JOURNAL OF SOLID STATE CHEMISTRY
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2012
·
IF 2.159
Si-Fu Tang,Xiao-Bo Pan,Xiao-Xia Lv,Xue-Bo Zhao
A new multifunctionalized phosphoric acid , (2-(diphosphonomethylamino)nicotinic acid, Py(COOH)(NHCH(PO 3 H 2 ) 2 ), H 5 L 1 ), has been employed as ligand for the construction of new metal phosphonates . By reacting it with different metal chlorides under hydrothermal condition, three new transition metal phosphonates, namely, [Co 2 (H L 1 )(H 2 O) 5 ][H 2 O] 3 ( 1 ), Zn(H 3 L 1 ) ( 2 ) and [Cd(H 3 L 1 )(H 2 O) 2 ][H 2 O] ( 3 ) were successfully obtained. The single-crystal structure measurements indicated that the coordination mode of ligand H 5 L 1 is metal-dependant and results in different structures. For compound 1 , it features 2D layered structure. Whereas compounds 2 and 3 have 1D chain structures. Under the excitation of 250 nm light, both compounds 2 and 3 show intraligand and ligand to metal charge transfer (LMCT) emission bands at about 415 and 420 nm, respectively. Magnetic study shows that compound 1 displays antiferromagnetic behavior.
研究领域:
化学
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材料科学
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DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Shuhui Sun,Chao Shan,Zhichao Yang,Shu Wang,Bingcai Pan
Phosphonate is an important category of highly soluble organophosphorus in contaminated waters, and its oxidative transformation into phosphate is usually a prerequisite step to achieve the in-depth removal of the total phosphorus. Currently, selective oxidation of phosphonate into phosphate is urgently desired as conventional advanced oxidation processes suffer from severe matrix interferences. Herein, we employed 1-hydroxyethylidene-1,1-diphosphonic acid (HEDP) as a model phosphonate and demonstrated its efficient and selective oxidation by the Cu(II)/H2O2 process at alkaline pH. In the presence of trace Cu(II) (0.020 mM), 90.8% of HEDP (0.10 mM) was converted to phosphate by H2O2 in 30 min at pH 9.5, whereas negligible conversion was observed by UV/H2O2 or a Fenton reaction (pH = 3.0). The oxidation of HEDP by Cu(II)/H2O2 was insignificantly affected by natural organic matters (10.0 mg TOC/L) and various anions including chloride, sulfate, and nitrate (10.0 mM). The complexation of Cu(II) with HEDP coupling Cu(III) produced in situ enabled an intramolecular electron transfer process, which features high selective oxidation. Selective degradation of HEDP was further validated by adding stoichiometric H2O2 into an industrial effluent, where the existing Cu(II) could serve as the catalyst. This study also provides a successful case to trigger selective oxidation of trace pollutants of concern upon synergizing with the nature of the contaminated water.
研究领域:
环境科学
·
水处理技术
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jinglin Zhu,Yutao Huang,Juanjuan Peng,Shaomin Liu
Developing simple and effective activation approaches to degrade phosphonate is crucial due to its potential aquatic environmental risks. Recently, Cu(II)-mediated activation processes provide a feasible method via nonradical oxidation mechanism to remove phosphonate, but is yet challenged under neutral conditions. Herein, a strategy for enhancing the Cu(II)/peroxymonosulfate (PMS) process by adding hydroxylamine (HA) could efficiently degrade 1-hydroxyethane1,1-diphosphonic acid (HEDP) at pH = 7.0. After 15-min reaction, 85.7% of total phosphorus (TP) in HEDP transformed into PO 4 3− in the Cu(II)/PMS/HA process is observed, which is 3.4 times than that in the Cu(II)/PMS process. The results of multiple experiments confirm that the presence of HA accelerates the reduction of Cu(II) and the generation of reactive species, SO 4 •− and Cu(III) induced intramolecular electron transfer as the primary reactive species play a significant role in the degradation of HEDP. Additionally, the removal of HEDP is inhibited with the addition of Cl − and HCO 3 − in the Cu(II)/PMS/HA process. However, the Cu(II)/PMS/HA process demonstrates a superior removal effectiveness of HEDP in different actual wastewater samples compared to the Cu(II)/PMS process under neutral conditions. This study provides an effective method for removing phosphonate from actual wastewater.
研究领域:
环境科学
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水处理工程
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DOI
高影响因子
CHEMOSPHERE
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2022
·
IF 8.943
Chaocheng Zeng,Huimin Hu,Chao Wang,Qing Shi,Qiwu Zhang,Mengfei Chen,Qian Wang,Tingting Zhang
Due to the stable chelating effect of organic phosphonates in wastewater, phosphonates with increasing emission are difficult to be removed effectively by traditional ferric salt flocculation , which has posed tough challenges for reducing total phosphorus pollution in recent years. In this work, calcium carbonate (CaCO 3 ) was introduced to work together with the widely investigated flocculant of ferric chloride (FeCl 3 ) to realize an efficient removal of nitrilotrismethylenephosphonic acid (NTMP) at much lower dosage of FeCl 3 . With an aid of synergy effect from together use of CaCO 3 and FeCl 3 , the remaining concentration as low as 0.16 mg−P/L, far below the sewage discharge limit (0.5 mg−P/L), was simply obtained with a significantly reduced Fe/P molar ratio at only 4, resulting from calcium source donor to form more stable Fe–Ca–P tridentate bridging complexes, high affinity towards ferric ions on CaCO 3 surface and slow-release alkaline from CaCO 3 . A comparison among sodium hydroxide (NaOH), calcium hydroxide (Ca(OH) 2 ) and CaCO 3 as additives, was carried out to highlight the advantages of using CaCO 3 and clarify the mechanism for the greatly improved performance by a set of characterizations including XRD, FTIR, Zeta potential , XPS , SEM−EDS and TG analyses. The addition of CaCO 3 in ferric flocculation resulted in further obvious advantages such as 75% shortened settling time and only one−third of sludge volume of the precipitant, beneficial to the sample handling in engineering application. The proposed new approach has been further confirmed to work efficiently on real phosphonate-containing wastewater. Discussion on the interaction between CaCO 3 and ferric salts in phosphonate solutions shed new insights into the working mechanism of using CaCO 3 for the treatment of phosphonates-containing wastewater.
研究领域:
环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF DRUG DELIVERY SCIENCE AND TECHNOLOGY
·
2025
·
IF 4.9
Jiayu Li,Huanfan He,Jun Zhu,Shujing Li,Yifan He,Ze Zhang,Xiaojing Pei
Nanoemulsions (NE) are attractive for cosmetic applications due to ensure improved steadiness and efficient penetration of bioactive components, leading to enhanced efficacy. Hydroxypinacolone Retinoate (HPR) is an ingredient with great potential in combating the effects of aging, but its formulation is often unstable. In order to improve the solubility, bioavailability and stability of HPR, two kinds of oil-in-water (O/W) nanoemulsions were developed by high-pressure homogenization technology. These two nanoemulsions used GTCC and dimethyl isosorbide as the oil phase, respectively, which leads to different properties. Average particle size was (101 ± 0.02 nm) (72 ± 0.03 nm), Zeta potential was (-16.23 ± 0.15) (-18.21 ± 0.02). Particle size, polydispersity index, and potential were recorded for seven different conditions, which showed good physical and chemical stability over 90 days. Compared to free HPR, the retention of NE at 60 days under light and 45 °C was improved by 10% (G-NE) and 8% (D-NE), respectively. Encapsulation resulted in improved stability and bioavailability of HPR. In the in vitro diffusion cell assay, the skin retention of the two nanoemulsions was 17.02 μg/mL and 29.17 μg/mL, which was much higher than that of the free HPR, which was 4.08 μg/mL (P<0.01). Both the erythrocyte hemolysis test and the human patch test showed that the nanoemulsion reduced the stimulation of HPR. This study provides a practical method to increase the utilization of HPR in cosmetic formulations, thereby improving efficacy.
研究领域:
化妆品科学
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药剂学
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生物医学工程
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DOI
高影响因子
WATER RESEARCH
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2023
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IF 12.8
Sainan Sun,Meng Qiao,Guanghua Huang,Junke Zhang,Bo Yang,Xu Zhao
Phosphonate used as scale inhibitor is a non-negligible eutrophic contaminant in corresponding polluted waters. Besides, its conversion to orthophosphate (ortho-P) is a precondition for realizing bioavailable phosphorus recovery. Due to the feeble degradation efficiency with less than 30 % from classical Fenton commonly used in industrial wastewater treatment and itself vulnerable to strong inhibition interference of matrix chloride ions, we proposed an electrochemical approach to transform the native salt in the solution into oxidizing substances, sort of achieving beneficial utilization of matrix waste, and enhanced the ortho-P conversion rate of 1-Hydroxyethane-1,1-diphosphonic acid (HEDP) to 89.2 % (± 3.6 %). In electrochlorination system, it was found that HEDP rapidly complexed with Fe(II) and then coordinated in-situ Fe(III) to release free HEDP via intramolecular metal-ligand electron transfer reaction. The subsequent degradation mainly rooted in the oxidation of pivotal reactive species HClO, Fe IV O 2+ and 1 O 2 , causing C-P and C C bonds to fracture in sequence. Eventually the organically bound phosphorus of HEDP was recovered as ortho-P. This study acquainted the audiences with the rare mechanism of chloridion-triggered HEDP degradation under electrochemical way, as well as offered a feasible technology for synchronous transformation of organically bound phosphorus to ortho-P and elimination from phosphonates.
研究领域:
环境科学
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废水处理
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电化学工程
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Xing Yan,Jieshu Qian,Shu Wang,Xiaolin Zhang,Yanyang Zhang,Bingcai Pan
Phosphonates, featuring organic skeletons binding phosphonic acid group, are ubiquitous in wastewaters and natural waters. Highly efficient removal of trace phosphonates is desirable to ensure the water quality and to prevent eutrophication. Commercially available hyper-cross-linked resins modified by amino groups have been proved to exhibit preferable adsorption of various organic acids from aqueous systems via synergetic effect of various interactions (electrostatic interaction, van der Waals interaction, π-π interaction, etc.) but seem relatively ineffective for phosphonates. In this study, we proposed a new strategy via coupling a commercial resin NDA88 with nanoconfinement of Hydrated ferric oxide (HFO) for selective removal of phosphonates. The resultant HFO@NDA88 shows an adsorption capacity of 15.0 mg P/g towards a model phosphonate (nitrilotris(methylenephosphonic acid)), higher than those of the NDA88 host (7.9 mg P/g) and the bare HFO (7.4 mg P/g). Remarkably, compared to NDA88 and HFO, HFO@NDA88 exhibits much higher resistance to the interference of various anions and other substances at much greater levels, particularly the organic analogue nitrilotriacetic acid and phosphate. Such superior selectivity is believed to result from the cooperative contributions of the host NDA88 as well as the embedded nano-HFO. Moreover, HFO@NDA88 shows excellent reusability and satisfactory performance in fixed-bed water treatment. This work provides a rational design of nanocomposite adsorbents for highly selective removal of phosphonates from complicated water matrix.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
CEMENT & CONCRETE COMPOSITES
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2024
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IF 10.8
Jingjie Wei,Changle Fang,Bo Zhou,Zhuorui Wu
The strong early hydration reaction and short setting time of alkali-activated slag composites limit its practical engineering application . Compared with traditional chemical admixture , organic phosphates show higher efficiency in delaying the hydration rate of alkali-activated slag system . However, there is limited research on the performance of alkali-activated materials modified by different organic phosphonate type, and their modification mechanism is also unclear. In this study, three typical organic phosphonates, hydroxyethylidene diphosphonic acid Tetrasodium (HEDP-4Na), aminotris (methylene phosphonic acid) tetrasodium (ATMP-4Na), and diethylenetriamine penta (methylene phosphonic acid) pentasodium (DTPMP-5Na), were selected to clarify the effect of organic phosphonate type on the properties of alkali-activated slag materials (AASM) and its mechanism under different dosage and alkali content . The results indicate that DTPMP-5Na has the most significant effect on the improvement of fresh properties of AASM, compared to other two types of organic phosphonates. Using 0.3 % DTPMP-5Na can delay the initial and final setting time of AASM by 240 % and 190 % respectively, increase the slump flow by 20 %, and reduce yield stress and plastic viscosity by 57 % and 65 % respectively. This was because DTPMP-5Na has the largest number of monomolecular phosphonic acid groups, which can chelate Ca 2+ in AASM, form stable complex and cover the surface of slag particles to prevent further hydration reaction . The phosphonate reduced the hydration rate and increased the surface negative potential of slag particles. The use of phosphonates and the increase in alkali content can significantly enhance the mechanical properties of AASM. Using 0.3 % of ATMP-4Na increased the 28-day compressive and flexural strengths of AASM made with 5 % alkali content by 155 % and 53 %, respectively, compared to the reference AASM with 3 % alkali content. Additionally, the 28-day compressive and flexural strengths of reference at 7 % alkali content increased by 115 % and 12 %, respectively, compared to that at 3 % alkali content. This improvement was mainly attributed to the consumption of organic phosphonates at the early stage, which provides more activation channels for slag later, resulting in a denser structure and improved pore structure of AASM, thus enhancing its long-term mechanical properties. However, with the increase of alkali content, the effect of organic phosphonates in strengthening fresh and hardened properties of AASM decreased. The use of 0.3 % HEDP-4Na increased 28-day compressive and flexural strengths of AASM with 3 % alkali contents increased by 25 % and 27 %, respectively, compared to the reference AASM. Such improvement was limited to 4 % and 19 % for AASM made with 5 % alkali content. This can be attributed to the significant promotion of OH − concentration in the system, increasing the yield of hydration products at early age on the surface of slag, and reduced activation channels for slag over the long term. In summary, the use of ATMP-4Na is recommended in AASM, as it can significantly improve the fresh properties of AASM and provide excellent mechanical properties.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
DALTON TRANSACTIONS
·
2018
·Vol. 47
·期 32
·11226-11238
·
IF 4.099
Hailong Xu,Hong Zhou,Lu Feng,Qiaoyun Wang,Rui Chen,Wentao Huang,Xixi Wu
Six coordination polymers of metal phosphonates, [Co3(HL)2(H2O)4]·2H2O (1), [Cu(H2L)H2O] (2), [Fe3(L)2(H2O)3OH]·2H2O (3), [Cu2(L)(4,4′-bipy)1.5]·5H2O (4), [Co(H2L)(4,4′-bipy)0.5] (5), and [Ni(H2L)(4,4′-bipy)0.5] (6) (H4L = 4-F-C6H4CH2N(CH2PO3H2)2), have been synthesized by hydrothermal methods and structurally characterized by X-ray single-crystal diffraction, infrared spectroscopy, elemental analysis and thermogravimetric analysis. Complexes 1–3 exhibit a 2D inorganic layer structure with a regular and alternate arrangement of metal ions and PO3 groups, where the layers are connected by moderately strong hydrogen bonds to form a supramolecular 3D network. Complexes 4–6 have a one-dimensional chain structure connected through similar coordination modes with 1–3, where each chain is rejoined by 4,4′-bipy bridges, forming layer coordination polymers. In addition, three complexes contain abundant water molecules, which exhibit different aggregation modes, clusters and chains, respectively. The magnetic properties of complexes 1–6 have been quantificationally studied using the Curie–Weiss law and the PHI program package.
研究领域:
无机化学
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材料科学
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物理化学
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产品关联
DOI
PubMed
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2016
·Vol. 32
·期 3
·605-610
·
IF 0.844
CHEN Feng-Feng,DONG Yan,SANG Xiao-Yan,ZHOU Yan,TAO Duan-Jian
Four tetrabutylphosphonium carboxylate ionic liquids ([P4444][CA]) were prepared, and their densities, viscosities, refractive indices, and conductivities were measured and correlated with thermodynamic and empirical equations in the temperature range of 298.15-348.15 K.
The influence of temperature on these four properties of [P4444][CA] was discussed, and their thermal expansion coefficient values were calculated. The CO2 absorption capacity of [P4444][CA] was studied at 313.15 K and 100 kPa. The results indicated that [P4444][Buty]
had the highest CO2 capture capacity among these ionic liquids, with an absorption capacity of 0.4 mol·mol-1 and balance time of less than 5 min.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Jiazhi Yang,Xuejun Long,Xiaonan Feng,Jun Wan
Orthophosphate and phosphonate are the main phosphorus (P) species in membrane concentrate, and they should be removed before discharge to prevent eutrophication in the aquatic environment. A variety of factors affect orthophosphate and phosphonate removal performance, while their contribution to the sorption process in the complex environment was not clear. In this study, the novel kaolin/lanthanum carbonate (KLC) composites were prepared for the simultaneous sorption of phosphate and phosphonate, and their surface morphology and crystal structure were characterized. The sorption kinetics and isotherms results indicated the competitive sorption of orthophosphate and phosphonate on the surface of KLC. The two phosphorus species’ maximum sorption capacities were both achieved at the equilibrium pH around 4.9, and the ionic strength showed negligible effect on their sorption capacity. The sorption capacities and rates were applied to explore the effects of sorbent dosage, pH and co-existing ions on the sorption process. To predict the simultaneous orthophosphate and phosphonate removal performance under different conditions, a multi-objective artificial neural network (ANN) model was established based on seven input variables (dosage, reaction time, pH, and concentrations of SO 4 2- , HCO 3 - , Ca 2+ and Mg 2+ ). The model was trained with experimental data, and could well predict the orthophosphate and phosphonate removal efficiency. In addition, the relative significance of these variables was also evaluated. This study provides a reliable ANN model to predict simultaneous orthophosphate and phosphonate removal, and insights into factors for phosphorus removal by Lanthanum-based sorbent.
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2013
·
IF 2.206
Duan-Jian Tao,Fan Ouyang,Zhang-Min Li,Na Hu,Zhen Yang,Xiang-Shu Chen
Four tetrabutylphosphonium carboxylate ionic liquids ([P4444][CA]) were prepared, characterized, and used as catalysts for the synthesis of propylene glycol methyl ether (PGME) from the alcoholysis reaction of propylene oxide (PO) with methanol. The effects of various parameters such as the kind of ILs, temperature, reaction time, catalyst loading, and molar ratio of the reactants on PGME yield and selectivity were also studied in detail. The results indicated that tetrabutylphosphonium butyrate ([P4444][Buty]) exhibited the best catalytic activity in comparison to three other carboxylate ILs, and PGME was produced in nearly 94% yield under mild conditions. In addition, [P4444][Buty] was found to exhibit good catalytic activities and selectivities in other alcoholysis reactions of epoxides with various alcohols, such as PO with n-propanol, PO with n-butanol, 1-(allyloxy)-2,3-epoxypropane with methanol, and 1,2-epoxybutane with methanol. [P4444][Buty] could also be recovered easily and used repetitively at least 10 times without an obvious decrease in activity and quantity. Therefore, [P4444][Buty] proved to be an effective recyclable homogeneous catalyst for the synthesis of PGME and showed potential application in industry.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）