Atomically dispersed materials: Ideal catalysts in atomic era

Nano Research, Journal Year: 2023, Volume and Issue: 17(1), P. 18 - 38

Published: May 25, 2023

Language: Английский

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Electrocatalytic water splitting: Mechanism and electrocatalyst design

Nano Research, Journal Year: 2023, Volume and Issue: 16(7), P. 9142 - 9157

Published: April 2, 2023

Language: Английский

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Lattice Strain Engineering of Ni₂P Enables Efficient Catalytic Hydrazine Oxidation‐Assisted Hydrogen Production

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(42)

Published: July 11, 2023

Hydrazine-assisted water electrolysis provides new opportunities to enable energy-saving hydrogen production while solving the issue of hydrazine pollution. Here, synthesis compressively strained Ni2 P as a bifunctional electrocatalyst for boosting both anodic oxidation reaction (HzOR) and cathodic evolution (HER) is reported. Different from multistep synthetic method that induces lattice strain by creating core-shell structures, facile strategy developed tune via dual-cation co-doping. The obtained with compressive -3.62% exhibits significantly enhanced activity HzOR HER than counterparts tensile without strain. Consequently, optimized delivers current densities 10 100 mA cm-2 at small cell voltages 0.16 0.39 V hydrazine-assisted electrolysis, respectively. Density functional theory (DFT) calculations reveal promotes dissociation concurrently tunes adsorption strength intermediates, thereby facilitating process on P. As HzOR, reduces energy barrier potential-determining step dehydrogenation *N2 H4 H3 . Clearly, this work paves pathway lattice-strained electrocatalysts

Language: Английский

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Fluorinated Ni‐O‐C Heterogeneous Catalyst for Efficient Urea‐Assisted Hydrogen Production

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(44)

Published: June 20, 2023

Abstract Constructing multiple heterogeneous structures allows for improving the electrocatalytic activity of NiO by incorporating active sites. Unfortunately, poor conductivity makes efficient charge transfer within difficult, thereby inhibiting improvement its intrinsic activity. Herein, F‐doped NiO/Ni@C catalyst (F‐NiO/Ni@C) is fabricated via a new organic‐inorganic hybrid approach, showing both advanced hydrogen evolution reaction (HER) and urea oxidation (UOR) The targeted F‐doping increases electron delocalization, facilitates from Ni to at nano‐interfaces. This interphase synergy provides ready‐to‐use F‐NiO sites, allowing F‐NiO/Ni@C achieve optimum H* adsorption Gibbs free energy HER lower barrier UOR. As result, as‐configured || cell requires an ultra‐low voltage 1.37 V 10 mA cm −2 in alkaline media (with 0.3 M urea), outperforming state‐of‐the‐art benchmark Pt/C|| RuO 2 (1.45 V). study reveals positive impact anion doping on useful guidelines designing monometallic catalysts UOR as well generation.

Language: Английский

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Ru/Ir‐Based Electrocatalysts for Oxygen Evolution Reaction in Acidic Conditions: From Mechanisms, Optimizations to Challenges

Advanced Science, Journal Year: 2024, Volume and Issue: 11(21)

Published: March 19, 2024

Abstract The generation of green hydrogen by water splitting is identified as a key strategic energy technology, and proton exchange membrane electrolysis (PEMWE) one the desirable technologies for converting renewable sources into hydrogen. However, harsh anode environment PEMWE oxygen evolution reaction (OER) involving four‐electron transfer result in large overpotential, which limits overall efficiency production, thus efficient electrocatalysts are needed to overcome high overpotential slow kinetic process. In recent years, noble metal‐based (e.g., Ru/Ir‐based metal/oxide electrocatalysts) have received much attention due their unique catalytic properties, already become dominant acidic OER process applied commercial devices. these still face thorny problem conflicting performance cost. this review, first, metal briefly classified according forms existence, mechanisms outlined. Then, focus on summarizing improvement strategies with respect activity stability over years. Finally, challenges development prospects discussed.

Language: Английский

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Cooperative Ni(Co)‐Ru‐P Sites Activate Dehydrogenation for Hydrazine Oxidation Assisting Self‐powered H₂ Production

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(35)

Published: July 10, 2023

Water electrolysis for H2 production is restricted by the sluggish oxygen evolution reaction (OER). Using thermodynamically more favorable hydrazine oxidation (HzOR) to replace OER has attracted ever-growing attention. Herein, we report a twisted NiCoP nanowire array immobilized with Ru single atoms (Ru1 -NiCoP) as superior bifunctional electrocatalyst toward both HzOR and hydrogen (HER), realizing an ultralow working potential of -60 mV overpotential 32 current density 10 mA cm-2 , respectively. Inspiringly, two-electrode electrolyzer based on overall splitting (OHzS) demonstrates outstanding activity record-high 522 at cell voltage 0.3 V. DFT calculations elucidate cooperative Ni(Co)-Ru-P sites in Ru1 -NiCoP optimize H* adsorption, enhance adsorption *N2 significantly lower energy barrier dehydrogenation. Moreover, self-powered system utilizing OHzS device driven direct fuel (DHzFC) achieve satisfactory rate 24.0 mol h-1 m-2 .

Language: Английский

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Regulating Hydrogen/Oxygen Species Adsorption via Built‐in Electric Field ‐Driven Electron Transfer Behavior at the Heterointerface for Efficient Water Splitting

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(16)

Published: Feb. 29, 2024

Abstract Alkaline water electrolysis (AWE) plays a crucial role in the realization of hydrogen economy. The design and development efficient stable bifunctional catalysts for both evolution reaction (HER) oxygen (OER) are pivotal to achieving high‐efficiency AWE. Herein, WC 1‐x /Mo 2 C nanoparticle‐embedded carbon nanofiber (WC C@CNF) with abundant interfaces is successfully designed synthesized. Benefiting from electron transfer behavior Mo , electrocatalysts C@CNF exhibit superior HER OER performance. Furthermore, when employed as anode cathode membrane electrode assembly devices, catalyst exhibits enhanced catalytic activity remarkable stability 100 hours at high current density 200 mA cm −2 towards overall splitting. experimental characterizations theoretical simulation reveal that modulation d‐band center C@CNF, achieved through asymmetric charge distribution resulting built‐in electric field induced by work function, enables optimization adsorption strength hydrogen/oxygen intermediates, thereby promoting kinetics This provides promising strategies designing highly active energy conversion fields.

Language: Английский

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Microwave Quasi‐Solid State to Construct Strong Metal‐Support Interactions with Interfacial Electron‐Enriched Ru for Anion Exchange Membrane Electrolysis

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 14(8)

Published: Dec. 28, 2023

Abstract Regulating the metal‐support interaction of anchored metal nanoclusters is recognized as valid approach to optimize electrocatalytic performance through tuning interfacial electronic structure. However, developing novel support and understanding electron accumulation on modulating reaction kinetics are still elusive. Herein, highly‐dispersed Ruthenium (Ru) onto phosphorous doped molybdenum boride (Ru/P‐MoB) developed ultrafast microwave‐plasma (60 s) approach. The synthesized Ru/P‐MoB impressively promote hydrogen evolution with low overpotentials 34, 45, 40 mV drive 10 mA cm −2 in alkaline freshwater, seawater acid media. Specially, it presents superior turnover frequency mass/specific activity relative Pt/C, Ru/C, Ru/MoB. Moreover, anion exchange membrane (AEM) electrolyzer cell based can achieve 500 1000 small voltages 1.71 1.78 V good durability. Experimental density functional theoretical (DFT) analysis reveal that strong interactions (Ru─Mo Ru─P bonds) generated electron‐enriched Ru, then favoring water‐molecule adsorption/dissociation optimal H intermediate adsorption free energy. This work provides designing avenue exploit electrocatalysts outstanding catalytic under high current at practical high‐temperature.

Language: Английский

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Interfacial Hydrogen Spillover on Pd-TiO₂ with Oxygen Vacancies Promotes Formate Electrooxidation

ACS Energy Letters, Journal Year: 2023, Volume and Issue: 8(9), P. 3945 - 3954

Published: Aug. 28, 2023

Pd-based catalysts are crucial in direct formate fuel cells owing to their high stability and selectivity for the oxidation reaction (FOR) CO2, avoiding carbonaceous poisoning species (e.g., COad, CHx) alkaline media. However, kinetics of electrocatalysts considerably impeded by unfavorable adsorption hydrogen (Had), which serve as primary intermediators occlude active sites. Herein, we crafted electron-rich Pd nanoparticles on a TiO2 support with oxygen vacancies (Pd/Ov-TiO2) improve Had desorption. The as-prepared Pd/Ov-TiO2 exhibited mass activity 4.16 A mgPd–1, outperforming Pd/TiO2 without commercial Pd/C 1.41 2.72 times, respectively. Experimental characterizations density functional theory calculations revealed that oxygen-vacant can concurrently downshift d-band center facilitate spillover, thereby accelerating desorption FOR kinetics. Our findings provide strategy refine broader electrochemical uses.

Language: Английский

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Optimizing Electrocatalytic Nitrogen Reduction via Interfacial Electric Field Modulation: Elevating d‐Band Center in WS₂‐WO₃ for Enhanced Intermediate Adsorption

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(29)

Published: May 25, 2023

Electrocatalytic nitrogen reduction reaction (ENRR) has emerged as a promising approach to synthesizing green ammonia under ambient conditions. Tungsten (W) is one of the most effective ENRR catalysts. In this reaction, protonation intermediates rate-determining step (RDS). Enhancing adsorption crucial increase intermediates, which can lead improved catalytic performance. Herein, we constructed strong interfacial electric field in WS2 -WO3 elevate d-band center W, thereby strengthening intermediates. Experimental results demonstrated that led significantly Specifically, exhibited high NH3 yield 62.38 μg h-1 mgcat-1 and promoted faraday efficiency (FE) 24.24 %. Furthermore, situ characterizations theoretical calculations showed upshifted W towards Fermi level, leading enhanced -NH2 -NH on catalyst surface. This resulted rate RDS. Overall, our study offers new insights into relationship between provides strategy enhance during process.

Language: Английский

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