Wenwu Zhong

Direct seawater oxygen evolution reaction (OER) is critically hampered by chloride‐induced competitive oxidation, corrosion, and active‐site poisoning, driving the urgent need for highly active and chlorine‐tolerant electrocatalysts. Herein, a surface‐engineered electrocatalyst comprising osmium nanoparticles (Os NPs) anchored onto CoFe layered double hydroxide (Os/CoFe LDH) was prepared. X‐ray photoelectron spectroscopy revealed that the incorporated Os NPs stabilized high‐valence Co/Fe species, which preferentially promote OH ⁻ adsorption over Cl ⁻ and function as the genuine active centers for OER. Furthermore, in situ Raman spectroscopy demonstrates that Os NPs anchoring modulates the interfacial water structure, thereby enhancing water adsorption and facilitating seawater OER kinetics. The optimized Os/CoFe LDH‐40 achieves an overpotential of only 244 mV at 10 mA cm ⁻² in simulated alkaline seawater and operates stably for over 300 h in an anion exchange membrane electrolyzer at 300 mA cm ⁻² . This work not only develops a high‐performance catalyst for alkaline seawater OER but also offers new perspectives for advancing osmium‐based materials in electrocatalysis.

The oxide path mechanism (OPM) offers a compelling route to bypass the activity–stability trade‐off of conventional oxygen evolution catalysis. However, its deliberate activation has largely relied on doping strategies to create heterometallic dual sites, which suffer from limited electronic tunability. Here, we demonstrate a fundamentally different approach that combines heterojunction engineering with guided in situ reconstruction. By integrating ruthenium oxide with a cobalt–nickel telluride heterostructure, we exploit the pronounced surface reconstruction of tellurides under anodic potentials to in situ generate a metastable CoO ₂ phase featuring high‐valent cobalt. This reconstructed phase intimately couples with neighboring RuO ₂ to form well‐defined Co–O–Ru bridged dual sites, which are proposed as the pivotal centers for OPM‐enabled O─O coupling. The telluride framework further acts as an electronic modulator, stabilizing ruthenium while promoting high‐valent cobalt formation. This synergy yields a catalyst with an overpotential of 213 mV at 100 mA cm ⁻² and a mass activity 103 times that of commercial RuO ₂ . When deployed in an anion‐exchange membrane electrolyzer, it operates at 1 A cm ⁻² with a cell voltage of 1.78 V for over 800 h. Our work establishes heterojunction‐induced reconstruction as a powerful strategy to unlock OPM catalysis, moving beyond conventional doping toward dynamically assembled active interfaces.

Hydrogenolysis of waste plastics offers a promising route to valorize them into fuels, light olefins, and aromatics (BTX). Despite extensive studies, rational catalyst design and process optimization remain challenging. Although conventional catalysts (homogeneous, nanoparticle, bulk) have driven progress through interfacial and ensemble effects, the activity and stability of these systems ultimately originate from elementary steps at the atomic scale motivating a shift toward atomically precise active-site design. This Perspective highlights atomic active centers and key mechanistic factors and underscores the importance of techno-economic and life cycle analyses for atomically precise catalysts, providing guidance for designing efficient hydrogenolysis systems.

Ruthenium phosphide electrocatalysts for the hydrogen evolution reaction (HER) still face challenges such as insufficient active site utilization and limited durability. This work addresses these challenges via a synergistic strategy that integrates heterojunction engineering with a hollow confinement structure, resulting in RuP₂-Ni₂P nanoparticles embedded within N,P-codoped hollow carbon spheres (RuP₂-Ni₂P/NPC). The interfacial coupling between RuP₂ and Ni₂P optimizes the electronic structure toward a near-ideal hydrogen adsorption energy, while the unique embedded architecture ensures abundant accessible active sites and exceptional structural robustness. As a result, the RuP₂-Ni₂P/NPC catalyst exhibits superior HER performance across a wide pH range, achieving ultralow overpotentials of 3 mV in 1 M KOH and 17.3 mV in 0.5 M H₂SO₄ at 10 mA cm^-2, ranking among the best of reported RuP₂-based catalysts. It also demonstrates excellent long-term durability in both alkaline and acidic electrolytes. This work provides a feasible design strategy toward efficient and robust electrocatalysts for hydrogen production.

The oxygen evolution reaction (OER) mechanism on layered double hydroxides (LDHs) involves a delicate balance between the adsorbate evolution mechanism (AEM) and the lattice oxygen mechanism (LOM), with intercalated anions serving as a critical yet underexplored regulatory factor. Herein, four different anions (CO ₃ ²⁻ , VO ₄ ³⁻ , WO ₄ ²⁻ , MoO ₄ ²⁻ ) are intercalated into high‐entropy LDHs to systematically investigate their structure‐dependent effects. The results demonstrate that intercalated anion engineering governs the electronic structure of Ru active sites and concurrently promotes lattice oxygen participation in the OER. Although all anions promote a mixed AEM/LOM pathway, MoO ₄ ²⁻ induces the most pronounced electronic modification, lowering the Ru oxidation state and upshifting its d‐band center. This electronic configuration reduces the reaction energy barrier, thereby optimizing the AEM pathway, while simultaneously enabling moderate activation of lattice oxygen to facilitate the LOM route. As a result, the HE–MoO ₄ ²⁻ –LDH catalyst exhibits outstanding OER performance, achieving a low overpotential of 229.5 mV at 10 mA cm ⁻² with excellent operational stability. This work provides a key design guideline for tailoring reaction pathways in high‐entropy electrocatalysts through anion intercalation.

Electrooxidation of sterols is recognized as a promising approach for synthesizing value‐added steroid hormone pharmaceuticals. However, enhancing current density while delivering market‐required steroidal carbonyl products with high selectivity remains a significant challenge. Herein, we report a rational design of Ni ³⁺ ‐rich active sites on nickel nitride (Ni ₃ N) nanosheets via Pd‐induced electronic modulation, which is utilized for sterol oxidation coupled with hydrogen evolution reaction (HER). Experimental and theoretical analyses demonstrated that the strong electron‐withdrawing capability of Pd acts as an “electron pump,” accelerating the formation of high‐valent Ni ³⁺ active centers by attracting electrons from Ni ₃ N to Pd, facilitating the adsorption and activation of N‐(1‐hydroxy‐2,2,6,6‐tetramethylpiperidin‐4‐yl)acetamide (ACTH) during the oxidation process, thereby enhancing catalytic activity. The Pd‐Ni ₃ N composite as a bifunctional electrocatalyst for producing carbonyl product 1b (19‐Hydroxy‐4‐androstene‐3,17‐dione) and H ₂ concurrently at an industrial‐scale current of 5 A in a large flow electrolyzer, achieving productivities of 70.9 mmol/h for 1b (with 99% selectivity) and 93.1 mmol/h for H ₂ . This work provides a novel strategy for the electrosynthesis of valuable steroid intermediates alongside H ₂ production.

The industrial implementation of water electrolysis for hydrogen production is significantly hindered by the sluggish kinetics of the oxygen evolution reaction, while the high cost of state-of-the-art iridium-based catalysts remains a critical challenge. This work demonstrates an innovative heterojunction-doping synergy strategy through rational design of SrPd_3-xRu_xO₄/SrRuO₃ composite electrocatalysts. The strategy combines the structural advantages of cubic-phase SrPd₃O₄ and perovskite-type SrRuO₃, where their inherent compatibility facilitates atomic-level interface formation through oxygen-bridge coordination. Simultaneously, controlled Ru substitution in the SrPd₃O₄ lattice induces beneficial structural strain and precisely modulates the electronic environment to optimize intermediate adsorption energetics. The optimized catalyst exhibits exceptional electrocatalytic performance in 1 M KOH, delivering an overpotential as low as 227.6 mV at 10 mA cm^-2 and notably retaining stability for 300 hours at 50 mA cm^-2. In situ Raman spectroscopy confirms the dominance of the adsorbate evolution mechanism, while theoretical calculations reveal that the synergistic effects diminish the activation energy barrier governing the rate-determining step. This work not only provides fundamental insights into the design of Pd-based oxide catalysts but also establishes a generalizable approach for developing high-performance electrocatalysts through synergistic structural engineering.

Hydrogen energy has attracted much attention as a clean energy source, but its large-scale application faces storage and transportation challenges. Negative hydrogen medium (metal hydrides and borohydrides) materials have become a research hotspot due to their efficient hydrogen storage capacity. Investigating the role of negative hydrogen in the structure of materials can improve our understanding of the various structural properties of hydrogen and provide valuable insights into the design of hydrogen-containing materials with new functionalities. This paper reviews the research progress on negative hydrogen medium in recent years. Specifically, they include magnesium hydride (MgH₂), sodium aluminum hydride (NaAlH₄), lithium borohydride (LiBH₄), ammonia borane (AB, NH₃BH₃), sodium borohydride (NaBH₄), and potassium borohydride (KBH₄). The catalytic performance of different catalysts used for hydrogen storage and release in the negative hydrogen medium in the last three years is summarized, and the structure–performance relationship of different catalysts for negative hydrogen medium is described on the nanoscale and atomic scale. The reasons for monolithic catalyst and light-enhanced hydrogen release performances are also described. The research progress on the regeneration of negative hydrogen materials is summarized from both computational and experimental perspectives. Finally, the main challenges and development prospects of the negative hydrogen medium in the future are put forward. This review contributes to the basic understanding of the design and mechanism studies of negative hydrogen medium catalysts and provides effective design principles for overcoming the problems of low rates of hydrogen storage and release and the difficulty of cyclic regeneration.

This review systematically explores strategies to enhance product selectivity in PEC CO ₂ RR, and further analyzes recent advances in C ₁ /C ₂ product synthesis, challenges in selectivity control, and future directions.