The Effect of the Coordination Environment of Atomically Dispersed Fe and N Co‐doped Carbon Nanosheets on CO<sub>2</sub> Electroreduction

Tuo, Jinqin; Zhu, Yihua; Jiang, Hongliang; Shen, Jianhua; Li, Chunzhong

doi:10.1002/celc.202001437

Cited by 20 publications

(13 citation statements)

References 45 publications

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“…The TEM image of MMC-1/Se in Figure 4A shows a solid Se-carbon composite with no bulk Se on the surface, which agrees with the SEM image in Figure S3B. The high-resolution image and blurry SAED pattern in Figure 4B 32,64,65 The Se 3d spectrum of MMC-1/Se in Figure 4E contained two sharp peaks at 54.7 and 55.6 eV for Se 3d 5/2 and Se 3d 3/2 , respectively. 33,48 A minute peak at 57.3 eV stemmed from the surface oxidation of Se and the formation of Se-C bonds.…”

Section: Resultssupporting

confidence: 76%

Deliberate introduction of mesopores into microporous activated carbon toward efficient Se cathode of Na−Se batteries

Kim

Kang

2021

Intl J of Energy Research

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Sodium-selenium (NaÀSe) batteries are garnering increasing attention as promising energy storage systems because of the low cost of Na resources and the high volumetric capacity of Se. Nevertheless, their practical application is hindered by the low utilization rate of Se and the shuttle effect of polyselenide, which lead to unstable cycling performance. Therefore, extensive efforts are necessary to develop suitable carbon-based Se hosts. Here, we propose a simple method to introduce a controlled amount of mesopores into microporous carbon, which can remarkably improve the electrochemical performance of NaÀSe batteries. The Se encapsulated in the optimized micro-mesoporous carbon exhibited a substantially improved cycling stability, with a capacity of 572 mA h g À1 at 0.5C after 150 cycles, which represents a 93% capacity retention from the second cycle. In addition, the Se could achieve a high reversible capacity of 214 mA h g À1 , even at 20C. The results of this study provide guidance for distinguishing the roles of the micropores and mesopores of carbon in the Se host of NaÀSe batteries: (a) Micropores are ideal reservoirs to confine Se in an amorphous form for stable electrochemical reactions with Na, and (b) mesopores provide pathways for Na + ion diffusion and a buffer for the volume change of Se. The proposed method would be widely applicable to other types of microporous carbon with much higher specific surface areas, which can afford higher Se loading for more advanced alkali metalÀSe batteries.

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Section: Resultssupporting

confidence: 76%

Deliberate introduction of mesopores into microporous activated carbon toward efficient Se cathode of Na−Se batteries

Kim

Kang

2021

Intl J of Energy Research

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“…Ni−S−C 1000 exhibited the highest value of 1.38 among them, hinting that a large number of detects exist, which is more beneficial to exposing the active site. 36,37 We performed the XPS tests on each Ni−S−C T catalyst to obtain each element's valence state. The full XPS spectra showed that Ni, N, C, O, and S are included in all catalysts (Figure 4a).…”

Section: ■ Results and Discussionmentioning

confidence: 99%

S-Doped Ni^II-Triazolate Derived Ni–S–C Catalyst for Electrochemical CO₂ Reduction to CO

Zhang

Chen

Zheng

et al. 2022

ACS Appl. Energy Mater.

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Metal heteroatom doped carbon materials display remarkable catalytic performance in the electrochemical CO 2 reduction (ECR) because the doped heteroatoms can significantly change the local density of state and electronic structure of carbon, which induces charge polarization or structural defects. Herein, we synthesized S-doped Ni II -triazolate precursors with high purity and crystallinity through a simple one-step hydrothermal method. The high-temperature pyrolysis process produced a series of Ni−S−C T (T = 800, 900, 1000 °C) materials with Ni 3 S 2 as the main component. It resulted in significant carbon structure defects in the catalyst, which increased the specific surface area and pore volume, providing a basis for improving the ECR activity. Through the structural characterizations of powder X-ray diffraction (PXRD), Raman, X-ray photoelectron (XPS), Brunauer−Emmett−Teller (BET), transmission electron microscopy (TEM), and electrochemical characterizations of linear sweep voltammetry (LSV), chronoamperometry (i−t curve), electrochemical impedance spectroscopy (EIS), and electrochemical active surface area (ECSA), as well as gaseous product analysis, we can build the structural-performance relationship. Ni−S−C T catalysts all reached the highest CO Faraday efficiency at −1.5 V vs Ag/AgCl potential, among which Ni−S−C 1000 exhibited the best catalytic activity (FE CO of 66.6% and j CO of 1.28 mA/ cm 2 ). It also displayed excellent stability and recyclability, which could realize the efficient reuse of the catalyst. In addition, the density functional theory (DFT) calculation was carried out on Ni 3 S 2 to illustrate the ECR activity origination. It is the first report on Ni 3 S 2 -based catalysts in the application of ECR.

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“…The achievement of obtaining simple Ni(I) atoms was attributed to the low electronegativity of the pyridinic species N and S, and this last heteroatom was added by the authors for the dipping of graphene catalysts in addition to nitrogen. The result was a good electrochemical performance with mean overpotentials of 0.61 V, excellent stability (100 h) at high current densities such as 22 mA cm −2 , and high faradic efficiency of 97% for CO. Tou and co-workers [113] investigated different local coordination environments and their effects on catalytic activity by experimenting with changes in the synthesis temperature. Single Fe atoms were uniformly anchored on N-doped graphene nanosheets.…”

Section: Smas-n-graphenementioning

confidence: 99%

From CO2 to Value-Added Products: A Review about Carbon-Based Materials for Electro-Chemical CO2 Conversion

et al. 2021

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The global warming and the dangerous climate change arising from the massive emission of CO2 from the burning of fossil fuels have motivated the search for alternative clean and sustainable energy sources. However, the industrial development and population necessities make the decoupling of economic growth from fossil fuels unimaginable and, consequently, the capture and conversion of CO2 to fuels seems to be, nowadays, one of the most promising and attractive solutions in a world with high energy demand. In this respect, the electrochemical CO2 conversion using renewable electricity provides a promising solution. However, faradaic efficiency of common electro-catalysts is low, and therefore, the design of highly selective, energy-efficient, and cost-effective electrocatalysts is critical. Carbon-based materials present some advantages such as relatively low cost and renewability, excellent electrical conductivity, and tunable textural and chemical surface, which show them as competitive materials for the electro-reduction of CO2. In this review, an overview of the recent progress of carbon-based electro-catalysts in the conversion of CO2 to valuable products is presented, focusing on the role of the different carbon properties, which provides a useful understanding for the materials design progress in this field. Development opportunities and challenges in the field are also summarized.

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The Effect of the Coordination Environment of Atomically Dispersed Fe and N Co‐doped Carbon Nanosheets on CO₂ Electroreduction

Cited by 20 publications

References 45 publications

Deliberate introduction of mesopores into microporous activated carbon toward efficient Se cathode of Na−Se batteries

Deliberate introduction of mesopores into microporous activated carbon toward efficient Se cathode of Na−Se batteries

S-Doped Ni^II-Triazolate Derived Ni–S–C Catalyst for Electrochemical CO₂ Reduction to CO

From CO2 to Value-Added Products: A Review about Carbon-Based Materials for Electro-Chemical CO2 Conversion

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The Effect of the Coordination Environment of Atomically Dispersed Fe and N Co‐doped Carbon Nanosheets on CO2 Electroreduction

Cited by 20 publications

References 45 publications

Deliberate introduction of mesopores into microporous activated carbon toward efficient Se cathode of Na−Se batteries

Deliberate introduction of mesopores into microporous activated carbon toward efficient Se cathode of Na−Se batteries

S-Doped NiII-Triazolate Derived Ni–S–C Catalyst for Electrochemical CO2 Reduction to CO

From CO2 to Value-Added Products: A Review about Carbon-Based Materials for Electro-Chemical CO2 Conversion

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Product

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The Effect of the Coordination Environment of Atomically Dispersed Fe and N Co‐doped Carbon Nanosheets on CO₂ Electroreduction

S-Doped Ni^II-Triazolate Derived Ni–S–C Catalyst for Electrochemical CO₂ Reduction to CO