Cover Image, Volume 4, Number 1, January 2022

Shu, Chengyong; Tan, Qiang; Deng, Chengwei; Du, Wei; Gan, Zhuofan; Liu, Yan; Fan, Chao; Jin, Hui; Tang, Wei; Yang, Xiaodong; Yang, Xiaohua; Wu, Yuping

doi:10.1002/cey2.183

Cited by 10 publications

(10 citation statements)

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Section: Resultsmentioning

confidence: 99%

“…Only two broad peaks located at 26.0° and 43.7° are presented in three kinds of samples, which can be ascribed to the (002) and (101) planes of carbon (Figure S10, Supporting Information), indicating the Fe species are probably atomically dispersed in the whole skeletons. [26,27] Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) was employed to observe the Fe moiety in FeN 4 OC/Gr at the atomic scale. The isolated bright spots confirm the atomically dispersed Fe sites in FeN 4 OC/Gr (Figure 2a).…”

Section: Resultsmentioning

confidence: 99%

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FeN₄OC Nanoplates Covalently Bonding on Graphene for Efficient CO₂ Electroreduction and ZnCO₂ Batteries

Chen

Tan

et al. 2023

Adv Funct Materials

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Electrochemical carbon dioxide (CO2) reduction into value‐added products holds great promise in moving toward carbon neutrality but remains a grand challenge due to lack of efficient electrocatalysts. Herein, the nucleophilic substitution reaction is elaborately harnessed to synthesize carbon nanoplates with a FeN4O configuration anchored onto graphene substrate (FeN4OC/Gr) through covalent linkages. Density functional theory calculations demonstrate the unique configuration of FeN4O with one oxygen (O) atom in the axial direction not only suppresses the competing hydrogen evolution reaction, but also facilitates the desorption of *CO intermediate compared with the commonly planar single‐atomic Fe sites. The FeN4OC/Gr shows excellent performance in the electroreduction of CO2 into carbon monoxide (CO) with an impressive Faradaic efficiency of 98.3% at −0.7 V versus reversible hydrogen electrode (RHE) and a high turnover frequency of 3511 h−1. Furthermore, as a cathode catalyst in an aqueous zinc (Zn)‐CO2 battery, the FeN4OC/Gr achieves a high CO Faradaic efficiency (≈91%) at a discharge current density of 3 mA cm−2 and long‐term stability over 74 h. This work opens up a new route to simultaneously modulate the geometric and electronic structure of single‐atomic catalysts toward efficient CO2 conversion.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

FeN₄OC Nanoplates Covalently Bonding on Graphene for Efficient CO₂ Electroreduction and ZnCO₂ Batteries

Chen

Tan

et al. 2023

Adv Funct Materials

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“…In order to promote good dispersion of Fe ions in the precursor and achieve high content of FeN x coordination structure, N-rich compounds such as polyaniline, [87,88] polyphenylenediamine, [89][90][91][92][93][94][95][96] polydopamine, [85] diaminopyridine, [83,[97][98][99][100] melamine, [101,102] and N-containing MOFs, [103][104][105][106][107][108] have been employed as the ideal N sources. For example, the ZIFs with a large Brunauer−Emmett−Teller (BET) surface and abundant pores that can disperse and hold Fe, are identified to be promising candidates for synthesizing Fe-N-C catalysts.…”

Section: Production Of High-density Active Sitesmentioning

confidence: 99%

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

Yang

Chen

Zhang

et al. 2023

Adv Funct Materials

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

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“…[ 8–10 ] Currently, the emerging metal–nitrogen–carbon (M–N–C) electrocatalysts with atomic metal–nitrogen (M–N 4 ) active sites have been proved to be promising candidates due to their low cost and favorable electrocatalytic ORR activities. [ 11–14 ] However, the large electronegativity of coordinated N atoms in M–N 4 active sites of M–N–C electrocatalysts would cause strong adsorption of ORR intermediates, resulting in unsatisfied sluggish ORR kinetics. [ 15,16 ] Thanks to the efforts of many researchers, highly efficient M–N–C electrocatalysts with tuning heteroatoms coordination, such as B, P, S, and their combinations, have been proposed to optimize the adsorption energy for boosting ORR kinetics.…”

Section: Introductionmentioning

confidence: 99%

Coordination Engineering of Defective Cobalt–Nitrogen–Carbon Electrocatalysts with Graphene Quantum Dots for Boosting Oxygen Reduction Reaction

Geng

Huang

Yuan

et al. 2023

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According to the report "Global Carbon Budget 2021," the concentration of atmospheric CO 2 reaches 414.7 ppm in 2021, which is 50% above pre-industrial levels. [1] Moreover, the average fossil CO 2 emissions (E FOS ) in 2020 is about 9.5 ± 0.5 Gt Cy −1 due to the rapid growth of global energy consumption. To decrease Developing efficient and robust metal-nitrogen-carbon electrocatalysts for oxygen reduction reaction (ORR) is of great significance for the application of hydrogen-oxygen fuel cells and metal-air batteries. Herein, a coordination engineering strategy is developed to improve the ORR kinetics and stability of cobalt-nitrogen-carbon (Co-N-C) electrocatalysts by grafting the oxygenrich graphene quantum dots (GQDs) onto the zeolite imidazole frameworks (ZIFs) precursors. The optimized oxygen-rich GQDs-functionalized Co-N-C (G-CoNOC) electrocatalyst demonstrates an increased mass activity, nearly two times higher than that of pristine defective Co-N-C electrocatalyst, and retains a stability of 90.0% after 200 h, even superior to the commercial Pt/C. Comprehensive investigations demonstrate that the GQDs coordination can not only decrease carbon defects of Co-N-C electrocatalysts, improving the electron transfer efficiency and resistance to the destructive free radicals from H 2 O 2 , but also optimize the electronic structure of atomic Co active site to achieve a desired adsorption energy of OOH − , leading to enhanced ORR kinetics and stability by promoting further H 2 O 2 reduction, as confirmed by theoretical calculations and experimental results. Such a coordination engineering strategy provides a new perspective for the development of highly active noble-metal-free electrocatalysts for ORR.

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Cover Image, Volume 4, Number 1, January 2022

Cited by 10 publications

References 0 publications

FeN₄OC Nanoplates Covalently Bonding on Graphene for Efficient CO₂ Electroreduction and ZnCO₂ Batteries

FeN₄OC Nanoplates Covalently Bonding on Graphene for Efficient CO₂ Electroreduction and ZnCO₂ Batteries

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

Coordination Engineering of Defective Cobalt–Nitrogen–Carbon Electrocatalysts with Graphene Quantum Dots for Boosting Oxygen Reduction Reaction

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Cover Image, Volume 4, Number 1, January 2022

Cited by 10 publications

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FeN4OC Nanoplates Covalently Bonding on Graphene for Efficient CO2 Electroreduction and ZnCO2 Batteries

FeN4OC Nanoplates Covalently Bonding on Graphene for Efficient CO2 Electroreduction and ZnCO2 Batteries

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

Coordination Engineering of Defective Cobalt–Nitrogen–Carbon Electrocatalysts with Graphene Quantum Dots for Boosting Oxygen Reduction Reaction

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FeN₄OC Nanoplates Covalently Bonding on Graphene for Efficient CO₂ Electroreduction and ZnCO₂ Batteries

FeN₄OC Nanoplates Covalently Bonding on Graphene for Efficient CO₂ Electroreduction and ZnCO₂ Batteries