Catalysis

Adsorption

Engineering

Chemical physics

Boron

Electrochemistry

Materials science

Density functional theory

Biochemistry

Chemical engineering

Dissociation (chemistry)

Hydrogen storage

Electrocatalyst

Physical chemistry

Hydrogen

Nanotechnology

Organic chemistry

Desorption

Computational chemistry

Ruthenium

Chemistry

Electrode

Electrolyte

Osmium

Nature Communications

Developing high-performance electrocatalysts for hydrogen evolution reaction (HER) is crucial for sustainable hydrogen production, yet still challenging. Here, we report boron-modulated osmium (B-Os) aerogels with rich defects and ultra-fine diameter as a pH-universal HER electrocatalyst. The catalyst shows the small overpotentials of 12, 19, and 33 mV at a current density of 10 mA cm −2 in acidic, alkaline, and neutral electrolytes, respectively, as well as excellent stability, surpassing commercial Pt/C. Operando X-ray absorption spectroscopy shows that interventional interstitial B atoms can optimize the electron structure of B-Os aerogels and stabilize Os as active sites in an electron-deficient state under realistic working conditions, and simultaneously reveals the HER catalytic mechanisms of B-Os aerogels in pH-universal electrolytes. The density functional theory calculations also indicate introducing B atoms can tailor the electronic structure of Os, resulting in the reduced water dissociation energy and the improved adsorption/desorption behavior of hydrogen, which synergistically accelerate HER.

Interstitial boron-triggered electron-deficient Os aerogels for enhanced pH-universal hydrogen evolution