Substantial Impact of Built‐in Electric Field and Electrode Potential on the Alkaline Hydrogen Evolution Reaction of Ru−CoP Urchin Arrays

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(12)

Опубликована: Янв. 30, 2024

Although great efforts on the delicate construction of a built-in electric field (BIEF) to modify electronic properties active sites have been conducted, substantial impact BIEF coupled with electrode potential electrochemical reactions has not clearly investigated. Herein, we designed an alkaline hydrogen evolution reaction (HER) catalyst composed heterogeneous Ru-CoP urchin arrays carbon cloth (Ru-CoP/CC) strong guidance density functional theory (DFT) calculations. Impressively, despite its unsatisfactory activity at 10 mA cm

Язык: Английский

---

Organocatalyst Supported by a Single‐Atom Support Accelerates both Electrodes used in the Chlor‐Alkali Industry via Modification of Non‐Covalent Interactions

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(8)

Опубликована: Янв. 6, 2024

Consuming one of the largest amount electricity, chlor-alkali industry supplies basic chemicals for society, which mainly consists two reactions, hydrogen evolution (HER) and chlorine reaction (CER). Till now, state-of-the-art catalyst applied in this field is still dimensional stable anode (DSA), consumes a large noble metal Ru Ir. It thus necessary to develop new types catalysts. In study, an organocatalyst anchored on single-atom support (SAS) put forward. exhibits high catalytic efficiency towards both HER CER with overpotential 21 mV 20 at 10 mA cm

Язык: Английский

---

Manipulating the Microenvironment of Single Atoms by Switching Support Crystallinity for Industrial Hydrogen Evolution

Angewandte Chemie International Edition, Год журнала: 2023, Номер 63(7)

Опубликована: Дек. 28, 2023

Abstract Modulating the microenvironment of single‐atom catalysts (SACs) is critical to optimizing catalytic activity. Herein, we innovatively propose a strategy improve local reaction environment Ru single atoms by precisely switching crystallinity support from high crystalline and low crystalline, which significantly improves hydrogen evolution (HER) The catalyst anchored on low‐crystalline nickel hydroxide (Ru−LC−Ni(OH) 2 ) reconstructs distribution balance interfacial ions due activation effect metal dangling bonds support. Single‐site with oxidation state induces aggregation hydronium (H 3 O + ), leading formation acidic in alkaline media, breaking pH‐dependent HER As comparison, high‐crystalline (Ru−HC−Ni(OH) exhibits sluggish Volmer step conventional environment. expected, Ru−LC−Ni(OH) requires overpotentials 9 136 mV at 10 1000 mA cm −2 conditions operates stably 500 for h an seawater anion exchange membrane (AEM) electrolyzer. This study provides new perspective constructing highly active electrocatalysts.

Язык: Английский

---

Tailored Metal‐Organic Framework‐Based Nanozymes for Enhanced Enzyme‐Like Catalysis

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 19, 2024

Abstract The global crisis of bacterial infections is exacerbated by the escalating threat microbial antibiotic resistance. Nanozymes promise to provide ingenious solutions. Here, we reported a homogeneous catalytic structure Pt nanoclusters with finely tuned metal–organic framework (ZIF‐8) channel structures for treatment infected wounds. Catalytic site normalization showed that active aggregates fine‐tuned pore modifications had capacity 14.903×10 5 min −1 , which was 18.7 times higher than particles in monodisperse state ZIF‐8 (0.793×10 ). In situ tests revealed change from homocleavage heterocleavage hydrogen peroxide at interface nanozyme one key reasons improvement activity. Density‐functional theory and kinetic simulations reaction jointly determine role center substrate together. Metabolomics analysis developed nanozyme, working conjunction reactive oxygen species, could effectively block energy metabolic pathways within bacteria, leading spontaneous apoptosis rupture. This pioneering study elucidates new ideas regulation artificial enzyme activity provides perspectives development efficient substitutes.

Язык: Английский

---

Enhancing Ni/Co Activity by Neighboring Pt Atoms in NiCoP/MXene Electrocatalyst for Alkaline Hydrogen Evolution

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(20)

Опубликована: Фев. 27, 2024

Density functional theory (DFT) calculations demonstrate neighboring Pt atoms can enhance the metal activity of NiCoP for hydrogen evolution reaction (HER). However, it remains a great challenge to link and NiCoP. Herein, we introduced curvature bowl-like structure construct Pt/NiCoP interface by adding minimal 1 ‰-molar-ratio Pt. The as-prepared sample only requires an overpotential 26.5 181.6 mV accordingly achieve current density 10 500 mA cm

Язык: Английский

---

Advances of Synergistic Electrocatalysis Between Single Atoms and Nanoparticles/Clusters

Nano-Micro Letters, Год журнала: 2024, Номер 16(1)

Опубликована: Июль 9, 2024

Combining single atoms with clusters or nanoparticles is an emerging tactic to design efficient electrocatalysts. Both synergy effect and high atomic utilization of active sites in the composite catalysts result enhanced electrocatalytic performance, simultaneously provide a radical analysis interrelationship between structure activity. In this review, recent advances single-atomic site coupled are emphasized. Firstly, synthetic strategies, characterization, dynamics types clusters/nanoparticles introduced, then key factors controlling discussed. Next, several clean energy catalytic reactions performed over synergistic illustrated. Eventually, encountering challenges recommendations for future advancement energy-transformation electrocatalysis outlined.

Язык: Английский

---

The hybrid Pt nanoclusters/Ru nanowires catalysts accelerating alkaline hydrogen evolution reaction

Advanced Powder Materials, Год журнала: 2024, Номер 3(5), С. 100214 - 100214

Опубликована: Июнь 13, 2024

Water electrolysis via alkaline hydrogen evolution reaction (HER) is a promising approach for large-scale production of high-purity at low cost, utilizing renewable and clean energy. However, the sluggish kinetics derived from high energy barrier water dissociation impedes seriously its practical application. Herein, series hybrid Pt nanoclusters/Ru nanowires (Pt/Ru NWs) catalysts are demonstrated to accelerate HER. And optimized Pt/Ru NWs (10 ​% wt Pt) exhibits exceptional performance with an ultralow overpotential (24 ​mV 10 ​mA ​cm−2), small Tafel slope (26.3 dec−1), long-term stability, outperforming benchmark commercial Pt/C-JM-20 catalyst. This amazing also occurred in anion-exchange membrane devices, where it delivered cell voltage about 1.9 ​V 1 ​A ​cm−2 outstanding stability (more than 100 ​h). The calculations have revealed such superior exhibited by stems formed heterointerfaces, which significantly reduce decisive rate step cooperative-action between cluster Ru substance. work provides valuable perspectives designing advanced materials toward HER beyond.

Язык: Английский

---

Microwave‐Assisted PtRu Alloying on Defective Tungsten Oxide: A Pathway to Improved Hydroxyl Dynamics for Highly‐Efficient Hydrogen Evolution Reaction

Advanced Energy Materials, Год журнала: 2024, Номер unknown

Опубликована: Сен. 3, 2024

Abstract Platinum (Pt)‐based compounds are the benchmarked catalysts for hydrogen evolution reaction (HER) but exhibit slow kinetics in alkaline environments. The * OH accumulation on Pt surface can block active sites, affecting proton reduction and water re‐adsorption. Alloying Ruthenium (Ru) with sites significantly modulate adsorption desorption of dissociation intermediates. Choosing suitable supports utilizing metal‐support interaction (MSI) is crucial site optimization. PtRu alloy anchored tungsten oxide (WO 3 ) rich oxygen vacancies (O V prepared through an ultrafast microwave‐assisted approach. Benefiting from coupling effects between alloying MSI, PtRu/WO ‐O exhibits exceptionally high HER activity. In 1 m KOH, KOH + seawater, 0.5 H 2 SO 4 , it requires ultralow overpotentials 9, 26, 6 mV to achieve 10 mA cm −2 respectively. designed catalyst surpasses commercial Pt/C mass activity demonstrates considerable potential intermittent energy integration. Density functional theory reveals that Ru reduces barrier dissociating OH, modulating blockage then promoting overall process. This study offers insights into rapid synthesis non‐carbon supported modulation generation.

Язык: Английский

---

Leveraging Dual‐Atom Catalysts for Electrocatalysis Revitalization: Exploring the Structure‐Performance Correlation

Advanced Energy Materials, Год журнала: 2024, Номер 14(18)

Опубликована: Фев. 27, 2024

Abstract In light of the profound shift toward renewable fuels, dual‐atom catalysts (DACs) are impressively prospected as auspicious for electrocatalysis revitalization, accomplishing environmental remediation and sustainable global energy security. Leveraging appealing attributes such inspiring synergistic effect, additional adjacent adsorption sites, ultrahigh atom utilization, DACs endowed with unprecedented stability, activity, selectivity in multifarious energy‐related applications. By virtue addressing time technological prominence to review this ground‐breaking atomic electrocatalyst, first encompasses a correlation elucidation between substrate, dual‐atoms, facile synthetic approaches intriguing modification strategies. Furthermore, state‐of‐the‐art characterization techniques specially employed spotlighted, alongside rigorously unveiling novel mechanistic insights’ milestone gained from both theoretical modeling experimental research multitudes environmentally benign electrocatalytic applications, including O 2 reduction, CO H evolution, N other fundamental reactions. As final note, presents brief conclusion highlighting current challenges outlining prospects frontier. Importantly, deciphers structure‐performance while excavating advancement DACs, thus is anticipated shed catalysis community on bolstering an intense evolution triggering sapient inspiration more robust next‐generation catalysts.

Язык: Английский

---

Iron Molybdenum Sulfide‐Supported Ultrafine Ru Nanoclusters for Robust Sulfion Degradation‐Assisted Hydrogen Production

Advanced Functional Materials, Год журнала: 2024, Номер 34(27)

Опубликована: Март 5, 2024

Abstract Electrocatalytic hydrogen evolution and (S 2− ) recycling present promising strategies for cost‐effective production simultaneous removal of environmental pollutants. However, the advancement this technology is hindered by limited availability affordable, efficient, stable catalysts. Herein, study synthesizes ultrafine ruthenium (Ru) nanoclusters on a substrate iron molybdenum sulfide (FeMo‐S) nanosheets, creating new heterointerface catalyst (FeMo‐S/Ru) reaction (HER) sulfion oxidation (SOR). Experimental theoretical calculations suggest that strong electron interactions between Ru FeMo‐S substrate, optimizing *H adsorption promoting HER activity one side while facilitating sulfur intermediates other side, effectively catalyzing SOR. Additionally, assembled electrocatalytic coupling system with FeMo‐S/Ru displays an ultralow cell voltage 0.57 V at 100 mA cm −2 , achieving high Faradaic efficiencies (>96%) H 2 production, also exhibiting remarkable durability over 1 month (838 h). This work paves way development highly efficient durable supported catalysts, enabling energy‐saving environmentally friendly recycling.

Язык: Английский

---