Ir Nanoparticles Anchored on Metal‐Organic Frameworks for Efficient Overall Water Splitting under pH‐Universal Conditions

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(17)

Опубликована: Март 2, 2023

The construction of high-activity and low-cost electrocatalysts is critical for efficient hydrogen production by water electrolysis. Herein, we developed an advanced electrocatalyst anchoring well-dispersed Ir nanoparticles on nickel metal-organic framework (MOF) Ni-NDC (NDC: 2,6-naphthalenedicarboxylic) nanosheets. Benefiting from the strong synergy between MOF through interfacial Ni-O-Ir bonds, synthesized Ir@Ni-NDC showed exceptional electrocatalytic performance evolution reaction (HER), oxygen (OER) overall splitting in a wide pH range, superior to commercial benchmarks most reported electrocatalysts. Theoretical calculations revealed that charge redistribution bridge induced optimization H2 O, OH* H* adsorption, thus leading accelerated electrochemical kinetics HER OER. This work provides new clue exploit bifunctional pH-universal splitting.

Язык: Английский

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Metastabilizing the Ruthenium Clusters by Interfacial Oxygen Vacancies for Boosted Water Splitting Electrocatalysis

Advanced Energy Materials, Год журнала: 2024, Номер 14(21)

Опубликована: Фев. 2, 2024

Abstract Metal–support interaction (MSI) is witnessed as an essential manner to stabilize active metals and tune catalytic activity for heterogonous water splitting. Kinetically driving the electrolysis (WE) appeals a rational MSI system with coupled electron‐donating/accepting (e‐D/A) characters hydrogen/oxygen evolution reactions (HER/OER). However, metal stabilization effect by will in turn restrict deblocking of e‐D/A properties challenge full electrocatalytic optimization. This study profiles heterostructure featuring metastable Ru clusters on defective NiFe hydroxide (Ru/d‐NiFe LDH) support low‐precious (≈2 wt%) platform efficient WE. It indicated that interfacial oxygen vacancies can deviate stable 4d 5 orbit 2+δ state, regulate d‐band center levels toward facilitated HER/OER processes. Resultantly, Ru/d‐NiFe LDH attains ultralow overpotentials at 10 mA cm −2 Pt‐beyond alkaline HER (18 mV) OER (220 fast kinetics durability. The symmetrical electrolyzer delivers promising voltage 1.49 V 1 m KOH seawater splitting performance. work carries interesting opportunities rationalizing sophisticated metal‐support electrocatalysts through metal‐site metastabilization engineering.

Язык: Английский

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Graphene Quantum Dot-Mediated Atom-Layer Semiconductor Electrocatalyst for Hydrogen Evolution

Nano-Micro Letters, Год журнала: 2023, Номер 15(1)

Опубликована: Сен. 28, 2023

The hydrogen evolution reaction performance of semiconducting 2H-phase molybdenum disulfide (2H-MoS2) presents a significant hurdle in realizing its full potential applications. Here, we utilize theoretical calculations to predict possible functionalized graphene quantum dots (GQDs), which can enhance HER activity bulk MoS2. Subsequently, design GQD-induced in-situ bottom-up strategy fabricate near atom-layer 2H-MoS2 nanosheets mediated with GQDs (ALQD) by modulating the concentration electron withdrawing/donating functional groups. Experimental results reveal that introduction series during synthesis ALQD plays crucial role. Notably, higher and strength electron-withdrawing groups on GQDs, thinner more active resulting are. Remarkably, synthesized ALQD-SO3 demonstrate significantly improved performance. Our provides simple efficient approach for expanding catalytic application Furthermore, it holds substantial developing other transition-metal dichalcogenide materials.

Язык: Английский

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Electrochemical Co-Production of Ammonia and Biodegradable Polymer Monomer Glycolic Acid via the Co-Electrolysis of Nitrate Wastewater and Waste Plastic

ACS Catalysis, Год журнала: 2023, Номер 13(15), С. 10394 - 10404

Опубликована: Июль 25, 2023

Electrochemical reformation of nitrate wastewater and poly(ethylene terephthalate) (PET) plastic waste into ammonia (NH3) fine chemicals is a sustainable strategy for resource utilization. Herein, co-production system glycolic acid (GA, degradable polymer monomer) constructed by coupling reduction ethylene glycol (EG, in PET hydrolysate) oxidation. Low-crystalline CoOOH (LC-CoOOH/CF) Pd nanothorns (Pd NTs/NF) grown situ on the metal foam substrates are employed as cathode anode, respectively. The high density amorphous regions LC-CoOOH/CF enables enhanced adsorption provides abundant active sites, ultimately leading to an Faradic efficiency (FE) 97.38 ± 1.0% at −0.25 V vs reversible hydrogen electrode (RHE). Meanwhile, unique nanothorn morphology endows NTs/NF with high-curvature tip, triggering tip effect (TE) promote highly selective oxidation EG GA. Furthermore, two-electrode system, NH3 GA operated low energy consumption (onset voltage: 0.5 V), much lower than traditional electrolysis process (1.4 V). This study method utilization co-produce value-added chemicals.

Язык: Английский

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Manipulation of Electron Spins with Oxygen Vacancy on Amorphous/Crystalline Composite-Type Catalyst

ACS Nano, Год журнала: 2023, Номер 18(1), С. 1214 - 1225

Опубликована: Дек. 27, 2023

By substituting the oxygen evolution reaction (OER) with anodic urea oxidation (UOR), it not only reduces energy consumption for green hydrogen generation but also allows purification of urea-rich wastewater. Spin engineering d orbital and oxygen-containing adsorbates has been recognized as an effective pathway enhancing performance electrocatalysts. In this work, we report fabrication a bifunctional electrocatalyst composed amorphous RuO2-coated NiO ultrathin nanosheets (a-RuO2/NiO) abundant amorphous/crystalline interfaces (HER) UOR. Impressively, 1.372 V voltage is required to attain current density 10 mA cm–2 over electrolyzer. The increased vacancies in a-RuO2/NiO by incorporation RuO2 enhance total magnetization entail numerous spin-polarized electrons during reaction, which speeds up UOR kinetics. functional theory study reveals that promote charge-carrier transfer, tailored d-band center endows optimized adsorption oxygen-generated intermediates. This kind vacancy induced toward boosting HER kinetics provides reliable reference exploration advanced

Язык: Английский

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Enlarging the Ni–O Bond Polarizability in a Phosphorene-Hosted Metal–Organic Framework for Boosted Water Oxidation Electrocatalysis

ACS Nano, Год журнала: 2023, Номер 17(17), С. 17254 - 17264

Опубликована: Авг. 31, 2023

The emerging lattice-oxygen oxidation mechanism (LOM) presents attractive opportunities for breaking the scaling relationship to boost oxygen evolution reaction (OER) with direct OLattice-*O interaction. However, currently LOM-triggering rationales are still debated, and a streamlined physicochemical paradigm is extremely desirable design of LOM-defined OER catalysts. Herein, Ni metal-organic framework/black phosphorene (NiMOF/BP) heterostructure theoretically profiled constructed as catalytic platform LOM-derived studies. It found that p-type BP host can enlarge Ni-O bond polarizability NiMOF through stretching valence declining synergically. Such an enlarged will in principle alleviate lattice confinement benefit LOM pathway performance. As result, optimized NiMOF/BP catalyst exhibits promising performance low overpotential 260 mV at 10 mA cm-2 long-term stability 1 M KOH electrolyte. Both experiment calculation results suggest activated more balanced step barrier catalyst. This research puts forward criterion LOM-scaled electrocatalysts water oxidation.

Язык: Английский

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Recent Progress of Non‐Noble Metallic Heterostructures for the Electrocatalytic Hydrogen Evolution

Small Science, Год журнала: 2023, Номер 3(9)

Опубликована: Авг. 2, 2023

Developing energy production, storage, and conversion technologies based on sustainable or renewable is essential to address the environmental crisis. Electrochemical water splitting one of most promising approaches realize production green hydrogen. The design catalytic materials with low cost, high activity, long‐term stability exploration specific reaction mechanisms are key focus for involved electrochemical hydrogen evolution (HER). Recently, substantial efforts have been devoted rational synthesis non‐noble metallic heterostructures fascinating synergistic effects among different components. These heterostructured demonstrate comprehensive properties exceeding estimations by rule mixtures display activity in industrial conditions HER. Herein, mechanism parameters improving performance HER process discussed detail. latest advances synthetic methods electrocatalytic characteristics from experimental computational perspectives summarized according role various insights provided this review into an in‐depth understanding as electrocatalysts, opportunities challenges scale up future‐oriented developments highlighted.

Язык: Английский

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A self-circulating pathway for the oxygen evolution reaction

Energy & Environmental Science, Год журнала: 2023, Номер 16(11), С. 5210 - 5219

Опубликована: Янв. 1, 2023

The self-circulation between Ni(OH) 2 and NiOOH during water oxidation significantly lowers the overpotential of oxygen evolution reaction (OER).

Язык: Английский

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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

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Lithiation Enhances Electrocatalytic Iodine Conversion and Polyiodide Confinement in Iodine Host for Zinc–Iodine Batteries

Advanced Functional Materials, Год журнала: 2023, Номер 33(45)

Опубликована: Июль 5, 2023

Abstract Aqueous static zinc–iodine batteries attract tremendous attention because of their abundant reserves iodine, nonflammable electrolyte, and facile assembly. Currently, scientific challenges for include self‐discharge sluggish kinetics. Herein, a lithiation approach the iodine host to suppress shuttle effect catalyze conversion is reported. Through regulating d ‐ p ‐band center lowering I − /I 0 barrier, Li + intercalation into VS 2 reinforces interaction with 3 achieves catalytic ameliorating self‐discharge, accelerating Zinc–iodine featuring LiVS as reach high utilization, Coulombic efficiencies, long cyclic lifespan. Notably, performance enhancement mechanism thermodynamically favorable reaction, inhibition appearance, promotion consumption due insertion. The findings provide fundamental insights tackling issues batteries.

Язык: Английский

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