Single-Atom Cr–N₄ Sites with High Oxophilicity Interfaced with Pt Atomic Clusters for Practical Alkaline Hydrogen Evolution Catalysis

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(39), P. 21432 - 21441

Published: Sept. 20, 2023

Although dispersing Pt atomic clusters (ACs) on a conducting support is promising way to minimize the amount required in hydrogen evolution reaction (HER), catalytic mass activity and durability of ACs are often unsatisfactory for alkaline HER due their unfavorable water dissociation challenges stabilizing them against agglomeration detachment. Herein, we report class single-atom Cr-N4 sites with high oxophilicity interfaced mesoporous carbon achieving highly active stable an anion-exchange-membrane electrolyzer (AEMWE). The as-made catalyst achieves highest reported (37.6 times higher than commercial Pt/C) outstanding operational stability. Experimental theoretical studies elucidate that formation unique Pt-Cr quasi-covalent bonding interaction at interface effectively suppresses migration thermal vibration atoms stabilize contributes greatly enhanced Moreover, oxophilic adjacent favorable adsorption hydroxyl species facilitate nearly barrierless thus enhance activity. An AEMWE using this (with only 50 μgPt cm-2) can operate stably industrial-level current density 500 mA cm-2 1.8 V >100 h small degradation rate 90 μV h-1.

Language: Английский

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Tunable Built‐In Electric Field in Ru Nanoclusters‐Based Electrocatalyst Boosts Water Splitting and Simulated Seawater Electrolysis

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(7)

Published: Oct. 31, 2023

Abstract The development of bifunctional electrocatalysts suitable for a wide pH range and seawater splitting under simulated industrial electrolysis conditions is expected to advance practical applications clean hydrogen energy. Here, the study reports built‐in electric field approach assemble heterogeneous Ru nanoclusters (Ru NCs) anchored in P,O co‐doped NiFe layered double hydroxide NCs/P,O‐NiFe LDH) overall water splitting. It revealed that BEF ensures electron enrichment via unidirectional transfer from P,O‐NiFe LDH due difference corresponding Fermi levels. optimized LDH/NF shows excellent electrocatalytic activity toward evolution reaction, oxygen range, as well industry‐relevant conditions. long‐term catalyst stability high currents process temperatures also demonstrated. Density functional theory calculations further confirm active sites at interface effectively reduce energy barrier electrolysis, thereby facilitating processes.

Language: Английский

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Dual role of sulfur doping in NiCr LDH for water oxidation: Promoting surface reconfiguration and lattice oxygen oxidation

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 351, P. 123994 - 123994

Published: April 24, 2024

Language: Английский

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Acidic enol electrooxidation-coupled hydrogen production with ampere-level current density

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: July 14, 2023

Hydrogen production coupled with biomass upgrading is vital for future sustainable energy developments. However, most electrooxidation reactions suffer from high working voltage and low current density, which substantially hinder large-scale industrial applications. Herein, we report an acidic hydrogen system that combined anodic ascorbic acid cathodic evolution. Unlike C-H O-H bonds cleavage slow kinetics in conventional organic oxidation, the highly active enol structure allows ultralow overpotential of only 12 mV@10 mA/cm2 using Fe single-atom catalysts, reaches 1 A/cm2 at 0.75 V (versus reversible electrode) approximately 100% Faraday efficiency production. Furthermore, fabricated two-electrode membrane-free electrolyser delivers density 2 A/[email protected] 60 °C (2.63 kWh/Nm3 H2), requires half electricity consumption water electrolysis (~5 H2). This work provides a new avenue achieving industrial-scale biomass.

Language: Английский

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The Guest Doping Effects of Fe on Bimetallic NiCo Layered Double Hydroxide for Enhanced Electrochemical Oxygen Evolution Reaction: Theoretical Screening and Experimental Verification

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(48)

Published: July 12, 2023

Abstract Exploring efficient transition‐metal‐based electrocatalysts for oxygen evolution reaction (OER) is imperative but remain challenging sustainable energy storage and conversion systems. Foreign species doping a significant regulation strategy to enhance the intrinsic activity of host matrix. However, potential relationship structure‐activity caused by guest elements seldom tracked systematically. In this case, both theoretical screening experimental verification are complementarily employed investigate effects ten first‐row transition metals (Sc∼Zn) on bimetallic NiCo layered double hydroxide (NiCo‐LDH). As result, optimized Fe‐doped NiCo‐LDH identified as most promising candidate toward alkaline electrocatalytic OER, which exhibits quasi‐industrial current density 1000 mA cm −2 at overpotential 400 mV. Meanwhile, it also shows impressively long‐term stability 500 h with negligible loss. Moreover, in situ electrochemical Raman spectroscopy unveils dynamic structure from pre‐catalytic state (Fe‐NiCo‐LDH) metal oxyhydroxide (Fe‐(NiCo)OOH) during oxidation reaction, ab‐initio molecular dynamics simulations further performed confirm thermodynamic activated Fe‐(NiCo)OOH phase. This work provides platform exploring critical role matrix developing industrially required OER electrocatalysts.

Language: Английский

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Emerging Amorphous to Crystalline Conversion Chemistry in Ca‐Doped VO₂ Cathodes for High‐Capacity and Long‐Term Wearable Aqueous Zinc‐Ion Batteries

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(11)

Published: Aug. 10, 2023

Amorphous transition metal oxides have attracted significant attention in energy storage devices owing to their potentially desirable electrochemical properties caused by abundant unsaturated dangling bonds. However, the amorphization further amplifies shortcoming of poor intrinsic electronic conductivity oxides, resulting unsatisfying rate capability and power density. Herein, freestanding amorphous Ca-doped V

Language: Английский

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Flexible tungsten disulfide superstructure engineering for efficient alkaline hydrogen evolution in anion exchange membrane water electrolysers

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: July 8, 2024

Abstract Anion exchange membrane (AEM) water electrolysis employing non-precious metal electrocatalysts is a promising strategy for achieving sustainable hydrogen production. However, it still suffers from many challenges, including sluggish alkaline evolution reaction (HER) kinetics, insufficient activity and limited lifetime of ampere-level-current-density HER. Here, we report an efficient HER at industrial-level current density wherein flexible WS 2 superstructure designed to serve as the cathode catalyst AEM electrolysis. The features bond-free van der Waals interaction among low Young’s modulus nanosheets ensure excellent mechanical flexibility, well stepped edge defect structure realize high catalytic favorable interface micro-environment. unique can effectively withstand impact high-density gas-liquid exchanges facilitate mass transfer, endowing long-term durability under industrial-scale density. An electrolyser containing this exhibits cell voltage 1.70 V deliver constant 1 A cm −2 over 1000 h with negligible decay rate 9.67 μV −1 .

Language: Английский

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Construction of Pt Single-Atom and Cluster/FeOOH Synergistic Active Sites for Efficient Electrocatalytic Hydrogen Evolution Reaction

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(10), P. 7867 - 7876

Published: May 6, 2024

The design of efficient catalysts that synergistically promote *H2O decomposition, H2 formation, and desorption is critical to accelerate hydrogen evolution reaction (HER) kinetics but remains a significant challenge. Herein, we an catalyst Pt/FeOOH@NiFe LDHs with Pt single-atom cluster distribution induced by amorphous FeOOH. low content 2 wt % exhibit ultralow HER overpotentials 20 85 mV in alkaline media (5 40 acidic media) achieve the current densities 10 100 mA cm–2. specific activity normalized electrochemically active surfaces (ECSA) are [email protected] cmECSA–2 140 [email protected] cmECSA–2. Tafel slope 51 dec–1, process follows Volmer-Hyrovsky mechanism. Moreover, overall water splitting requires only voltages 1.46 V@10 cm–2 1.61 V@100 cm–2, which better than most reported catalysts. Experimental theoretical studies show FeOOH can induce formation electron redistribution, formed cluster/FeOOH synergistic sites superior performance. facilitates adsorption activation H2O, play key role H2, accelerating kinetics.

Language: Английский

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Advances of layered double hydroxide electrocatalysts for high-current-density alkaline water/seawater splitting

Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 510, P. 215832 - 215832

Published: March 28, 2024

Language: Английский

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Modulating interfacial charge distribution of Ni2P-NiSe2 by multiple interface engineering for accelerating water splitting with industry-level activity and stability

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 347, P. 123817 - 123817

Published: April 24, 2024

Language: Английский

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