ACS Applied Materials & Interfaces
·
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
·
化学工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2025
·
IF 1.6
He Yan,Du Wenlong,Fu Xiaolei,Yuan Dingzhong,Na Bing,Zhang Shaoze,Liu Honglai
Developing new porous polymer to separate uranium in water is an urgent task. In our work, a novel hypercross-linked porous polymer bearing phosphonate ligand (HCP-PL) was constructed by a simple Friedel–Crafts alkylation strategy. The obtained polymer HCP-PL was showed an excellent uranium adsorption capacity and outstanding selectivity in aqueous solution. The adsorption isotherm model is consistent with Langmuir monolayer isotherm. It is worth mentioned that the maximum uranium adsorption capacity ( q max ) by HCP-PL reached up to 553.4 mg/g, which was much higher than most reported porous materials. The polymer HCP-PL exhibits a pronounced selective adsorption capacity for uranium in the existence of other impurity ions, including Cu 2+ , Co 2+ , Sn 2+ , La 3+ , Ce 3+ , and Pb 2+ . This excellent selectivity is attributed to the strong affinity between uranium and phosphonate ligand, as demonstrated by experimental results and by density functional theory calculations. Moreover, the porous polymer HCP-PL remained removal uranium percentage of 82% after 5 adsorption–desorption cycles. Therefore, the novel hypercross-linked porous materials bearing phosphonate ligand have good application prospects in the removal of uranium ions in water.
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 CLUSTER SCIENCE
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2020
·Vol. 32
·期 2
·437-443
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IF 1.731
Li Hong-Jing,Wei Xue-Wen,Liu Kuan-Guan,Yan Xiao-Wei
For investigating the template effects and the ligand roles in constructing structurally charming silver clusters, we isolated and analyzed a new cluster compound, namely, [(CO 3 ) 2 @Ag 25 (C≡C t Bu) 15 (CF 3 CO 2 ) 3 (Ph 2 PO 2 ) 2 I] , 1 . We report here the synthesis, crystal structure, characterization by various spectroscopic (IR, solid-state NMR, XPS) techniques and the luminescent property of this cluster. Its X-ray crystal structure reveals that the cluster is a 25-nuclearity silver cage with double CO 3 2− ions encapsulated in. Two diphenylphosphinates in new coordination mode (μ 2 :O 1 ,O 1 ) are co-protecting on the surface of cluster 1 . Also, the cluster emits orange-red light in the solid-state at 77 K.
研究领域:
无机化学
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材料科学
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产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2023
·Vol. 35
·期 12
·2210223
·
IF 29.4
Jungang Wang,Yuhang Che,Yuwei Duan,Zhike Liu,Shaomin Yang,Dongfang Xu,Zhimin Fang,Xuruo Lei,Yong Li,Shengzhong (Frank) Liu
Cesium lead triiodide (CsPbI 3 ) is a promising light-absorbing material for constructing perovskite solar cells (PSCs) owing to its favorable bandgap and thermal tolerance. However, the high density of defects in the CsPbI 3 film not only act as recombination centers, but also facilitate ion migration, leading to lower PCE and inferior stability compared with the state-of-the-art organic–inorganic hybrid PSC counterpart. Theoretical analyses suggest that the effective suppression of defects in CsPbI 3 film is helpful for improving the device performance. Herein, the stable and efficient γ -CsPbI 3 PSCs are demonstrated by developing an acyloin ligand (1,2-di(thiophen-2-yl)ethane-1,2-dione (DED)) as a phase stabilizer and defect passivator. The experiment and calculation results confirm that carbonyl and thienyl in DED can synergistically interact with CsPbI 3 by forming a chelate to effectively passivate Pb-related defects and further suppress ion migration. Consequently, DED-treated CsPbI 3 PSCs yield a champion PCE of 21.15%, which is one of the highest PCE among all the reported CsPbI 3 PSCs to date. In addition, the unencapsulated DED-CsPbI 3 PSC can retain 94.9% of itsinitial PCE when stored under ambient conditions for 1000 h and 92.8% of its initial PCE under constant illumination for 250 h.
研究领域:
材料科学
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太阳能
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光伏技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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