The synthesis of atomic Fe embedded in bamboo-CNTs grown on graphene as a superior CO<sub>2</sub> electrocatalyst

Zhang, Huinian; Wang, Jie; Zhao, Zheng; Zhao, Huifang; Cheng, Miao; Li, Anni; Wang, Congwei; Wang, Junying; Wang, Junzhong

doi:10.1039/c8gc01466c

Cited by 46 publications

(16 citation statements)

References 65 publications

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“…1e ). For Mn–C 3 N 4 /CNT and C 3 N 4 /CNT, peaks at 25.8° and 42.8° can be ascribed to the (002) and (100) facets of the CNTs 14 , respectively, and no peak of g-C 3 N 4 is observed. However, a peak appears at 27.4° after the amount of DCD is increased (Supplementary Fig.…”

Section: Resultsmentioning

confidence: 98%

A Mn-N3 single-atom catalyst embedded in graphitic carbon nitride for efficient CO2 electroreduction

et al. 2020

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Developing effective catalysts based on earth abundant elements is critical for CO 2 electroreduction. However, simultaneously achieving a high Faradaic efficiency (FE) and high current density of CO (j CO) remains a challenge. Herein, we prepare a Mn single-atom catalyst (SAC) with a Mn-N 3 site embedded in graphitic carbon nitride. The prepared catalyst exhibits a 98.8% CO FE with a j CO of 14.0 mA cm −2 at a low overpotential of 0.44 V in aqueous electrolyte, outperforming all reported Mn SACs. Moreover, a higher j CO of 29.7 mA cm −2 is obtained in an ionic liquid electrolyte at 0.62 V overpotential. In situ X-ray absorption spectra and density functional theory calculations demonstrate that the remarkable performance of the catalyst is attributed to the Mn-N 3 site, which facilitates the formation of the key intermediate COOH * through a lowered free energy barrier.

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Section: Resultsmentioning

confidence: 98%

A Mn-N3 single-atom catalyst embedded in graphitic carbon nitride for efficient CO2 electroreduction

et al. 2020

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“…The ever‐increasing energy shortage and environmental crisis facing mankind have stimulated the rapid development of energy conversion systems using renewable energies including solar, wind, geothermal, and tidal, etc . One promising strategy for this purpose is the carbon dioxide reduction reaction (CO 2 RR), which can be driven by renewable electric energies to generate value‐added chemicals and simultaneously consume the excessive CO 2 in the atmosphere . Compared with C 1 products, e.g., carbon monoxide (CO) and methane (CH 4 ) from the CO 2 RR, C 2 products, e.g., ethanol (EtOH) and ethylene (C 2 H 4 ) are more meritorious .…”

Section: Introductionmentioning

confidence: 99%

AuCu Alloy Nanoparticle Embedded Cu Submicrocone Arrays for Selective Conversion of CO₂ to Ethanol

Shen

Peng

Song

et al. 2019

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The CO2 reduction reaction (CO2RR) driven by renewable electricity represents a promising strategy toward alleviating the energy shortage and environmental crisis facing humankind. Cu species, as one type of versatile electrocatalyst for the CO2RR, attract tremendous research interest. However, for C2 products, ethanol formation is commonly less favored over Cu electrocatalysts. Herein, AuCu alloy nanoparticle embedded Cu submicrocone arrays (AuCu/Cu‐SCA) are constructed as an active, selective, and robust electrocatalyst for the CO2RR. Enhanced selectivity for EtOH is gained, whose Faradaic efficiency (FE) reaches 29 ± 4%, while ethylene formation is relatively inhibited (16 ± 4%) in KHCO3 aqueous solution. The ratio between partial current densities of EtOH and C2H4 (jEtOH/jC2H4) can be tuned in the range from 0.15 ± 0.27 to 1.81 ± 0.55 by varying the Au content of the electrocatalysts. The combined experimental and theoretical calculation results identify the importance of Au in modifying binding energies of key intermediates, such as CH2CHO*, CH3CHO*, and CH3CH2O*, which consequently modify the activity and selectivity (jEtOH/jC2H4) for the CO2RR. Moreover, AuCu/Cu‐SCA also shows high durability with both the current density and FEEtOH being largely maintained for 24 h electrocatalysis.

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“…For instance, atomically dispersed Fe on N‐doped graphene (Fe‐NG) with Fe‐N 4 sites (as revealed by XAS studies and HRTEM) exhibited a FE CO of 80% at an applied potential of −0.5 V, compared to metallic Fe nanoparticles supported on same N‐doped graphene, which demonstrated a FE CO of merely 12% at the sample applied potential . Similarly, atomic Fe dispersed on CNT embedded Fe nanoparticles were also recently reported to be highly active for CO 2 RR to CO with a FE CO > 95% . In fact, as indicated in Figure 15 , the introduction of a iron nitride core facilitates CO desorption from the Fe–N x –C sites and this allows the attainment of high selectivity, stability and moderate j during long term CO 2 RR.…”

Section: Active Sites In Metal‐carbon Catalystsmentioning

confidence: 92%

A Disquisition on the Active Sites of Heterogeneous Catalysts for Electrochemical Reduction of CO₂ to Value‐Added Chemicals and Fuel

Daiyan

Saputera

Masood

et al. 2020

Advanced Energy Materials

135

104

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Renewable‐electricity‐powered electrocatalytic CO2 reduction reactions (CO2RR) have been identified as an emerging technology to address the issue of rising CO2 emissions in the atmosphere. While the CO2RR has been demonstrated to be technically feasible, further improvements in catalyst performance through active sites engineering are a prerequisite to accelerate its commercial feasibility for utilization in large CO2‐emitting industrial sources. Over the years, the improved understanding of the interaction of CO2 with the active sites has allowed superior catalyst design and subsequent attainment of prominent CO2RR activity in literature. This review tracks the evolution of the understanding of CO2RR active sites on different electrocatalysts such as metals, metal‐oxides, single atoms, metal‐carbon, and subsequently metal‐free carbon‐based catalysts. Despite the tremendous research efforts in the field, many scientific questions on the role of various active sites in governing CO2RR activity, selectivity, stability, and pathways are still unanswered. These gaps in knowledge are highlighted and a discussion is set forth on the merits of utilizing advanced in‐situ and operando characterization techniques and machine learning (ML). Using this technique, the underlying mechanisms can be discerned, and as a result new strategies for designing active sites may be uncovered. Finally, this review advocates an interdisciplinary approach to discover and design CO2RR active sites (rather than focusing merely on catalyst activity) in a bid to stimulate practical research for industrial application.

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The synthesis of atomic Fe embedded in bamboo-CNTs grown on graphene as a superior CO₂ electrocatalyst

Abstract: Synthesized atomic Fe/bamboo-CNTs/graphene exhibits ∼95% faradaic efficiency in the electroreduction of CO2 into CO at 0.55 V overpotential over 12 h.

Cited by 46 publications

References 65 publications

A Mn-N3 single-atom catalyst embedded in graphitic carbon nitride for efficient CO2 electroreduction

A Mn-N3 single-atom catalyst embedded in graphitic carbon nitride for efficient CO2 electroreduction

AuCu Alloy Nanoparticle Embedded Cu Submicrocone Arrays for Selective Conversion of CO₂ to Ethanol

A Disquisition on the Active Sites of Heterogeneous Catalysts for Electrochemical Reduction of CO₂ to Value‐Added Chemicals and Fuel

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The synthesis of atomic Fe embedded in bamboo-CNTs grown on graphene as a superior CO2 electrocatalyst

Abstract: Synthesized atomic Fe/bamboo-CNTs/graphene exhibits ∼95% faradaic efficiency in the electroreduction of CO2 into CO at 0.55 V overpotential over 12 h.

Cited by 46 publications

References 65 publications

A Mn-N3 single-atom catalyst embedded in graphitic carbon nitride for efficient CO2 electroreduction

A Mn-N3 single-atom catalyst embedded in graphitic carbon nitride for efficient CO2 electroreduction

AuCu Alloy Nanoparticle Embedded Cu Submicrocone Arrays for Selective Conversion of CO2 to Ethanol

A Disquisition on the Active Sites of Heterogeneous Catalysts for Electrochemical Reduction of CO2 to Value‐Added Chemicals and Fuel

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Product

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The synthesis of atomic Fe embedded in bamboo-CNTs grown on graphene as a superior CO₂ electrocatalyst

AuCu Alloy Nanoparticle Embedded Cu Submicrocone Arrays for Selective Conversion of CO₂ to Ethanol

A Disquisition on the Active Sites of Heterogeneous Catalysts for Electrochemical Reduction of CO₂ to Value‐Added Chemicals and Fuel