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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CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Huilin Lun,Yi Zeng,Xiang Xiong,Houbu Li,Ziming Ye,Xiaoxu Liu
This work introduces fabricating single-phase ternary-anion carbide solid solution via solid-state diffusion of B and N. Initially, non-stoichiometric (Zr,Hf,Ti)C x with carbon vacancies was synthesized by modified spark plasma sintering. Then, using B 2 O 3 and g -C 3 N 4 as sources, (Zr 0.3 Hf 0.5 Ti 0.2 )(C 0.87 B 0.03 N 0.07 ) with face-centered-cubic structure was produced via B diffusion at 1100 °C and N diffusion at 1600 °C. Trace B (0.23 wt%) and N (0.71 wt%) in (Zr 0.3 Hf 0.5 Ti 0.2 )(C 0.87 B 0.03 N 0.07 ) was found to significantly enhance the oxidation resistance (higher onset temperature 520 ± 3 °C (particle size 2.5 ± 1.3 μm) than 475 ± 3 °C of (Zr 0.3 Hf 0.5 Ti 0.2 )C 0.85 and improve structural stability with more negative binding energy.
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JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Yu Liu,Mingyang Xu,Lingxin Zhao,Shufei He,Likui Feng,Liangliang Wei
The dissemination of antimicrobial resistance (AMR) in wastewater treatment poses a severe threat to the global ecological environment. This study explored the effectiveness of photocatalysis in inactivating antibiotic resistant bacteria (ARB) and quantitatively clarified the inhibiting rate of the transfer of antibiotics resistance genes (ARGs). Herein, the magnetic heterojunction as UiO-66-NH 2 @CuFe LDH-Fe 3 O 4 (UN-66@LDH-Fe) effectively facilitated the electron-hole separation and accelerated the photogenerated charge transfer, thereby guaranteeing the stable practical application in aeration tanks. Notably, the internal electric field of heterogeneous photocatalyst resulted in significant increase of ARGs inactivation, achieving 5.63 log of ARB, 3.66 log of tet A and 3.57 log of Ampr genes were photodegraded under optimal reaction conditions within 6 h. Based on the complex microbial and molecular mechanism of multiple-ARB communities inactivation in photo-treatment, the photogenerated reactive oxygen species (ROSs, ·OH and ·O 2 − ) effectively destroyed bacterial membrane protein, thereby the intracellular ROSs and redox cycles further induced oxidative stress, attributing to the abundance reduction of ARGs and their host bacteria. Moreover, long-term (7 days) continuous operation preliminarily verified the practical potential in reducing AMR spread and developing wastewater treatment efficacy. Overall, this study presented an advantageous synergistic strategy for mitigating the AMR-associated environmental risk in wastewater treatment.
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Journal of Physical Chemistry C
·
2025
·
IF 3.2
Xuan Liu,Yujie Yan,Feifei Guo,Liangliang Chang,Zengzhe Xi,Chunsheng Zhou
This study demonstrates a tripartite strategy to significantly enhance the piezo-photocatalytic degradation of ofloxacin (OFL) using modified BTO@BGFZ9 composite nanoparticles. Gd/Zr codoping optimizes the band structure and ferroelectricity of BFO, while heterojunction construction with BTO promotes interfacial charge separation. Corona poling treatment further aligns ferroelectric domains to amplify the piezoelectric field. The optimized 0.4BTO@BGFZ9 composite achieved 88.96% OFL degradation within 120 min under ultrasonic and visible-light synergy with a first-order rate constant of 0.0175 min–1. Mechanistic studies reveal that VO and a type-II heterojunction facilitate the generation of dominant reactive species (•O2– and h+), enabling efficient OFL mineralization via piperazine ring cleavage and defluorination.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2025
·Vol. 46
·期 2
·117844
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IF 6.2
Zhuangzhuang Ma,Yunhao Wang,Tianhao Rui,Yulin Lan,Linyuan Lu,Yang Yu,Mingxuan Deng,Tianxing Lan,Zhekang Zhao,Zhen Teng,Haibin Zhang
High-entropy pyrochlore ceramics with the nominal composition Eu 2 B 2 O 7 , incorporating up to five equiatomic B-site cations, were synthesized via a solid-state reaction method and evaluated their aqueous chemical durability for nuclear waste immobilization. Comprehensive characterization using XRD, Raman, and SEM analyses confirmed the formation of a single-phase pyrochlore structure with uniform and random elemental distribution. However, secondary phases were observed in the Ce- and Nb-doped samples, which is attributed to the larger ionic radius of Ce and the higher valence state of Nb. The 42 days leaching tests revealed normalized element release rates ranging from 10 −5 to 10 −7 g/(m 2 ∙d), significantly lower than those of conventional pyrochlore materials. This enhanced durability is attributed to synergistic effects of electronegativity, ionic radius, and atomic number, which together hinder cation diffusion and strengthen chemical durability at the B site. These findings demonstrate the potential of Eu 2 B 2 O 7 high-entropy pyrochlore ceramics as long-term host materials for high-level radioactive waste. This study provides a valuable resource for enriching the thermophysical properties database of B-site high-entropy pyrochlore solidification, thereby supporting their engineering development.
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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 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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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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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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FUEL
·
2022
·
IF 8.035
Ruolan Li,Zongqian Wu,Ya Chen,Xingyan Liu,Weiwei Guo,Yumin Huang,Min Fu,Youzhou He
An efficient bifunctional porphyrin-based MOF is fabricated for photocatalytic hydrogen evolution and NO removal, in which the mixed Zr/Ti-oxo clusters are the metal nodes and uniformly distributed Pt nanoparticles (Pt NPs) are the co-catalysts. It is worth noting that the optimal Zr-MOF-s(Pt)(Zr/Ti)-R is obtained through replacing partial Zr(IV) with Ti(IV) in the original Zr-based porphyrin MOFs and in-situ generating confined Pt NPs with a relatively small size within the internal cavities. Compared with the majority of reported Zr-based porphyrin MOFs, the Zr-MOF-s(Pt)(Zr/Ti)-R exhibits an extremely high hydrogen evolution activity (2545.11 μmol·g −1 ·h −1 ) and NO removal rate (46.6 %) under visible light irradiation. The excellent photocatalytic performance should be ascribed to the reason that the mixed Zr/Ti-oxo cluster and the in-situ generated Pt NPs significantly promote the rate of charge transfer and separation. Moreover, the photocatalytic NO oxidation process was also monitored by in - situ DRIFTS, which indicates the Zr-MOF-s(Pt)(Zr/Ti)-R could realize the effective oxidation of NO and intermediates to the final product (NO 3 – ). This work provides us with a practical route to further improve the photocatalytic performance by synergistically modifying the original metal clusters to adjust the ligand-to-metal charge transfer efficiency and in-situ introducing metal nanoparticles to form Schottky junctions.
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危险品化学品经营许可证（带存储）