Coordinatively unsaturated nickel–nitrogen sites towards selective and high-rate CO<sub>2</sub>electroreduction

Yan, Cairong; Li, Haobo; Ye, Yifan; Wu, Hongpeng; Fan, Caimei; Si, Rui; Xiao, Jianping; Miao, Shu; Xie, Songhai; Yang, Fan; Li, Yanshuo; Wang, Qianqian; Bao, Xinhe

doi:10.1039/c8ee00133b

Cited by 685 publications

(596 citation statements)

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“…[26,27] In our study however, a lower concentration of pyridinic N correlates with a higher selectivity towards the CO2RR. As we have previously discussed, the ECSA has an effect on the catalyst activity.…”

Section: Resultscontrasting

confidence: 56%

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: Resultscontrasting

confidence: 56%

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

et al. 2019

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“…We compare the performance of AuCe‐47.3 with other electrocatalysts in Table S1 in the Supporting Information. High KHCO 3 solution concentration could increase CO FE, and CO FE of AuCe‐47.3 (Figure S7, Supporting Information) could reach 81.1% at −0.4 V in 0.5 m KHCO 3 . When the quantity of NaBH 4 pretreatment increases to 200 mg, the Ce 3+ concentration is 46.8% (Figure S8, Supporting Information), which indicates the limitation of Ce 3+ increase by NaBH 4 pretreatment .…”

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confidence: 99%

Abundant Ce³⁺ Ions in Au‐CeO_x Nanosheets to Enhance CO₂ Electroreduction Performance

Dong

Zhang

et al. 2019

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The electroreduction of CO2 to CO provides a potential way to solve the environmental problems caused by excess fossil fuel utilization. Loading transition metals on metal oxides is an efficient strategy for CO2 electroreduction as well as for reducing metal usage. However, it needs a great potential to overcome the energy barrier to increase CO selectivity. This paper describes how 8.7 wt% gold nanoparticles (NPs) loaded on CeOx nanosheets (NSs) with high Ce3+ concentration effectively decrease the overpotential for CO2 electroreduction. The 3.6 nm gold NPs on CeOx NSs containing 47.3% Ce3+ achieve CO faradaic efficiency of 90.1% at −0.5 V in 0.1 m KHCO3 solution. Furthermore, the CO2 electroreduction activity shows a strong relationship with the fractions of Ce3+ on Au‐CeOx NSs, which has never been reported. In situ surface‐enhanced infrared absorption spectroscopy shows that Au‐CeOx NSs with high Ce3+ concentration promote CO2 activation and *COOH formation. Theoretical calculations also indicate that the improved performance is attributed to the enhanced *COOH formation on Au‐CeOx NSs with high Ce3+ fraction.

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“…[1][2][3] Adv. These active moieties for catalysis reactions can be commonly exposed by increasing the specific areas of the materials or by tailoring the densities of metal-nitrogen moieties in composites.…”

Section: Metallic Porous Single Crystalsmentioning

confidence: 99%

“…[1][2][3] www.advmat.de www.advancedsciencenews.com metal nitride single crystals with high density of active metalnitrogen moieties have long-range ordering and interconnected open frameworks, which could provide long-range electronic connectivity, and thus reduce energy losses at grain boundaries and maintain high stability and activity. These active moieties for catalysis reactions can be commonly exposed by increasing the specific areas of the materials or by tailoring the densities of metal-nitrogen moieties in composites.…”

Section: Metallic Porous Single Crystalsmentioning

confidence: 99%

“…[4][5][6] These results indeed give an in-depth insight at the atomic level into structural dependence of catalytic activity of metal nitride nanoparticles by closely correlating the average structural information with catalytic performances. [1][2][3] Adv. The state-of-the-art pyrolysis technique of specific precursors is commonly used to construct metal-nitrogen moieties.…”

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confidence: 99%

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Metallic Porous Iron Nitride and Tantalum Nitride Single Crystals with Enhanced Electrocatalysis Performance

Zhang

Lin

et al. 2018

Advanced Materials

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Previous studies show that the metalnitrogen moieties with unsaturated nitrogen coordination numbers possess higher catalytic activities and the reported smallest nitrogen coordination number is confirmed to be ≈2 for Co-N 2 and Fe-N 2 moieties using extended X-ray absorption fine structure spectra analysis. [4][5][6] These results indeed give an in-depth insight at the atomic level into structural dependence of catalytic activity of metal nitride nanoparticles by closely correlating the average structural information with catalytic performances. However, the active metalnitrogen moieties confined at the surface layer of materials that host catalysis reactions still remain unclear.Building metal-nitrogen moieties with unsaturated nitrogen coordination numbers to enhance material's catalytic activity remains a fundamental challenge. The state-of-the-art pyrolysis technique of specific precursors is commonly used to construct metal-nitrogen moieties. However, the simultaneous presence of multiple metal species in most composite catalysts makes it highly complex to understand the nature of metal-nitrogen moieties. [7][8][9][10] The short length scale of nanostructured catalysts makes it extremely challenging to quantify metal-nitrogen moiety structure and distributions and to correspondingly elucidate the electronic structure features and unusual activity. The metal-nitrogen moieties are indeed a kind of active clusters at atomic level, which are strictly confined at lattice in local structures in crystalline composites. The polycrystalline or amorphous states of composites make it highly uncertain to construct resolved metal-nitrogen moieties and to accordingly expose these active centers on material's surfaces to host catalysis reactions. Another consideration should be given to the resolved structural feature and chemical composition of moieties that tailor electronic structures to facilitate catalysis functionalities.Single crystals with porosity, combining the advantages of long-range structural coherence of bulk crystals and large surface areas of porous materials, could provide opportunities to host the metal-nitrogen moieties with unsaturated nitrogen coordination on surface. The long-range structural coherence in single crystals offers the possibility to stabilize the metalnitrogen moieties in lattice of local structures on crystalline surfaces especially on the condition that the surface moieties have similar chemical compositions to bulk crystals. Porous Altering a material's catalytic properties would require identifying structural features that deliver electrochemically active surfaces. Single-crystalline porous materials, combining the advantages of long-range ordering of bulk crystals and large surface areas of porous materials, would create sufficient active surfaces by stabilizing 2D active moieties confined in lattice and may provide an alternative way to create high-energy surfaces for electrocatalysis that are kinetically trapped. Here, a radical concept of building active metalnitrogen moieties ...

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Coordinatively unsaturated nickel–nitrogen sites towards selective and high-rate CO₂electroreduction

Abstract: Coordinatively unsaturated Ni–N active sites facilitate CO2electroreduction and inhibit the competitive hydrogen evolution reaction, demonstrating selective and high-rate CO2electroreduction.

Cited by 685 publications

References 25 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

Abundant Ce³⁺ Ions in Au‐CeO_x Nanosheets to Enhance CO₂ Electroreduction Performance

Metallic Porous Iron Nitride and Tantalum Nitride Single Crystals with Enhanced Electrocatalysis Performance

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Coordinatively unsaturated nickel–nitrogen sites towards selective and high-rate CO2electroreduction

Abstract: Coordinatively unsaturated Ni–N active sites facilitate CO2electroreduction and inhibit the competitive hydrogen evolution reaction, demonstrating selective and high-rate CO2electroreduction.

Cited by 685 publications

References 25 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

Abundant Ce3+ Ions in Au‐CeOx Nanosheets to Enhance CO2 Electroreduction Performance

Metallic Porous Iron Nitride and Tantalum Nitride Single Crystals with Enhanced Electrocatalysis Performance

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Coordinatively unsaturated nickel–nitrogen sites towards selective and high-rate CO₂electroreduction

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

Abundant Ce³⁺ Ions in Au‐CeO_x Nanosheets to Enhance CO₂ Electroreduction Performance