Evidence map›Paper›PMID 38228851›Full record

ArticleNature chemistry2024

A molecular-level mechanistic framework for interfacial proton-coupled electron transfer kinetics.

Noah B Lewis, Ryan P Bisbey, Karl S Westendorff, Alexander V Soudackov, Yogesh Surendranath

Abstract read
PubMed Publisher
In one paragraph

Article in Nature chemistry, 2024. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 17 papers.

0numbers the graph read from it
0cells of the map it votes in
17citing papers in PubMed
–field-weighted citation impact
1 · What the graph read from it

What it found

Each row is one number read from the abstract, on the scale the paper reported it, with its interval. Left of the dashed line favours the treatment, right favours the comparator. Under each row is the sentence it came from. New to these charts? A ten-minute tutorial.

The abstract states no effect estimate the extractor could read, or names no intervention and outcome on the map, so this paper lights no cell and moves no belief. It is still indexed, cited and linked below.

2 · The registry

The trial behind it

Trials whose registry record cites this paper, or whose number appears in the abstract. A trial that started after this paper was published is citing it as background, not reporting it.

Neither the registry nor the abstract names a trial number. If this is a trial report, that itself is worth knowing.

3 · Its place in the literature

Who cites it

17 citing papers in PubMed.

  1. Article
  2. Tailored Catalytic Microenvironments Enable Efficient Electrochemical Ammonia Production.Advanced science (Weinheim, Baden-Wurttemberg, Germany) · 2026
    Article
  3. Article
  4. Ionic Liquids as Interfacial Media for Metal-Free Electrochemical COACS sustainable chemistry & engineering · 2026
    Article
  5. Article
  6. Article
  7. Article
  8. Article
  9. Structured electrolytes facilitate Grotthuss-type transport for enhanced proton-coupled electron transfer reactions.Proceedings of the National Academy of Sciences of the United States of America · 2026
    Article
  10. Synthesis of 4,5-DisubstitutedThe Journal of organic chemistry · 2025
    Article
  11. Article
  12. Article
  13. Article
  14. Review
  15. Article
  16. Article
  17. Article
4 · The record

Corrections and comments

PubMed lists nothing against this paper. Absence here is not a guarantee, only a check that was made.

5 · Who and what money

Authors and funding

5 authors.

Noah B LewisDepartment of Chemistry, Massachusetts Institute of Technology, Cambridge, MA, USA.ORCID http://orcid.org/0000-0003-4646-2481
Ryan P BisbeyDepartment of Chemistry, Massachusetts Institute of Technology, Cambridge, MA, USA.ORCID http://orcid.org/0000-0001-8699-5077
Karl S WestendorffDepartment of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA.ORCID http://orcid.org/0000-0001-6565-1945
Alexander V SoudackovDepartment of Chemistry, Yale University, New Haven, CT, USA.ORCID http://orcid.org/0000-0001-9581-8494
Yogesh SurendranathDepartment of Chemistry, Massachusetts Institute of Technology, Cambridge, MA, USA. yogi@mit.edu.ORCID http://orcid.org/0000-0003-1016-3420

Funding

DOE | SC | Basic Energy Sciences (BES) DE-SC0020973
6 · The paper itself

Abstract

Electrochemical proton-coupled electron transfer (PCET) reactions can proceed via an outer-sphere electron transfer to solution (OS-PCET) or through an inner-sphere mechanism by interfacial polarization of surface-bound active sites (I-PCET). Although OS-PCET has been extensively studied with molecular insight, the inherent heterogeneity of surfaces impedes molecular-level understanding of I-PCET. Herein we employ graphite-conjugated carboxylic acids (GC-COOH) as molecularly well-defined hosts of I-PCET to isolate the intrinsic kinetics of I-PCET. We measure I-PCET rates across the entire pH range, uncovering a V-shaped pH-dependence that lacks the pH-independent regions characteristic of OS-PCET. Accordingly, we develop a mechanistic model for I-PCET that invokes concerted PCET involving hydronium/water or water/hydroxide donor/acceptor pairs, capturing the entire dataset with only four adjustable parameters. We find that I-PCET is fourfold faster with hydronium/water than water/hydroxide, while both reactions display similarly high charge transfer coefficients, indicating late proton transfer transition states. These studies highlight the key mechanistic distinctions between I-PCET and OS-PCET, providing a framework for understanding and modelling more complex multistep I-PCET reactions critical to energy conversion and catalysis.

Identifiers

What OpenQuestion holds

Textmetadata
Read underepoch 390

Registered trials

None linked

Read under generation 80e0d062 · epoch 390. Bibliography from PubMed, PubMed Central and OpenAlex; grants from NIH RePORTER; trial links from ClinicalTrials.gov; estimates, votes and beliefs from the OpenQuestion graph.