Platinum-Ruthenium Dual-Atomic Sites Dispersed in Nanoporous Ni0.85Se Enabling Ampere-Level Current Density Hydrogen Production.

Alkaline anion-exchange-membrane water electrolyzers (AEMWEs) using earth-abundant catalysts is a promising approach for the generation of green H2. However, the AEMWEs with alkaline electrolytes suffer from poor performance at high current density compared to proton exchange membrane electrolyzers. Here, atomically dispersed Pt-Ru dual sites co-embedded in nanoporous nickel selenides (np/Pt1Ru1-Ni0.85Se) are developed by a rapid melt-quenching approach to achieve highly-efficient alkaline hydrogen evolution reaction. The np/Pt1Ru1-Ni0.85Se catalyst shows ampere-level current density with a low overpotential (46 mV at 10 mA cm-2 and 225 mV at 1000 mA cm-2), low Tafel slope (32.4 mV dec-1), and excellent long-term durability, significantly outperforming the benchmark Pt/C catalyst and other advanced large-current catalysts. The remarkable HER performance of nanoporous Pt1Ru1-Ni0.85Se is attributed to the strong intracrystal electronic metal-support interaction (IEMSI) between Pt-Se-Ru sites and Ni0.85Se support which can greatly enlarge the charge redistribution density, reduce the energy barrier of water dissociation, and optimize the potential determining step. Furthermore, the assembled alkaline AEMWE with an ultralow Pt and Ru loading realizes an industrial-level current density of 1 A cm-2 at 1.84 volts with high durability.

Constructing Nanoporous Ir/Ta2 O5 Interfaces on Metallic Glass for Durable Acidic Water Oxidation.

Although proton exchange membrane water electrolyzers (PEMWE) are considered as a promising technique for green hydrogen production, it remains crucial to develop intrinsically effective oxygen evolution reaction (OER) electrocatalysts with high activity and durability. Here, a flexible self-supporting electrode with nanoporous Ir/Ta2O5 electroactive surface is reported for acidic OER via dealloying IrTaCoB metallic glass ribbons. The catalyst exhibits excellent electrocatalytic OER performance with an overpotential of 218 mV for a current density of 10 mA cm-2 and a small Tafel slope of 46.1 mV dec-1 in acidic media, superior to most electrocatalysts. More impressively, the assembled PEMWE with nanoporous Ir/Ta2 O5 as an anode shows exceptional performance of electrocatalytic hydrogen production and can operate steadily for 260 h at 100 mA cm-2 . In situ spectroscopy characterizations and density functional theory calculations reveal that the modest adsorption of OOH* intermediates to active Ir sites lower the OER energy barrier, while the electron donation behavior of Ta2 O5 to stabilize the high-valence states of Ir during the OER process extended catalyst's durability.

Pd Atomic Engineering of Nanoporous Ni/NiO for Efficient Nitrophenol Hydrogenation Reaction.

The catalytic hydrogenation of nitrophenols is widely utilized for both industrial synthesis and environmental protection, thus efficient and cost-effective catalysts are in urgent need. Still, the cost and scarcity of the materials still inhibit their application and the active sites are not well specified, especially in the complex catalysts. Herein, we developed an atomic Pd-doped nanoporous Ni/NiO (Pd1@np-Ni/NiO) catalyst via facial dealloying for efficient nitrophenol hydrogenation reaction under mild conditions. Pd1@np-Ni/NiO achieves an excellent specific activity (1301 min-1 mgPd-1, 35.2 times that of commercial Pd/C), nearly 100% selectivity, and continuous reproducibility. The catalytic performance is highly relevant to the Ni sites on the catalysts regarding the exposure sites and the intrinsic property. The metal/metal oxide interfacial structure could cooperatively accelerate the catalytic reaction kinetics. The atomic dopants could effectively modulate the electronic structure, facilitate the absorption of molecules, and reduce the energy barrier of catalytic hydrogenation reaction. Based on the efficient catalyst, the protype nitrophenol//NaBH4 battery is designed for efficient material conversion and power output, which is very attractive for green energy systems.

Rapid Melt-Quenching Enables General Synthesis of High-Loading Single-Atom Catalysts with Bicontinuous Nanoporous Structure.

Single-atom catalysts have attracted extensive attention due to their unique atomic structures and extraordinary activities in catalyzing chemical reactions. However, the lack of general and efficient approaches for producing high-density single atoms on suitably tailored supporting matrixes hinders their industrial applications. Here, a rapid melt-quenching strategy with high throughput to synthesize single atoms with high metal-atom loadings of up to 9.7 wt% or 2.6 at% on nanoporous metal compounds is reported, representing several-fold improvements compared to benchmarks in the literature. Mechanism characterizations reveal that the high-temperature melting provides the essential liquid environment and activation energy to achieve the atomization of metals, while the following rapid-quenching pins the isolated metal atoms and stabilizes the coordination environment. In comparison with carbon-supported single-atom catalysts, various collaboration combinations of single atoms and nanoporous metal compounds can be synthesized using the strategy, thus achieving efficient hydrazine oxidation-assisted H2 production. This synthesis protocol is highly compatible with automatic operation, which provides a feasible and general route to design and manufacture specific single-atom catalysts with tunable atomic metal components and supporting matrixes, thus promoting the deployment of single-atom catalysts for various energy technology applications.