Abstract
The scarcity of protons in alkaline media limits many proton-coupled energy conversion processes, particularly the hydrogen evolution reaction (HER). Here, we introduce a strategy to create a confined acidic microenvironment within strongly alkaline solution. Ultramicroporous Brønsted acidic zeolites stabilize hydrated protons through a size-exclusion effect, in the presence of bulky quaternary ammonium bases. In situ diffuse reflectance infrared Fourier transform spectroscopy and first-principles simulations reveal that confined protons derived from Brønsted acid sites migrate into the hydrogen-bond network of water, forming a Zundel–Eigen continuum that supports Grotthuss transport. Complementary inelastic neutron scattering and solid-state nuclear magnetic resonance confirm the persistence of hydrated protons under highly alkaline conditions. Guided by this principle, we developed a composite catalyst combining proton-donating nanoparticles with active, conductive layers, which delivers a 19–25% reduction in overpotential, a 20-fold enhancement in Pt mass activity, and accelerated kinetics compared with commercial Pt/C. These findings establish a broadly applicable framework for decoupling local proton activity from bulk pH, opening new pathways for HER and other proton-coupled reactions in alkaline environments.
| Original language | English |
|---|---|
| Pages (from-to) | 17294-17302 |
| Number of pages | 9 |
| Journal | Journal of the American Chemical Society |
| Volume | 148 |
| Issue number | 16 |
| DOIs | |
| State | Published - Apr 29 2026 |
Funding
This work was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under contract number DE-AC05-00OR22725 with the U.S. Department of Energy (DOE). The U.S. government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for U.S. government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). This research used resources at the Spallation Neutron Source, DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. Oak Ridge National Laboratory is managed by UT-Battelle, LLC, for U.S. DOE under Contract No. DEAC05-00OR22725. The beam time was allocated to VISION on proposal number IPTS-36037. This research used computing resources of National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231 using NERSC award ERCAP0024340. AEM tests performed by XL and AS are supported by the U.S. DOE through the Hydrogen from Next-generation Electrolyzers of Water (H2NEW) consortium and the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy.
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