Small
·
2025
·
IF 12.1
Jiajie Xu,Tenghui Jin,Wei Qu,Kaizhou Huang,Zhiyu Liu,Ping Zhang,Jiaping Paul Chen
Development of high-performance photocatalysts for persulfate activation is often limited by rapid electron–hole recombination and insufficient quantum efficiency. To overcome the challenges, electronic metal–support interaction (EMSI) structure is designed. The innovative structure has several key benefits: recombination rates are significantly reduced, charge separation is enhanced, and content of active sites and intrinsic catalytic activity are increased. ZrO 2 /Co 3 O 4 bimetallic oxides featuring a synergistic Co─O─Zr EMSI coordination are synthesized via a sol-gel method. Strong EMSI effects markedly modulate and stabilize the Co 3d electronic structure, creating an electron-rich center on Co sites to promote persulfate activation, and an electron-deficient center on Zr sites to adsorb atrazine. The Gibbs free energy analysis reveals that Zr incorporation reduces the overpotential of oxygen evolution reaction, thereby facilitating electron transfer, promoting hole consumption and suppressing charge recombination. More importantly, it promotes the generation of reactive oxygen species—predominantly via a singlet oxygen ( 1 O 2 )-dominated non-radical mechanism. The optimized catalyst achieves 97.3% degradation of atrazine (a model compound) under visible light, outperforming commercial catalysts (e.g., 4.5-fold of Co 3 O 4 ). The work elucidates the cooperative mechanism of dual-site engineering and EMSI-mediated electron redistribution, providing a rational strategy for designing efficient photocatalysts toward sustainable advanced oxidation processes.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Longjiang Jiang,Kaikai Ba,Yanhong Lin,Dejun Wang,Meng Cui,Tengfeng Xie
The extensive solid-liquid interface between the photoanode and the electrolyte solution impedes the kinetics of the oxygen evolution reaction (OER), resulting in a photoelectrochemical (PEC) water splitting efficiency that falls short of theoretical predictions. In this study, by depositing a metal-phytate complex (CoCu-PA) coating onto Ti, Zr co-doped Fe 2 O 3 via a hydrothermal method, we successfully fabricated a CoCu-PA/Ti,Zr:Fe 2 O 3 composite photoanode for water oxidation. Various characterization techniques and electrochemical analyses indicated that Ti, Zr co-doping enhanced the conductivity of Fe 2 O 3 . More importantly, owing to the highly hydrophilic property of CoCu-PA, the charge transfer resistance at the interface between the composite photoanode and the solution is significantly reduced. Furthermore, a built-in electric field was formed within the photoanode, facilitating the rapid migration of photogenerated charges and their efficient injection into the electrolyte to participate in the OER. As a result, the CoCu-PA coating enhanced the OER kinetics of the composite photoanode and led to a photocurrent density of 3.4 mA/cm 2 . This study offers new insights into the design of composite photoanodes to improve charge migration efficiency both within the bulk material and at the solid-liquid interface.
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高影响因子
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2025
·
IF 6.2
Feihong Li,Lei Zheng,Zhanjun Liu,Mingyu Zhang,Qizhong Huang
This work delves into the fascinating transformation from organic precursors to dense SiC-modified (Ti, Zr, Hf)C solid solution ceramics. Nanocrystalline powder was crafted through an innovative sol-gel process coupled with carbothermal reduction, followed by spark plasma sintering (SPS) to obtain the multi-phase ceramics. The results indicate that the addition of silicone alkoxide is required for forming a robust multi-phase gel network, which facilitates the formation of oxide intermediates (e.g., ZrSiO 4 , HfSiO 4 ), accelerates phase transformation, and inhibits grain from coarsening by encapsulating Ti/Zr/Hf compounds while reinforcing grain boundaries. After pyrolysis at 1400 °C, the precursors gradually evolved into a highly crystalline, medium-entropy solid solution. The optimal sintered composite achieves a relative density of 97.8 % and an open porosity of 0.4 %. The mechanical properties were improved by induced lattice distortion and effect of fine-grained strengthening with the incorporation of SiC. Nanoindentation tests reveal that the hardness and elastic modulus of the (Ti, Zr, Hf)C-SiC composite reach 22.39 GPa and 342.78 GPa, respectively.
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高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Jinjie Hou,Pei Jia,Kairong Yang,Tong Bu,Shuang Zhao,Longwen Li,Li Wang
As a special heavy metal ion, copper ions (Cu2+) play an indispensable role in the fields of environmental protection and safety. Their excessive intake not only easily leads to diseases but also affects human health. Therefore, it is particularly important to construct a facile, effective, and highly selective Cu2+ probe. Herein, a novel Zr–tetraphenylporphyrin tetrasulfonic acid hydrate (TPPS) metal–organic framework (ZTM) was fabricated using TPPS as the ligand and exhibited strong red fluorescence with a high quantum yield of 12.22%. In addition, we designed a ratiometric fluorescent probe by introducing green fluorescein isothiocyanate (FITC), which was not subject to environmental interference and had high accuracy. When exposed to different amounts of Cu2+, the fluorescence emission at 667 nm from ZTMs is remarkably quenched, while that at 515 nm from FITC is enhanced, accompanied by a change in the solutions’ fluorescence color from red to green under a UV lamp. Besides, the ZTMs solutions display an excellent ratiometric colorimetric response for Cu2+ and produce an obvious color change (from green to colorless) that is visible to the naked eye. The fabricated ZTMs@FITC fluorescent probe exhibits distinguished performance for Cu2+ detection with linear ranges of 0.1 to 5 μM and 5 to 50 μM, as well as a low detection limit of 5.61 nM. Moreover, a colorimetric sensor based on ZTMs exhibits a good linear range from 0.1 to 20 μM for Cu2+ with the detection limit of 4.96 nM. Furthermore, the dual-signal ratiometric sensor has significant specificity for Cu2+ and is successfully applied for monitoring Cu2+ in water samples, which proves its practical application value in the environment and biological systems.
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高影响因子
ENERGY
·
2022
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IF 8.857
Xiaopeng Shi,Pan Li,Xianhua Wang,Jiande Song,Shuqi Fang,Chun Chang,Shusheng Pang
The main purpose of this work was to explore the effect of metal modified biochar and multi-catalysts on improving the quality of products by microwave pyrolysis (MVP) of biomass. Single-component catalysts and multi-catalysts were prepared by Zn/Zr impregnation methods. The prepared catalysts were evaluated by XRD , BET, FT-IR and SEM. The properties, composition and product distribution of bio-oil and bio-syngas were analyzed. The results showed that ZSM-5 obtained more bio-oil (42.16 wt%) at the expense of gas product yield, and BC obtained the highest gas yield (43.10 wt%). Zn promoted the selectivity of aromatic hydrocarbons in bio-oil, Zr could effectively improve the yield of syngas and upgrading bio-oil, respectively. Zr-modified multi-catalyst was prepared, and the highest syngas yield (91.54 vol%) and aromatic hydrocarbon products were obtained. Among them, the selectivity of monocyclic aromatic hydrocarbons (MAHs) reached 21.82%. The mechanism of MVP of biomass under the effect of Zn/Zr modified different catalysts was proposed. The study has successfully demonstrated an approach for producing high-value bio-oil and bio-syngas from microwave multi-catalyst pyrolytic system.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Chongfu Wu,Zhenhua Sun,Changshen Ye,Zhaoyang Qi,Jie Chen,Zhixian Huang,Ting Qiu
The development of catalysts with excellent performance in oxidative desulfurization (ODS) at room temperature will greatly facilitate the advancement of desulfurization technology. An efficient novel strategy, 4-aminopyridine molecular bridging combined with manual grinding, was presented to encapsulate HPW into UiO-66 for achieving stable loading of PW and to produce abundant defects that contribute to the formation of active complexes with strong oxidation ability. The prepared catalyst showed outstanding catalytic activity in the ODS system, achieving full desulfurization in 15 min at room temperature and a low O/S molar ratio. Further investigations reveal that the synergistic catalytic effect of the faulty UiO-66 and PW is mostly responsible for superior catalytic performance. UiO-66 rich in defects promote the decomposition of H 2 O 2 into radicals, and PW can combine with the radicals to form more stable active peroxide intermediates, then exerting the catalytic ability of ODS at room temperature. Such a synergistic catalytic mechanism provides a guide to improving the oxidation ability of PW-based catalysts at room temperature.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Ning Zhang,Dan Li,Mengyao Mu,Minghua Lu
Increasing the stability of materials and affinity to the target has always been the pursuit. In this paper, the strategy of partially fluorinated metal–organic framework materials (MOFs) was introduced into the field of sample preparation for the first time, and the potential of this method to prepare materials with improved stability and extraction performance against environmental pollutants was verified. The UiO-66-(NH 2 ) 0.58 (4F) 0.42 coating was successfully prepared on carboxyl functionalized stainless steel fiber through covalent bonding method. Owing to the introduction of F element, the UiO-66-(NH 2 ) 0.58 (4F) 0.42 coating exhibited enhanced metal node acidity, hydrophobicity and stability, thus its extraction performance for phthalates (PAEs) was higher than that of pure UiO-66-NH 2 and commercial fiber coatings. The UiO-66-(NH 2 ) 0.58 (4F) 0.42 -coated fiber was coupled with GC–MS to detect PAEs, and the wide linear range (0.03–1000 ng/L), good correlation coefficients (0.9732–0.9998) and low detection limit (0.0039–0.016 ng/L) were obtained. The established method had also been successfully applied to detection of trace PAEs in plastic bags packed milk and bottled liquor with satisfactory recoveries (83.7 ± 5.1–118.1 ± 4.1 %). This research provides a new path for the preparation of environmental pollutant enrichment and removel materials with good performance.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 27
·13021-13029
·
IF 3.925
Xinlei Zhang,Peng Liu,Bohan Li,Xianliang Li,Yan Xu
Hydrogen-bond driven self-assembly of carbon dot-based luminescent materials has been widely studied in the fields of sensor and optoelectronic devices. However, the uniform confinement of carbon-dots (CDs) into crystalline porous materials through hydrogen bond interactions has rarely been reported. Herein, an O-phenylenediamine (O-PD) mediated Zr-based MOF material denoted as CDs@UiO-66(COOH)2 was successfully synthesized via an efficient solvent-free synthetic method. The O-PD molecules were grafted to the structural pyromellitic acid ligands in the UiO-66(COOH)2 framework via H-bonding interactions, and during the subsequent thermal treatment process the O-PD molecules were partially decomposed and converted into luminescent CDs. The resultant CDs@UiO-66(COOH)2 composites retained the crystallinity of UiO-66(COOH)2, and the confined CDs in UiO-66(COOH)2 show excitation-independent stable green emitting properties when dispersed in a variety of solvents. The CDs@UiO-66(COOH)2 composite exhibits excellent chlortetracycline detection performance with high selectivity, anti-interference and low limit of detection (LOD = 0.102 μM) in a wide linear range of 0–100 μM. Also, it shows an excellent stimuli-response in fluorescence intensities toward pH and temperature changes. Acting as an optical thermometer, the maximum relative temperature sensitivity (Sr) is 0.82% °C−1 in the range of 10–80 °C. This work opens a new way for exploring fluorescent CD-integrated MOF composites via a hydrogen-bond driving strategy for multifunctional fluorescent sensing applications.
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高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Xue Ma,Jinghua Zhang,Chong Zhang,Xiaoqing Yang,Ajuan Yu,Yanjie Huang,Shusheng Zhang,Gangfeng Ouyang
Aminothiols are closely related to chronic kidney disease, but little is known regarding levels of related aminothiols in the urine of immunoglobulin A vasculitis with nephritis (IgAVN) patients. Herein, a well-defined core–shell Zr-based metal–organic framework (Zr-MOF) composite SiO2@50Benz-Cys was constructed as a mercury ion affinity material via a solvent-assisted ligand exchange strategy for the selective extraction and enrichment of low-concentration aminothiols in IgAVN patient urine. SiO2@50Benz-Cys was competent to enrich the total glutathione (GSH) and total homocysteine (Hcy) in virtue of the excellent affinity after chelation with mercury ions. The extraction efficiencies were closely related to the pH, dithiothreitol amount, and the dose of functional Zr-MOF. Coupled with HPLC–MS/MS in optimized conditions, GSH and Hcy were determined with low detection limits of 0.5 and 1 nmol L–1, respectively. The recoveries of GSH and Hcy for the urine sample at three spiked levels were in the range of 85.3–105% and 79.5–103%, which showed good precision and accuracy. Benefiting from the matrix interference elimination in the process of extraction, the simultaneous detection of aminothiols in the urine of the healthy group and immunoglobulin A vasculitis (IgAV) and IgAVN patients was successfully carried out, suggesting that the Zr-MOF and the robust method together provided a potential application in the analysis of urinary biomolecules. The analysis of variance (ANOVA) showed that the levels of GSH and Hcy had significant differences between the patients and the control. This work is very valuable as it provides a better understanding of concentration alterations of GSH and Hcy in urine involved with IgAVN for clinical research.
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高影响因子
Catalysis Science & Technology
·
2021
·Vol. 12
·期 3
·894-905
·
IF 6.119
Jihui Yao,Yuzi Rong,Zeyan Gao,Xiaohua Tang,Fei Zha,Haifeng Tian,Yue Chang,Xiaojun Guo
To introduce a hierarchical porous structure into SAPO-34 zeolites and adjust their acid properties and crystalline size, a series of Zr-modified SAPO-34 zeolites (Zrx-SAPO-34 (x = 0.25, 0.50 and 0.75)) with hierarchical porous structure were synthesized by hydrothermal crystallization using palygorskite as a silicon and partial aluminum source, morpholine and tetraethylammonium hydroxide as organic structure directing agents and UiO-66 as a co-template agent. The obtained catalysts were characterized via XRD, SEM, TEM, EDX, N2-adsorption–desorption, NH3-TPD, FTIR, Py-IR, XRF, 29Si MAS NMR and TG analyses. The catalytic performance of Zrx-SAPO-34 in the methanol-to-olefin (MTO) transformation was investigated in a fixed bed reactor. The introduction of a hierarchical porous structure effectively enhanced the diffusion and mass transfer of the reactants/products, prolonging the catalytic lifetime. Additionally, the optimization of the acidity dramatically improved the selectivity for light olefins. Under the reaction conditions wherein the reaction temperature was 400 °C, the feed of WHSV was 2.0 h−1, the mass of the catalyst was 0.5 g and at atmospheric pressure, the Zr0.50-SAPO-34 zeolites exhibited optimum catalytic performance, where the methanol conversion was 100%, the light olefin selectivity was 98.66% and the catalytic lifetime was more than 1500 min.
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
·
IF 4.551
Jun Yao,Ming Xie,Yang Li
In order to protect human health from the threat of excessive acrylamide in heat-processed foods, swift, uncomplicated, highly selective and sensitive online monitoring methods for acrylamide are urgently needed. In this study, a rare earth metal/transition metal-organic frameworks Eu/Zr-MOFs fluorescence sensor with dual-band luminescence was prepared by the solvothermal method for detection of acrylamide in fried potatoes and cookie crumbs. This sensor exhibited two different fluorescence emission peaks at 430 and 615 nm under excitation of 365 nm, and the ratio of fluorescence intensity was linear with the experimental concentration of acrylamide in the range of 1 × 10 −4 to 1 × 10 −3 M. Under the optimal conditions, the proposed fluorescence analysis method showed that the detection limit of acrylamide was as low as 2.4 × 10 −8 M, and the satisfactory recoveries of 94.05–104.04% were obtained for various spiked samples. More importantly, the sensor has ultra-high selectivity for the detection of acrylamide while other small organic molecules hardly interfere with it in the measurement environment. These studies confirmed that the ratiometric fluorescence sensing method was expected to achieve on-line rapid detection of acrylamide in real foods. In addition, the mechanism of Eu/Zr-MOFs sensing of acrylamide was analyzed and discussed in depth, and the analog computation was carried out by Materials Studio software, and the entire sensing system was studied at the micro level in combination with density functional theory.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xiang Li,Xueqian Wang,Li Yuan,Langlang Wang,Yixing Ma,You Wu,Yibing Xie,Rui Cao,Yiran Xiong,Ping Ning
The lengthy processes and cumbersome operations for the separate removal of COS and H 2 S have severely limited the development of blast furnace gas recycling process. CuO exhibits excellent H 2 S oxidation performance, but weak COS hydrolysis performance; in contrast, ZrO 2 shows the opposite trend. However, the functional combination of CuO and ZrO 2 has never been used for simultaneous removal of COS and H 2 S. In this study, a Cu/Zr co-doped K@TiO 2 bifunctional catalyst was tailored to simultaneously remove COS and H 2 S. The combined COS and H 2 S capacity of this catalyst reaches 340.5 mg/g at a low temperature of 60 °C, which is much higher than those of other reported bifunctional catalysts. The microcrystal structure formed by Cu/Zr co-doping increases the specific surface area of the catalyst and promotes the adsorption of COS/H 2 S. Specifically, Zr doping increases the content of moderate basic sites and significantly improves the hydrolysis efficiency of COS. Moreover, Cu doping induces lattice distortion of TiO 2 , while CuO captures 4 s valence electrons of K to form Cu 2 O. These two processes lead to the release of lattice oxygen from TiO 2 and CuO, generating oxygen vacancies and ·O 2 − , which promotes H 2 S oxidation. By proposing a simple route for the bifunctionalization of a desulfurization catalyst, this study drives innovation in both the theory and application of simultaneous removal of COS and H 2 S.
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