Reasonable design of electrocatalysts with rapid self-reconstruction for efficient oxygen evolution reaction (OER) under commercially demanded current density is highly desired, but really challenging. Herein, ultrathin Fe-modified Ni hydroxysulfide (Fe-NiSOH)...

Designing efficient and durable electrocatalysts for seawater splitting to avoid undesired chlorine evolution reaction and resist the corrosive seawater is crucial for seawater electrolysis technology. Herein, a functional bimetal (Co and Fe) is designed specifically to modify nickel phosphide (denoted as CoFe‐Ni2P) for boosting seawater splitting, where the Fe atom improves the conductivity of Ni2P for improving electron transfer, and the Co atom accelerates the self‐reconstruction process to favorably generate bimetal co‐incorporated NiOOH (CoFe‐NiOOH) species on the electrode surface. Additionally, these in situ‐generated CoFe‐NiOOH species remarkably inhibit the adsorption of Cl− ions but selectively adsorb OH− ions, which contributes to excellent performance of the CoFe‐Ni2P electrode for large‐current‐density seawater splitting. Therefore, the CoFe‐Ni2P electrode only requires low overpotentials of 266 and 304 mV to afford current densities of 100 and 500 mA cm−2 in a harsh 6 m KOH + seawater electrolyte, and can work stably for 600 h. Impressively, a flow‐type anion exchange membrane electrolyzer assembled by the CoFe‐Ni2P/Ni‐felt bifunctional electrode is demonstrated to run stably at an industrially large current density of 1.0 A cm−2 in 6 m KOH + seawater electrolyte for 350 h, which shows promising application prospects.

Green syngas production from Earth-abundant and renewable resources is a viable means to achieve carbon neutrality.

Light-driven hydrogen production from renewable liquid biomass derivatives rather than fossil fuels offers an ideal path towards carbon neutrality.1–3 It is often however operated under an anaerobic condition with the limitations of sluggish kinetics and severe coking. Herein, a disruptive air-promoted strategy is explored for exceptionally efficient and durable light-driven hydrogen production from bioethanol over a core/shell Cr2O3@GaN nanowires semiconducting architecture. Owing to the unique catalytic attributes of Cr2O3@GaN, bioethanol is energetically favorable to be adsorbed on the Cr2O3@GaN interface, followed by dehydrogenation toward acetaldehyde and protons by photoexcited holes. The released protons are then consumed for H2 evolution by photogenerated electrons. After that, O2 can be evolved into active oxygen species and promote the continuous deprotonation and C-C cleavage of the key C2 intermediate, thus significantly lowering the reaction energy barrier of hydrogen evolution from bioethanol and removing the carbon residual with inhibited bioethanol overoxidation. As a result, hydrogen is produced at a high rate of 76.9 mole H2 per gram Cr2O3@GaN per hour by only feeding bioethanol, air, and light. Notably, an unprecedented light-to-hydrogen efficiency of 17.6% is achieved under concentrated light illumination of 7 W∙cm-2. A distinguished turnover frequency of > 2,314,000 mole H2 per mole Cr2O3 per hour, in conjunction with a superior stability of 180 hours, leads to the achievement of a record-high turnover number of 266,943,000 mole H2 per mole Cr2O3. The simultaneous generation of aldehyde from bioethanol dehydrogenation enables the process more economically promising.