ACS Applied Materials & Interfaces
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2019
·
IF 8.456
Wen Zhang,An Bu,Qingyuan Ji,Luofu Min,Song Zhao,Yuxin Wang,Jing Chen
We report a class of pKa-directed, precise incorporation of phosphonate ligands into a zirconium-based metal–organic framework (Zr-MOF), MOF-808, via ligand exchange. By replacing of formate ligands with methylphosphonic acid (MPA), ethanephosphonic acid (EPA), and vinylphosphonic acid (VPA), whose pKa values are slightly higher than that of the benzenetricarboxylic acid (BTC) linker in MOF-808, daughter MOFs can be synthesized without controlling the stoichiometric amounts of added MPA. The methylphosphonate MOFs (808-MPAs) demonstrate high porosities, with only small changes in the pore diameter and specific surface area when compared with the parent MOF-808. PXRD patterns and structure refinements indicate the expansion of the lattice for all MOFs after decorating with methylphosphonate ligands. The XPS spectra reveal a charge redistribution of the Zr6 node after ligand exchange. FTIR and 31P MAS NMR spectra, combined with DFT calculation, suggest that the methylphosphonate ligand is connected to the Zr6 node as CH3P(O)(OZr)(OH) species with an accessible acidic P–OH group. Besides, 808-MPAs demonstrate excellent chemical stability in concentrated HCl, concentrated HNO3, hot water, and 0.2 mol/L trifluoroacetic acid solutions. Impressively, 808-MPAs show ultrafast adsorption performance for uranyl ions using the ion-exchange property of P–OH sites in their cavity environment, with an equilibrium time of 10 min, much quicker than the previous adsorbents. The present study demonstrates a series of important proof-of-concept examples of the pKa-directed Zr-MOFs with tunable phosphonate-terminated ligands, which can extend to other phosphonate-functionalized Zr-based framework platforms in the near future.
研究领域:
材料科学
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环境科学
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化学工程
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PubMed
高影响因子
Environmental Science-Nano
·
2018
·Vol. 5
·期 7
·1584-1594
·
IF 6.087
Peipei Yang,Qi Liu,Hongsen Zhang,Jingyuan Liu,Rongrong Chen,Rumin Li,Di Wu,Xuefeng Bai,Jun Wang
A novel kind of graphene oxide-based (GO-based) adsorbent was successfully prepared by chemical modification with cetyltrimethylammonium bromide (C16TAB) and phytic acid (PA) for adsorbing uranium (U(VI)). A close relationship between PA and GO interlayer spacing was investigated; the optimal spacing was 3.88 Å with 4.5 mL PA. A series of adsorption experiments were carried out with the as-prepared product (denoted as GO–C16TAB–PA) to capture U(VI) ions. The adsorption capacity of the GO–C16TAB–PA adsorbent can reach 923 mg g−1 (298.15 K) with an excellent removal rate (∼90%), which demonstrates a 527% increment compared with that of pristine GO in the same environment (pH = 8, Co = 500 mg L−1). Meanwhile, the adsorption equilibrium time of GO–C16TAB–PA was shortened by 50% compared with that of pristine GO. In addition, the GO–C16TAB–PA adsorbent exhibited superior recyclability with a six-adsorption–desorption-cycle test. Finally, the fabricated GO–C16TAB–PA adsorbent exhibited excellent adsorption performance in simulated seawater, providing a theoretical guide and methodology for further seawater extraction of uranium(VI).
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
JOURNAL OF MEMBRANE SCIENCE
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2017
·
IF 6.035
Yali Zhao,Zhiguang Zhang,Lei Dai,Suobo Zhang
A novel diacyl chloride monomer dimethyl (3,5-bis(chlorocarbonyl)phenyl)phosphonate (compound(I)) with a phosphonate group (–PO(OCH 3 ) 2 ) was successfully synthesized and then blended with 2,2′,4,4′-biphenyl tetraacyl chloride (BTEC) as organic phase monomers to prepare RO membranes for brackish water desalination. BM-X was utilized to represent RO membranes prepared by compound (I). X represented the concentration percent of compound (I) (%) in Isopar G solutions，which was the ratio of the concentration of compound (I) to the concentrations of compound (I) and BTEC. When X increased from 0% to 50%, the water flux of BM-X improved from 35 L/m 2 h to 79 L/m 2 h while holding high salt rejections (99.1–99.5%). The enhancement of membrane hydrophilicity was certified by the contact angle decreasing from 83° to 38° with compound (I) content increasing from 0% to 50%. Because the improvement of membrane hydrophilicity made for the enhancement of membrane antifouling, BM-50 exhibited a lower water flux decline and irreversible fouling degree compared with a commercial RO membrane (BW30FR, Dow Filmtec). The irreversible fouling degree reached 6.8% after 1500 min three cycles fouling which was lower than 14.1% of BW30FR. Finally, BM-50 showed a very good and stable desalination performance for 30 days measured in a pH=6.0 and 2000 ppm NaCl solution.
研究领域:
材料科学
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环境工程
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DOI
高影响因子
FIRE AND MATERIALS
·
2021
·Vol. 46
·期 1
·130-137
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IF 2.407
Changchen Cai,Qian Sun,Kai Zhang,Xiaoyu Bai,Peng Liu,Aixiang Li,Zijian LYu,Qiuhong Li
Summary Propylene oxide (PO) was used to block polycarboxyethyl phenyl ethylene phosphinate (PCEPEP) synthesized by 2-carboxyethylphenylphosphinic acid (CEPPA) and ethylene glycol (EG) to obtain a reactive phosphonate polyol. The results of chemical titration analysis and Fourier transform infrared spectrum (FT-IR) showed that the end-capping effect was best when the molar ratio of PO to acidic functional groups in PCEPEP was 6:1. Moreover, the obtained phosphorus-containing polyol was used as a reactive monomer to be introduced into thermoplastic polyurethane (TPU) to prepare flame retardant TPU. Cone calorimetry results demonstrated that TPU containing 20 wt% phosphorus-containing polyol showed a reduction of 3.8%, 72.2%, and 39.3% in the peak heat release rate, total heat release and total smoke release, and an increment of 351.9% in mass retention. The addition of phosphonate polyol enhanced the char-forming performance of TPU, which effectively prevented the transfer of combustible gas and heat, and displayed a good flame retardant effect.
研究领域:
材料科学
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高分子化学
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DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
·
IF 5.4
Cuicui Shao,Kai Tuo,Weifeng Hou,Chuyao Liang,Yi Li,Yuxin Sun,Wei Xu,Shuyang Cao,Zhijian Li,Shouzhi Pu,Chunhui Deng
Extraction of uranium represents one of the valuable but challenging processes in the fields of resource recycling and environmental protection. Here, a low-cost and efficient phosphate-based hydrogen-bond organic framework (P-HOF) was designed for the adsorption of uranium with abundant phosphate groups on its surface, exhibiting superior removal performance (Q m = 1066.0 mg g −1 ) for uranium. It had high selectivity and good recyclability for U(VI) in simulated seawater, and after five adsorption-desorption cycles, the adsorption capacity of uranium decreased slightly, but it can still be maintained at more than 80 %. Impressively, P-HOF demonstrated excellent uranium removal capabilities across a wide pH range, with removal rates exceeding 70 % even under acidic conditions (pH = 1), and the P-HOF adsorbed 7.58 mg g −1 of uranium from natural seawater under 13 days. This work indicates that the phosphonate-based P-HOF could be utilized as a promising adsorbent for the effective removal of uranium from seawater.
研究领域:
材料科学
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环境科学
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核能技术
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
·
IF 4.539
Lili Liang,Hao Zhang,Xiaoyan Lin,Kaiyin Yan,Mengsha Li,Xunhai Pan,Yang Hu,Yan Chen,Xuegang Luo,Ran Shang
Although various kinds of adsorbents have good uranium adsorption capacity, they still meet the challenge in capturing uranium under highly acidic condition. Therefore, efficiently extracting uranium under strong acidic condition become the pursuit of researchers. In this study, a new phytic acid decorated porous organic polymers (POPs) named MA-U-PA was prepared by synthesizing a organic framework (MA-U) using melamine and uracil and with subsequent phytic acid modification. The results showed that the excellent stability of the prepared organic framework and strong uranium chelating ability of phytic acid endowed the as-prepared material being an excellent adsorbent under strong acidic condition. The adsorption capacity achieved 106.7 mg·g -1 at the pH of 1 which was much higher than that of MA-U and most of other adsorbents. The study of modification mechanism confirmed that the hydrogen bonds interaction of phytic acid with MA-U lead to the successful modification. In addition, the phosphonate groups of PA was mainly the active groups chelated with uranium. Moreover, the uranium adsorption process of MA-U-PA was in accordance with the pseudo-second-order kinetic and Langmuir isothermal model. The newly prepared phytic acid decorated porous organic material could achieve efficient uranium capturing from highly acidic nuclear wastewater.
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
FIRE AND MATERIALS
·
2017
·Vol. 42
·期 1
·99-108
·
IF 1.352
Xiaomeng Wang,Xueqing Liu,Sha Peng,Panrui Peng,Liyong Zou,Jia Chen,Jiyan Liu
Summary A novel phosphorus-containing acrylate monomer (AOPA) was synthesized starting from 2-methy-2,5-dioxo-1,2-oxaphospholane and hydroxyethyl acrylate. The structure of AOPA was characterized with FTIR and 1 H NMR. AOPA shows good compatibility with polyethylene glycol diacrylate (PEGDA) and can polymerize with PEGDA under UV light irradiation at different mass ratios to form membranes with high transparency (above 88.9% of light transmittance in the range of 400-800 nm) and flexibility. Incorporating 20 wt% of AOPA in PEGDA reduced the total heat release and peak rate by 50.3% and 38.4%, respectively, as measured by micro combustion calorimeter. The membrane containing 40 wt% of AOPA with 0.4 mm thickness can pass the UL94 V0 rating, and limiting oxygen index reaches 33.4%. TG-FTIR and SEM-EDX analysis show that the presence of AOPA depresses the thermal degradation and promotes the char formation.
研究领域:
材料科学
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化学工程
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高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
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2020
·Vol. 137
·期 37
·49090
·
IF 2.52
Jianwen Cheng,Huajun Duan,Shuang Yang,Jun Wang,Qianqian Zhang,Guoping Ding,Yefa Hu,Siqi Huo
A P/N-containing flame retardant (PPT) constructed by phosphaphenanthrene, phosphonate, and triazole groups was successfully synthesized and used as a reactive co-curing agent for epoxy resin (EP). The curing behavior, thermal property, combustion behavior, and flame retardant mechanism of EP thermosets were comprehensively investigated. According to the analysis of DSC and TGA, PPT accelerated the crosslinking reaction and enhanced the charring ability for EP thermosets at high temperature. The results of combustion test indicated that PPT endowed epoxy thermoset with outstanding flame retardancy. When the phosphorus content was 0.71 wt%, EP/DDS/PPT-2 achieved a LOI value of 33.2% and passed V-0 rating in UL-94 test, and its peak heat release rate and total heat release were decreased by 63.7 and 30.5%, respectively, relative to EP/DDS. Moreover, the FIGRA of EP/DDS/PPT-2 was reduced from 9.7 to 3.5 kW m −2 s −1 , manifesting the significantly improved fire safety of EP thermoset. The flame retardant mechanism was summarized as two parts: (a) the barrier effect of continuous phosphorus-rich char layers in condensed phase, (b) the quenching effect of phosphorous radicals and diluting effect of nonflammable gases in gaseous phase.
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
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Junhua Ding,Jinggang Wang,Weihong Cao,Huajun Zheng,Zhenghong Guo,Zhengping Fang,Peng Chen,Juan Li
A bio-based phosphonate 4-(7-((diphenylphosphoryl)oxy)-5-hydroxy-4-oxo-4H-chromen-3-yl)phenyl diphenylphosphinate (DPGE) was synthesized using diphenylphosphinic chloride and genistein. DPGE was used to modify the flame retardancy of poly(ethylene 2,5-furandicarboxylate-co-ethylene terephthalate) (PEFT20) containing 20 mol % 2,5-furandicarboxylic acid. PEFT20 containing 8 wt % DPGE displays a UL-94 V0 rating and a limiting oxygen index of 29.8 vol %. The flame retardant mode is the comprehensive effects of melting-away, gas phase, and condensed phase induced by DPGE. In addition, triglycidyl isocyanurate (TGIC) was incorporated to regulate the mechanical performance of PEFT20/DPGE. The flexural and impact strengths of PEFT20/DPGE are modified greatly. The coupling reactions between PEFT20 and TGIC increase the molecular weight and mechanical properties of PEFT20 blends. But, TGIC counteracts the melting-away effect caused by DPGE. Therefore, too much TGIC causes the decrease in flame retardancy.
研究领域:
材料科学
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生物化学
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DOI
高影响因子
Polymers
·
2025
·Vol. 17
·期 10
·1341
·
IF 4.9
Min Zhou,Zhenglin Liu,Dandan Lu,Jiajun Wang,Zili Chen,Yunren Qiu
Due to the similar physicochemical properties of rare earth ions, their separation presents significant challenges. In this study, acidic phosphonic chitosan (aPCS) was prepared by modifying chitosan with phosphite and formaldehyde for improving the water solubility and complexing ability of rare earth ions in acidic aqueous solutions. DFT calculations revealed that its phosphonic groups serve as preferred reaction sites, forming stable bidentate complexes with rare earth cations. The complexation abilities of aPCS and phosphorylated chitosan (PCS) for La(III) were compared at various pHs by complexation–ultrafiltration. The results showed that aPCS achieved a 97% rejection for La(III), while 70% for PCS at pH 5 and P/RE 10. Furthermore, aPCS maintained higher rejection than PCS at pH of 3 to 7. In conclusion, aPCS demonstrates excellent potential for the selective extraction and purification of rare earth ions.
研究领域:
化学
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材料科学
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稀土分离
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DOI
PubMed
高影响因子
MICROCHIMICA ACTA
·
2019
·Vol. 186
·期 7
·1-10
·
IF 5.479
Yue Yuhua,Jiang Li,Li Zhen,Yuan Jie,Shi Haizhu,Feng Shun
A glassy carbon electrode (GCE) was consecutively modified with amino groups and phosphate groups, and then loaded with Zr(IV) ions. Fourier transform infrared spectrophotometry, field-emission scanning electron microscopy, energy dispersive X-ray spectroscopy and cyclic voltammetry were used to characterize the morphologies and electrochemical properties. The sensor was used to detect p-nitrophenyl-substituted organophosphorus pesticides, with methyl-parathion (MP) as the model analyte. Under optimized conditions, the oxidation current of square wave voltammetry (typically measured at around −0.28 V vs. saturated calomel electrode) increases linearly in the 1.0 to 100 ng mL −1 MP concentration range, and the detection limit is 0.25 ng mL −1 (at a signal to noise ratio of 3). Average recoveries from (spiked) real water samples are 99.9–102.2%, with relative standard deviations of 0.3–2.6% ( n = 3) at three levels. The reliability and accuracy of the method was validated by HPLC.
Zr(IV) modified GCE is prepared via three steps. The electrode shows high specificity and selectivity towards methyl‐parathion. And the linear range is 1.0 ‐ 100.0 ng mL‐ 1 with the detection limit as low as 0.25 ng mL‐ 1 with SWV.
研究领域:
分析化学
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环境科学
·
农药检测
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DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Tingting Xiao,Chen Tan,Gary Histand,Dongen Lin
Latent imidazolium phosphinate ionic liquids (IMPILs) with innovative structures were developed as high-performance curing agents for one-component epoxy systems. These room-temperature liquid IMPILs exhibit exceptional compatibility with liquid epoxy resin (EP, E-51), overcoming the immiscibility limitations of conventional curing agents. These IMPILs efficiently cure EP (E-51) at moderate temperatures (109–180 °C) in the mass ratio range of 100:10–100:15, while maintaining storage stability with a 15-day pot life at 25 °C. The cured thermosets achieve impressive overall performance: tensile strength of 88 MPa (surpassing thermosets cured with 1-methylimidazole or 1,2-dimethylimidazole), good thermal stability (T10% = 374–407 °C), and unexpected flame retardancy (LOI = 30.7–35.1%, surpassing standard epoxy resins). This work establishes IMPILs as a novel class of liquid latent curing agents that satisfy both long-term storage requirements and excellent thermal-curing performance for advanced epoxy composites.
研究领域:
材料科学
·
化学工程
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DOI
高影响因子
危险品化学品经营许可证（带存储）