Identification of Fenton-like active Cu sites by heteroatom modulation of electronic density

Proceedings of the National Academy of Sciences, Journal Year: 2022, Volume and Issue: 119(8)

Published: Feb. 14, 2022

Developing heterogeneous catalysts with atomically dispersed active sites is vital to boost peroxymonosulfate (PMS) activation for Fenton-like activity, but how controllably adjust the electronic configuration of metal centers further improve kinetics still remains a great challenge. Herein, we report systematic investigation into heteroatom-doped engineering tuning structure Cu-N4 by integrating electron-deficient boron (B) or electron-rich phosphorus (P) heteroatoms carbon substrate PMS activation. The electron-depleted Cu-N4/C-B found exhibit most oxidation capacity among prepared single-atom catalysts, which at top rankings Cu-based and superior state-of-the-art catalysts. Conversely, electron-enriched Cu-N4/C-P induces decrease in Both experimental results theoretical simulations unravel that long-range interaction B atoms decreases density Cu down-shifts d-band center, thereby optimizes adsorption energy This study provides an approach finely control atomic level expected guide design smart

Language: Английский

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Water splitting performance of metal and non-metal-doped transition metal oxide electrocatalysts

Coordination Chemistry Reviews, Journal Year: 2022, Volume and Issue: 474, P. 214864 - 214864

Published: Oct. 12, 2022

Language: Английский

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Co/CoP Heterojunction on Hierarchically Ordered Porous Carbon as a Highly Efficient Electrocatalyst for Hydrogen and Oxygen Evolution

Advanced Energy Materials, Journal Year: 2021, Volume and Issue: 11(42)

Published: Oct. 8, 2021

Abstract Designing non‐precious electrocatalysts to synergistically achieve a facilitated mass/electron transfer and exposure of abundant active sites is highly desired but remains significant challenge. Herein, composite electrocatalyst consisting dispersed Co/CoP heterojunction embedded within hierarchically ordered macroporous‐mesoporous‐microporous carbon matrix (Co/CoP@HOMC) rationally designed through the pyrolysis polystyrene sphere‐templated zeolite imidazolate framework‐67 (ZIF‐67) assemblies. The combined experimental theoretical calculations reveal that interfaces not only provide richly exposed also optimize hydrogen/water absorption free energy via electronic coupling, while interconnected macroporous structure enables superior mass all accessible sites. As result, as‐developed Co/CoP@HOMC composites exhibit outstanding catalytic activity with overpotentials 120 260 mV at 10 mA cm −2 for hydrogen evolution reaction oxygen in 1.0 m KOH, respectively. Moreover, an alkaline electrolyzer constructed by requires ultralow cell voltage 1.54 V , outperforming Pt@C||IrO 2 @C couple (1.64 V).

Language: Английский

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Rational Design of Transition Metal Phosphide‐Based Electrocatalysts for Hydrogen Evolution

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 33(7)

Published: Dec. 9, 2022

Abstract Developing efficient and inexpensive electrocatalysts for the hydrogen evolution reaction (HER) is critical to commercial viability of electrochemical clean energy technologies. Transition metal phosphides (TMPs), with merits abundant reserves, unique structure, tunable composition, high electronic conductivity, are recognized as attractive HER catalytic materials. Nevertheless, electrocatalytic activity TMPs still limited by various thorough issues inherent performance bottlenecks. In this review, these carefully sorted, corresponding reasonable explanations solutions elucidated on basis origins TMPs. Subsequently, highly targeted multiscale strategies improve comprehensively presented. Additionally, scientific constructing high‐efficiency TMP‐based proposed. Finally, process, mechanism research, catalyst construction, their application expansion mentioned challenges future directions research field. Expectedly, review offers professional guidelines rational design practical catalysts.

Language: Английский

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Dual synergistic effects between Co and Mo2C in Co/Mo2C heterostructure for electrocatalytic overall water splitting

Chemical Engineering Journal, Journal Year: 2021, Volume and Issue: 430, P. 132697 - 132697

Published: Sept. 30, 2021

Language: Английский

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Progress and Perspectives for Solar‐Driven Water Electrolysis to Produce Green Hydrogen

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(16)

Published: March 9, 2023

Abstract Solar‐driven water electrolysis has been considered to be a promising route produce green hydrogen, because the conventional system is not completely renewable as it requires power from nonrenewable fossil fuel sources. This review emphasizes strategies for solar‐driven electrolysis, including construction of photovoltaic (PV)‐water electrolyzer systems, PV‐rechargeable energy storage device‐water systems with solar sole input energy, and photoelectrochemical splitting systems. The basic discussions above are first presented. Meanwhile, replacing oxygen evolution reaction electrooxidation organic compounds can effectively improve efficiency splitting. Also, seawater greatly broadens practical applications due abundant reserves seawater. Recent years have witnessed great development in field electrolysis. recent research area subsequently reviewed. Finally, perspectives on existing challenges along some opportunities further provided.

Language: Английский

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Electronic structural engineering of transition metal-based electrocatalysts for the hydrogen evolution reaction

Nano Energy, Journal Year: 2022, Volume and Issue: 104, P. 107882 - 107882

Published: Oct. 11, 2022

Language: Английский

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A membrane-free flow electrolyzer operating at high current density using earth-abundant catalysts for water splitting

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: July 6, 2021

Electrochemical water splitting is one of the most sustainable approaches for generating hydrogen. Because inherent constraints associated with architecture and materials, conventional alkaline electrolyzer emerging proton exchange membrane are suffering from low efficiency high materials/operation costs, respectively. Herein, we design a membrane-free flow electrolyzer, featuring sandwich-like cyclic operation mode, decoupled overall splitting. Comprised two physically-separated compartments flowing H

Language: Английский

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Heteroatom‐Driven Coordination Fields Altering Single Cerium Atom Sites for Efficient Oxygen Reduction Reaction

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(28)

Published: April 4, 2023

For current single-atom catalysts (SACs), modulating the coordination environments of rare-earth (RE) single atoms with complex electronic orbital and flexible chemical states is still limited. Herein, cerium (Ce) SAs supported on a P, S, N co-doped hollow carbon substrate (Ce SAs/PSNC) for oxygen reduction reaction (ORR) are reported. The as-prepared Ce SAs/PSNC possesses half-wave potential 0.90 V, turnover frequency value 52.2 s

Language: Английский

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Tailoring a local acid-like microenvironment for efficient neutral hydrogen evolution

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

Published: July 14, 2023

Electrochemical hydrogen evolution reaction in neutral media is listed as the most difficult challenges of energy catalysis due to sluggish kinetics. Herein, Ir-HxWO3 catalyst readily synthesized and exhibits enhanced performance for reaction. HxWO3 support functioned proton sponge create a local acid-like microenvironment around Ir metal sites by spontaneous injection protons WO3, evidenced spectroscopy electrochemical analysis. Rationalize revitalized lattice-hydrogen species located interface are coupled with Had atoms on metallic surfaces via thermodynamically favorable Volmer-Tafel steps, thereby fast Elaborated demonstrates activity low overpotential 20 mV at 10 mA cm-2 Tafel slope 28 dec-1, which even comparable those acidic environment. The concept exemplified this work offer possibilities tailoring regulate catalytic pathway.

Language: Английский

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