M-N-C-based single-atom catalysts for H2, O2 &amp; CO2 electrocatalysis: activity descriptors, active sites identification, challenges and prospects

Kumar, Anuj; Vashistha, Vinod Kumar; Das, Dipak K.; Ibraheem, Shumaila; Yasin, Ghulam; Iqbal, Rashid; Nguyen, Tuan Anh; Gupta, Ram K.; Islam, Md. Rasidul

doi:10.1016/j.fuel.2021.121420

Cited by 76 publications

(22 citation statements)

References 162 publications

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“…The state-of-the-art PGM-free ORR catalysts are composed of heat-treated metal–nitrogen–carbon (M–N–C) precursors. − Despite their many attributes, their undefined structure makes it very difficult to improve them, which hinders their further development. , Non-heat-treated molecular catalysts are well-defined and can be systematically modified to tune their catalytic properties to reach high selectivity, high reaction kinetics at low overpotential, and high durability. − …”

Section: Introductionmentioning

confidence: 99%

Application of Molecular Catalysts for the Oxygen Reduction Reaction in Alkaline Fuel Cells

Friedman

Mizrahi

Levy

et al. 2021

ACS Appl. Mater. Interfaces

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The development of precious group metal-free (PGM-free) catalysts for the oxygen reduction reaction is considered as the main thrust for the cost reduction of fuel cell technologies and their mass production. Within the PGM-free category, molecular catalysts offer an advantage over other heattreated PGM-free catalysts owing to their well-defined structure, which enables further design of more active, selective, and durable catalysts. Even though non-heat-treated molecular catalysts with exceptional performance have been reported in the past, they were rarely tested in a fuel cell. Herein, we report on a molecular catalyst under alkaline conditions: fluorinated iron phthalocyanine (FeFPc) supported on cheap and commercially available high-surface area carbonBP2000 (FeFPc@BP2000). It exhibits the highest activity ever reported for molecular catalysts under alkaline conditions in half-cells and fuel cells.

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Section: Introductionmentioning

confidence: 99%

Application of Molecular Catalysts for the Oxygen Reduction Reaction in Alkaline Fuel Cells

Friedman

Mizrahi

Levy

et al. 2021

ACS Appl. Mater. Interfaces

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“…Today, electrocatalysis plays a key role in achieving defossilization in minimizing carbon emission and hence in supporting the ambitious goals necessary to fight climate change. The electrochemical conversion of abundant small molecules like H 2 O, N 2 , O 2 , and CO 2 into chemical feedstocks or energy carriers using renewable electricity is considered a promising approach to the global supply of sustainable energy. − Consequently, the development of (electro)catalysts that can maximize the rates of reaction and minimize the overpotentials of these conversions is crucial for the large-scale industrialization of this green technology. , To enable a rational design of electrocatalysts, an in-depth understanding of the complex chemical occurrences at the electrochemical interface during a reaction (e.g., adsorption and desorption, charge and electron transfer, solvation and desolvation, and electrostatic interactions) is of high importance and the basis for engineering and optimizing electrocatalytic systems. ,,− …”

Section: Introductionmentioning

confidence: 99%

Operando Scanning Electrochemical Probe Microscopy during Electrocatalysis

et al. 2023

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Scanning electrochemical probe microscopy (SEPM) techniques can disclose the local electrochemical reactivity of interfaces in single-entity and sub-entity studies. Operando SEPM measurements consist of using a SEPM tip to investigate the performance of electrocatalysts, while the reactivity of the interface is simultaneously modulated. This powerful combination can correlate electrochemical activity with changes in surface properties, e.g., topography and structure, as well as provide insight into reaction mechanisms. The focus of this review is to reveal the recent progress in local SEPM measurements of the catalytic activity of a surface toward the reduction and evolution of O2 and H2 and electrochemical conversion of CO2. The capabilities of SEPMs are showcased, and the possibility of coupling other techniques to SEPMs is presented. Emphasis is given to scanning electrochemical microscopy (SECM), scanning ion conductance microscopy (SICM), electrochemical scanning tunneling microscopy (EC-STM), and scanning electrochemical cell microscopy (SECCM).

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“…Meanwhile, in the study of applying a catalyst that replaces Pt in fuel cells, a clear understanding of the reaction mechanism is required, and the identification of the active site of the catalyst must precede. In this context, experimental results describing the reaction mechanisms and active sites of non−Pt or carbon-based catalysts have been reported for decades [ 15 , 16 , 17 , 18 , 19 ]. For instance, the atomically dispersed transition metal (M = Fe, Co, Mn, etc.)…”

Section: Introductionmentioning

confidence: 99%

Activity Quantification of Fuel Cell Catalysts via Sequential Poisoning by Multiple Reaction Inhibitors

Kim

Min

et al. 2022

Nanomaterials

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The development of non−Pt or carbon−based catalysts for anion exchange membrane fuel cells (AEMFCs) requires identification of the active sites of the catalyst. Since not only metals but also carbon materials exhibit oxygen reduction reaction (ORR) activity in alkaline conditions, the contribution of carbon-based materials to ORR performance should also be thoroughly analyzed. However, the conventional CN− poisoning experiments, which are mainly used to explain the main active site of M−N−C catalysts, are limited to only qualitative discussions, having the potential to make fundamental errors. Here, we report a modified electrochemical analysis to quantitatively investigate the contribution of the metal and carbon active sites to ORR currents at a fixed potential by sequentially performing chronoamperometry with two reaction inhibitors, CN− and benzyl trimethylammonium (BTMA+). As a result, we discover how to quantify the individual contributions of two active sites (Pt nanoparticles and carbon support) of carbon−supported Pt (Pt/C) nanoparticles as a model catalyst. This study is expected to provide important clues for the active site analysis of carbon-supported non−Pt catalysts, such as M−N−C catalysts composed of heterogeneous elements.

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M-N-C-based single-atom catalysts for H2, O2 & CO2 electrocatalysis: activity descriptors, active sites identification, challenges and prospects

Cited by 76 publications

References 162 publications

Application of Molecular Catalysts for the Oxygen Reduction Reaction in Alkaline Fuel Cells

Application of Molecular Catalysts for the Oxygen Reduction Reaction in Alkaline Fuel Cells

Operando Scanning Electrochemical Probe Microscopy during Electrocatalysis

Activity Quantification of Fuel Cell Catalysts via Sequential Poisoning by Multiple Reaction Inhibitors

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