Pulsed Electrocatalysis Driven Efficient Ammonia Synthesis by Facilitating *NOOH Formation and Balancing *H Supply.

Electrochemical nitrate reduction emerges as a promising approach for ammonia generation; however, its efficiency is hindered by the sluggish hydrogenation of nitrogen-containing intermediates and limited active hydrogen supply at constant applied potentials. Driven by the pulsed electrocatalysis, in this work, efficient nitrate-to-ammonia conversion is realized by facilitating *NOOH formation and balancing *H supply on a Janus Cu@Co/NC electrocatalyst. In detail, the Cu sites could activate NO at low overpotentials, while the Co sites could facilitate *NOOH formation with sufficient *H provided by the Co sites at high overpotentials.

Promoting the Intermediates Hydrogenation for Urea Electrosynthesis Over an "Active Hydrogen Pump" Catalyst.

Electrocatalytic coupling of CO and NO offers a sustainable approach for urea production. However, the limited supply of active hydrogen (*H) hinders the formation of the key carbon- and nitrogen-containing intermediates, thus impeding the selective C─N coupling. Herein, we developed copper molybdate (CuMoO) nanorods, which could serve as "active hydrogen pump" catalysts by regulating the water dissociation and hydrogen adsorption.

A Multiagent-Driven Robotic AI Chemist Enabling Autonomous Chemical Research On Demand.

The successful integration of large language models (LLMs) into laboratory workflows has demonstrated robust capabilities in natural language processing, autonomous task execution, and collaborative problem-solving. This offers an exciting opportunity to realize the dream of autonomous chemical research on demand. Here, we report a robotic AI chemist powered by a hierarchical multiagent system, ChemAgents, based on an on-board Llama-3.

Accelerating the Discovery of Efficient High-Entropy Alloy Electrocatalysts: High-Throughput Experimentation and Data-Driven Strategies.

High-entropy alloys (HEAs) present both significant potential and challenges for developing efficient electrocatalysts due to their diverse combinations and compositions. Here, we propose a procedural approach that combines high-throughput experimentation with data-driven strategies to accelerate the discovery of efficient HEA electrocatalysts for the hydrogen evolution reaction (HER). This enables the rapid preparation of HEA arrays with various element combinations and composition ratios within a model system.

In Situ Synthesis and Microfabrication of High Entropy Alloy and Oxide Compounds by Femtosecond Laser Direct Writing under Ambient Conditions.

Synthesis and coating of multi-metal oxides (MMOs) and alloys on conductive substrates are indispensable to electrochemical applications, yet demand multiple, resource-intensive, and time-consuming processes. Herein, an alternative approach to the synthesis and coating of alloys and MMOs by femtosecond laser direct writing (FsLDW) is reported. A solution-based precursor ink is deposited and dried on the substrate and illuminated by a femtosecond laser.

Efficient Electrocatalyst Nanoparticles from Upcycled Class II Capacitors.

To move away from fossil fuels, the electrochemical reaction plays a critical role in renewable energy sources and devices. The anodic oxygen evolution reaction (OER) is always coupled with these reactions in devices but suffers from large energy barriers. Thus, it is important for developing efficient OER catalysts with low overpotential.

Reversible Al Metal Anodes Enabled by Amorphization for Aqueous Aluminum Batteries.

Aqueous aluminum metal batteries (AMBs) are regarded as one of the most sustainable energy storage systems among post-lithium-ion candidates, which is attributable to their highest theoretical volumetric capacity, inherent safe operation, and low cost. Yet, the development of aqueous AMBs is plagued by the incapable aluminum plating in an aqueous solution and severe parasitic reactions, which results in the limited discharge voltage, thus making the development of aqueous AMBs unsuccessful so far. Here, we demonstrate that amorphization is an effective strategy to tackle these critical issues of a metallic Al anode by shifting the reduction potential for Al deposition.

Confining High-Valence Iridium Single Sites onto Nickel Oxyhydroxide for Robust Oxygen Evolution.

Enhancing activity and stability of iridium- (Ir-) based oxygen evolution reaction (OER) catalysts is of great significance in practice. Here, we report a vacancy-rich nickel hydroxide stabilized Ir single-atom catalyst (Ir-Ni(OH)), which achieves long-term OER stability over 260 h and much higher mass activity than commercial IrO in alkaline media. In situ X-ray absorption spectroscopy analysis certifies the obvious structure reconstruction of catalyst in OER.

Synergic Reaction Kinetics over Adjacent Ruthenium Sites for Superb Hydrogen Generation in Alkaline Media.

Ruthenium (Ru)-based electrocatalysts as platinum (Pt) alternatives in catalyzing hydrogen evolution reaction (HER) are promising. However, achieving efficient reaction processes on Ru catalysts is still a challenge, especially in alkaline media. Here, the well-dispersed Ru nanoparticles with adjacent Ru single atoms on carbon substrate (Ru -NC) is demonstrated to be a superb electrocatalyst for alkaline HER.

Dynamic Restructuring of Cu-Doped SnS Nanoflowers for Highly Selective Electrochemical CO Reduction to Formate.

With ever-increasing energy consumption and continuous rise in atmospheric CO concentration, electrochemical reduction of CO into chemicals/fuels is becoming a promising yet challenging solution. Sn-based materials are identified as attractive electrocatalysts for the CO reduction reaction (CO RR) to formate but suffer from insufficient selectivity and activity, especially at large cathodic current densities. Herein, we demonstrate that Cu-doped SnS nanoflowers can undergo in situ dynamic restructuring to generate catalytically active S-doped Cu/Sn alloy for highly selective electrochemical CO RR to formate over a wide potential window.

Anomalous self-optimization of sulfate ions for boosted oxygen evolution reaction.

Broadly, the oxygen evolution reaction (OER) has been deeply understood as a significant part of energy conversion and storage. Nevertheless, the anions in the OER catalysts have been neglected for various reasons such as inactive sites, dissolution, and oxidation, amongst others. Herein, we applied a model catalyst s-Ni(OH) to track the anionic behavior in the catalyst during the electrochemical process to fill this gap.

Tuning the Electronic Structures of Multimetal Oxide Nanoplates to Realize Favorable Adsorption Energies of Oxygenated Intermediates.

Highly active oxygen evolution reaction (OER) electrocatalysts are important to effectively transform renewable electricity to fuel and chemicals. In this work, we construct a series of multimetal oxide nanoplate OER electrocatalysts through successive cation exchange followed by electrochemical oxidation, whose electronic structure and diversified metal active sites can be engineered the mutual synergy among multiple metal species. Among the examined multimetal oxide nanoplates, CoCeNiFeZnCuO nanoplates exhibit the optimal adsorption energy of OER intermediates.

An All-Organic D-A System for Visible-Light-Driven Overall Water Splitting.

Direct water splitting over photocatalysts is a prospective strategy to convert solar energy into hydrogen energy. Nevertheless, because of the undesirable electron accumulation at the surface, the overall water-splitting efficiency is seriously restricted by the poor charge separation/transfer ability. Here, an all-organic donor-acceptor (D-A) system through crafting carbon rings units-conjugated tubular graphitic carbon nitride (C-TCN) is proposed.

A Unique Ru-N-P Coordinated Structure Synergistically Waking Up the Nonmetal P Active Site for Hydrogen Production.

Numerous experiments have demonstrated that the metal atom is the active center of monoatomic catalysts for hydrogen evolution reaction (HER), while the active sites of nonmetal doped atoms are often neglected. By combining theoretical prediction and experimental verification, we designed a unique ternary Ru-N-P coordination structure constructed by monodispersed Ru atoms supported on N,P dual-doped graphene for highly efficient hydrogen evolution in acid solution. The density functional theory calculations indicate that the charge polarization will lead to the most charge accumulation at P atoms, which results in a distinct nonmetallic P active sites with the moderate H∗ adsorption energy.

NiAg 3D porous nanoclusters with epitaxial interfaces exhibiting Pt like activity towards hydrogen evolution in alkaline medium.

The necessity of Earth-abundant low-cost catalysts with activity similar to noble metals such as platinum is indispensable in order to realize the production of hydrogen through electrolysis of water. Herein, we report a relatively low-cost NiAg 3D porous nanocluster catalyst whose activity matches with that of the state-of-the-art Pt/C in 1 M KOH solution. The catalyst is designed on the principle of creating an interface between a metal having a positive Gibbs energy of hydrogen adsorption and a metal of negative Gibbs energy based on the volcano plot, to tune the Gibbs energy of hydrogen adsorption near zero for enhanced hydrogen evolution.

Edge-Rich Fe-N Active Sites in Defective Carbon for Oxygen Reduction Catalysis.

Controllably constructing nitrogen-modified divacancies (ND) in carbon substrates to immobilize atomic Fe species and unveiling the advantageous configuration is still challenging, but indispensable for attaining optimal Fe-N-C catalysts for the oxygen reduction reaction (ORR). Herein, a fundamental investigation of unfolding intrinsically superior edge-ND trapped atomic Fe motifs (e-ND-Fe) relative to an intact center model (c-ND-Fe) in ORR electrocatalysis is reported. Density functional theory calculations reveal that local electronic redistribution and bandgap shrinkage for e-ND-Fe endow it with a lower free-energy barrier toward direct four-electron ORR.

Achieving Efficient Alkaline Hydrogen Evolution Reaction over a Ni P Catalyst Incorporating Single-Atomic Ru Sites.

Developing efficient electrocatalysts for alkaline water electrolysis is central to substantial progress of alkaline hydrogen production. Herein, a Ni P electrocatalyst incorporating single-atom Ru (Ni P -Ru) is synthesized through the filling of Ru species into the metal vacancies of nickel hydroxides and subsequent phosphorization treatment. Electron paramagnetic resonance spectroscopy, X-ray-based measurements, and electron microscopy observations confirm the strong interaction between the nickel-vacancy defect and Ru cation, resulting in more than 3.

Carbon Microtube Aerogel Derived from Kapok Fiber: An Efficient and Recyclable Sorbent for Oils and Organic Solvents.

A carbon microtube aerogel (CMA) with hydrophobicity, strong adsorption capacity, and superb recyclability was obtained by a feasible approach with economical raw material, such as kapok fiber. The CMA possesses a great adsorption capacity of 78-348 times its weight. Attributed to its outstanding thermal stability and excellent mechanical properties, the CMA can be used for many cycles of distillation, squeezing, and combustion without degradation, which suggests a potential practical application in oil-water separation.

Electrochemical Conversion of CO to Syngas with Controllable CO/H Ratios over Co and Ni Single-Atom Catalysts.

The electrochemical CO reduction reaction (CO RR) to yield synthesis gas (syngas, CO and H ) has been considered as a promising method to realize the net reduction in CO emission. However, it is challenging to balance the CO RR activity and the CO/H ratio. To address this issue, nitrogen-doped carbon supported single-atom catalysts are designed as electrocatalysts to produce syngas from CO RR.

Facile and eco-friendly preparation of super-amphiphilic porous polycaprolactone.

Super-amphiphilic (highly oleophilic and hydrophilic) materials have attracted tremendous interest for fundamental research and potential applications, owing to their unique affinity for both oil and water. In this work, a novel super-amphiphilic porous polycaprolactone (PCL) was fabricated via an efficient and eco-friendly method, in which stearic acid (SA) was used as both a porogen and a dopant precursor. The porous PCL had an interconnected hierarchical pore structure and was capable of absorbing oil and water rapidly.

Amorphous Fe-Ni-P-B-O Nanocages as Efficient Electrocatalysts for Oxygen Evolution Reaction.

Electrocatalysts are one of the most important parts for oxygen evolution reaction (OER) to overcome the sluggish kinetics. Herein, amorphous Fe-Ni-P-B-O (FNPBO) nanocages as efficient OER catalysts are synthesized by a simple low-cost and scalable method at room temperature. The samples are chemically stable, in clear contrast to reported unstable or even pyrophoric boride samples.

Metal-Oxide-Mediated Subtractive Manufacturing of Two-Dimensional Carbon Nitride for High-Efficiency and High-Yield Photocatalytic H Evolution.

g-CN is a promising visible-light-driven photocatalyst for H evolution reaction; however, the achievement of the high photocatalytic performance is primarily limited by the low separation efficiency of the photogenerated charge carriers and partly restricted by the slow kinetics of charge transfer. 2D g-CN can significantly improve the charge generation, transfer, and separation efficiencies. The 2D g-CN-based Z-scheme heterostructure can further enhance the charge-carrier separation and simultaneously increase the redox ability, thereby further boosting the photocatalytic performance.

Engineering the In-Plane Structure of Metallic Phase Molybdenum Disulfide Co and O Dopants toward Efficient Alkaline Hydrogen Evolution.

Molybdenum disulfide (MoS) has attracted much attention as a promising alternative to Pt-based catalysts for highly efficient hydrogen generation. However, it suffers sluggish kinetics for driving the hydrogen evolution reaction (HER) process because of inert basal planes, especially in alkaline solution. Here, we show a combination of heteroatom doping and phase transformation strategies to engineer the in-plane structure of MoS, that trigger their catalytic activities.