CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zhuoyao Fang,Siyuan Pan,Xiaolin Zhang,Lu Lv,Bingcai Pan
Efficient removal of As(III) from groundwater remains an urgent but still challenging task. The X-Mn (X = Fe, Zr, Al…) binary oxide nanoparticles enable simultaneous oxidation and sequestration of As(III), yet facing the challenges in facile synthesis of the ultra-small nanoparticles with extraordinary decontamination reactivity, and in effective regeneration of oxidation capability. Herein, we prepared a novel nanocomposite Zr-Mn@N201 by conducting stepwise precipitation of hydrated oxides of zirconium (HZO) and manganese (HMO) inside the commercial gel-type anion exchanger N201, i.e. , the quaternary ammoniated poly(styrene-co-divinylbenzene) bead. Owing to restriction of nanopores, the HZO/HMO inside N201 possessed an ultra-small size around 4.78 nm. The kinetics and spectroscopic results suggested that As(III) was transformed into As(V) by HMO prior to adsorption onto HZO, and the negatively charged HMO captured most of the produced Mn 2+ ions. Alkaline treatment could regenerate Zr-Mn@N201 through simultaneously desorbing As(V) and transforming Mn 2+ into HMO again. During a 10-cyclic adsorption-regeneration assay, Zr-Mn@N201 could steadily reduce As(III) from 500 μg/L to < 10 μg/L with negligible HMO loss (<0.3%) in each run. In fixed-bed assays, the integration of HMO increased the effective treatment amounts of the Zr-Mn@N201 column toward the realistic groundwater by ∼ 11.5 times over the single nano-HZO ( i.e. , HZO@N201) column, reaching to ∼ 4600 bed volume with < 1% HMO loss.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Qinzhi Wang,Yijian Zhao,Zhan Shi,Xinyu Sun,Tong Bu,Changqiu Zhang,Zexiang Mao,Xiaohan Li,Li Wang
Azo dyes in soft drinks present a serious risk to human health and are strictly limited in many countries. Herein, we demonstrate that covalent-organic framework (COF) can be facilely grown on magnetic metal–organic framework (MOF) to form three kinds of porous Fe 3 O 4 @MOF(M = Fe, Ti, Zr)@COFs composites for efficient azo dyes adsorption. Adsorption performances of Fe 3 O 4 @MOF(M = Fe, Ti, Zr)@COFs toward azo dyes were systemically investigated by adsorption kinetics , adsorption isotherms and adsorption thermodynamics. Under optimized conditions, the maximum adsorption capacities of both Fe 3 O 4 @MOF(Fe)@COF and Fe 3 O 4 @MOF(Zr)@COF for Congo red (CR) are 1250.02 and 625.13 mg g −1 , and the Fe 3 O 4 @MOF(Ti)@COF for Chrysoidine (CYD) is 294.12 mg g −1 , all which are higher than those of mostly previous reports. Furthermore, possible mechanisms of adsorption were revealed through Fourier-transform infrared spectra and X-ray photoelectron spectroscopy analysis. These Fe 3 O 4 @MOF(M = Fe, Ti, Zr)@COFs composites also present good biocompatibility, and exhibit high adsorption capacities for CR or CYD in soft drinks, which can be suggested as effective adsorbents for the azo dyes removal from soft drinks.
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Metals
·
2025
·Vol. 15
·期 3
·307
·
IF 2.5
Ziyang Ruan,Zifan Zhao,Jing Feng
Rare-earth tantalates (RETaO4) are considered as a type of emerging thermal barrier coating materials applied to the hot components of gas turbines and aerospace engines due to their excellent thermal stability, high-temperature fracture toughness, corrosion resistance and extremely low thermal conductivity. However, the relatively low hardness and thermal expansion coefficients may limit their service lifetime in a harsh engine environment. To address the current limitation of rare-earth tantalates and further optimize the mechanical and thermal properties, the defective fluorite-structured Y₂Zr₂O₇ (YZ) was introduced as a second phase into the YTaO4(YT) matrix to form YT1−x–YZx(x = 0, 0.25, 0.5, 0.75, 1) composite ceramics in this work. The mechanical and thermal properties of YT1−x–YZxcomposite ceramics are significantly improved compared to pure-phase YTaO4ceramics. The Vickers hardness of YT1−x–YZx(x = 0.25, 0.5, 0.75) composite ceramics is 9.1~11.3 GPa, which are 2~2.5 times higher than that of YTaO4(4.5 GPa). Among them, YT0.75–YZ0.25exhibits a maximum fracture toughness (3.7 ± 0.5 MPa·m1/2), achieving a 23% improvement compared to YTaO4(3.0 ± 0.23 MPa·m1/2) and a 118% improvement compared to Y2Zr2O7(1.73 ± 0.28 MPa·m1/2). The enhancement is attributed to the combined effect of the intrinsic strengthening of the second phase, as well as the residual stress and grain refinement caused by the introduction of a second phase. Additionally, the thermal expansion coefficients of YT1−x–YZxcomposite ceramics at 1673 K range from 10.3 × 10⁻⁶ K⁻1to 11.0 × 10⁻⁶ K⁻1, which is also higher than that of YTaO4(10.0 × 10−6K−1). Consequently, the superior mechanical and thermal properties indicate that YT–YZ composite ceramics possess promising application prospects for thermal barrier coatings.
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 10
·5875-5884
·
IF 10.7
Hui Guo,Yifeng Li,Lulu Jiang,Yenan Sha,Shihang Guo,Donglin Han
Proton conducting oxides are attracting increasing attention due to their promising application as electrolytes in solid-state electrochemical devices for energy conversion and chemical production, including protonic ceramic fuel cells, electrolyzers and membrane reactors. BaZrO3 and Ba(Zr,Ce)O3 substituted by acceptor dopants are currently the most promising proton conductors. In principle, replacing Zr or Ce with one kind of trivalent element (e.g., Y or Yb) can generate oxygen vacancies, which are necessary for the hydration reaction to introduce charge carriers of protons. However, it is commonly recognized that substituting Zr or Ce with Y and Yb simultaneously leads to high performance of the devices, but the reason is not clear. In this work, we studied the transport properties of four different compositional classes: BaZr0.8−xCexY0.2O3−δ (BZCY20), BaZr0.8Y0.2−xYbxO3−δ (BZYYb), BaZr0.1Ce0.7Y0.2−xYbxO3−δ (BZCYYb) and BaCe0.8Y0.2−xYbxO3−δ (BCYYb), at 600, 650 and 700 °C. For BZCY20, the ionic conductivity decreases on replacing Zr in BZY20 with x = 0.1 of Ce, increases with increasing Ce content within x = 0.1–0.5, and decreases on further increasing Ce content from x = 0.5 to 0.8. The ionic transport number increases with increasing Ce content. The ionic conductivity, partial conductivity of oxide ions and hole conductivity of BZCYYb and BCYYb increase with increasing Yb content. Since the increment of hole conductivity is larger, the ionic transport number decreases. For BZYYb, the ionic conductivity decreases and the hole conductivity increases with increasing Yb content, leading to decreasing ionic transport number. Both the high ionic conductivity and transport number are vital factors governing the performance of protonic ceramic cells (PCCs). Therefore, the improved performance of PCCs by adding both Y and Yb into the electrolyte cannot be explained from the viewpoint of electrical properties of the electrolytes. Thereby, we summarized our recent series of studies on the chemical compatibility between the electrolyte and NiO negatrode substrate, and suggested that the loss of dopant was suppressed by partly replacing Y with Yb. The high ionic conduction of the electrolyte can be maintained after co-sintering at high temperature to fabricate PCCs. This might be the real reason for the high performance of the devices using Y and Yb co-substituted electrolytes, prepared by the co-sintering method.
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Materials Today Communications
·
2025
·
IF 4.5
Xiaojing Liu,Chonghe Xu,Lin Wang,Rongchao Jiang,Liguang Yang,Wenyu Yang,Xuetao Yue
Ceramic fibers have emerged as a promising candidate for advanced thermal insulation applications due to their exceptional thermomechanical properties and chemical resistance. In this work, Mg(-Al/Zr)-Si ceramic fibers were successfully prepared via electrospinning technology using a dual-source precursor strategy, combining magnesium citrate complex and metal chlorides as metal oxides precursors. The crystalline phase formation, thermal decomposition behavior, microstructure, and properties of the fibers were systematically investigated using X-ray diffraction (XRD), thermogravimetric-differential scanning calorimetry (TG-DSC), Fourier transform infrared spectroscopy (FT–IR), and scanning electron microscopy (SEM). The heterogeneous sol precursor notably influenced the fiber crystallization process and facilitated more gradual thermal decomposition, as evidenced by reduced weight loss rates. Consequently, the Mg(-Al/Zr)-Si ceramic fibers maintained good structural integrity after exposure to 1200 °C. Moreover, the incorporation of aluminum or zirconium enhanced the tensile strengths of fibers (heat treated at 800 °C) to 1.56–1.79 MPa, representing a significant improvement over pure magnesium silicate fibers. Furthermore, the fibers exhibited good thermal insulation performance with low room-temperature thermal conductivity values ranging from 0.0282 to 0.0333 W·m −1 ·K −1 , further highlighting their suitability for high-temperature insulation applications. These findings underscore the significant potential of the developed fibers for use in high temperature thermal management and insulation systems.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2026
·Vol. 47
·期 1
·118754
·
IF 6.3
Junyao Wu,Sai Liu,Shenxiang Luo,Jinwei Guo,Haonan Shi,Fan Zhang,Wang Zhu
High-entropy A 6 B 2 O 17 (A = Hf, Zr; B = Ta, Nb)/8YSZ double-layer ceramic coatings with three compositions are fabricated by atmospheric plasma spraying (APS). Thermal cycling tests are performed at 1150 °C with a 5 min heating hold followed by 5 min air cooling, while isothermal oxidation tests are performed at 1150 °C. Among the three coatings, H 3 Z 1 T 2 N 1 coating exhibits the longest thermal cycling lifetime (1823 ± 153 cycles), followed by the H 1 Z 1 T 2 N 1 coating (1123 ± 136 cycles) and H 1 Z 3 T 2 N 1 coating (826 ± 114 cycles). After 180 h oxidation, the thermally grown oxide (TGO) thicknesses are 5 μm, 5.6 μm, and 6.6 μm, respectively. The H 3 Z 1 T 2 N 1 coating possesses the lowest oxidation rate constant ( k p = 0.1263 μm 2 ·h −1 ). This superior performance is attributed to dense vertical cracks induced by higher thermal expansion, which relieve thermal stress, suppress oxygen ingress, and delay interfacial failure.
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JOURNAL OF CHROMATOGRAPHY A
·
2026
·
IF 4
Mingjie Guo,Weihong Xie,Suling Zhang,Xiaofei Li,Jianwei Zhang,Zhongshi Xu,Ying pan,Dong zhang,Lulu Xu,Ting Lü,Linlin Qiu
Etomidate and its analogs can produce euphoria and addiction, and their recent abuse has led to an increasing number of poisoning and fatal cases. Thus, they are classified as controlled psychotropic drugs. This work proposed small-sized wood aerogel-supported zirconium metal-organic framework (UiO-66) particles for the extraction of trace etomidate and its analogs from urine and e-cigarette samples. Owing to the removal of lignin and hemicellulose, the delignified wood aerogel exhibited enhanced internal pore structures and exposed functional groups, which facilitated the immobilization of more UiO-66 crystals and achieved a high loading efficiency of 61.3 %. The lightweight UiO-66/wood aerogel composite enables facile separation, avoiding UiO-66 powder leakage while retaining its adsorption capacity. The composite was mechanically stable and kept commendable reusability over nine consecutive cycles. Benefiting from its high specific surface area and multiple chemical interactions with target drugs, the extraction method achieved enrichment factors of 22.9–30.0. Key factors influencing extraction—including solution pH, extraction time, the type and volume of desorption solvent, and desorption time—were investigated. Under the optimal conditions, the UiO-66/wood aerogel-based micro-solid phase extraction coupled with GC–MS method showed wide linear ranges and good precision (1.1%–3.2% for intra-day; 3.4%–5.1% for inter-day). The limits of detection and quantification were in the range of 0.02–0.04 μg/L and 0.05–0.1 μg/L, respectively. The recoveries for the urine and e-cigarette oil samples ranged from 86.2%–110.2% and 80.1%–107.9%, respectively. This method is eco-friendly, simple, and sensitive for the determination of new psychotropic drugs in clinical and forensic applications.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Zihao Sun,Lin Dai,HuanHuan Li,Ning Ma,Lengyuan Niu,Yinyan Gong,Can Li
A mechanistic design paradigm beyond the conventional high-entropy effect is established. • Short-range ordering and electronic redistribution synergistically optimize OER kinetics. • Element-specific functional assignment enables efficient and stable oxygen evolution. The development of non-noble metal electrocatalysts with high intrinsic activity and long-term durability for the oxygen evolution reaction (OER) remains a major challenge. Herein, we report a series of FeCoNiMoZr high-entropy oxides (HEOs) synthesized via a sol-gel method, and systematically investigate the synergistic effects of high-valent Zr incorporation and sintering temperature on the structural, electronic, and catalytic properties. Comprehensive characterization reveals that the optimal HEO-Zr 1.5 -T 600 achieves a unique local optimization window where localized nanocrystalline domains coexist with a disordered matrix. It exhibits exceptional OER performance in 1.0 M KOH, with low overpotentials of 219/279 mV at 10/100 mA cm −2 , a small Tafel slope of 48.3 mV dec −1 , and an 18-fold enhancement in turnover frequency compared to its counterparts. Furthermore, it demonstrates remarkable long-term stability (4.7% current decay over 100 h) and a high Faradaic efficiency of 90.7%. Results suggest distinct functional roles for the constituent elements, Zr and Mo primarily regulate macroscopic structural distortions, framework stability, and electronic redistribution, while Fe, Co, and Ni serve as the principal active centers. This work moves beyond the generic high-entropy effect to establish a design paradigm: rational enhancement in HEOs arises from an element-specific, functionally complementary catalytic architecture within a compositionally and thermally defined local optimization window. Download: Download high-res image (166KB) Download: Download full-size image
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APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Wenmei Wuxia,Yu Chen,HuanHuan Li,Ning Ma,Lengyuan Niu,Yinyan Gong,Can Li
Zr 4+ incorporation drives a complete transition to an amorphous phase and increases the electrochemically active surface area. • Zr 4+ incorporation induces a downward shift in the core-level binding energies of Fe, Co, and Ni sites. • Optimized S-CrMnFeCoNiZr 1.5 specimen achieves overpotentials of 240/287 mV at 10/100 mA/cm 2 . • S-CrMnFeCoNiZr 1.5 specimen exhibits outstanding stability and a 16-fold enhancement in TOF relative to S-CrMnFeCoNi specimen. Developing efficient and durable electrocatalysts for oxygen evolution reaction (OER) is pivotal to advancing renewable energy conversion technologies. Herein, a series of amorphous CrMnFeCoNi-based high-entropy compounds (HECs) with varied Zr content were synthesized, and the role of Zr doping in modulating the atomic/electronic structures were investigated, as well as the OER activity. Experimental characterization reveals that Zr 4+ incorporation drives a complete transition to an amorphous phase, increases the electrochemically active surface area, and induces a downward shift in the core-level binding energies of Fe, Co, and Ni. Relative to the Zr-free analogue, the optimized catalyst S-CrMnFeCoNiZr 1.5 delivers a 57/69 mV reduction in overpotential at 10/100 mA cm −2 , exhibits a 17-fold higher turnover frequency, and maintains exceptional operational stability over 72 h. This OER activity outperforms most previously reported HECs. Density functional theory calculations corroborate these observations, demonstrating that Zr doping upshifts the d-band centers of Fe, Co, and Ni, thereby strengthening adsorption of intermediates and optimizing the free-energy profile for the rate-determining steps. Collectively, this study establishes a rigorous structure–electronic property–performance correlation and demonstrates Zr-mediated electronic modulation as a rational, scalable strategy for engineering high-entropy electrocatalysts. Download: Download high-res image (70KB) Download: Download full-size image
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Reaction Kinetics Mechanisms and Catalysis
·
2026
·
IF 2.1
Wang Jiahao,Liu Feng,Xie Lei,Yang Hailiang,Ma Sanjian,Lin Zixia,Liu Xin,Wang Suqin
Refractory wastewater treatment via Fenton reactions is hindered by iron sludge. Herein, fluorinated UiO-66(Zr)-F4 was employed as a hydrogen-storage carrier to confine Pd⁰ catalytic centers, and an [H]-mediated (H 2 -precursored) Fenton-like system was constructed for carbamazepine degradation under ambient conditions. With 25 μM Fe 2 + and 60 mL min⁻ 1 H 2 flow, 53% carbamazepine removal was achieved in 1 h via ⋅OH/ 1 O 2 oxidation, and > 59% efficiency was retained over six 3-h cycles. However, [H]-driven hydrogen spillover reduced C-F bonds, causing a 92.3% drop in specific surface area that compromised long-term stability. It was concluded that fluorination is suboptimal; modulating the carrier’s hydrophobicity via electron-donating groups (instead of fluorination) is critical for stable Zr-MOF-based catalysts in [H]-assisted advanced oxidation, offering alternative perspectives for process optimization. Graphical abstract
The alternative text for this image may have been generated using AI.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Jiacong Wu,Juan Han,Yanli Mao,Lei Wang,Yi Wang,Yuanyuan Li,Yun Wang
A metal–organic frameworks (MOFs) with adjustable mesopores was prepared through bionic mineralization using protein as template in this paper. By regulating the content of bovine serum, pore structures of different sizes (6.46, 7.55, 10.80 nm) were obtained, used for the immobilization of enzymes (HRP, laccase and cellulase). It was found that the UIO-66 with a pore size of 6.46 nm exhibited the highest loading capacities for the investigated three enzymes. Under optimized conditions for immobilization, the maximum loading capacity of HRP, laccase and cellulase was 205.7, 214.2 and 203.9 mg g −1 , respectively. It should be noted that the stabilities of the three immobilized HRP@UIO-66, laccase@UIO-66 and cellulase@UIO-66 were significantly improved due to the favorable fitting between the pore size of the carrier material and the enzyme molecular size. In particular, the substrate affinity of the immobilized HRP@UIO-66 (0.120 g L −1 ) is similar to that of free HRP (0.122 g L −1 ). It is mainly due to that the appropriate porous structure of the carrier could avoid the obstruction of the substrate mass transfer channel after the adsorption of enzyme molecules. Moreover, the porous structure has a certain enrichment effect on the substrate, which promotes the catalytic efficiency of immobilized enzymes.
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Foods
·
2023
·Vol. 12
·期 4
·707
·
IF 5.2
Linzhi Li,Xiaofeng Wang,Jian Chen,Tianzeng Huang,Hongmei Cao,Xing Liu
In this study, an electrochemiluminescence (ECL) immunosensor based on nanobody heptamer and resonance energy transfer (RET) between g-C3N4(g-CN) and NU-1000(Zr) was proposed for ultrasensitive ochratoxin A (OTA) detection. First, OTA heptamer fusion protein was prepared by fusing OTA-specific nanometric (Nb28) with a c-terminal fragment of C4 binding protein (C4bpα) (Nb28-C4bpα). Then, Nb28-C4bpα heptamer with the high affinity used as a molecular recognition probe, of which plenty of binding sites were provided for OTA-Apt-NU-1000(Zr) nanocomposites, thereby improving the immunosensors’ sensitivity. In addition, the quantitative analysis of OTA can be achieved by using the signal quenching effect of NU-1000(Zr) on g-CN. As the concentration of OTA increases, the amount of OTA-Apt-NU-1000(Zr) fixed on the electrode surface decreases. RET between g-CN and NU-1000(Zr) is weakened leading to the increase of ECL signal. Thus, OTA content is indirectly proportional to ECL intensity. Based on the above principle, an ultra-sensitive and specific ECL immunosensor for OTA detection was constructed by using heptamer technology and RET between two nanomaterials, with a range from 0.1 pg/mL to 500 ng/mL, and the detection limit of only 33 fg/mL. The prepared ECL-RET immunosensor showed good performance and can be successfully used for the determination of OTA content in real coffee samples, suggesting that the nanobody polymerization strategy and the RET effect between NU-1000(Zr) and g-CN can provide an alternative for improving the sensitivity of important mycotoxin detection.Keywords:Nb28-C4bpα heptamer;electrochemiluminescence immunosensor;resonance energy transfer;ochratoxin A
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