Construction of atomically dispersed Cu-N4 sites via engineered coordination environment for high-efficient CO2 electroreduction

Cheng, Huiyuan; Wu, Xuemei; Li, Xiangcun; Nie, Xiaowa; Fan, Shuai; Feng, Manman; Zhai, Fan; Tan, Mingqian; Chen, Yonggang; He, Gaohong

doi:10.1016/j.cej.2020.126842

Cited by 102 publications

(60 citation statements)

References 73 publications

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“…The results indicate the transfer of electrons from Cu to BmimNO 3 , caused by the coordination interaction between Cu and BmimNO 3 in the IL@Cu catalyst. [27,28] For the N 1s XPS spectrum of the IL@Cu catalyst (Figure 2c), there is a peak at a binding energy of 398.7 eV, which can be ascribed to CuÀ N. [29] The peaks centered at 400.5 and 401.7 eV correspond to CÀ N and C=N bonding on the imidazole rings of BmimNO 3 . [30,31] No signal was observed in this energy range for the Cu catalyst (Figure 2c).…”

Section: Methodsmentioning

confidence: 99%

Anchoring Ionic Liquid in Copper Electrocatalyst for Improving CO₂ Conversion to Ethylene

et al. 2022

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Electrochemical conversion of CO 2 to valuable fuels is appealing for CO 2 fixation and energy storage. The Cu-based catalysts feature unique superiorities, but achieving high ethylene selectivity is still restricted. In this study, we propose the anchoring of an ionic liquid (IL) on a Cu electrocatalyst for improving the electrochemical CO 2 reduction to ethylene. In a water-based electrolyte and a commonly used H-type cell, a high ethylene Faradaic efficiency of 77.3 % was achieved at À 1.49 V (vs. RHE). Experimental and theoretical studies reveal that an IL can modify the electronic structure of a Cu catalyst through its interaction with Cu, making it more conducive to *CO dimerization for ethylene formation.

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Section: Methodsmentioning

confidence: 99%

Anchoring Ionic Liquid in Copper Electrocatalyst for Improving CO₂ Conversion to Ethylene

et al. 2022

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“…Furthermore, great efforts have been made to enhance the selectivity of value-added products by optimizing MOF morphologies, grain boundaries, defects, etc. [35][36][37][38][39]. Particularly, MOFs or MOF-derived materials with different shapes, such as nanoparticles, nanosheets, and nanowires, have been proven to play a significant role in CO 2 RR performance [40][41][42][43][44].…”

Section: Introductionmentioning

confidence: 99%

Helical copper-porphyrinic framework nanoarrays for highly efficient CO2 electroreduction

et al. 2021

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In recent years, metal-organic frameworks (MOFs) have been extensively investigated as electrocatalysts due to their highly efficient electroreduction of CO 2 . Herein, the electrocatalytic CO 2 reduction reaction was investigated by growing helical Cu-porphyrinic MOF Cu meso-tetra(4-carboxyphenyl)porphyrin (TCPP) on Cu(OH) 2 nanoarrays (H-CuTCPP@Cu(OH) 2 ) using a sacrificial template method. The electrocatalytic results showed that the H-CuTCPP@Cu(OH) 2 nanoarrays exhibited a high acetic acid Faradaic efficiency (FE) of 26.1% at −1.6 V vs. Ag/Ag + , which is much higher than the value of 19.8% obtained for non-helical CuTCPP@ Cu(OH) 2 (nH-CuTCPP@Cu(OH) 2 ). The higher efficiency may be because space was more effectively utilized in the helical MOF nanoarrays, resulting in a greater number of active catalytic sites. Furthermore, in situ diffuse reflectance infrared Fourier transform spectra showed that the H-CuTCPP@ Cu(OH) 2 nanoarrays have much stronger CO linear adsorption, indicating a better selectivity of acetic acid than that of nH-CuTCPP@Cu(OH) 2 . In this study, we develop new helical nanomaterials and propose a new route to enhance the reduction of CO 2 .

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“…This is mainly due to the presence of Cu-N 4 sites, which highly facilitated the CO 2 activation step, whereas the graphene substrate promoted water dissociation, which provides protons involved in the CO 2 RR process. Cheng et al [87] confirmed the effectiveness of the Cu-N 4 site for the catalysis of the CO 2 RR to CO, since it can guarantee an appropriate binding energy strength in COOH*and CO* intermediates, and therefore boost CO generation. In particular, the authors successfully synthesized Cu single atoms dispersed on N-C support through a MOF-assisted method (named Cu-N 4 -C/1100).…”

Section: Other Metal-based Single-atom Catalystsmentioning

confidence: 93%

Single-Atom Catalysts for the Electro-Reduction of CO2 to Syngas with a Tunable CO/H2 Ratio: A Review

Scarpa

Sarno

2022

Catalysts

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Nowadays, transition towards green chemistry is becoming imperative. In this scenario, an attractive perspective consists in the generation of CO through the electrochemical reduction of CO2 under ambient conditions. This approach allows storage of the electrical energy from intermittent renewable sources in the form of chemical bonds, and simultaneously reduces greenhouse gas emissions, giving carbon a second chance of life. However, most catalysts adopted for this process, i.e., noble metal-based nanoparticles, still have several issues (high costs, low current densities, high overpotentials), and in the view of generating syngas through co-electrolysis of H2O and CO2, do not enable a widely tunable CO/H2 ratio. Single-atom catalysts with N-doped carbon supports have been recently introduced to face these challenges. The following review aims to answer the demand for an extended and exhaustive analysis of the metal single-atom catalysts thus far explored for the electro-reduction of CO2 in aqueous electrolyte solution. Moreover, focus will be placed on the objective of generating a syngas with a tunable CO/H2 ratio. Eventually, the advantages of single-atom catalysts over their noble metal-based nano-sized counterparts will be identified along with future perspectives, also in the view of a rapid and feasible scaling-up.

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Construction of atomically dispersed Cu-N4 sites via engineered coordination environment for high-efficient CO2 electroreduction

Cited by 102 publications

References 73 publications

Anchoring Ionic Liquid in Copper Electrocatalyst for Improving CO₂ Conversion to Ethylene

Anchoring Ionic Liquid in Copper Electrocatalyst for Improving CO₂ Conversion to Ethylene

Helical copper-porphyrinic framework nanoarrays for highly efficient CO2 electroreduction

Single-Atom Catalysts for the Electro-Reduction of CO2 to Syngas with a Tunable CO/H2 Ratio: A Review

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Construction of atomically dispersed Cu-N4 sites via engineered coordination environment for high-efficient CO2 electroreduction

Cited by 102 publications

References 73 publications

Anchoring Ionic Liquid in Copper Electrocatalyst for Improving CO2 Conversion to Ethylene

Anchoring Ionic Liquid in Copper Electrocatalyst for Improving CO2 Conversion to Ethylene

Helical copper-porphyrinic framework nanoarrays for highly efficient CO2 electroreduction

Single-Atom Catalysts for the Electro-Reduction of CO2 to Syngas with a Tunable CO/H2 Ratio: A Review

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Anchoring Ionic Liquid in Copper Electrocatalyst for Improving CO₂ Conversion to Ethylene

Anchoring Ionic Liquid in Copper Electrocatalyst for Improving CO₂ Conversion to Ethylene