Disentangling the Roles of Dissolved Oxygen, Common Salts, and pH on the Spontaneous Hydrogen Peroxide Production in Water: No O2, No H2O2

Himanshu Mishra; Muzzamil Ahmad Eatoo

REVIEW 3 major objections 6 minor 10 references

Disentangling the Roles of Dissolved Oxygen, Common Salts, and pH on the Spontaneous Hydrogen Peroxide Production in Water: No O2, No H2O2

T0 review · 3 major / 6 minor · reviewed 2026-08-07 · deepseek-v4-flash

Challenge this review Re-run · record.json Download PDF Read on arXiv ↗

Pith's one-line read This paper argues that spontaneous hydrogen peroxide in water microdroplets is produced by reduction of dissolved oxygen at solid-water interfaces, not at the air-water interface or by microdroplet geometry; removing oxygen removes the…

desk verdict A solid experimental argument that O2 is necessary for H2O2 in sprays, but the claim that solid surfaces are the only source depends on inference, not direct measurement in the spray. read the letter →

arxiv 2505.21175 v1 pith:SSNECFWN submitted 2025-05-27 cond-mat.soft

Muzzamil Ahmad Eatoo , Himanshu Mishra This is my paper · ORCID

classification cond-mat.soft

keywords hydrogenperoxidemicrodropletsair-waterinterfacesolid-waterdissolvedoxygencorrosionpittingpHdependence

verification ladder T0 review T1 audit T2 compute T3 formal

The pith

A machine-rendered reading of the paper's core claim, the machinery that carries it, and where it could break.

The reading

This paper argues that the long-reported spontaneous formation of hydrogen peroxide in sprayed water microdroplets does not happen at the air-water interface or because of microdroplet geometry. Instead, the authors claim, the peroxide is produced by reduction of dissolved oxygen at solid-water interfaces that are inevitably present in the apparatus; in their experiments, removing O2 eliminates H2O2 regardless of added salts. They reproduce the previously reported halide and pH trends but attribute them to corrosion of metal surfaces: chloride, bromide, and iodide differ in how strongly they pit aluminum, and Al versus Ti corrosion depends oppositely on pH. If right, the electric-field and ion-separation mechanisms proposed for microdroplet H2O2 formation would be replaced by a mundane surface-oxidation pathway.

What carries the argument

The load-bearing mechanism is oxygen reduction at a solid-water interface, coupled to oxidation (corrosion) of that solid: O2 is the electron acceptor and the solid is the electron donor, yielding H2O2. Halide ions enter through corrosion chemistry—Cl- pits the passive oxide film and then consumes H2O2 on fresh metal, I- scavenges H2O2 to triiodide, Br- sits between—so the reported halide order is a corrosion signature. pH enters only through its effect on which solid corrodes faster: Al oxidizes faster in acid, Ti in base. Quantification relies on HPAK fluorometry cross-validated by 1H-NMR, and corrosion rates are measured by potentiodynamic polarization.

What would settle it

The claim would be falsified by a single clean experiment in which H2O2 is detected in sprayed microdroplets after all dissolved O2 is removed to below 0.01 mg/L and all solid-water contacts are made from inert, non-corroding materials, or by detecting H2O2 in the presence of O2 when the collected droplets demonstrably never touched a wetted solid surface.

Watch

Extended reading notes

Core claim

The paper's central claim is that spontaneous H2O2 production in water microdroplets is not an interfacial water phenomenon: it is oxygen-reduction chemistry at solid-water interfaces. In sprays, O2-free solutions produced no H2O2 regardless of halide identity, while air-saturated solutions did, with yields ordered by the halide's effect on corrosion of the aluminum surface. Separate immersion experiments on Al and Ti showed H2O2 yield tracks oxidation rate: Al corrodes faster in acid and yields more H2O2 there; Ti corrodes faster in base and yields more H2O2 there. The authors therefore attribute the halide and pH trends reported in prior droplet studies to surface corrosion chemistry, not to charge separation or alkalinity at the air-water interface.

Load-bearing premise

The load-bearing premise is that the absence of H2O2 in O2-free sprays, together with bulk immersion experiments on Al and Ti, proves that all H2O2 in the sprays came from solid-water interfaces rather than from an oxygen-dependent air-water pathway.

Editorial extensions

If this is right

Any claimed air-water or microdroplet H2O2 generation should be re-examined with dissolved O2 removed and with every solid contact surface identified and passivated.
H2O2 yields in sprayed droplets should depend on the material of the capillary, tubing, collection vessel, and substrate, not just on solution composition.
Halide trends in H2O2 yield are not evidence for ion-specific interfacial chemistry; they track pitting propensity and H2O2 consumption rates.
pH trends in H2O2 yield are not universal; the same solution pH can increase or decrease yield depending on the solid surface.
Oxygen-free control experiments become a screening test for any purported interfacial oxidation reaction in water.

Reading between the lines

Editorial extensions of the paper, not claims the author makes directly.

If the mechanism generalizes, other reported 'spontaneous' microdroplet oxidations—beyond H2O2—may also be driven by trace corrosion or dissolution of solids rather than by interfacial electric fields.
The paper implies a practical design rule for microdroplet experiments: choose wetted materials by their corrosion resistance in the intended solution, and degas when trying to isolate interfacial effects.
A quantitative model combining pitting potential, corrosion current, and H2O2 consumption kinetics could predict the full concentration-dependent crossover (Cl > Br at low salt, Br > Cl at high salt) from electrochemical data alone.
The triiodide signature offers a cheap diagnostic: in iodide solutions, UV absorption at roughly 350 nm should track H2O2 production, providing a cross-check beyond fluorescence assays.

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Editorial analysis

A structured set of objections, weighed in public.

Desk editor's note, referee report, and a circularity audit.

Desk Editor's Note

read the letter

Colleague — this paper does something useful: it reproduces George's halide and pH trends and shows they line up with corrosion chemistry on Al and Ti. The O2-free spray control is clean and, combined with the NMR cross-checks, makes the necessity of O2 about as solid as these measurements get. The halide crossover (Cl > Br at low concentration, Br > Cl at high) and the pitting-consumption explanation are genuinely new and worth taking seriously. The triiodide observation for iodide is a nice supporting detail.

The soft spot is the locus of production. The no-O2 control removes the oxidant but not the air-water interface, so it does not by itself rule out an O2-dependent air-water mechanism. The bulk immersion experiments show that corroding Al and Ti make H2O2, but the spray rig uses silica and glass, not those coupons. The paper cites prior work for glass corrosion, but it does not quantify the solid-surface contribution inside the spray geometry. So the universal negative—'no O2, no H2O2, and therefore no air-water role'—is an interpretation that goes beyond the data. A reader who believes in an electric-field or ion-separation mechanism can accept the O2 requirement and still say the air-water interface contributes when O2 is present. To close that gap, the authors would need to vary the solid surface area/material in the spray itself or use a non-corroding surface and show zero H2O2.

I also noticed the paper gives no error bars or replicate counts in the main figures. The trends are large enough that I suspect they are real, but the quantitative claims—like the crossover concentrations—deserve more than a single curve. That is fixable with statistics.

Overall: the paper is an honest, well-executed challenge to a prominent claim, with several new observations that stand on their own. The central interpretation is underdetermined, but not in a way that makes the work unserious. It deserves a real peer review, and the referees should push for direct locus identification and error bars. I'd bring it to a reading group.

Referee Report

3 major / 6 minor

Summary. The paper reports experiments on spontaneous hydrogen peroxide (H2O2) production in sprayed water microdroplets and at solid–water interfaces. The authors find that removing dissolved O2 eliminates detectable H2O2 in sprays regardless of halide identity, while in O2-bearing solutions H2O2 yields depend on halide type and pH. They reproduce the halide trend (Br > Cl > I at 10 mM) and the pH dependence reported by George and co-workers, but attribute all H2O2 production to O2 reduction at solid–water interfaces driven by surface corrosion. Halide effects are explained by pitting corrosion and iodide oxidation, and pH effects by the contrasting pH-dependent corrosion of Al versus Ti. The central conclusion is the mnemonic 'no O2, no H2O2', which is presented as refuting air–water interfacial or microdroplet-geometry mechanisms.

Significance. If the central claim is correct, the paper would be an important experimental contribution to the ongoing debate on spontaneous H2O2 formation in microdroplets, providing evidence against air–water interfacial mechanisms and supporting a corrosion-based alternative. Strengths include dual quantification by 1H-NMR and HPAK, the O2-free control, the cross-validation of trends with corrosion current measurements, and falsifiable predictions such as the absence of H2O2 without dissolved O2. However, because the spray experiments do not directly isolate solid-surface contributions within the spray geometry itself, the universal negative claim is not fully demonstrated; the significance is therefore conditional on additional locus identification.

major comments (3)

[Results, Fig. 1c-d and Conclusion] The O2-free spray control establishes that dissolved O2 is necessary for the H2O2 observed in sprays, but it does not identify the reaction site; an O2-dependent air–water or microdroplet pathway is equally consistent with the null result. The paper's universal claim that 'the air–water interface or the microdroplet geometry ... do not form H2O2' is therefore an inference from the bulk immersion experiments (Fig. 2) and prior work (ref 14), not a direct measurement in the spray geometry. Please add a control that varies the solid–water surface area or material inside the spray and collection train (e.g., compare silica versus PTFE capillaries, or add/remove solid beads in the collection flask) to demonstrate that the H2O2 yield scales with solid contact and not with droplet surface area.
[Results, The Curious Case of Cl- and Br-, and Fig. S6] The pitting-consumption mechanism is invoked to reconcile the divergent ordering of H2O2 yields (Br > Cl > I at 10 mM and above) and corrosion currents (Cl > Br > I). The only direct evidence for H2O2 consumption is Fig. S6, which shows that a freshly polished Al surface consumes more H2O2 than an oxide-covered one in a 100 µM H2O2 solution; it does not quantify consumption during pitting in chloride solutions at the concentrations and times of the experiments. The reconciliation should be presented as a hypothesis and tested directly, for example by measuring H2O2 decay in pitting versus non-pitting conditions with matched solution chemistry.
[Results, Quantifying Oxidation Rates of Solid Surfaces] The sentence 'we compare the trends in measured H2O2 concentrations in sprays (Figure 2b) and the corrosion at the solid–water interface (Figures 3b-c)' mislabels Figure 2b, which reports bulk immersion measurements at the Al–water interface, not spray measurements; the spray data are in Figure 1c and Figure S2. This conflation obscures which dataset supports the solid-water attribution. Please correct the cross-reference and state explicitly which data come from sprays and which from bulk immersion.

minor comments (6)

[Abstract] In the sentence 'demonstrating that aluminum and titanium surfaces more H2O2 in acidic and alkaline conditions', the verb 'produce' is missing.
[The Curious Case of I-] The phrase 'also noted by Georged & co-workers' contains a typo; it should read 'George'.
[Section S4] The references to 'Fig. 4a' in the text should be 'Fig. S4a' to match the supplementary numbering.
[Methods S2.4] The sentence 'The tests were carried out at a scan rate of 0.5 mV s−1 and were performed.' is grammatically incomplete; remove the trailing phrase.
[Figure 5c-d] The corrosion current values appear to mix units (mA/cm2 and µA/cm2); please verify and unify the units in the text and figure.
[Conclusion] The mnemonic 'no O2, no H2O2' should be qualified as 'under the conditions and detection limits tested' to avoid overgeneralization.

Circularity Check

0 steps flagged · score 0.0 of 10

No significant circularity: the central claims rest on new measurements; the no-O2 control is a necessary-condition test rather than a construction, and the same-author citation is supporting rather than definitional.

full rationale

The paper's main empirical content is self-contained and not circular by construction. The halide and pH trends are obtained from new spray experiments, immersion experiments on Al and Ti, and potentiodynamic polarization measurements, with H2O2 quantified independently by NMR and HPAK. No parameter is fitted and then renamed as a prediction. The 'no O2, no H2O2' result is an experimental necessary-condition observation, not a definitional identity: the paper does not define O2 reduction as H2O2 formation, nor does any equation equate the conclusion with an input. The inference that the solid-water interface, rather than the air-water interface, is the site in the spray is underdetermined by the O2-free control alone, but underdetermination is a scientific-inference limitation, not circularity. The one same-author citation (ref. 14) is used to extend the solid-water mechanism to glass and other non-metallic surfaces, and the paper also cites external corrosion reviews (refs. 38, 39); this is ordinary evidential reliance rather than a self-citation chain that forces the conclusion. The central claims are falsifiable by independent measurement and do not reduce to their inputs.

Assumptions & free parameters 0 free parameters · 3 assumptions · 0 invented entities

The ledger is small because the paper is an experimental refutation rather than a theory with derived parameters. The main assumptions concern the site of H2O2 production in sprays and the mechanistic roles of pitting and iodide scavenging.

assumptions (3)

domain assumption The H2O2 detected in sprayed microdroplets originates from O2 reduction at solid-water interfaces, not at air-water interfaces.
Inferred from the O2-free spray control and from separate bulk immersion experiments; the paper does not directly measure the solid-surface contribution in the spray geometry. Appears in Results, first section.
ad hoc to paper Pitting corrosion exposes fresh metal surfaces that consume H2O2, explaining why H2O2 is lower in high-concentration chloride solutions.
Supported qualitatively by SEM, polarization curves, and the fresh-metal consumption test (Fig. S6), but the quantitative relationship between pit density and the H2O2 deficit is not measured. Introduced in 'The Curious Case of Cl- and Br-'.
domain assumption The pH dependence of H2O2 formation is governed by the oxidation rate of the specific solid surface, not by water alkalinity.
Established for Al and Ti in this paper; its generality to other surfaces and to sprays is assumed.

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Cite this review

Pith. "Pith review of Disentangling the Roles of Dissolved Oxygen, Common Salts, and pH on the Spontaneous Hydrogen Peroxide Production in Water: No O2, No H2O2." pith.science (2026). https://pith.science/paper/SSNECFWN

@misc{pith2026250521175,
  author       = {Pith},
  title        = {Pith review of: Disentangling the Roles of Dissolved Oxygen, Common Salts, and pH on the Spontaneous Hydrogen Peroxide Production in Water: No O2, No H2O2},
  year         = {2026},
  howpublished = {\url{https://pith.science/paper/SSNECFWN}},
  note         = {Machine review of arXiv:2505.21175}
}

read the original abstract

Despite the mounting evidence proving that the air-water interface or the microdroplet geometry has nothing to do with the spontaneous formation of hydrogen peroxide (H2O2), the myth persists. Three recent studies by George and co-workers give credence to the myth by showing connections between the spontaneous formation of hydroxyl (HO) radicals and hydrogen peroxide (H2O2) in sprayed microdroplets with the solution pH, dissolved salts, nebulizing gas, and the gaseous environment. They report that among halides (chloride, bromide, and iodide), bromide dominates the H2O2 formation because of its ability to donate electrons. Also, they conclude that the H2O2 production at the air-water interface scales with waters alkalinity. In response, we apply a broad set of techniques, spanning NMR, potentiodynamic polarization, electron microscopy, and hydrogen peroxide assay kit (HPAK) fluorometry, to reexamine these claims. Our experiments reveal that regardless of the halide present in water, the air-water interface or the microdroplet geometry does not drive the H2O2 formation. It is the reduction of O2 at the solid-water interface that produces H2O2, i.e., in the absence of O2, no H2O2 is formed regardless of the halide ions. We explain the relative dependence of H2O2 concentrations on the halides based on their propensity to drive pitting corrosion (Chloride > Bromide > Iodide). As the pits appear in the passivating layer, exposing the metal, H2O2 is consumed in further oxidation. Next, we disprove the claim of alkalinity-driven H2O2 formation by demonstrating that aluminum and titanium surfaces produce more H2O2 in acidic and alkaline conditions, respectively. Taken together, these findings refute the conclusions of George and co-workers and others regarding spontaneous H2O2 generation at the air-water interface. The following mnemonic captures our conclusion: no O2, no H2O2.

Discussion (0). Continue with ORCID to comment.

Reference graph

Works this paper leans on

10 extracted references · 9 canonical work pages

[1]

K.; Walker, K

(1) Lee, J. K.; Walker, K. L.; Han, H. S.; Kang, J.; Prinz, F. B.; Waymouth, R. M.; Nam, H. G.; Zare, R. N. Spontaneous generation of hydrogen peroxide from aqueous microdroplets. Proceedings of the National Academy of Sciences of the United States of America 2019, 116 (39), 19294-19298. (2) Lee, J. K.; Han, H. S.; Chaikasetsin, S.; Marron, D. P.; Waymout...

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(25) Nguyen, D.; Lyu, P.; Nguyen, S. C. Experimental and Thermodynamic Viewpoints on Claims of a Spontaneous H2O2 Formation at the Air–Water Interface. The Journal of Physical Chemistry B 2023, 127 (11), 2323-2330. (26) Nguyen, D.; Nguyen, S. C. Revisiting the Effect of the Air –Water Interface of Ultrasonically Atomized Water Microdroplets on H2O2 Format...

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(28) LaCour, R. A.; Heindel, J. P.; Zhao, R.; Head -Gordon, T. The Role of Interfaces and Charge for Chemical Reactivity in Microdroplets. J Am Chem Soc 2025, 147 (8), 6299-6317. (29) Li, K.; Guo, Y .; Nizkorodov, Sergey A.; Rudich, Y .; Angelaki, M.; Wang, X.; An, T.; Perrier, S.; George, C. Spontaneous dark formation of OH radicals at the interface of a...

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The results revealed that H 2O2 is consumed more by the fresh metal surface as compared to one covered with an oxide layer. Fig. S6 Comparison of H 2O2 consumption by fresh metal surface vs the surface with oxide layer. References: (1) Eatoo, M. A.; Mishra, H. Busting the myth of spontaneous formation of H 2O2 at the air- water interface: contributions of...

work page Pith review arXiv 2024
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deionized

DOI: https://doi.org/10.1016/B978-0-7506-5924-6.X5000-4. (38) Frankel, G. S.; Vienna, J. D.; Lian, J.; Scully, J. R.; Gin, S.; Ryan, J. V .; Wang, J. W.; Kim, S. H.; Windl, W.; Du, J. C. A comparative review of the aqueous corrosion of glasses, crystalline ceramics, and metals. Npj Materials Degradation 2018, 2 (1). (39) Gin, S.; Dillmann, P.; Birbilis, N...

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[2015]

NMR characterization of H2O2 hydrogen exchange

(34) Kakeshpour, T.; Bax, A. NMR characterization of H2O2 hydrogen exchange. Journal of Magnetic Resonance 2021, 333, 107092. DOI: https://doi.org/10.1016/j.jmr.2021.107092. (35) Frankel, G. S. Pitting corrosion of metals - A review of the critical factors. Journal of the Electrochemical Society 1998, 145 (6), 2186-2198. (36) Fontana, M. G. Corrosion Engi...

arXiv 2021
[2022]

M.; Kuo, I

(6) Kathmann, S. M.; Kuo, I. F. W.; Mundy, C. J.; Schenter, G. K. Understanding the Surface Potential of Water. Journal of Physical Chemistry B 2011, 115 (15), 4369-4377. (7) Ben-Amotz, D. Electric buzz in a glass of pure water. Science 2022, 376 (6595), 800-801. (8) Heindel, J. P.; Hao, H.; LaCour, R. A.; Head-Gordon, T. Spontaneous formation of hydrogen...

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[2024]

J.; Williams, E

(20) Chen, C. J.; Williams, E. Are Hydroxyl Radicals Spontaneously Generated in Unactivated Water Droplets? Angewandte Chemie International Edition 2024, e202407433. DOI: https://doi.org/10.1002/anie.202407433 . (21) Chen, C. J.; Williams, E. R. A Source of the Mysterious m/z 36 Ions Identified: Implications for the Stability of Water and Unusual Chemistr...

work page doi:10.1002/anie.202407433 2024

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[2025]

(22) Asserghine, A.; Baby, A.; N’Diaye, J.; Romo, A

DOI: 10.1021/acscentsci.5c00306. (22) Asserghine, A.; Baby, A.; N’Diaye, J.; Romo, A. I. B.; Das, S.; Litts, C. A.; Jain, P. K.; Rodríguez-López, J. Dissolved Oxygen Redox as the Source of Hydrogen Peroxide and Hydroxyl Radical in Sonicated Emulsive Water Microdroplets. Journa...

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(10) Colussi, A. J. Mechanism of Hydrogen Peroxide Formation on Sprayed Water Microdroplets. Journal of the American Chemical Society 2023, 145 (30), 16315-16317. (11) Colussi, A. J. Physical Chemistry of Water Microdroplets. The Journal of Physical Chemistry Letters 2025, 16 ...

2023

Pith tools

Reviewed August 7, 2026 · model on record in the stance chip above.

[1] [1]

K.; Walker, K

(1) Lee, J. K.; Walker, K. L.; Han, H. S.; Kang, J.; Prinz, F. B.; Waymouth, R. M.; Nam, H. G.; Zare, R. N. Spontaneous generation of hydrogen peroxide from aqueous microdroplets. Proceedings of the National Academy of Sciences of the United States of America 2019, 116 (39), 19294-19298. (2) Lee, J. K.; Han, H. S.; Chaikasetsin, S.; Marron, D. P.; Waymout...

work page 2019

[2] [6]

(25) Nguyen, D.; Lyu, P.; Nguyen, S. C. Experimental and Thermodynamic Viewpoints on Claims of a Spontaneous H2O2 Formation at the Air–Water Interface. The Journal of Physical Chemistry B 2023, 127 (11), 2323-2330. (26) Nguyen, D.; Nguyen, S. C. Revisiting the Effect of the Air –Water Interface of Ultrasonically Atomized Water Microdroplets on H2O2 Format...

work page arXiv 2023

[3] [7]

A.; Heindel, J

(28) LaCour, R. A.; Heindel, J. P.; Zhao, R.; Head -Gordon, T. The Role of Interfaces and Charge for Chemical Reactivity in Microdroplets. J Am Chem Soc 2025, 147 (8), 6299-6317. (29) Li, K.; Guo, Y .; Nizkorodov, Sergey A.; Rudich, Y .; Angelaki, M.; Wang, X.; An, T.; Perrier, S.; George, C. Spontaneous dark formation of OH radicals at the interface of a...

work page 2025

[4] [10]

The results revealed that H 2O2 is consumed more by the fresh metal surface as compared to one covered with an oxide layer. Fig. S6 Comparison of H 2O2 consumption by fresh metal surface vs the surface with oxide layer. References: (1) Eatoo, M. A.; Mishra, H. Busting the myth of spontaneous formation of H 2O2 at the air- water interface: contributions of...

work page Pith review arXiv 2024

[5] [2006]

deionized

DOI: https://doi.org/10.1016/B978-0-7506-5924-6.X5000-4. (38) Frankel, G. S.; Vienna, J. D.; Lian, J.; Scully, J. R.; Gin, S.; Ryan, J. V .; Wang, J. W.; Kim, S. H.; Windl, W.; Du, J. C. A comparative review of the aqueous corrosion of glasses, crystalline ceramics, and metals. Npj Materials Degradation 2018, 2 (1). (39) Gin, S.; Dillmann, P.; Birbilis, N...

work page doi:10.1016/b978-0-7506-5924-6.x5000-4

[6] [2015]

NMR characterization of H2O2 hydrogen exchange

(34) Kakeshpour, T.; Bax, A. NMR characterization of H2O2 hydrogen exchange. Journal of Magnetic Resonance 2021, 333, 107092. DOI: https://doi.org/10.1016/j.jmr.2021.107092. (35) Frankel, G. S. Pitting corrosion of metals - A review of the critical factors. Journal of the Electrochemical Society 1998, 145 (6), 2186-2198. (36) Fontana, M. G. Corrosion Engi...

arXiv 2021

[7] [2022]

M.; Kuo, I

(6) Kathmann, S. M.; Kuo, I. F. W.; Mundy, C. J.; Schenter, G. K. Understanding the Surface Potential of Water. Journal of Physical Chemistry B 2011, 115 (15), 4369-4377. (7) Ben-Amotz, D. Electric buzz in a glass of pure water. Science 2022, 376 (6595), 800-801. (8) Heindel, J. P.; Hao, H.; LaCour, R. A.; Head-Gordon, T. Spontaneous formation of hydrogen...

work page 2011

[8] [2024]

J.; Williams, E

(20) Chen, C. J.; Williams, E. Are Hydroxyl Radicals Spontaneously Generated in Unactivated Water Droplets? Angewandte Chemie International Edition 2024, e202407433. DOI: https://doi.org/10.1002/anie.202407433 . (21) Chen, C. J.; Williams, E. R. A Source of the Mysterious m/z 36 Ions Identified: Implications for the Stability of Water and Unusual Chemistr...

work page doi:10.1002/anie.202407433 2024