Mn- and N- doped carbon as promising catalysts for oxygen reduction reaction: Theoretical prediction and experimental validation

Liu, Kexi; Qiao, Zhi; Hwang, Sooyeon; Liu, Zhenyu; Zhang, Hanguang; Su, Dong; Xu, Hui; Wu, Gang; Wang, Guofeng

doi:10.1016/j.apcatb.2018.10.034

Cited by 184 publications

(138 citation statements)

References 48 publications

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“…In Table S7 and Figure S15a in the Supporting Information, we compare the off‐plane distortion (Δ h ) of carbon layers and the oxygen adsorption energy of the modelled FeN 4 sites. At first, we used the value of the limiting potential defined as the maximum applied electrode potential to make ORR thermodynamically favorable, as a parameter gauging the ORR activity of the differently strained FeN 4 sites …”

Section: Resultsmentioning

confidence: 99%

Thermally Driven Structure and Performance Evolution of Atomically Dispersed FeN₄ Sites for Oxygen Reduction

et al. 2019

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FeN4 moieties embedded in partially graphitized carbon are the most efficient platinum group metal free active sites for the oxygen reduction reaction in acidic proton‐exchange membrane fuel cells. However, their formation mechanisms have remained elusive for decades because the Fe−N bond formation process always convolutes with uncontrolled carbonization and nitrogen doping during high‐temperature treatment. Here, we elucidate the FeN4 site formation mechanisms through hosting Fe ions into a nitrogen‐doped carbon followed by a controlled thermal activation. Among the studied hosts, the ZIF‐8‐derived nitrogen‐doped carbon is an ideal model with well‐defined nitrogen doping and porosity. This approach is able to deconvolute Fe−N bond formation from complex carbonization and nitrogen doping, which correlates Fe−N bond properties with the activity and stability of FeN4 sites as a function of the thermal activation temperature.

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Section: Resultsmentioning

confidence: 99%

Thermally Driven Structure and Performance Evolution of Atomically Dispersed FeN₄ Sites for Oxygen Reduction

et al. 2019

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“…Despite having high activity, FeN x catalysts can catalyze the undesirable Fenton side reaction to generate free radicals, which causes carbon corrosion and active site loss. Thus, atomically dispersed Co or Mn catalysts, which have relatively low catalytic activity for the Fenton reaction, have been developed for application in acidic ORR and realistic PEMFC application. Similar to FeN x , pyrolysis of Co or Mn modified MOFs is an effective method for the synthesis of CoN x and MnN x catalysts.…”

Section: Atomically Dispersed Single Metal Site Electrocatalysis For mentioning

confidence: 99%

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Zhu

Sokolowski

Song

et al. 2019

Advanced Energy Materials

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Carbon‐based heteroatom‐coordinated single‐atom catalysts (SACs) are promising candidates for energy‐related electrocatalysts because of their low‐cost, tunable catalytic activity/selectivity, and relatively homogeneous morphologies. Unique interactions between single metal sites and their surrounding coordination environments play a significant role in modulating the electronic structure of the metal centers, leading to unusual scaling relationships, new reaction mechanisms, and improved catalytic performance. This review summarizes recent advancements in engineering of the local coordination environment of SACs for improved electrocatalytic performance for several crucial energy‐convention electrochemical reactions: oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, CO2 reduction reaction, and nitrogen reduction reaction. Various engineering strategies including heteroatom‐doping, changing the location of SACs on their support, introducing external ligands, and constructing dual metal sites are comprehensively discussed. The controllable synthetic methods and the activity enhancement mechanism of state‐of‐the‐art SACs are also highlighted. Recent achievements in the electronic modification of SACs will provide an understanding of the structure–activity relationship for the rational design of advanced electrocatalysts.

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“…[ 77‐80 ] Similarly, other Co‐N‐C and Mn‐N‐C catalysts are constantly emerged. [ 81‐83 ] To eliminate the Fenton effect and expose more dense active sites, it is necessary to regulate the atomic chemical environment, improve the atomic dispersion catalyst, and enhance the co‐adsorption of oxygen reactions. [ 67 ] How to boost the ORR performance of atomical‐dispersed catalysts under acidic conditions is worthy of exploration.…”

Section: Structure–property Effects For Atomic Level Dispersed Metal–mentioning

confidence: 99%

Atomic Level Dispersed Metal–Nitrogen–Carbon Catalyst toward Oxygen Reduction Reaction: Synthesis Strategies and Chemical Environmental Regulation

Yin

Xia

Zhao

et al. 2020

Energy & Environ Materials

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For development and application of proton exchange membrane fuel cell (PEMFC) energy transformation technology, the cost performance must be elevated for the catalyst. At present, compared with noble metal‐based catalysts, such as Pt‐based catalysts, atomically dispersed metal–nitrogen–carbon (M–N–C) catalysts are popularity and show great potential in maximizing active site density, high atom utilization and high activity, making them the first choice to replace Pt‐based catalysts. In the preparation of atomically dispersed metal–nitrogen–carbon catalyst, it is difficult to ensure that all active sites are uniformly dispersed, and the structure system of the active sites is not optimal. Based on this, we focus on various approaches for preparing M–N–C catalysts that are conducive to atomic dispersion, and the influence of the chemical environmental regulation of atoms on the catalytic sites in different catalysts. Therefore, we discuss the chemical environmental regulation of the catalytic sites by bimetals, atom clusters, and heteroatoms (B, S, and P). The active sites of M–N–C catalysts are explored in depth from the synthesis and characterization, reaction mechanisms, and density functional theory (DFT) calculations. Finally, the existing problems and development prospects of the current atomic dispersion M–N–C catalyst are proposed in detail.

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Mn- and N- doped carbon as promising catalysts for oxygen reduction reaction: Theoretical prediction and experimental validation

Cited by 184 publications

References 48 publications

Thermally Driven Structure and Performance Evolution of Atomically Dispersed FeN₄ Sites for Oxygen Reduction

Thermally Driven Structure and Performance Evolution of Atomically Dispersed FeN₄ Sites for Oxygen Reduction

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Atomic Level Dispersed Metal–Nitrogen–Carbon Catalyst toward Oxygen Reduction Reaction: Synthesis Strategies and Chemical Environmental Regulation

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Mn- and N- doped carbon as promising catalysts for oxygen reduction reaction: Theoretical prediction and experimental validation

Cited by 184 publications

References 48 publications

Thermally Driven Structure and Performance Evolution of Atomically Dispersed FeN4 Sites for Oxygen Reduction

Thermally Driven Structure and Performance Evolution of Atomically Dispersed FeN4 Sites for Oxygen Reduction

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Atomic Level Dispersed Metal–Nitrogen–Carbon Catalyst toward Oxygen Reduction Reaction: Synthesis Strategies and Chemical Environmental Regulation

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Thermally Driven Structure and Performance Evolution of Atomically Dispersed FeN₄ Sites for Oxygen Reduction

Thermally Driven Structure and Performance Evolution of Atomically Dispersed FeN₄ Sites for Oxygen Reduction