On a New Point of View Toward the Mechanism of Those Electrochemical Reactions Driven by the External Potential

You yi Sun

doi:doi:10.11648/j.sf.20240503.13

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On a New Point of View Toward the Mechanism of Those Electrochemical Reactions Driven by the External Potential

You yi Sun^*

Published in Science Frontiers (Volume 5, Issue 3)

Received: 2 September 2024 Accepted: 14 September 2024 Published: 29 September 2024

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Abstract

In the search of electrochemical reaction, uncovering the reaction mechanism plays a decisive role in analyzing the production of diverse products. We believe that all types of electrochemical reaction driven by external potential should follow a general process. In this paper, we propose that in those electrochemical reactions driven by the external potential, the formation of radicals via electron transfer between electrode and the species carrying electric charge serves as the first step, triggering subsequent reactions. This suggestion might be considerable electrochemical interest.

Published in	Science Frontiers (Volume 5, Issue 3)
DOI	10.11648/j.sf.20240503.13
Page(s)	123-129
Creative Commons	This is an Open Access article, distributed under the terms of the Creative Commons Attribution 4.0 International License (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution and reproduction in any medium or format, provided the original work is properly cited.
Copyright	Copyright © The Author(s), 2024. Published by Science Publishing Group

Keywords

Electrochemical Reaction, Reaction Mechanism, Electron-Transfer Step, Radical Reaction, Mechanistic Model

1. Introduction

The using of electrochemistry on synthetic chemistry, energy supply and removal of chemical pollution has a long history beginning with the decomposing water into hydrogen and oxygen by electrolysis using Volta's battery and which is still a hot topic until today. Electrochemistry offers an advantage of having no spent oxidant or reductant for disposal. However, electrochemical processes fell out of favour in the face of conventional chemical reactions because the outcome from electrochemistry was often far from the predictability. Understanding the mechanisms of these processes plays a critical role in designing reaction system to avoid the pitfalls.

Electrons, in electrochemical reaction, are transferred at an electrode singly, not in pairs. The primary reactive species to be generated by electron-transfer is usually considered to be either a delocalized radical-ion or a radical.

[1]

For various reactions, corresponding processes have been proposed for understanding the outcome of electrochemical reactions, however, most of them are still in debate. In general, when the primary reactant species are neutral (without an electric charge), it is considered that these neutral species are going to achieve the electron-transfer with electrode in initial reaction step, forming a negatively or positively charged particle. For example, carbon dioxide (CO₂) molecule in CO₂ reduction reaction is considered to accept an electron from cathodic electrode to form CO₂^•- anion in the first step.

[2]

The standard potential for formation of CO₂^•- anion in an aqueous media is -1.90 V,

[3]

however, almost all products, including CO, C₁, C₂ and C₃, can form under a low potential of -1.0 V in experimental CO₂ reduction reaction.

[4]

This strongly suggests that the actual process of reducing CO₂ into various valuable products may not involve the formation of CO₂^•- anion.

In addition, it is widely accepted that in electrochemical nitrate (NO₃^-) reduction to ammonia (NH₃), the negatively charged NO₃^- ions are adsorbed on cathode surface in the reduction process for the formation of NH₃ or other products.

[5]

However, some experiments carried out using surface-enhanced infrared absorption spectroscopic, suggesting that nitrate ion adsorption on electrode surface only occurs under positive potential.

[6]

Thus, in our opinion, it might be impossible for anions (NO₃^-) ions to be adsorbed on cathode surface in the reaction process because anions tend to move away from cathode under the external electric field, the cathodic electrode surface might be surrounded by cations and neutral particles during reaction process.

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Figure 1. Representation of (a) reduction and (b) oxidation process of a species, A⁺ and B^-, in solution for the occurrence of those electrochemical reactions required the applying of external potential. The molecular orbitals (MO) of species A⁺ which is reduced into A^▪ reducing radical on cathode surface are the highest occupied MO and the lowest vacant MO, the MO of species B^- which is oxidized into B^▪ oxidizing radical on anode surface are the highest occupied MO and the lowest vacant MO as well. These correspond in an approximate way to the E⁰_s of the A⁺/A^▪ and B^-/B^▪ couples, respectively.

In electrochemical reactions driven by the external potential, the external electric field on electrode exerts an electrostatic force to ions in electrolyte, which makes cations tend to move to cathode and anions tend to move to anode. It has been widely accepted that the primary adsorbed species on surface of electrode are some species with an electric charge (cations adsorbed on cathode and/or anions adsorbed on anode).

[7]

Therefore, the reactant species in electron-transfer steps (electrochemical reaction step) should be the species with an electric charge. Namely, cations are in favour of achieving electron-transfer with electrode of cathode, and anions are in favour of achieving electron-transfer with electrode of anode.

In the present paper it is shown that on the ground of the above discussion, if we assume that in initial step of electrochemical reaction requiring the driving of external potential, the species with an electric charge is firstly converted to a reactive radical with an unpaired electron via electron transfer on the electrode as showed in Figure 1 and consider that this reactive radical can react with other radical or spin-paired species for bond forming or bond cleaving in following steps, we can obtain a well understanding of reaction mechanism and illuminating explanation of formation of various products in various types of electrochemical reactions.

In view of the radicals formed from species with an electric charge in initial electrochemical reaction step, we suggest that those radicals formed from positively charged species by accepting a single electron on cathodic electrode have a strong reducing property, it can attack the oxidizing radical on spin-paired species by abstraction or addition. Relatively, radicals formed from negatively charged species by donating a single electron on anodic electrode is a strong oxidizing agent, which can attack the reducing radical on spin-paired species by abstraction or addition. Notice that radicals formed on anode or cathode also can dimerize to produce a new spin-paired product or intermediate in electrochemical reaction. In the following, several reactions as examples, are concerned, we wish to present a clear line of thought and the facts which have led us to this point of view, hoping that our assumption may be useful to the investigator in area of electrochemistry.

2. Concerning Nitrate Reduction Reaction

We start first with the point of view taken in the electrochemical nitrate reduction, which is a typical reduction reaction driven by the negative potential. There are two reactants: protons (H⁺) and NO₃^- ions. The former one is positively charged, and the latter is negatively charged. It seems to us that on cathode surface, it is impossible for NO₃^- ions being absorbed on electrode surface to achieve electrons accepting, and it might be the protons to achieve this forming reactive H^• radicals. As H^• radical is a type of strong reducing agents,

[7]

which can react with the oxidizing group on NO₃^-, it is our opinion that the processes of NO₃^- reduction to various products are a sequence of radical reactions with H^• radicals as illustrated in Figure 2. We assume that NO₃^- is initially converted into N-centred O-N^•=O radical (NO₂) by abstraction of O^•- from NO₃^- by H^• radical (H^• formed from H⁺ by accepting an electron from electrode). An O-centred O^•-N=O radical (NO₂) may then be formed by displacement of electrons of this N-centred O-N^•=O radical. Following this, a radical dimerization reaction with H^• radical may occur on NO₂ forming nitrite (HNO₂), which can be converted to a new N-centred N^•=O radical (nitrogen monoxide (NO), one side product and important intermediate in electrochemical NO₃^--to-NH₃) by abstraction of ^•O-H from HO-N=O by H^• radical. In addition, the NO₂ may also react with H₂O forming HNO₃ and NO as shown in Figure 2 (blue line). If N-centred N^•=O radical undergoes a radical dimerization reaction with H^• radical forming a spin-paired intermediate (HN=O), another side product (NH₂OH) and useful product (NH₃) may then be formed via stepwise reactions with reducing H^• radicals. However, if two N-centred N^•=O radicals encounter and dimerize, a spin-paired intermediate (O=N-N=O) will form, N₂H₄ or N₂O molecule might be produced through radical reactions with H^• radicals, but the O on N₂O might be removed by further reactions with H^• radicals forming N₂ in final step.

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Figure 2. The proposed reaction pathways for nitrate reduction reactions; (1) proton (H⁺) is converted into H^• radicals via electron-transfer step, (2) the possible reaction pathway for electrochemical nitrate reduction reaction on cathodic bias; NO₃^- ions are converted into various products by H^• radicals, which are formed via electron-transfer to proton from cathode under negative potential.

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Figure 3. The proposed reaction pathways for oxygen reduction reaction and oxygen evolution reaction; a) reaction pathways for oxygen reduction reaction; O₂ molecules are converted into hydrogen peroxides or water by H^• radicals, and Pt metal as catalysts can increase the reaction rate by activating O₂ into reactive radical state, b) reaction pathways for oxygen evolution reaction; this reaction starts with the conversion of HO^- ions into oxidizing HO^• radicals by electron-transfer to anode, two HO^• radicals may undergo dimerization forming hydrogen peroxide, which is then converted into O₂ molecule by abstraction of H^• groups by another two HO^• radicals. On Pt electrocatalysts surface, part HO^• radicals formed via electron-transfer are in-situ bonded on surface atoms forming HO-Pt, which may be converted into O₂ molecule with stepwise reactions with HO^• radicals. c) reaction pathways for α-substitution of methylbenzenes in acetic acid media, this reaction starts with ^-OAc ion conversion into ^•OAc radical with strong oxidizing property, the reducing H^• agent on α position of methylbenzenes forming α-substitution product with a further radical dimerization.

As it is impossible for NO₃^- ions to be absorbed on cathode during reaction process, and the conversion of a NO₃^- ion into NH₃ requires eight H^• radicals, it is our opinion, furthermore, that those catalysts that can promote the formation of H^• radicals will be beneficial for the reduction of NO₃^- ions to NH₃. It is intriguing that, in practice, Pd metal is experimentally proved to be effective for the formation of H^• radicals,

[8]

and that Pd metal cathode also can support a high selectivity of reduction of NO₃^- to NH₃.

[9, 10]

Thus, it might be that the study of electrocatalysts for conversion of NO₃^- ions into NH₃ should focus on the improvement of formation of H^• radicals (avoiding dimerization of H^• radicals to form H₂ side-products), rather than the relationship between catalysts and NO₃^- ions.

3. Concerning CO₂ Reduction Reaction (CO₂RR)

There are two reactants in this reaction: protons (H⁺) and CO₂ molecules. The assumption of formation of CO₂^•- anion in the initial step of electrochemical CO₂RR is doubtable as discussed above. Here, we have assumed that the electron-transfer may be achieved by protons, rather than CO₂ molecule. Protons receive electrons from cathode forming reducing H^• radicals. As CO₂ molecules are inert and H^• radicals are easy to dimerize to form H₂, catalysts are required for this reaction to convert CO₂ molecules into active state for reaction spontaneously occurring. It is experimentally proved that Cu metal is active in this reaction and can produce a wide range of products. We have assumed that in our previous publication,

[11]

Cu with single unpaired can activate CO₂ molecules into reactive C-centred radicals (O=C^•-O-Cu), followed by various radical reactions with H^• radicals and/or other type of radicals to form various products. See the detailed reaction processes for the formation of various products in our previous publication,

[11]

we will not discuss more in this work. Besides nitrate reduction reaction and CO₂ reduction reaction, we wish to discuss more reactions. The following treatments are several other types of electrochemical reactions.

4. Concerning Oxygen Reduction Reaction (ORR)

O₂ molecules and protons (H⁺) are reactants in ORR. We believe that it is the proton that achieves electron-transfer with cathode forming reactive H^• radicals in the initial step. Then, the O₂ is gradually reduced into hydrogen peroxide or water by H^• radicals (Figure 3a). The radical addition of H^• radical to an O₂ molecule leads to the formation of a O^•-OH radical, which is then converted into spin-paired hydrogen peroxide molecule (HO-OH) by dimerization with a H^• radical. With further stepwise reactions of radical abstraction and radical dimerization with H^• radicals, an O₂ molecule is gradually converted into two H₂O molecule.

Free H^• radicals tend to dimerize into H₂ molecule and solubility of O₂ usually is low in electrolyte, these make the kinetics of ORR reactions much slow, and an efficient electrocatalyst is required to adsorb and activate O₂ molecule.

[12]

It is experimentally confirmed that Pt or Pd metals are active in this reaction.

[13]

Recent experimental studies have confirmed that O₂ molecule can react with surface atom of Pt metal.

[14]

This makes us assume that surface atoms of Pt metal might have the potential to adsorb and activate O₂ molecule into reactive O-centred radical (O^•-O-Pt), which can make the reaction with H^• radicals more convenient and faster. As shown in Figure 3a (on Pt metal surface), O₂ interacts with Pt to give reactive O^•-O-Pt intermediate, which then reacts with H^• radical by dimerization to give H-O-O-Pt. Hydrogen peroxide (H-O-O-H) might be generated when H-O-O^• group is abstracted by H^• radical from H-O-O-Pt. Yet, if H-O^• group of H-O-O-Pt is abstracted by H^• radical forming H₂O and O^•-Pt intermediate, O₂ in this reaction pathway will be converted into H₂O with further reaction with H^• radicals.

5. Concerning Oxygen Evolution Reaction (OER)

The following treatments focus on the electrochemical reactions driven by the positive potential. OH^- ions are only one reactant in OER and are negatively charged. Thus, it must be that under positive potential, OH^- ions lose electrons forming reactive O-centred radicals (HO^•), which is a strong oxidizing agent.

[15]

As shown in Figure 3b, two free HO^• radicals dimerize to give a spin-paired hydrogen peroxide (HO-OH). Due to the strong oxidation of HO^•, the HO-OH might be converted into O₂ molecule by abstraction of two H groups by another two free ^•OH radicals in final step.

It should be noticed that part noble metals as electrocatalysts (such as Pt) can improve the kinetics of this reaction. Recently, it is detected that OH is adsorbed on Pt surface at positive potential by using in-situ vibrational spectroscopy, in-situ X-ray absorption spectroscopy, and ex-situ X-ray photoelectron spectroscopy.

[14, 16, 17]

This makes us assume that OER on Pt metal surface follows the pathways as showed in Figure 3b (on Pt metal surface), two HO^• radicals formed via electron-transfer step are in-site bonded on Pt surface forming H-O-Pt-O-H intermediate, which might result in the formation of H-O-O-H (the formation of O-O bond). Then, the H^• group of H-O-O-H might also undergo an attack by oxidizing HO^• radical to give an O₂ and two H₂O molecules.

Besides the H⁺ and HO^- can be converted to relative reducing or oxidizing radicals on electrode by a single electron transfer, and then involving in sequence of radical reactions for formation of products in electrochemical reaction, we also assume that other types of positively or negatively charged species in electrolyte could achieve it as well. For example, methylbenzenes can be oxidized to a α-substitution product on anodic bias in acetic acid.

[18]

It is our assumption that in initial step, ^-OAc with negative charge is converted to an oxidizing O-centred radical (^•OAc) by removing a single electron to anode (Figure 3c), then C-centred radical could be made by abstraction of H^• from α position of methylbenzenes by ^•OAc radical. In final step, α-substitution product could then be formed by dimerization with another ^•OAc radical.

6. Conclusions

Thus far, we have already discussed several reaction processes of electrochemical reactions driven by external potential—based on our assumptions—including reduction reaction on cathodic bias and oxidation reaction on anodic bias. From reactant species to final products in these electrochemical reactions, the pathways are clear and straightforward. We hope that some experiments will carry out to proof those assumptions in our future work.

In addition, we believe that the electrocatalysts play a normal catalytic role in electrochemical reaction, such as activation of spin-paired reactant and/or supporting the dimerization reaction of radical (the formation of new chemical bond).

[11, 19-21]

The assumption of mechanism of electrochemical reaction as discussed above may be considered as different interpretations in the description of the process of electrochemical reactions. The viewpoint of conversion of ions into strong reducing or oxidizing radicals via electron-transfer, as well as the assumption of the radical reactions in process for formation of various products as above discussed, are hoped to find applications more widely to problems on the mechanism of electrochemical reactions.

Abbreviations

MO	Molecular Orbitals
OER	Oxygen Evolution Reaction
ORR	Oxygen Reduction Reaction
CO₂RR	CO₂ Reduction Reaction

Acknowledgments

I would like to thank my mom for her encouragement for the publication of this work.

Author Contributions

Youyi Sun is the sole author. The author read and approved the final manuscript.

Conflicts of Interest

The authors declare no conflicts of interest.

References

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Sun, Y. Y. (2024). On a New Point of View Toward the Mechanism of Those Electrochemical Reactions Driven by the External Potential. Science Frontiers, 5(3), 123-129. https://doi.org/10.11648/j.sf.20240503.13

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Sun, Y. Y. On a New Point of View Toward the Mechanism of Those Electrochemical Reactions Driven by the External Potential. Sci. Front. 2024, 5(3), 123-129. doi: 10.11648/j.sf.20240503.13

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Sun YY. On a New Point of View Toward the Mechanism of Those Electrochemical Reactions Driven by the External Potential. Sci Front. 2024;5(3):123-129. doi: 10.11648/j.sf.20240503.13

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@article{10.11648/j.sf.20240503.13,
  author = {You yi Sun},
  title = {On a New Point of View Toward the Mechanism of Those Electrochemical Reactions Driven by the External Potential
},
  journal = {Science Frontiers},
  volume = {5},
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  doi = {10.11648/j.sf.20240503.13},
  url = {https://doi.org/10.11648/j.sf.20240503.13},
  eprint = {https://article.sciencepublishinggroup.com/pdf/10.11648.j.sf.20240503.13},
  abstract = {In the search of electrochemical reaction, uncovering the reaction mechanism plays a decisive role in analyzing the production of diverse products. We believe that all types of electrochemical reaction driven by external potential should follow a general process. In this paper, we propose that in those electrochemical reactions driven by the external potential, the formation of radicals via electron transfer between electrode and the species carrying electric charge serves as the first step, triggering subsequent reactions. This suggestion might be considerable electrochemical interest.
},
 year = {2024}
}

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TY  - JOUR
T1  - On a New Point of View Toward the Mechanism of Those Electrochemical Reactions Driven by the External Potential

AU  - You yi Sun
Y1  - 2024/09/29
PY  - 2024
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DO  - 10.11648/j.sf.20240503.13
T2  - Science Frontiers
JF  - Science Frontiers
JO  - Science Frontiers
SP  - 123
EP  - 129
PB  - Science Publishing Group
SN  - 2994-7030
UR  - https://doi.org/10.11648/j.sf.20240503.13
AB  - In the search of electrochemical reaction, uncovering the reaction mechanism plays a decisive role in analyzing the production of diverse products. We believe that all types of electrochemical reaction driven by external potential should follow a general process. In this paper, we propose that in those electrochemical reactions driven by the external potential, the formation of radicals via electron transfer between electrode and the species carrying electric charge serves as the first step, triggering subsequent reactions. This suggestion might be considerable electrochemical interest.

VL  - 5
IS  - 3
ER  -

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Author Information

You yi Sun

Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, China

Research Fields: Youyi Sun: Catalytic reaction mechanism, electrochemical reaction, renewable energy storage, electrochemical reaction mechanism, catalytic ammonia synthesis, Fischer-Tropsch reaction.

Contact Email

http://orcid.org/0009-0001-2117-4021

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Sun, Y. Y. (2024). On a New Point of View Toward the Mechanism of Those Electrochemical Reactions Driven by the External Potential. Science Frontiers, 5(3), 123-129. https://doi.org/10.11648/j.sf.20240503.13

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Sun, Y. Y. On a New Point of View Toward the Mechanism of Those Electrochemical Reactions Driven by the External Potential. Sci. Front. 2024, 5(3), 123-129. doi: 10.11648/j.sf.20240503.13

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Sun YY. On a New Point of View Toward the Mechanism of Those Electrochemical Reactions Driven by the External Potential. Sci Front. 2024;5(3):123-129. doi: 10.11648/j.sf.20240503.13

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@article{10.11648/j.sf.20240503.13,
  author = {You yi Sun},
  title = {On a New Point of View Toward the Mechanism of Those Electrochemical Reactions Driven by the External Potential
},
  journal = {Science Frontiers},
  volume = {5},
  number = {3},
  pages = {123-129},
  doi = {10.11648/j.sf.20240503.13},
  url = {https://doi.org/10.11648/j.sf.20240503.13},
  eprint = {https://article.sciencepublishinggroup.com/pdf/10.11648.j.sf.20240503.13},
  abstract = {In the search of electrochemical reaction, uncovering the reaction mechanism plays a decisive role in analyzing the production of diverse products. We believe that all types of electrochemical reaction driven by external potential should follow a general process. In this paper, we propose that in those electrochemical reactions driven by the external potential, the formation of radicals via electron transfer between electrode and the species carrying electric charge serves as the first step, triggering subsequent reactions. This suggestion might be considerable electrochemical interest.
},
 year = {2024}
}

Copy | Download

TY  - JOUR
T1  - On a New Point of View Toward the Mechanism of Those Electrochemical Reactions Driven by the External Potential

AU  - You yi Sun
Y1  - 2024/09/29
PY  - 2024
N1  - https://doi.org/10.11648/j.sf.20240503.13
DO  - 10.11648/j.sf.20240503.13
T2  - Science Frontiers
JF  - Science Frontiers
JO  - Science Frontiers
SP  - 123
EP  - 129
PB  - Science Publishing Group
SN  - 2994-7030
UR  - https://doi.org/10.11648/j.sf.20240503.13
AB  - In the search of electrochemical reaction, uncovering the reaction mechanism plays a decisive role in analyzing the production of diverse products. We believe that all types of electrochemical reaction driven by external potential should follow a general process. In this paper, we propose that in those electrochemical reactions driven by the external potential, the formation of radicals via electron transfer between electrode and the species carrying electric charge serves as the first step, triggering subsequent reactions. This suggestion might be considerable electrochemical interest.

VL  - 5
IS  - 3
ER  -

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