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<p>The search for efficient adsorbents to capture harmful heavy metal (HM) cations is crucial for environmental remediation. This study explores the adsorption performance of pristine and functionalized CTFs for removing Cd<sup>2+</sup>, Hg<sup>2+</sup>, and Pb<sup>2+</sup> from water using both computational and experimental methods. A molecular-level understanding of host–guest interactions is essential for designing functionalized nanoporous materials. DFT calculations at the ωB97XD level predict complexation energies of the cations on CTF fragments in the order: <InlineEquation ID="IEq1"> <InlineMediaObject> <ImageObject Color="BlackWhite" FileRef="13738_2025_3253_Article_IEq1.gif" Format="GIF" Height="19" Rendition="HTML" Resolution="72" Type="Linedraw" Width="74" /> </InlineMediaObject> <EquationSource Format="TEX">\({\text{E}}_{{\text{Pb}}^{2+}@\text{CTF}}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mtext>E</mtext> <mrow> <msup> <mrow> <mtext>Pb</mtext> </mrow> <mrow> <mn>2</mn> <mo>+</mo> </mrow> </msup> <mo>@</mo> <mtext>CTF</mtext> </mrow> </msub> </math></EquationSource> </InlineEquation> &gt; <InlineEquation ID="IEq2"> <InlineMediaObject> <ImageObject Color="BlackWhite" FileRef="13738_2025_3253_Article_IEq2.gif" Format="GIF" Height="21" Rendition="HTML" Resolution="72" Type="Linedraw" Width="74" /> </InlineMediaObject> <EquationSource Format="TEX">\({\text{E}}_{{\text{Hg}}^{2+}@\text{CTF}}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mtext>E</mtext> <mrow> <msup> <mrow> <mtext>Hg</mtext> </mrow> <mrow> <mn>2</mn> <mo>+</mo> </mrow> </msup> <mo>@</mo> <mtext>CTF</mtext> </mrow> </msub> </math></EquationSource> </InlineEquation>  &gt; <InlineEquation ID="IEq3"> <InlineMediaObject> <ImageObject Color="BlackWhite" FileRef="13738_2025_3253_Article_IEq3.gif" Format="GIF" Height="19" Rendition="HTML" Resolution="72" Type="Linedraw" Width="75" /> </InlineMediaObject> <EquationSource Format="TEX">\({\text{E}}_{{\text{Cd}}^{2+}@\text{CTF}}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mtext>E</mtext> <mrow> <msup> <mrow> <mtext>Cd</mtext> </mrow> <mrow> <mn>2</mn> <mo>+</mo> </mrow> </msup> <mo>@</mo> <mtext>CTF</mtext> </mrow> </msub> </math></EquationSource> </InlineEquation>. Based on the theoretical results, carboxylic acid (COOH)-functionalized CTF (COOH-CTF) is selected as the optimal adsorbent. COOH-CTF is synthesized through ZnCl<sub>2</sub>-catalyzed ionothermal cyclotrimerization of the 2,5-dicyanobenzoic acid monomer and characterized by XRD, FT-IR, BET, and XPS techniques. The COOH-CTF adsorbent demonstrates medium to high adsorption capacities for Cd<sup>2+</sup> (88.02 mg g<sup>−1</sup>), Hg<sup>2+</sup> (247.28 mg g<sup>−1</sup>), and Pb<sup>2+</sup> (360.39 mg g<sup>−1</sup>). NCI analysis shows that in the HM@CTF-1 system, HM cations interact mainly via Van der Waals and strong electrostatic forces with nitrogen atoms of the triazine ring. In HM@COOH-CTF, additional strong electrostatic interactions occur with oxygen atoms of carboxylic groups, indicating a synergistic adsorption effect at N and O sites.</p> Graphical abstract <p></p>

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Removal of heavy metal cations (Cd2+, Hg2+, and Pb2+) from water using carboxylic acid-functionalized covalent triazine frameworks: Computational design and experimental validation

  • 期刊论文

  • 发表日期：

    2025年7月28日

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  • Rana Rafiei,
  • Majid Pirooz,
  • Sina Pourebrahimi

摘要

The search for efficient adsorbents to capture harmful heavy metal (HM) cations is crucial for environmental remediation. This study explores the adsorption performance of pristine and functionalized CTFs for removing Cd2+, Hg2+, and Pb2+ from water using both computational and experimental methods. A molecular-level understanding of host–guest interactions is essential for designing functionalized nanoporous materials. DFT calculations at the ωB97XD level predict complexation energies of the cations on CTF fragments in the order: \({\text{E}}_{{\text{Pb}}^{2+}@\text{CTF}}\) E Pb 2 + @ CTF > \({\text{E}}_{{\text{Hg}}^{2+}@\text{CTF}}\) E Hg 2 + @ CTF  >  \({\text{E}}_{{\text{Cd}}^{2+}@\text{CTF}}\) E Cd 2 + @ CTF . Based on the theoretical results, carboxylic acid (COOH)-functionalized CTF (COOH-CTF) is selected as the optimal adsorbent. COOH-CTF is synthesized through ZnCl2-catalyzed ionothermal cyclotrimerization of the 2,5-dicyanobenzoic acid monomer and characterized by XRD, FT-IR, BET, and XPS techniques. The COOH-CTF adsorbent demonstrates medium to high adsorption capacities for Cd2+ (88.02 mg g−1), Hg2+ (247.28 mg g−1), and Pb2+ (360.39 mg g−1). NCI analysis shows that in the HM@CTF-1 system, HM cations interact mainly via Van der Waals and strong electrostatic forces with nitrogen atoms of the triazine ring. In HM@COOH-CTF, additional strong electrostatic interactions occur with oxygen atoms of carboxylic groups, indicating a synergistic adsorption effect at N and O sites.

Graphical abstract