Layered Confinement Reaction: Atomic‐level Dispersed Iron–Nitrogen Co‐Doped Ultrathin Carbon Nanosheets for CO<sub>2</sub> Electroreduction

Tuo, Jinqin; Zhu, Yihua; Cheng, Ling; Li, Yuhang; Yang, Xin; Shen, Jianhua; Li, Chunzhong

doi:10.1002/cssc.201901058

Cited by 24 publications

(14 citation statements)

References 45 publications

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“…Based on the EXAFS fitting results, the Fe‐N coordination number is around four at temperatures higher than 400 °C (Table S4). The possible FeN 4 moieties have been theoretically predicted active for the CO2RR [3, 7, 48] . Unlike previous reports, [7, 49] we found that mild thermal activation is sufficient to generate active FeN 4 sites for the CO2RR.…”

Section: Resultscontrasting

confidence: 58%

Engineering Atomically Dispersed FeN₄ Active Sites for CO₂ Electroreduction

et al. 2020

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Atomically dispersed FeN4 active sites have exhibited exceptional catalytic activity and selectivity for the electrochemical CO2 reduction reaction (CO2RR) to CO. However, the understanding behind the intrinsic and morphological factors contributing to the catalytic properties of FeN4 sites is still lacking. By using a Fe‐N‐C model catalyst derived from the ZIF‐8, we deconvoluted three key morphological and structural elements of FeN4 sites, including particle sizes of catalysts, Fe content, and Fe−N bond structures. Their respective impacts on the CO2RR were comprehensively elucidated. Engineering the particle size and Fe doping is critical to control extrinsic morphological factors of FeN4 sites for optimal porosity, electrochemically active surface areas, and the graphitization of the carbon support. In contrast, the intrinsic activity of FeN4 sites was only tunable by varying thermal activation temperatures during the formation of FeN4 sites, which impacted the length of the Fe−N bonds and the local strains. The structural evolution of Fe−N bonds was examined at the atomic level. First‐principles calculations further elucidated the origin of intrinsic activity improvement associated with the optimal local strain of the Fe−N bond.

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Section: Resultscontrasting

confidence: 58%

Engineering Atomically Dispersed FeN₄ Active Sites for CO₂ Electroreduction

et al. 2020

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“…Interestingly, the improvement in catalytic activity by increasing dispersion of active sites owing to confinement effect has also been extended to electrocatalytic reduction of CO 2 . [45,46] Especially, Tuo e al reported a new strategy to synthesize metal porphyrin-hybridized porous and ultra-thin carbon nanosheets (MPPCN) by the confinement function of the layered template. In the preparation process, the layered confinement reaction protects the coordination structure of metal and nitrogen atoms during subsequent hightemperature treatment while ensuring the formation of ultrathin structures.…”

Section: Increasing Metal Dispersionmentioning

confidence: 99%

Catalytic Conversion of Carbon Oxides in Confined Spaces: Status and Prospects

Zhao

2020

ChemCatChem

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Owing to the depletion of fossil reserves and the global warming by released greenhouse gas from the consumption of fossil resources, the catalytic conversion of carbon oxide (COx, including CO2 and CO) into fuels and high‐value chemicals has attracted tremendous interest in the field of catalysis. Developing high‐performance and practical catalysts with high activity, selectivity, and stability is of great importance but remains a huge challenge. A variety of new strategies were developed to take advantage of confinement effect to address the challenges that are relevant to the highly‐efficient transformation and utilization of COx by performing catalytic reactions in a confined space. The status on this issue can be divided into three aspects: improvement in catalytic activity, increase in catalytic selectivity and enhancement in catalytic stability. In this review, the progress in the field of promoted catalytic conversion of COx in confined spaces will be presented and discussed. Especially, the specific promoting mechanism in terms of the confinement effect for COx‐related transformations in confined spaces and the relationship between the impact of the confined space on the catalytic activity, selectivity, and stability regarding of COx conversions are highlighted. Finally, the future prospects on the opportunities and challenges of catalytic conversion of COx in confined spaces are outlined.

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“…Excessive CO 2 emission form combustion of fossil fuels has caused a series of environmental problems. Electrocatalytic CO 2 reduction to value added chemicals by renewable electricity is of great significance for tackling the carbon emissions and recycle use of CO 2 …”

Section: Introductionmentioning

confidence: 99%

Controllable Synthesis of Leaf‐Like CuO Nanosheets for Selective CO₂ Electroreduction to Ethylene

et al. 2020

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The carbon dioxide reduction reaction (CO 2 RR) driven by renewable electricity is a promising way to tackle the CO 2 emission woes and recycle use of CO 2 . The synthesis of electrocatalysts with high activity and selectivity for CO 2 RR to ethylene remains a great challenge. Herein, leaf-like CuO nanosheets are fabricated in situ on nitrogen-doped graphene (NG) by using a novel reduction-oxidation-reconstruction process. When used as a catalyst for the CO 2 RR in 0.1 M KHCO 3 , a high faradaic efficiency of approximately 30 % for ethylene with an ultra-high ethylene/methane ratio of 190 was achieved at À 1.3 V vs. the reversible hydrogen electrode. The SEM and TEM images confirm the leaf-like CuO nanosheets display highcurvature structures, while multiple distinguished grain boundaries constructed by CuO(110) and CuO(111) planes are verified by HRTEM. For the first time, we present a facile method to combine the high-curvature structure and the grain boundary to enhance the selectivity of the CO 2 RR to ethylene over a CuO catalyst.

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Layered Confinement Reaction: Atomic‐level Dispersed Iron–Nitrogen Co‐Doped Ultrathin Carbon Nanosheets for CO₂ Electroreduction

Cited by 24 publications

References 45 publications

Engineering Atomically Dispersed FeN₄ Active Sites for CO₂ Electroreduction

Engineering Atomically Dispersed FeN₄ Active Sites for CO₂ Electroreduction

Catalytic Conversion of Carbon Oxides in Confined Spaces: Status and Prospects

Controllable Synthesis of Leaf‐Like CuO Nanosheets for Selective CO₂ Electroreduction to Ethylene

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Layered Confinement Reaction: Atomic‐level Dispersed Iron–Nitrogen Co‐Doped Ultrathin Carbon Nanosheets for CO2 Electroreduction

Cited by 24 publications

References 45 publications

Engineering Atomically Dispersed FeN4 Active Sites for CO2 Electroreduction

Engineering Atomically Dispersed FeN4 Active Sites for CO2 Electroreduction

Catalytic Conversion of Carbon Oxides in Confined Spaces: Status and Prospects

Controllable Synthesis of Leaf‐Like CuO Nanosheets for Selective CO2 Electroreduction to Ethylene

Contact Info

Product

Resources

About

Layered Confinement Reaction: Atomic‐level Dispersed Iron–Nitrogen Co‐Doped Ultrathin Carbon Nanosheets for CO₂ Electroreduction

Engineering Atomically Dispersed FeN₄ Active Sites for CO₂ Electroreduction

Engineering Atomically Dispersed FeN₄ Active Sites for CO₂ Electroreduction

Controllable Synthesis of Leaf‐Like CuO Nanosheets for Selective CO₂ Electroreduction to Ethylene