Identification and Understanding of Active Sites of Non‐Noble Iron‐Nitrogen‐Carbon Catalysts for Oxygen Reduction Electrocatalysis

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(26)

Published: March 14, 2023

Non‐noble iron‐nitrogen‐carbon (Fe‐N‐C) catalysts have been explored as one type of the most promising alternatives precious platinum (Pt) in catalyzing oxygen reduction reaction (ORR). However, their catalytic ORR activity and stability still cannot meet requirement practical applications. Active sites such are key factors determining performance. This review gives a critical overview on identification understanding active sties non‐pyrolytic pyrolytic Fe‐N‐C terms design strategies, synthesis, characterization, functional mechanisms performance validation. The diversity complexity that greatly dominate progress include Fe‐containing (Fe‐based nanoparticles single‐atom Fe‐species) metal‐free (heteroatoms doping defects). Meanwhile, synergistic effects also discussed this with emphasis interaction among multiple sites. Although substantial endeavors devoted to develop efficient catalysts, some challenges remain. To facilitate further research toward applications, perspectives prospected aspects innovative synthesis methods, active‐sites modulation high‐resolution ex situ/in situ/operando characterization techniques, theoretical calculations, so on. may provide guideline for identifying developing high‐performance catalysts.

Language: Английский

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Non-noble metal-based electro-catalyst for the oxygen evolution reaction (OER): Towards an active & stable electro-catalyst for PEM water electrolysis

International Journal of Hydrogen Energy, Journal Year: 2024, Volume and Issue: 58, P. 556 - 582

Published: Jan. 26, 2024

Language: Английский

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Electronic Structure Design of Transition Metal-Based Catalysts for Electrochemical Carbon Dioxide Reduction

ACS Nano, Journal Year: 2024, Volume and Issue: 18(14), P. 9823 - 9851

Published: March 28, 2024

With the increasingly serious greenhouse effect, electrochemical carbon dioxide reduction reaction (CO2RR) has garnered widespread attention as it is capable of leveraging renewable energy to convert CO2 into value-added chemicals and fuels. However, performance CO2RR can hardly meet expectations because diverse intermediates complicated processes, necessitating exploitation highly efficient catalysts. In recent years, with advanced characterization technologies theoretical simulations, exploration catalytic mechanisms gradually deepened electronic structure catalysts their interactions intermediates, which serve a bridge facilitate deeper comprehension structure-performance relationships. Transition metal-based (TMCs), extensively applied in CO2RR, demonstrate substantial potential for further modulation, given abundance d electrons. Herein, we discuss representative feasible strategies modulate catalysts, including doping, vacancy, alloying, heterostructure, strain, phase engineering. These approaches profoundly alter inherent properties TMCs interaction thereby greatly affecting rate pathway CO2RR. It believed that rational design modulation fundamentally provide viable directions development toward conversion many other small molecules.

Language: Английский

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Electron Lock Manipulates the Catalytic Selectivity of Nanozyme

ACS Nano, Journal Year: 2024, Volume and Issue: 18(4), P. 3814 - 3825

Published: Jan. 17, 2024

Nanomaterials with enzyme-mimicking functions, termed nanozymes, offer attractive opportunities for biocatalysis and biomedicine. However, manipulating nanozyme selectivity poses an insurmountable hurdle. Here, we propose the concept of energy-governed electron lock that controls transfer between substrates to achieve manipulation enzyme-like catalysis. An can be constructed opened, via modulating nanozyme's energy match barrier enzymatic reactions. iron-doped carbon dot (FeCD) easy-to-regulate is selected as a proof concept. Through regulating conduction band which dominates energy, activatable oxidase selective peroxidase (POD) substrate affinity 123-fold higher than natural horseradish (HRP) achieved. Furthermore, while maintaining selectivity, FeCDs exhibit catalytic kinetics comparable HRP upon transforming photons into electrons. Superior efficient catalysis, undetectable biotoxicity energize potent targeted drugs on antibiotic-resistant bacterial abscesses. provides robust strategy manipulate toward advanced nanozymes.

Language: Английский

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Electronegativity Matching of Asymmetrically Coordinated Single‐Atom Catalysts for High‐Performance Lithium–Sulfur Batteries

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(19)

Published: March 13, 2024

Abstract Asymmetrically coordinated single‐atom catalysts are attractive for the implementation of high‐performance lithium–sulfur (Li─S) batteries. However, design principle asymmetric coordination that can efficiently promote bidirectional conversion polysulfides has not been fully realized. Herein, a series Co─N 3 X 1 ( refers to F, O, Cl, S, or P) configurations established, and theoretically unravel relative electronegativity value (REV) be used as an index parameter characterizing catalytic activity. By virtue enhanced chemical affinity with sulfur species lowered Li 2 S decomposition, chlorine‐atom‐constructed optimal REV exhibit stronger effect inhibit shuttling. Such REV‐related is termed effect. Following this principle, novel catalyst dominated Cl configuration successfully synthesized through inside‐out thermal reaction strategy modified layer on cathode‐side separator. Interestingly, assembled Li─S batteries quite high rate capacity (804.3 mAh g −1 at 5.0 C), durable cyclability (0.023% decay per cycle), competitive areal (7.0 cm −2 under 7.5 mg loading lean electrolyte). The guideline provided in work gives impetus pursuit highly efficient practical

Language: Английский

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