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Formation of Complex Ions03:45

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A type of Lewis acid-base chemistry involves the formation of a complex ion (or a coordination complex) comprising a central atom, typically a transition metal cation, surrounded by ions or molecules called ligands. These ligands can be neutral molecules like H2O or NH3, or ions such as CN− or OH−. Often, the ligands act as Lewis bases, donating a pair of electrons to the central atom. These types of Lewis acid-base reactions are examples of a broad subdiscipline called coordination...
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Complexation reactions take place when dative or coordinate covalent bonds form between metal ions and ligands. The compounds formed in these reactions are called coordination compounds. The number of bonds formed between the metal ion and the ligands is called its coordination number. Generally, most metal ions in an aqueous solution are solvated by water molecules and thus exist as aqua complexes.
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In complexation reactions, metal atoms or cations interact with ligands to form donor-acceptor adducts called metal complexes. Ligands that bind through one donor site are monodentate, ligands with two donor sites are bidentate, and those with more than two donor sites are polydentate ligands. For example, ethylene diamine is a bidentate ligand that binds through two nitrogen donor atoms, forming a five-membered ring. EDTA is a polydentate ligand that binds through four oxygen and two nitrogen...
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Precipitation and coprecipitation methods can be used to separate a mixture of ions in a solution. In qualitative inorganic analysis, ions that form sparingly soluble precipitates with the same reagent are separated based on the differences in solubility products. For example, consider the separation of Cu(II) and Fe(II) ions by precipitation as insoluble sulfides. First, copper(II) sulfide is precipitated by the addition of acidic H2S, where the dissociation of H2S is suppressed. Adding H2S...
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Electrodeposition is a technique used to separate an analyte from interferents by electrochemical processes. Here, the analyte is a metal ion that can be deposited on an electrode immersed in the sample solution. The electrochemical setup consists of an anode and a cathode. When an electric current is applied to the setup, oxidation occurs at the anode. At the cathode, which consists of a large metal surface, metal ions undergo reduction and deposit onto the surface.
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Metal ions can be separated from one another by complexation with organic ligands–the chelating agent– to form uncharged chelates. Here, the chelating agent must contain hydrophobic groups and behave as a weak acid, losing a proton to bind with the metal. Since most organic ligands used in this process are insoluble or undergo oxidation in the aqueous phase, the chelating agent is initially added to the organic phase and extracted into the aqueous phase. The metal-ligand complex is...
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Excess Cations Alter *CO Intermediate Configuration and Product Selectivity of Cu in Acidic Electrochemical CO2

Suhwan Yoo1,2, Sejin Park1, Jihoon Son3

  • 1Department of Chemistry, Seoul National University, Seoul 08826, Republic of Korea.

Journal of the American Chemical Society
|April 2, 2025
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Excess cations like Cs+ can hinder electrochemical CO2 reduction (CO2RR) by altering CO adsorption on copper, favoring hydrogen evolution over C2+ products. Polymeric binders can restore CO2RR performance.

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Area of Science:

  • Electrochemistry
  • Surface Science
  • Catalysis

Background:

  • Electrochemical CO2 reduction (CO2RR) is crucial for sustainable chemistry.
  • Cation concentration is known to influence CO2RR selectivity in acidic media.

Purpose of the Study:

  • To investigate how excess cations affect CO adsorption configurations and CO2RR product distribution.
  • To elucidate the mechanism behind cation-induced changes in CO2RR selectivity.

Main Methods:

  • Operando attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) to monitor CO adsorption.
  • Density functional theory (DFT) simulations to understand cation-CO interactions.
  • Electrochemical experiments with varying cation concentrations and polymeric binders.

Main Results:

  • Increasing Cs+ concentration shifts CO adsorption from atop to bridge configuration on Cu surfaces.
  • High Cs+ concentrations promote hydrogen evolution reaction (HER) and suppress C-C coupling.
  • Polymeric binders on Cu surfaces restore CO2RR selectivity by preventing cation interference.

Conclusions:

  • Cation concentration significantly impacts CO adsorption intermediates and CO2RR pathways.
  • Stabilization of CObridge by Cs+ hinders C-C coupling, favoring HER.
  • Catalyst surface modification with polymeric binders offers a strategy to mitigate detrimental cation effects and enhance CO2RR.