Efficient CO<sub>2</sub> to CO electrolysis on solid Ni–N–C catalysts at industrial current densities

Möller, Tim; Ju, Wen; Bagger, Alexander; Wang, Xingli; Luo, Fengjian; Thanh, Trung Ngo; Varela, Ana Sofía; Rossmeisl, Jan; Strasser, Peter

doi:10.1039/c8ee02662a

Cited by 409 publications

(383 citation statements)

References 49 publications

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“…X-Ray Diffraction (XRD) patterns for the 5 catalysts are shown in Figure S1, showing an amorphous character of the materials. Similar to previous works, [30,32] we observed that on the samples prepare at temperatures � 900°C there are nanoparticles embedded in the carbon structure, which makes them difficult to be removed via acid leaching. In addition, residual crystalline inorganic Fe x S y species, namely pyrrhotite and pyrite, can be detected on the catalysts prepared at higher temperatures.…”

Section: Resultssupporting

confidence: 88%

“…To understand the differences in selectivity, we turn to the different N functionalities. Consistently, experimental studies on NiNC catalysts containing exclusively NiN 4 reported faradaic efficiency up to 99 % towards CO. [32] Therefore, the difference in catalytic activity of our tested materials can be attributed mainly to the concentration of FeN x sites, which are not only the predominant active sites on MNC catalysts, but they are also highly selective in reducing CO 2 to CO. [26,27] In our study however, a lower concentration of pyridinic N correlates with a higher selectivity towards the CO2RR.…”

Section: Resultsmentioning

confidence: 91%

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Optimizing FeNC Materials as Electrocatalysts for the CO₂ Reduction Reaction: Heat‐Treatment Temperature, Structure and Performance Correlations

et al. 2019

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The direct CO 2 electrochemical reduction reaction (CO2RR) into carbon-based chemicals has attracted tremendous attention as a sustainable process for CO 2 utilization. The viability of the process, however, is contingent on finding efficient catalysts based on earth abundant elements. Carbon-based solid catalyst materials doped with nitrogen and transition metals (MÀ NÀ C) have emerged as a cost-efficient alternative for the direct electrochemical reduction of CO 2 into CO. These materials contain different N functionalities and MN x moieties which could be involved in the catalytic process. With the aim of gaining insight into the role of these different active sites and how to control their concentration we have prepared 5 polyani-line derived FeNC catalysts by changing the temperature of the heat treatment (750-1050°C). We observed that it is possible to tune the ratio of the different N functionalities by changing the pyrolysis temperature. Furthermore, this had a clear impact on the catalytic performance of this family of FeNC materials. In particular, a higher temperature correlated with a larger FeN x concentration resulting in a high selectivity toward the CO2RR. These results indicate that FeN x moieties play a predominant role in the catalytic process and that the incorporation of such sites to the carbon structure is enhanced by the heat-treatment temperature.

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Section: Resultssupporting

confidence: 88%

Section: Resultsmentioning

confidence: 91%

Optimizing FeNC Materials as Electrocatalysts for the CO₂ Reduction Reaction: Heat‐Treatment Temperature, Structure and Performance Correlations

et al. 2019

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“…The Jaouen and Fontecave groups demonstrated that the Fe nanoparticle, which is inevitably formed during the preparation for FeN 4 , directly correlates to the HER and decreases CO selectivity due to its favorable proton reduction feature (Figure D) . In the case of Ni‐N‐C, Ni centers binding with more than one vacancy, that is, coordinated unsaturated state, stronger *COOH bindings than the NiN 4 site by DFT calculations (Figure E) . Practically, it was further suggested that intentionally synthesized Ni with a 3 N coordination (Ni‐CTF) exhibited higher activity toward CO production than the Ni with a 4N coordination (Ni‐TPP) (Figure F) .…”

Section: Carbon‐based Materialsmentioning

confidence: 98%

Progress in development of electrocatalyst for CO₂ conversion to selective CO production

et al. 2019

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The conversion of carbon dioxide (CO2) to valuable fuels and chemicals offers a new pathway for sustainable and clean carbon fixation. Recently, the focus has been on electrochemical CO2 reduction on heterogeneous electrode catalysts, leading to remarkable achievements in the reaction performance. To date, CO2 to carbon monoxide (CO) conversion is considered as the most promising candidate reaction for the industrial market, owing to its high efficiency and reasonable technoeconomic feasibility. Moreover, CO has been proposed as a key intermediate species for further reduced hydrocarbons, which can pave the way for various fuel production. This study sets out to describe recent progress on the electrochemical CO2 reduction to CO in a heterogeneously catalyzed system. The review includes understanding of the catalytic material employed and engineering strategies implemented by adjusting the binding energy of key adsorbates. These material design approaches, such as nanostructuring, alloying, doping, and so forth, have pioneered breakouts in the intrinsic catalytic nature of transition metal elements. Moreover, recent advances in systematic design are summarized, with focus on practical industrial applications. Finally, perspectives on the design of electrocatalyst materials for CO production by electrochemical CO2 reduction are presented.

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“…However, it was recently reported that when Ni is coordinated with defective carbon or with nitrogen doped graphene, HER can be suppressed and as a result CO 2 RR can be promoted in these catalysts. For instance, Ni–N 4 –C active sites were reported to display very high FE CO > 90% at moderate overpotentials, whereas Ni–N coordinated with single and double vacancy in nickel–nitrogen–graphene catalyst can generate CO with a selectivity of 97% . In fact, by tuning the coordination number of Ni, the electron transfer from the active sites to CO 2 reactants is improved and this allows the attainment of high FE CO of 97% at low applied overpotential of merely 0.61 V .…”

Section: Active Sites In Metal‐carbon Catalystsmentioning

confidence: 99%

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

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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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Efficient CO₂ to CO electrolysis on solid Ni–N–C catalysts at industrial current densities

Cited by 409 publications

References 49 publications

Optimizing FeNC Materials as Electrocatalysts for the CO₂ Reduction Reaction: Heat‐Treatment Temperature, Structure and Performance Correlations

Optimizing FeNC Materials as Electrocatalysts for the CO₂ Reduction Reaction: Heat‐Treatment Temperature, Structure and Performance Correlations

Progress in development of electrocatalyst for CO₂ conversion to selective CO production

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

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Efficient CO2 to CO electrolysis on solid Ni–N–C catalysts at industrial current densities

Cited by 409 publications

References 49 publications

Optimizing FeNC Materials as Electrocatalysts for the CO2 Reduction Reaction: Heat‐Treatment Temperature, Structure and Performance Correlations

Optimizing FeNC Materials as Electrocatalysts for the CO2 Reduction Reaction: Heat‐Treatment Temperature, Structure and Performance Correlations

Progress in development of electrocatalyst for CO2 conversion to selective CO production

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

Contact Info

Product

Resources

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Efficient CO₂ to CO electrolysis on solid Ni–N–C catalysts at industrial current densities

Optimizing FeNC Materials as Electrocatalysts for the CO₂ Reduction Reaction: Heat‐Treatment Temperature, Structure and Performance Correlations

Optimizing FeNC Materials as Electrocatalysts for the CO₂ Reduction Reaction: Heat‐Treatment Temperature, Structure and Performance Correlations

Progress in development of electrocatalyst for CO₂ conversion to selective CO production

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