Yun Zu

Developing efficient and durable electrocatalysts for oxygen and hydrogen evolution reactions (OER/HER) remains fundamentally challenging due to the intrinsic trade‐off between activity and stability. We herein report a high‐entropy‐engineered strategy to stabilize single Ru atoms on FeCoNiCrMn spinel oxides to overcome the dilemma. The resulting catalyst delivers excellent bifunctional activity and stability, revealed by low overpotentials of merely 280 mV at 100 mA cm ⁻² for OER and 37 mV at 10 mA cm ⁻² for HER, a low cell voltage of 1.66 V at 1 A cm ⁻² for anion exchange membrane water electrolyzer and undamped cell performance at 1 A cm ⁻² for 1500 h. Experimental and theoretical results illustrate that single Ru atoms coordinated by O ₄ Cl species are active centers with the lowest theoretical overpotentials for OER and HER. Uniquely, reversible oxyhydroxides reconstructed from spinel oxides occur in the OER process. Meanwhile, Ru single atoms anchored on the oxyhydroxides has much higher dissolution potential than RuO ₂ and catalyzes OER following the stable adsorbate evolution mechanism pathway, resulting in excellent stability. This work highlights high‐entropy engineering for stabilizing and activating single‐atom catalysts, offering new insights into rational design of advanced catalysts for future sustainable energy device development.

Developing efficient and durable electrocatalysts for oxygen and hydrogen evolution reactions (OER/HER) remains fundamentally challenging due to the intrinsic trade‐off between activity and stability. We herein report a high‐entropy‐engineered strategy to stabilize single Ru atoms on FeCoNiCrMn spinel oxides to overcome the dilemma. The resulting catalyst delivers excellent bifunctional activity and stability, revealed by low overpotentials of merely 280 mV at 100 mA cm ⁻² for OER and 37 mV at 10 mA cm ⁻² for HER, a low cell voltage of 1.66 V at 1 A cm ⁻² for anion exchange membrane water electrolyzer and undamped cell performance at 1 A cm ⁻² for 1500 h. Experimental and theoretical results illustrate that single Ru atoms coordinated by O ₄ Cl species are active centers with the lowest theoretical overpotentials for OER and HER. Uniquely, reversible oxyhydroxides reconstructed from spinel oxides occur in the OER process. Meanwhile, Ru single atoms anchored on the oxyhydroxides has much higher dissolution potential than RuO ₂ and catalyzes OER following the stable adsorbate evolution mechanism pathway, resulting in excellent stability. This work highlights high‐entropy engineering for stabilizing and activating single‐atom catalysts, offering new insights into rational design of advanced catalysts for future sustainable energy device development.

Alloying Ni with another metal on γ‐Al ₂ O ₃ support holds considerable promise to enhance carbon‐resistance in dry reforming of methane (DRM), yet its effectiveness is constrained by poorly controlled alloy structure and surface Al‐OH groups. Herein, bimetallic NiCo/γ‐Al ₂ O ₃ catalysts were designated using electropositive NiCo complexes via a strong electrostatic adsorption strategy. The NiCo alloy and oxygen vacancy were primarily derived from the evolution of surface Al‐ μ ₂ ‐OH and Al‐ μ ₃ ‐OH groups anchored NiCo layered structures. The optimized Ni _3.0 Co _3.0 Al catalyst achieved near‐thermodynamic‐equilibrium CH ₄ and CO ₂ conversions, along with ultra‐low coke deposition rate (0.03 mg _coke ·g _cat ⁻¹ ·h ⁻¹ ) after 200 h on‐stream at 600°C. Microkinetic and in situ FTIR studies elucidated the reaction mechanism, wherein CH _x * species from CH ₄ decomposition on atomically uniform NiCo alloys were rapidly eliminated by surface Al–OH and reactive O* generated from CO ₂ dissociation on limited oxygen vacancies, forming labile HCOO* and CH _x O* intermediates, while effectively suppressing the Boudouard reaction, thereby ensuring exceptional catalyst longevity.

A confining-coupling growth method is developed to prepare high-performance NiFe&FeNCL/G catalyst with abundant atomic Fe–N ₄ moieties and ultrasmall FeNi hydroxides, showing a low potential gap of 0.68 V for electrocatalytic oxygen reactions.

Using a solid-state ligand assistance strategy, we tailor metal–support interactions via precise Ni-complex modulation to fabricate highly dispersed Ni/beta catalysts with exceptional n -hexane hydroisomerization performance.