Unlocking a Water Coordination Environment in Co-Based Metal-Organic Frameworks for Advanced Nitrate-to-Ammonia Electroreduction.

Electrochemical nitrate reduction to ammonia (-NORR) offers a promising and sustainable alternative to the traditional Haber-Bosch process, enabling decentralized ammonia production under ambient conditions. However, the efficiency of -NORR is limited by the sluggish reaction kinetics due to the high activation energy barriers, poor mass transport, and the weaker adsorption affinity of the catalyst surface. In this study, we report the design and synthesis of a stable three-dimensional cobalt-based metal-organic framework (HUST-38), constructed from benzene-1,4-dicarboxylate ligand and DABCO, featuring water coordination within its framework.

Decoupled Control of CO and Nitrate Reduction Intermediates to Enable Efficient Tandem Urea Electrosynthesis.

The direct electrochemical coupling of CO and nitrate (NO) offers a sustainable alternative to the energy-intensive Bosch-Meiser process for urea synthesis. However, achieving efficient C-N coupling at single active sites remains challenging due to the kinetic mismatch between CO and NO reduction, as well as the intricate multistep proton-coupled electron transfer process. Here, we present a sacrificial template-based strategy to synthesize a two-dimensional (2D)/zero-dimensional (0D) FePS/AgS heterostructure catalyst, enabling the tandem coreduction of CO and nitrate for urea electrosynthesis.

Designing Molecular Reactor of Interlayer Dual-Atom Toward Urea Electrosynthesis.

Electrocatalytic C─N coupling offers a sustainable alternative to energy-intensive industrial processes for urea synthesis. Herein, we design conjugated polymer-based molecular reactors featuring interlayer diatomic Cu-N sites and precisely tunable spacings (4.0, 4.

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.

Realizing Unconventional Tandem Nitrate Reduction for Efficient Ammonia Electrosynthesis Enabled by Co, Fe Dual-Site Conjugated Metal Organic Frameworks.

The electrochemical nitrate-to-ammonia reduction reaction (NORR) offers a sustainable route for carbon-neutral chemical synthesis, while the intricate multi-electron/proton transfer processes and unstable intermediates pose significant challenges in attaining high selectivity and efficiency. This study demonstrates a Co, Fe bimetallic conjugated metal organic frameworks (CoFe-cMOFs) that enable efficient NORR via an unconventional [6 + 2] electron-transfer tandem pathway. Unlike the traditional [2 + 6] tandem pathway, the Fe sites predominantly reduce NO to *NHOH intermediate, which subsequently spills over onto the Co sites for further protonation.

Breaking low-strain and rapid-kinetics trade-off in heterostructured prussian blue cathode toward robust sodium storage.

Manganese-based hexacyanoferrate has garnered unprecedented attention for sodium-ion batteries due to their high theoretical capacity. However, the structural strain associated with Jahn-Teller distortion incurs fast capacity decline and poor rate capability. Effectively reconciling the trade-off between low-strain and rapid-kinetics in manganese-based hexacyanoferrate cathode poses a considerable challenge.

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.

Enabling Unconventional "Alternating-Distal" N Reduction Pathway for Efficient Ammonia Electrosynthesis.

The general understanding on the reaction path is that the electrocatalytic N reduction follows either individual associative alternating or distal pathways, where efficient N activation and selective NH production are very challenging. Herein, an unconventional "alternating-distal" pathway was achieved by shifting the "*NHNH→*NHNH" to "*NHNH→*NH + NH" step to boost NH synthesis with an amorphous CeMnO electrocatalyst. In this unconventional process, N activation was realized through π back donation on the Mn site, while the Mn/Ce dual active sites could regulate the intermediate configurations to avoid the nitrogen-containing by-product formation.

Boosting HO production via two-electron oxygen reduction with O-doped g-CN decorated with TiCT quantum dots.

Photocatalytic synthesis of HO with g-CN holds great promise for converting solar energy into chemical energy, but it remains constrained by the narrow optical absorption range and rapid charge recombination. To overcome these challenges, TiCT MXene quantum dots (TQDs), known for their ease of carrier regulation and strong visible light absorption, were incorporated into O-doped g-CN (O-CN) to form TQDs-modified O-CN (O-CN@TQDs) with a Schottky heterojunction. Attributed to such structural design, the HO production was promoted through the two-step two-electron oxygen reduction pathway, with O serving as the primary intermediate.

Electrocatalytic Reduction of CO to Long-Chain Hydrocarbons: Investigating the Asymmetric C-C Coupling Mechanism on PdAu Catalysts.

The electrochemical reduction of CO to high-energy-density hydrocarbons is pivotal for addressing energy and environmental challenges. Understanding the mechanisms underlying the conversion of CO to long-chain hydrocarbons is both crucial and complex. In this study, we employed density functional theory (DFT) calculations to investigate the C-C coupling mechanisms responsible for the formation of C2-C4 products on PdAu catalysts.

Tailoring Water-in-DMSO Electrolyte for Ultra-stable Rechargeable Zinc Batteries.

Rechargeable zinc batteries (RZBs) are hindered by two primary challenges: instability of Zn anode and deterioration of the cathode structure in traditional aqueous electrolytes, largely attributable to the decomposition of active HO. Here, we design and synthesize a non-flammable water-in-dimethyl sulfoxide electrolyte to address these issues. X-ray absorption spectroscopy, in situ techniques and computational simulations demonstrate that the activity of HO in this electrolyte is extremely compressed, which not only suppresses the side reactions and increases the reversibility of Zn anode, but also diminishes the cathode dissolution and proton intercalation.

Microplastic detection and remediation through efficient interfacial solar evaporation for immaculate water production.

Freshwater scarcity and microplastics (MPs) pollution are two concerning and intertwined global challenges. In this work, we propose a "one stone kills two birds" strategy by employing an interfacial solar evaporation platform (ISEP) combined with a MPs adsorbent. This strategy aims to produce clean water and simultaneously enhance MPs removal.

Interface engineering enabled by sodium dodecyl sulfonate surfactant for stable Zn metal batteries.

Aqueous zinc-ion batteries are emerging as powerful candidates for large-scale energy storage, due to their inherent high safety and high theoretical capacity. However, the inevitable hydrogen evolution and side effects of the deposition process limit their lifespan, which requires rational engineering of the interface between anode and aqueous electrolyte. In this paper, an anionic surfactant as electrolyte additive, sodium dodecyl sulfonate (SDS), is introduced to deliver highly reversible zinc metal batteries.

Achieving Dendrite-Free Zinc Metal Anodes via Molecule Anchoring and lon-Transport Pumping.

The potential for scale-up application has been acknowledged by researchers for rechargeable aqueous zinc-ion batteries (ZIBs). Nonetheless, the progress of the development is significantly impeded due to the instability of the interface between the zinc anode and electrolyte. Herein, efficient and environmentally benign valine (Val) were introduced as aqueous electrolyte additive to stabilize the electrode/electrolyte interface (EEI) via functional groups in additive molecules, thus achieving reversible dendrite-free zinc anode.

Nitroxyl radical triggered the construction of a molecular protective layer for achieving durable Zn metal anodes.

The issues of dendrite growth, hydrogen evolution reaction, and zinc anode corrosion have significantly hindered the widespread implementation of aqueous zinc-ion batteries (AZIBs). Herein, trace amounts of 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) additive is introduced into AZIBs to protect the zinc metal anode. Trace amounts of the TEMPO additive with nitroxyl radical can provide fast Zn transport and anode protection ability by forming an adsorbed molecular layer via Zn-O bond.

The Construction of Surface-Frustrated Lewis Pair Sites to Improve the Nitrogen Reduction Catalytic Activity of InO.

The construction of a surface-frustrated Lewis pairs (SFLPs) structure is expected to break the single electronic state restriction of catalytic centers of P-region element materials, due to the existence of acid-base and basic active canters without mutual quenching in the SFLPs system. Herein, we have constructed eight possible SFLPS structures on the InO (110) surface by doping non-metallic elements and investigated their performance as electrocatalytic nitrogen reduction catalysts using density functional theory (DFT) calculations. The results show that P atom doping (P@InO) can effectively construct the structure of SFLPs, and the doped P atom and In atom near the vacancy act as Lewis base and acid, respectively.

Tuning Main Group Element-based Metal-Organic Framework to Boost Electrocatalytic Nitrogen Reduction Under Ambient Conditions.

Main group element-based materials are emerging catalysts for ammonia (NH ) production via a sustainable electrochemical nitrogen reduction reaction (N RR) pathway under ambient conditions. However, their N RR performances are less explored due to the limited active behavior and unclear mechanism. Here, an aluminum-based defective metal-organic framework (MOF), aluminum-fumarate (Al-Fum), is investigated.

Interface Engineering for Aqueous Aluminum Metal Batteries: Current Progresses and Future Prospects.

Aqueous aluminum metal batteries (AMBs) have attracted numerous attention because of the abundant reserves, low cost, high theoretical capacity, and high safety. Nevertheless, the poor thermodynamics stability of metallic Al anode in aqueous solution, which is caused by the self-corrosion, surface passivation, or hydrogen evolution reaction, dramatically limits the electrochemical performance and hampers the further development of AMBs. In this comprehensive review, the key scientific challenges of Al anode/electrolyte interface (AEI) are highlighted.

Recent Advances in Metal-Organic Framework-Based Nanomaterials for Electrocatalytic Nitrogen Reduction.

The production of ammonia under moderate conditions is of environmental and sustainable importance. The electrochemical nitrogen reduction reaction (E-NRR) method has been intensively investigated in the recent decades. Nowadays, the further development of E-NRR is largely hindered by the lack of competent electrocatalysts.

Ammonia Electrosynthesis with a Stable Metal-Free 2D Silicon Phosphide Catalyst.

Metal-free 2D phosphorus-based materials are emerging catalysts for ammonia (NH ) production through a sustainable electrochemical nitrogen reduction reaction route under ambient conditions. However, their efficiency and stability remain challenging due to the surface oxidization. Herein, a stable phosphorus-based electrocatalyst, silicon phosphide (SiP), is explored.

An efficient and multifunctional S-scheme heterojunction photocatalyst constructed by tungsten oxide and graphitic carbon nitride: Design and mechanism study.

The design of multifunctional photocatalyst with strong redox performance is the key to achieve sustainable utilization of solar energy. In this study, an elegant S-scheme heterojunction photocatalyst was constructed between metal-free graphitic carbon nitride (g-CN) and noble-metal-free tungsten oxide (WO). As-established S-scheme heterojunction photocatalyst enabled multifunctional photocatalysis behavior, including hydrogen production, degradation (Rhodamine B) and bactericidal (Escherichia coli) properties, which represented extraordinary sustainability.

Emerging p-Block-Element-Based Electrocatalysts for Sustainable Nitrogen Conversion.

Artificial nitrogen conversion reactions, such as the production of ammonia via dinitrogen or nitrate reduction and the synthesis of organonitrogen compounds via C-N coupling, play a pivotal role in the modern life. As alternatives to the traditional industrial processes that are energy- and carbon-emission-intensive, electrocatalytic nitrogen conversion reactions under mild conditions have attracted significant research interests. However, the electrosynthesis process still suffers from low product yield and Faradaic efficiency, which highlight the importance of developing efficient catalysts.

Rechargeable Aqueous Aluminum-Ion Battery: Progress and Outlook.

The high cost and scarcity of lithium resources have prompted researchers to seek alternatives to lithium-ion batteries. Among emerging "Beyond Lithium" batteries, rechargeable aluminum-ion batteries (AIBs) are yet another attractive electrochemical storage device due to their high specific capacity and the abundance of aluminum. Although the current electrochemical performance of nonaqueous AIBs is better than aqueous AIBs (AAIBs), AAIBs have recently gained attention due to their low cost and enhanced safety.

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.

A Defect Engineered Electrocatalyst that Promotes High-Efficiency Urea Synthesis under Ambient Conditions.

Synthesizing urea from nitrate and carbon dioxide through an electrocatalysis approach under ambient conditions is extraordinarily sustainable. However, this approach still lacks electrocatalysts developed with high catalytic efficiencies, which is a key challenge. Here, we report the high-efficiency electrocatalytic synthesis of urea using indium oxyhydroxide with oxygen vacancy defects, which enables selective C-N coupling toward standout electrocatalytic urea synthesis activity.