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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Fabrication of EDTA modified silica gel toward highly efficient adsorptive removal of copper ions from methanol

Zilan Yin,Qidong Zhao,Chuyi Xie,Gaohong He,Yonghou Xiao

With the rapidly growing demand of high-purity methanol, developing high-efficiency adsorbents has become urgent to completely remove metal ions from methanol. Herein, a novel adsorbent, ethylenediaminetetraacetic acid (EDTA) modified silica gel (EDTA-2N-Silica) was successfully prepared for copper ions deep removal from methanol. EDTA-2N-Silica was constructed by using 3-(2-amino-ethylamino) propyl-trimethoxysilane (Silicone A-1120) to graft the EDTA molecules onto the silicon hydroxyl groups over silica gel. Dynamic adsorption experiments revealed that copper ions could be effectively removed from methanol prior to breakthrough point, with almost complete elimination achieved before adsorption column exhaustion. Correspondingly, the breakthrough and equilibrium adsorption capacities of copper ions over EDTA-2N-Silica-0.375 achieved 0.159 and 0.846 mmol g −1 at 40 °C, respectively. According to the density functional theory calculation, the enhanced copper ions capture performance of EDTA-2N-Silica was mainly attributed to the copper ions complexation with N-containing and the O-containing groups from EDTA. Furthermore, after the fifth regeneration, the equilibrium adsorption capacity of EDTA-2N-Silica-0.375 toward copper ions could retain 87.82 % that of the fresh sample, indicating its satisfactory regeneration performance. Considering its excellent adsorption and regeneration performance, EDTA-2N-Silica adsorbent is expected to be employed for efficient removal of trace copper ions from methanol.

CAS / MDL: 112926-00-8
研究领域: 化学工程 · 环境科学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Highly Dispersed AuCu Nanoparticles Confined in Zr-MOFs for Efficient Methanol Synthesis from CO2 Hydrogenation

Guiming Xie,Xingyang Bai,Yanrui Niu,Runduo Zhang,Jian Liu,Qingyuan Yang,Zhou-Jun Wang

Making use of novel materials to develop efficient catalysts is one of the research hotspots for CO2 hydrogenation to methanol. Herein, UiO-66, a typical Zr-MOF, was modified by ethylene diamine tetraacetic acid (EDTA) to serve as a substrate for the synthesis of AuCu bimetallic catalysts. The resultant AuCu@UiO-66-EDTA catalyst exhibited a superior methanol production rate, which delivered a high space-time yield of methanol (3.34 gMeOH gmetal–1 h–1) at 250 °C and 3.0 MPa. The EDTA modification was found to effectively confine AuCu nanoparticles inside the framework of MOFs, which significantly reduced the metal particle size and enriched the oxygen vacancy concentration. As a consequence, more active sites were generated for methanol synthesis. Moreover, the AuCu@UiO-66-EDTA catalyst yielded more favorable reaction intermediates that could be converted to methanol at a faster rate. This work develops unique MOFs-encapsulated bimetallic catalysts and illuminates the positive effect of confinement.

研究领域: 材料科学 · 催化化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2017 · IF 3.359

A positively charged composite nanofiltration membrane modified by EDTA for LiCl/MgCl2 separation

Wei Li,Chang Shi,Ayang Zhou,Xiao He,Yawei Sun,Jinli Zhang

For efficient recovery of lithium from brines, a composite nanofiltration (NF) membrane with positively charged skin layer (PA-B) was first synthesized via interfacial polymerization between branched poly(ethylene imine) (BPEI) and trimesoyl chloride (TMC) on the support of crosslinked polyetherimide, and the separation performance was assessed for simulative brine of mixed LiCl/MgCl 2 solution. To improve the permselectivity of Li + against Mg 2+ , then we adopted EDTA to modify the as-prepared positively charged PA-B NF membrane. The optimal EDTA modified NF membrane PA-B2-E3 showed the separation factor S Li , Mg about 9.2 for the LiCl/MgCl 2 mixed solution with a Mg 2+ /Li + mass ratio of 24, with excellent stability within 36   h filtration, which would have promising applications in the recovery of Li from brine.

研究领域: 材料科学 · 环境工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Post modification of Oxo-clusters in robust Zirconium-Based metal organic framework for durable SO2 capture from flue gas

Zhonghui Zhang,Bolun Yang,Yue Wu,Wenxiang Zhang,Heping Ma

The efficient capture of SO 2 after the combustion of fossil fuels is of great challenge as the low SO 2 concentration (<500 ppm) and coexisting with CO 2 , water, O 2 in flue gas . Robust zirconium-based MOFs possessing accessible polar sites usually have high SO 2 adsorption capacity but poor durably in adsorption desulfurization due to the acidic sulfate deposition on the Zr-O cluster. Herein, a Zr-O cluster post-modification method was introduced in a Zr-MOF (MOF-808) to form EDTA-MOF-808 (EDTA, ethylene diaminetetraacetic acid) for selective and durable removal of SO 2 . The introduction of EDTA not only improve their SO 2 adsorption capacity, but also sharply increase their SO 2 /CO 2 selectivity (57.2 vs 8.9) and SO 2 /N 2 selectivity (1915.8 vs 292.7) at low SO 2 partial pressure. Moreover, the synergistic effects of dipole and hydrogen bonding interaction between SO 2 and EDTA in EDTA-MOF-808 make the capture of SO 2 in a reversible manner, which can prevent the formation of S(VI) species in Zr-MOF. DFT calculation confirmed that SO 2 was interacted with EDTA through moderate dipole–dipole interaction (S(SO 2 ) with N(EDTA)) and hydrogen bonds (H(–COOH) with O(SO 2 )). Systematic investigations including thermodynamic SO 2 adsorption, dynamic breakthrough experiments, stability tests and DFT-calculations in both MOF-808 and EDTA-MOF-808 confirmed the efficient performance of post modification of Zr-O clusters with EDTA in Zr-MOFs for durable SO 2 capture.

研究领域: 环境科学 · 材料科学
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JOURNAL OF POROUS MATERIALS · 2020 ·Vol. 28 ·期 1 ·299-310 · IF 2.183

Facile synthesis of EDTA grafted 3D spherical-chain porous silica with high capacity for rapidly selective adsorption of Cu(II) from aqueous solutions

Ma Zixuan,Li Fang,Jia Aizhong,Zhang Xiao,Wang Yanji

The highly efficient adsorbents with fast adsorption rate, high adsorption capacity and selectivity as well as good reusability were successfully synthesized through fabricating 3D spherical-chain porous silica material and grafting modification with ethylenediaminetetraacetic acid (EDTA) for the selective removal Cu(II) from wastewater. The obtained adsorbents were characterized by XRD, FT-IR, SEM, TEM, XPS, N 2 adsorption–desorption and back titration. The results indicate that the 3D framework structure is adjustable in a certain range by varying the parameters of the synthesis system. And the adsorption performance of the materials was investigated under different conditions such as pH, contact time and initial metal ions concentration. Under the experiment conditions, the synthesized adsorbent is efficient in removing Cu(II) and the adsorption equilibrium could be achieved within only 5 min, and the kinetic data are well fitted by pseudo-second-order and Langmuir isotherm models. The prepared adsorbents display good selective adsorption of Cu(II) and can be feasibly regenerated without evident decrease even after five recycles. Basing on the obtained results, the plausible adsorption mechanism was proposed and analyzed.

CAS / MDL: 13822-56-5 57-09-0
研究领域: 材料科学 · 环境科学
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