JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2018
·Vol. 102
·期 5
·2415-2425
·
IF 2.956
Jingyuan Chu,Yue Zhao,Guangyu Jiang,Wei Wu,Zhiwei Zhang,Zhiyong Hong,Zhijian Jin
Tuning substrate properties is an effective methodology to modulate the texture development of MgO films deposited by ion beam-assisted deposition (IBAD) process for epitaxial oxide films. Herein, a solution deposition planarization (SDP) technique is employed to deposit Gd-Zr-O layer for engineering surface properties of the flexible metal substrate. The correlation between the Gd-Zr-O thin film microstructure and the IBAD-MgO texture is investigated. The coordinated study on atomic force microscopy (AFM) and reflection high-energy electron diffraction (RHEED) reveal that the grain coarsening during high-temperature sintering negatively influences the texture formation of IBAD-MgO. Moreover, the chemical environment of the atoms on the surface of Gd-Zr-O seed layer also plays a critical role, which is normally overlooked. The X-ray photoelectron spectroscopy (XPS) analysis indicates that the carbon residue and intermediate phase result in the poor texture of the IBAD-MgO. This phenomenon is related to the partial decomposition and synthesis reactions due to the lower sintering temperature or reduced surface to volume ratio. We demonstrate the high-quality texture of IBAD-MgO layer, deposited on mono-coated thick Gd-Zr-O film, by using optimal heat-treatment conditions. The cross-sectional TEM images present the dense Gd-Zr-O film with Gd 2 Zr 2 O 7 nanograins. The multifunctionalities, such as planarization, a barrier layer, and seed layer, of Gd-Zr-O layers are realized in full-stacked CeO 2 /LaMnO 3 /IBAD-MgO/SDP-Gd-Zr-O/C276 samples. This work demonstrates a route for simplifying the architecture of 2G-HTS using Gd-Zr-O layer and explores the effect of the surface properties on texture formation in IBAD-MgO layer.
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高影响因子
JOURNAL OF THE CHINESE CHEMICAL SOCIETY
·
2018
·Vol. 65
·期 11
·1398-1406
·
IF 0.862
Ruiying Wang,Jianjia Wang,Huimin Zi,Haijun Wang,Yongmei Xia,Xiang Liu
Three novel heterogeneous Zr-containing organic–inorganic hybrid catalysts were prepared for the transfer hydrogenation of biomass-derived ethyl levulinate (EL) to γ-valerolactone (GVL) with isopropyl alcohol (IPA) as the hydrogen donor and were characterized by Fourier transform infrared (FT-IR), Temperature-programmed desorption (TPD), Thermogravimetry (TG), X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET), energy dispersive X-ray spectroscopy (EDX), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). On their basis, the effects of temperature, time, the amount of catalyst, and the solvent were investigated on the yield of GVL. A GVL yield of 96.5% with 99% EL conversion was obtained using Zr-Pg, which was prepared by the reaction of ZrCl 4 and phloroglucinol (Pg) in N , N -dimethylformamide (DMF) at room temperature. The high catalytic activity may be attributed to the strong basicity, which was increased by the sufficient quantity of phenate in the structure of Zr-Pg. Meanwhile, Zr-Pg could be efficiently and easily recycled at least five times without any notable loss of activity and selectivity. Through the results of comparative experiments and characterization, we propose a plausible reaction mechanism for the high activity of Zr-Pg.
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高影响因子
Catalysis Science & Technology
·
2018
·Vol. 8
·期 10
·2624-2635
·
IF 5.365
Jingxia Tian,Wei Chen,Peng Wu,Zhirong Zhu,Xiaohong Li
A Cux–Mgy–Zrz/SiO2 catalyst with a total metal loading of 60 wt% prepared by a deposition–precipitation method was applied for the selective hydrogenation of ethylene carbonate to methanol and ethylene glycol in a fixed-bed reactor. As a result, the Cu8–Mg1–Zr0.47/SiO2 catalyst furnished 99% ethylene carbonate conversion with 85% selectivity to methanol and 99% selectivity to ethylene glycol under the optimized reaction conditions. Moreover, the Cu8–Mg1–Zr0.47/SiO2 catalyst also showed a good lifetime and neither the activity nor the selectivity decreased the during 208 h test. The reaction was found to depend sensitively on the Cu particle size, the surface acidity and the catalyst surface composition. The synergistic effect of balanced Cu0 and Cu+ sites was considered to play a critical role in attaining high yields of methanol and ethylene glycol. Boric oxide also had a positive effect on the hydrogenation of ethylene carbonate, affording higher selectivity to methanol under much milder conditions.
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高影响因子
CATALYSIS COMMUNICATIONS
·
2018
·
IF 3.463
Qinqin Wang,Mingyuan Zhu,Haiyang Zhang,Caixia Xu,Bin Dai,Jinli Zhang
Zr-modified ZSM-5 zeolite was successfully prepared, and Zn/Zr-ZSM-5 was employed as a catalyst for the acetylene hydration reaction. High catalytic activity, above 96% C 2 H 2 conversion, was achieved at 260 °C with a feed reactant ratio of H 2 O/C 2 H 4 = 4 and a GHSV of 90 h −1 . To understand the influence of zirconium addition in the zeolite, Fourier-transform infrared spectroscopy, X-ray diffraction, surface texture analysis (BET method), transmission electron microscopy, temperature programmed desorption of NH 3 , temperature programmed reduction by hydrogen and X-ray photoelectron spectroscopy techniques were used. The incorporation of zirconium in the zeolite enhanced Zn metal dispersion and metal–support interactions. Moreover, an enhanced concentration of weak acid sites and active catalytic sites were found to be responsible for the high catalytic activity of Zn/Zr-ZSM-5 for the acetylene hydration.
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高影响因子
COLLOID AND POLYMER SCIENCE
·
2025
·
IF 2.3
Zhang Fei,Xie Mingzhu,Zhao Jing
With the rapid development of nanotechnology, nanocarriers play an important role in achieving precise drug delivery and controlled release. Among them, nanoscale metal organic frameworks (NMOFs) have shown great potential due to ultra-high specific surface area, controllable size, tunable structure and open metal sites. The aim of this study is to enhance the multifunctionality of UiO-66-NH 2 NMOFs, such as physiological stability, biocompatibility, pH responsiveness, and targeting, by post-synthetic modification with hyaluronic acid-dopamine (HA-DA) functional material. The structure, size, and morphology were characterized by IR, XRD, DLS, and SEM, and the stability, drug-loading capacity, controlled release, and biocompatibility under different conditions were evaluated. The results showed that the particle size distribution and surface properties were improved after modification. This modification not only enhanced the stability in physiological environment, but also accelerated drug release in the acidic environment and improved drug bioavailability, which was of great significance for targeting acidic microenvironments. Cytotoxicity experiments further showed that the introduction of HA-DA effectively reduced the cytotoxicity and provided more suitable environment for cell growth. This study can achieve responsive release, alleviate inflammatory response, and promote tissue repair, especially for sports injuries, which provides a new approach for developing efficient and safe drug delivery systems. Graphical abstract Based on the structural properties of NMOF, a UiO-66-NH 2 NMOF drug delivery system was constructed by the post-synthetic modification of hyaluronic acid-dopamine (HA-DA). This kind of drug delivery system exhibits excellent stability and biocompatibility, and achieves responsive release, which may alleviate inflammatory response and promote tissue repair. This study provides a new approach for developing efficient and safe drug delivery systems.
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GREEN CHEMISTRY
·
2017
·Vol. 19
·期 20
·4829-4837
·
IF 9.125
Yufei Sha,Zhenhuan Xiao,Huacong Zhou,Keli Yang,Yinmin Song,Na Li,Runxia He,Keduan Zhi,Quansheng Liu
With the increasing demands for energy and carbon resources, exploration of novel utilization approaches of fossil resources and promotion of the conversion of sustainable resources become critical issues facing human society. In this study, we used humic acids (HAs), which are important derivatives from the low-rank coal, and the transition metal zirconium (Zr) to construct novel Zr-containing catalysts (Zr-HAs) for Meerwein–Ponndorf–Verley (MPV) reactions of biomass-derived platforms. Both commercial HAs and HAs extracted directly from lignite without any purification were used as raw materials to prepare the catalysts. The results showed that Zr-HAs catalysts were highly efficient for the conversion of furfural, with a high furfuryl alcohol yield of up to 97%, and also effective for the conversion of other carbonyl compounds with different structures under mild conditions. This novel strategy to construct catalysts using HAs as raw materials may be beneficial for both value-added utilization of low-rank coal and the conversion of biomass resources.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2016
·
IF 4.836
Shunlong Pan,Jiansheng Li,Gaojie Wan,Chao Liu,Wenhong Fan,Lianjun Wang
In this work, Fe 3 O 4 @Zr(OH) x yolk–shell nanospheres (YSNs) were synthesized via a two-step process and further examined as adsorbents for the removal of Pb(II). To understand the hollow structure on the adsorption properties of Pb(II), another adsorbent without hollow cavities, i.e., Fe 3 O 4 @SiO 2 @Zr(OH) x core–shell nanospheres (CSNs), was also prepared for comparison. The adsorption results showed that Fe 3 O 4 @Zr(OH) x YSNs exhibited 41.6% higher Pb(II) adsorption capacity as compared to that of Fe 3 O 4 @SiO 2 @Zr(OH) x CSNs. The isotherm was well fitted to Langmuir adsorption model with q max value of 310.8 mg/g after normalized by the weight of Zr in Fe 3 O 4 @Zr(OH) x YSNs. Scanning transmission electron microscopy (STEM) mapping results revealed that the existence of cavities between Fe 3 O 4 cores and Zr(OH) x shells is responsible for the improved adsorption performance. XPS analysis indicated the surface hydroxyl groups played a key role in the Pb(II) adsorption. The removal efficiency of Pb(II) was maintained above 90% in five consecutive adsorption–desorption cycles.
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PubMed
高影响因子
CHEMOSPHERE
·
2024
·
IF 8.1
Chengqiang He,Yue Sun,Yingpeng Gu,Hongyu Ji
Generally, the pH of fluorinated groundwater or many industrial wastewater is neutral, while the majority of metal-modified adsorbents can work efficiently only under acidic conditions. In this study, we synthesized a novel hybrid adsorbent, Mg–Zr-D213, by loading nano-Mg/Zr binary metal (hydrogen) oxides in a strong-base anion exchanger, D213, to enhance the adsorption of fluoride from neutral water. Mg–Zr-D213 exhibited a better fluoride-removal capacity in neutral water than monometallic modified resins. Under the interference of competing anions and coexisting organic acids, Mg–Zr-D213 exhibited superior selectivity. The Langmuir model indicated that the fitted maximum sorption capacity of Mg–Zr-D213 was 41.38 mg/g. The results of column experiments showed that the effective treatment volume of Mg–Zr-D213 was 8–16-times higher than that of D213 for both synthetic groundwater and actual industrial wastewater, and that NaOH–NaCl eluent could effectively recover more than 95% of fluoride. Adsorption experiments with Mg/Zr metal (hydrogen) oxide particles and D213 separately demonstrated a synergistic effect between –N + (CH 3 ) 3 and Mg/Zr metal (hydrogen) oxide particles. The ligand exchange or metal-ligand interaction of Mg/Zr metal (hydrogen) oxide particles on fluoride was further demonstrated via X-ray photoelectron spectroscopy. Overall, Mg–Zr-D213 has great potential for enhanced fluoride removal in neutral water.
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高影响因子
Journal of Water Process Engineering
·
2024
·
IF 6.3
Fangfang Liu,Mengnan Lu,Xiao Yang,Yuedi Wang,Chunmei Wang,Xiaomin Dou
This work proposed introducing nanoscale Fe-Zr oxides onto the layered-surfaces of MXene carriers to maintain well dispersion and anchoring stabilization. The results indicated that Fe-Zr oxide/MXene has a superior adsorption capacity of 209.1 mg/g at pH 7.0. The mass transfer of antimonite onto Fe-Zr oxide/MXene was investigated by numerical solving the homogeneous surface diffusion model. The external mass transfer coefficient ( k f ) and surface diffusion coefficient ( D S ) were determined to be 6.48 × 10 −4 and 1.86 × 10 −8 cm/min, respectively, and the latter was rate-limited. The 2-D profiles of Sb(III) diffusion within the adsorbents were visualized. Data mining and knowledge discovery using machine learning models indicated that the gradient boosting regression (GBR) model successfully predicted the test datasets. The operational conditions outweigh adsorbent properties in capacity prediction, and equilibrium concentration and adsorbent dose, are the most two important features. Using the trained GBR model, the Sb(III) adsorption capacities of MXene (Ti 3 C 2 ) and Fe-Zr/MXene were well predicted. This work provides insights on understanding the mass transfer mechanisms of Sb(III) in functionalized-MXene adsorbents and employing machine learning models for tuning the treatments for better achievements.
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高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2024
·
IF 8
Yijun Chen,Meina Cheng,Long Jin,Hailiang Yang,Sanjian Ma,Zixia Lin,Guoliang Dai,Xin Liu
The Fenton reaction is recognized as an effective technique for degrading persistent organic pollutants , such as the emerging pollutant trimethoprim (TMP). Recently, due to the excellent reducibility of active hydrogen ([H]), Pd–H 2 has been preferred for Fenton-like reactions and the specific H 2 activation of Pd-based catalysts. Herein, a heterogeneous Fenton catalyst named the hydrogen-accelerated oxygen reduction Fenton (MHORF@UiO-66(Zr)) system was prepared through the strategy of building ships in the bottle. The [H] has been used for the acceleration of the reduction of Fe(III) and self-generate H 2 O 2 . The systematic characterization demonstrated that the nano Pd 0 particle was highly dispersed into the UiO-66(Zr). The results found that 20 mg L −1 of TMP was thoroughly degraded within 90 min in the MHORF@UiO-66(Zr) system under conditions of initial pH 3, 30 mL min −1 H 2 , 2 g L −1 Pd@UiO-66(Zr) and 25 μM Fe 2+ . The hydroxyl radical as well as the singlet oxygen were evidenced to be the main reactive oxygen species by scavenging experiments and electron spin resonance . In addition, both reducing Fe(III) and self-generating H 2 O 2 could be achieved due to the strong metal-support interaction (SMSI) between the nano Pd 0 particles and UiO-66(Zr) confirmed by the correlation results of XPS and calculation of density functional theory. Finally, the working mechanism of the MHORF@UiO-66(Zr) system and the possible degradation pathway of the TMP have been proposed. The novel system exhibited excellent reusability and stability after six cyclic reaction processes.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 42
·18166-18176
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IF 2.7
Jing Xiao,Linshan Peng,Ailan Ouyang,Xin Mo,Yiping Yao,Chunyan Wang,Chunpei Yan
A phosphonate-functionalized Zr@FMA material was prepared in this work as an adsorbent for the efficient recovery and enrichment of Th(IV) from aqueous solutions. The adsorbent, prepared by functionalizing Zr@FMA with alendronate sodium (ALS), a well-known active bisphosphonate, demonstrates good water stability and a large surface area, making it suitable for the separation and enrichment of Th(IV) in aqueous solutions. A comparison of the adsorption behavior of Th(IV) on Zr@FMA-ALS with the unfunctionalized Zr@FMA reveals that the introduction of phosphonate groups significantly enhances the maximum adsorption capacity and rate of Zr@FMA-ALS. The adsorption data aligns well with the Langmuir isotherm model, suggesting a uniform distribution of Th(IV) on the adsorbent surface in a monolayer coverage. Thermodynamic analysis indicates an endothermic and spontaneous adsorption process. Zr@FMA-ALS also shows excellent selectivity for Th(IV) over other metal ions in mixed solutions. Insights into the adsorption mechanism are provided through SEM, XPS, and FT-IR analyses, indicating that ALS molecules play a crucial role in capturing Th(IV) on the surface of Zr@FMA-ALS.
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高影响因子
Journal of Water Process Engineering
·
2024
·
IF 6.3
Yijun Chen,Hailiang Yang,Sanjian Ma,Meina Cheng,Zixia Lin,Long Jin,Xin Liu
As a representative antibiotic, trimethoprim (TMP), the emerging pollutant has been frequently detected in water bodies, and its potential harm has aroused the attention of society. Although the emerging pollutant could be efficiently degraded by the advanced oxidation process (AOP) represented by the Fenton reaction , both the problem of iron sludge disposal and the safe use of H 2 O 2 have plagued the further promotion of this technology. The H 2 (precursor of the active hydrogen [H]) and catalyst Pd/UiO-66(Zr) were introduced into the Fenton reaction in this paper. It was found that the process of reducing Fe(III) and self-generating H 2 O 2 could be facilitated due to the reduction of [H]. Under certain reaction conditions (initial pH 3, trace total iron 25 μM, H 2 30 mL·min −1 , catalyst 2 g·L −1 ) and without H 2 O 2 , a Fenton-like system was constructed, named MHORF-UiO-66(Zr). While achieving zero iron sludge discharge, 100 % of 20 mg·L −1 TMP was rapidly degraded within 1 h. It was found that the degradation of TMP could be attributed to the attack of singlet oxygen and hydroxyl radical . Furthermore, the performance changes of catalyst before and after six rounds of reactions were studied and it was found that Pd/UiO-66(Zr) had excellent and stable catalytic performance.
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