Anti-dissolution Pt single site with Pt(OH)(O3)/Co(P) coordination for efficient alkaline water splitting electrolyzer

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: July 2, 2022

Abstract As the most well-known electrocatalyst for cathodic hydrogen evolution in water splitting electrolyzers, platinum is unfortunately inefficient anodic oxygen due to its over-binding with species and excessive dissolution oxidative environment. Herein we show that single Pt atoms dispersed cobalt phosphate an unique Pt(OH)(O 3 )/Co(P) coordination can achieve remarkable catalytic activity stability evolution. The catalyst yields a high turnover frequency (35.1 ± 5.2 s −1 ) mass (69.5 10.3 A mg at overpotential of 300 mV excellent stability. Mechanistic studies elucidate superior performance isolated herein stems from optimal binding energies intermediate also their strong electronic coupling neighboring Co suppresses formation soluble x >4 species. Alkaline electrolyzers assembled ultralow loading realizes industrial-level current density 1 cm −2 1.8 volts durability.

Language: Английский

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Neodymium‐Evoked Valence Electronic Modulation to Balance Reversible Oxygen Electrocatalysis

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 13(2)

Published: Nov. 23, 2022

Abstract Suffering from the competition adsorption between oxygen reduction reaction (ORR) and evolution (OER), development of high‐efficiency electrocatalysts with bifunctional properties still remains a challenge. Herein, novel effective neodymium‐evoked valence electronic perturbation strategy to improve balance reversible electrocatalysis metallic cobalt sites is proposed. To heighten coupling Nd Co, metal‐organic‐framework‐induced method chosen prepare target catalyst atomic Nd‐doped Co on an N‐doped carbon substrate. The as‐prepared presents excellent electrocatalytic low overpotential 288 mV at 10 mA cm −2 for OER high half‐wave potential 0.85 V ORR. robust stabilities both ORR are also proven. electrochemical in situ Raman spectra confirm surface dynamic change transformation intermediates by noting formation Co–OOH. Theoretical calculations verify that balanced owing strong 3d‐Nd 4f orbital effect below Fermi level. Moreover, practicability further demonstrated solid‐state rechargeable Zn‐Air batteries, which exhibit large power density long cycling life.

Language: Английский

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Advanced Support Materials and Interactions for Atomically Dispersed Noble‐Metal Catalysts: From Support Effects to Design Strategies

Advanced Energy Materials, Journal Year: 2021, Volume and Issue: 12(1)

Published: Nov. 21, 2021

Abstract Indisputably, noble‐metal single atom catalysts (SACs) are one of the most popular research topics in field catalysis because their low cost, ultrahigh atomic utilization, and distinctive performance for a wide variety catalytic reactions. Support materials play vital role preparation SACs. Thus, diverse support have been developed very rapidly elaborately designed last few years. In this review, effects SACs first systematically introduced, including anchoring effects, strong metal–support interactions, synergistic effects. Moreover, recent advances classified discussed detail with focus on mechanism. Importantly, design strategies advanced supports summarized guiding development utilization materials. To conclude possible future directions put forward to help overcome current issues facing

Language: Английский

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Pauling-type adsorption of O2 induced electrocatalytic singlet oxygen production on N–CuO for organic pollutants degradation

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Sept. 22, 2022

Due to environmentally friendly operation and on-site productivity, electrocatalytic singlet oxygen (1O2) production via O2 gas is of immense interest in environment purification. However, the side-on configuration on catalysts surface will lead formation H2O, which seriously limits selectivity activity 1O2 production. Herein, we show a robust N-doped CuO (N-CuO) with Pauling-type (end-on) adsorption at N-Cu-O3 sites for selective generation under direct-current electric field. We propose that not only lowers overall activation energy barrier, but also alters reaction pathway form instead key feature determining dissociation Cu-O bonds rather than O-O bonds. The proposed N dopant strategy applicable series transition metal oxides, providing universal electrocatalysts design scheme existing high-performance

Language: Английский

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Recent Developments of Microenvironment Engineering of Single‐Atom Catalysts for Oxygen Reduction toward Desired Activity and Selectivity

Advanced Functional Materials, Journal Year: 2021, Volume and Issue: 31(45)

Published: Aug. 7, 2021

Abstract Oxygen reduction reaction (ORR) is an essential process for sustainable energy supply and sufficient chemical production in modern society. Single‐atom catalysts (SACs) exhibit great potential on maximum atomic efficiency, high ORR activity, stability, making them attractive candidates pursuing next‐generation catalysts. Despite substantial efforts being made building diversiform single‐atom active sites (SAASs), the performance of obtained still unsatisfactory. Fortunately, microenvironment regulation SACs provides opportunities to improve activity selectivity ORR. In this review, first, mechanism pathways N‐coordinated SAAS, electrochemical evaluation, characterization SAAS are displayed. addition, recent developments tuning systematically summarized, especially, strategies modulation introduced detail boosting intrinsic 4e − /2e selectivity. Theoretical calculations cutting‐edge techniques united discussed fundamental understanding synthesis–construction–performance correlations. Furthermore, their comprehensively overviewed acquire outstanding SACs. Lastly, by proposing perspectives remaining challenges infant engineering, future directions other analogous procedures pointed out.

Language: Английский

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