A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
Disentangling Multiple pH-Dependent Factors on the Hydrogen Evolution Reaction at Au(111) (2025)


Zhen, E.-F., Liu, B.-Y., Zhang, M.-K., Zhang, L., Zhang, C.-Y., Cai, J., Melander, M. M., Huang, J., & Chen, Y.-X. (2025). Disentangling Multiple pH-Dependent Factors on the Hydrogen Evolution Reaction at Au(111). Precision Chemistry, Early online. https://doi.org/10.1021/prechem.4c00081


JYU-tekijät tai -toimittajat


Julkaisun tiedot

Julkaisun kaikki tekijät tai toimittajatZhen, Er-Fei; Liu, Bing-Yu; Zhang, Meng-Ke; Zhang, Lu−Lu; Zhang, Chen-Yu; Cai, Jun; Melander, Marko M.; Huang, Jun; Chen, Yan-Xia

Lehti tai sarjaPrecision Chemistry

eISSN2771-9316

Julkaisuvuosi2025

Ilmestymispäivä08.01.2025

VolyymiEarly online

KustantajaAmerican Chemical Society (ACS)

JulkaisumaaYhdysvallat (USA)

Julkaisun kielienglanti

DOIhttps://doi.org/10.1021/prechem.4c00081

Julkaisun avoin saatavuusAvoimesti saatavilla

Julkaisukanavan avoin saatavuusKokonaan avoin julkaisukanava

Julkaisu on rinnakkaistallennettu (JYX)https://jyx.jyu.fi/handle/123456789/99364


Tiivistelmä

Understanding how the electrolyte pH affects electrocatalytic activity is a topic of crucial importance in a large variety of systems. However, unraveling the origin of the pH effects is complicated often by the fact that both the reaction driving forces and reactant concentrations in the electric double layer (EDL) change simultaneously with the pH value. Herein, we employ the hydrogen evolution reaction (HER) at Au(111)-aqueous solution interfaces as a model system to disentangle different pH-dependent factors. In 0.1 M NaOH, the HER current density at Au(111) in the potential range of −0.4 V < ERHE < 0 V is up to 60 times smaller than that in 0.1 M HClO4. A reaction model with proper consideration of the local reaction conditions within the EDL is developed. After correcting for the EDL effects, the rate constant for HER is only weakly pH-dependent. Our analysis unambiguously reveals that the observed pH effects are mainly due to the pH-dependent reorganization free energy, which depends on the electrostatic potential and the local reaction conditions within the EDL. Possible origins of the pH and temperature dependence of the activation energy and the electron transfer coefficients are discussed. This work suggests that factors influencing the intrinsic pH-dependent kinetics are easier to understand after proper corrections of EDL effects.


YSO-asiasanatkemialliset reaktiotvetyelektrokatalyysipHpintakemiasähkökemia

Vapaat asiasanathydrogen evolution reaction; Au(111) electrode; pH effect; rate constants; EDL effects


Liittyvät organisaatiot

JYU-yksiköt:


OKM-raportointiKyllä

VIRTA-lähetysvuosi2025


Viimeisin päivitys 2025-25-01 klo 20:05