of porosity on lithium-ion transport. The percolation threshold was determined to be 47.91% porosity, indicating the minimum connectivity required for efficient ion migration. Based on these insights, a graphite-template sacrificial method was employed to fabricate a highly interconnected porous Li 6.25 Ga 0.25 La 3 Zr 2 O 12 (LGLZO) framework (P G LF). The ionic conductivity of the P G LF-LiPF 6 SSSE reached 3.02×10 -3 S cm -1 at room temperature. The constructed Li/Li cell can be stably cycled for more than 1600 h at 0.5 mA cm -2 , and the capacity retention rate of the LFP/Li cell was 91.62% after 2000 cycles at 2 C. In addition, similar properties can be achieved by replacing the formwork material (charcoal powder). This work established a correlation between porosity and ion transport performance, providing a promising preparation method for high-performance lithium metal batteries (LMBs).
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Feng Hong,Liangqiong Ren,Yiping Chen
In this work, we report a fluorescent and colorimetric dual readout bioassay for deoxynivalenol detection to ensure public food safety. A multifunctional fluorescent and colorimetric signal probe was constructed to develop the bioassay for deoxynivalenol detection based on the characteristics of Zr-MOF (PCN-224; i.e., high porosity, a large surface area, and excellent fluorescence quenching performance). Platinum nanoparticles (Pt NPs) were grown in situ outside, while glucose oxidase was stored inside (PPG). Glucose oxidase and Pt NPs are both enriched by Zr-MOF, achieving the first signal amplification, and cascade catalysis by the glucose-TMB system for colorimetric signal readout leads to the second signal amplification. PPG was quenched through the spontaneous formation of Zr O P bonds with fluorescent DNA to achieve a highly sensitive fluorescent readout. The self-supplied H 2 O 2 in the colorimetric detection further improved the self-accuracy of the dual-mode analysis strategy (the accuracy of independent signal readout modes from two different signal transduction mechanisms). This multifunctional PPG probe avoids the time-consuming assembly of different probes and reduces error accumulation from uncontrollable factors in complex experimental procedures. It allows for the sensitive and accurate detection of deoxynivalenol with excellent limits of detection (5.3 pg/mL for the fluorescent assay and 34 pg/mL for the colorimetric method). Overall, this work demonstrates a viable approach for the construction of a dual-signal biosensing platform based on multifunctional MOF probes for biological analysis.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Ruolan Li,Xingyan Liu,Yacen Tang,Jianning Yu,Ya Chen,Min Fu,Siqi Li,Youzhou He
In this study, a highly efficient bifunctional porphyrin-based MOFs with uniformly in-situ generated g-C 3 N 4 quantum dots (g-CNQDs) was fabricated for photocatalytic hydrogen evolution and NO removal, in which PtTCPP as the organic ligand and mixed Zr/Ti-oxo clusters as the metal nodes. Compared with most reported Zr-based porphyrin MOFs, the g-CNQDs@Zr-MOFs(Pt)(Zr/Ti) exhibited outstanding hydrogen evolution activity (14511.57 μmol g −1 ) and NO removal rate (31.9 %) under visible light irradiation. The obviously improved photocatalytic performance could be attributed to the significantly enhanced charge separation and transfer rates by the mixed Zr/Ti-oxo clusters via the rapid Ti 3+ /Ti 4+ process. Moreover, the uniformly in-situ generated g-CNQDs via confinement effect in the cavity of MOFs could also improve the utilization of visible light especially through the up-conversion effect, and promote charge carriers separation. This work provides an idea for us to expand the scope of light utilization and promote charge transfer and separation rates of MOFs via functionalizing host MOFs matrix and coupling guest active species to improve photocatalytic performance further.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 9.2
Dong-Chu Lu,Juan Xie,Yuan Gao,Cheng-Xin Li,Shan-Lin Zhang
The TEC of BFZYZ is lower to 13.8 × 10 −6 1/K, matching well with the electrolyte. • Y and Zn co-doping enhances hydration ability and surface oxygen vacancies. • BFZYZ yields an R p of 0.26 Ω cm 2 at 600 °C, 50% lower than that of BFZ. • PCFC with BFZYZ electrode achieved peak power density of 0.8 W/cm 2 at 600 °C. • The cell with BFZYZ electrode operates stably for 500 h. Developing active and durable oxygen electrodes for both oxygen reduction and oxygen evolution reactions at low temperatures remains a major challenge for proton ceramic electrochemical cells (PCECs). Herein, a cobalt-free Y and Zn co-doped Ba(Fe,Zr)O 3−δ perovskite (BFZYZ) is developed as a PCEC oxygen electrode, integrating excellent electrochemical performance and durability. At 600 °C, Y and Zn co-doping reduces the polarization resistance by 50%, mainly owing to enhanced hydration capability and surface oxygen exchange, which accelerate ORR/OER kinetics. Meanwhile, BFZYZ shows a lower average thermal expansion coefficient of 13.8 × 10 −6 1/K over 30–600 °C, improving its thermal compatibility with the electrolyte. The PCEC with BFZYZ electrode achieves a peak power density of 0.8 W/cm 2 in fuel cell mode and a current density of 0.82 A/cm 2 at 1.3 V in steam electrolysis mode at 600 °C, with stable operation, demonstrating the potential of BFZYZ for high-performance and durable PCECs.
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Sustainable Chemistry and Pharmacy
·
2023
·
IF 6
Qiuyun Zhang,Yaping Wu,Xingyue Hong,Zhenying Li,Yanting Lei,Rongfei Yu,Taoli Deng,Yutao Zhang,Peihua Ma
Different ligand functionalized bimetallic organic framework ((Zr/Ce)UiO-66- X ( X = H, NO 2 , NH 2 and (OH) 2 ) solids-supported phosphotungstic acid (HPW) has been fabricated through a facile impregnation process, and used in the esterification of methanol with oleic acid (OA). The obtained composites were characterized by FTIR , XRD, NH 3 -TPD, SEM-EDS, N 2 adsorption-desorption isotherm, TG , Py-FTIR, and XPS. The characterization analysis shows that the HPW/(Zr/Ce)UiO-66-NO 2 composite possesses the proper catalytic features, such as the greatest number of both strong Brønsted and Lewis acid sites, wider pores, relatively high surface area, and the existence of synergistic catalytic effects between HPW and (Zr/Ce)UiO-66-NO 2 framework. In the screening, the maximum OA conversion rate using (Zr/Ce)UiO-66-NO 2 , HPW/(Zr/Ce)UiO-66-NO 2 , HPW/(Zr/Ce)UiO-66, HPW/(Zr/Ce)UiO-66-NH 2 , HPW/(Zr/Ce)UiO-66-(OH) 2 catalysts is 13.7%, 91.6%, 81.6%, 80.7%, and 72.6% at 110 °C for 3 h, respectively. Moreover, the HPW/(Zr/Ce)UiO-66-NO 2 catalyst presents the better reusability over four cycles. Besides these, the HPW/(Zr/Ce)UiO-66-NO 2 catalyzed esterification reaction is estimated to have an activation energy of 33.7 kJ/mol. This present study provides an effective route for realizing biofuel production on an industrial scale involving heteropolyacids/bimetallic MOFs synergistic catalysts.
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ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Junning Wang,Yujie Zhou,Minqian Zeng,Yanhong Zhao,Xiaoxin Zuo,Fanrong Meng,Fang Lv,Yu Lu
Recently, metal-organic frameworks (MOFs) have great potential as an emerging peroxide-mimicking enzyme, and the improvement of its enzyme-like activity is desired. There are few studies on improving the peroxidase-like activity of MOFs by using the strategy of size reduction. Moreover, it is challenging to enhance the activity of Zr-based MOFs with peroxidase-mimicking activity by size reduction strategy. In this work, the synthesis of Zr-based MOFs capped with polyvinylpyrrolidone (Zr-MOF-PVP) was firstly reported to reduce crystal size of peroxidase-mimicking enzyme for enhanced catalytic activity . Using the 3,3′,5,5′-Tetramethylbenzidine (TMB) as substrate, the synthesized Zr-MOF-PVP nanocomposites with nanosize (about 45 nm) possessed obviously enhanced peroxidase-like activity compared with the pristine Zr-MOF. Based on the above, the Zr-MOF-PVP was also successfully applied in constructing colorimetric detection. By using hydrogen peroxide (H 2 O 2 ) and phenol as the model analytes, the satisfactory detection performance was obtained, indicating that the proposed method had an attractive application prospect in the field of peroxidase-related detection. Besides, this work also provided a new perspective for improving the catalytic activity of nanozymes.
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Jing Xia,Yanxin Gao,Gang Yu
The adsorptive removal of tetracycline (TC) was studied with three types of zirconium-based metal–organic frameworks (Zr-MOFs), UiO-66, NU-1000 and MOF-525. The adsorption kinetics best fitted with the pseudo-second-order kinetic model and the adsorption equilibrium was rapidly reached within 40 min on UiO-66 and NU-1000, and 120 min on MOF-525. The adsorption isotherms best fitted with Sips model, and the maximum Sips adsorption capacities of TC on UiO-66, NU-1000 and MOF-525 were 145 mg·g −1 , 356 mg·g −1 and 807 mg·g −1 respectively, which were much higher than common adsorbents. The X-ray photoelectron spectra measurements and the influence of pH suggested that the π-π interaction played a crucial role during the adsorption. Pore characteristics and topology of MOFs showed great effect on adsorption performance. The cages whose size match well with TC helped MOF-525 to get highest adsorption amount per surface area among MOFs we studied. The proper topology of NU-1000 contributed to its high adsorption rate. River water was also used to confirm the excellent adsorptive performance of these three Zr-MOFs in practical application. These results might aid us to comprehend the adsorption of TC on Zr-MOFs and expand the application of Zr-MOFs in water treatment for removal of emerging contaminants.
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