Constructing single Cu–N<sub>3</sub> sites for CO<sub>2</sub> electrochemical reduction over a wide potential range

Feng, Jiaqi; Zheng, Lirong; Jiang, Chongyang; Liu, Xiaona Chen Dandan He Zhipeng Chen Licheng; Liu, Lei; Zeng, Shaojuan; Bai, Lu; Zhang, Suojiang; Zhang, Xiangping

doi:10.1039/d1gc01914g

Cited by 27 publications

(16 citation statements)

References 44 publications

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“…The Cu‐N coordination of the DSAC PdN 4 /CuN 4 complex is lower than that of the original CuPc (CuN) complex. [ 20 ] The decrease in the CuN peak in PdN 4 /CuN 4 indicates that some Cu species may form copper oxide due to surface oxidation during air exposure. [ 21 ] , leading to the decrease in Cu in the macrocyclic structure host phthalocyanine (Pc 2– ).…”

Section: Resultsmentioning

confidence: 99%

Sustainable Synthesis of Dual Single‐Atom Catalyst of PdN₄/CuN₄ for Partial Oxidation of Ethylene Glycol

Moges

Chang

Huang

et al. 2022

Adv Funct Materials

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Catalysts assumed that properly designed bimetallic systems would provide superior catalytic performance due to the cooperative effects between two atoms. Dual single-atom catalyst (DSAC) PdN 4 /CuN 4 is synthesized using a simple, cost-effective, and efficient electrochemical reduction method. The palladium single-atom is prepared first by electrochemical reduction of copper phthalocyanine to create defective N 4 sites. The new structural feature is characterized by copper reduction from Cu-N 4 coordination and the formation of defected N 4 (▫ M -N 4 ) sites, which react with a Pd precursor and form PdN 4 on the host surface. The DSAC PdN 4 /CuN 4 technique synergistically improves electrocatalytic performance toward the ethylene glycol oxidation reaction. It possesses excellent glycolate selectivity (above 88%) in an alkaline solution with an onset oxidation potential as low as 0.6 V versus a reversible hydrogen electrode, compared to commercial Pd/C. The DSAC electrocatalyst is characterized by its high current density of 83.92 mA cm −2 and high faradic efficiency value (>80%) for glycolate at 1.0 V RHE . The findings suggest a promising method to synthesize the DSACs in varying transition metals to achieve highly efficient, selective, and environmentally friendly catalysts for different applications.

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Section: Resultsmentioning

confidence: 99%

Sustainable Synthesis of Dual Single‐Atom Catalyst of PdN₄/CuN₄ for Partial Oxidation of Ethylene Glycol

Moges

Chang

Huang

et al. 2022

Adv Funct Materials

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“…Therefore, among 11 Cu–N/C catalysts, CuN 3 V and CuN 2 V 2 with moderate adsorption strength of *COOH and *CO have better electrocatalytic CO 2 RR activity. In terms of the experiments, Feng et al 49 reported an unsaturated-coordinated Cu–N 3 catalyst with much higher catalytic performance than the saturated-coordinated Cu–N 4 catalyst. Zheng et al 48 reported an efficient CO 2 RR electrocatalyst with unsaturated-coordinated Cu–N 2 with better catalytic performance than the saturated-coordinated Cu–N 4 catalyst.…”

Section: Resultsmentioning

confidence: 99%

“…The active center of monatomic copper catalysts is the Cu atom. 48,49,66 The structures under each type of adsorption mode were calculated, and the structures of the CO 2 RR species on the Cu-N/C catalyst surface are shown in Fig. 4 and S3, † while the adsorption energies are shown in Table 1.…”

Section: Adsorption Of Reaction Species On Cu-n/cmentioning

confidence: 99%

“…The short bond length of Cu-N 2 accelerates electron transfer, which effectively improves the performance of the catalyst. Feng et al 49 reported an unsaturated structure catalyst (Cu-N 3 ) for efficient CO 2 RR. The experimental results showed that Cu-N 3 possessed better CO 2 RR activity than the previously reported Cu-N-doped carbon-based catalysts.…”

Section: Origin Of Catalytic Activity Of Cun 3 V and Cun 2 Vmentioning

confidence: 99%

“…20,21,46,47 For example, Zheng et al 48 reported a maximum CO FE of 81% for the unsaturated structure catalyst Cu-N 2 /GN, which is much higher than that of Cu-N 4 /GN. Feng et al 49 prepared an unsaturated structure catalyst (Cu-N 3 ) exhibiting a maximum CO FE of 98.7%, which is much higher than that of Cu-N 4 . Therefore, improving the catalytic activity by modulating the structure of single-atom copper is an effective method.…”

Section: Introductionmentioning

confidence: 99%

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Theoretical exploration on the activity of copper single-atom catalysts for electrocatalytic reduction of CO₂

et al. 2023

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Low‐Coordinated Single‐Atom Catalysts Modulated by Metal Ionic Liquids for Efficient CO₂ Electroreduction

Zeng

et al. 2023

Adv Funct Materials

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Modulating the coordination environment of single‐atom catalysts (SACs) is an attractive approach for maximizing the catalytic activity of single‐atom centers. Currently, the synthesis of low‐coordinated SACs is mainly confined to increasing the pyrolysis temperature (≥900 °C) to control C─N volatile fragments. Herein, a novel and universal strategy for the low‐coordinated SACs modulation is presented using transition metal (e.g., Ni, Co, Zn) ionic liquid precursors under relatively mild temperature of 600 °C, which regulates the L‐shell electronic structure and decreases nearly 50% electrophilic reactivity by ionization of 4‐position N atom, thereby orienting synthesis of the SACs with metal‐N3 centers. The Ni‐N3 SACs exhibit exceptional CO2 electroreduction performance of 99.7% CO Faraday efficiency with an ultra‐high CO partial current density of 467.55 mA·cm−2 as well as a CO production rate up to 10417.51 µmol·h−1·cm−2 in flow cell. The superior catalytic activity achieves over twofold increase compared with the Ni‐N4 SACs prepared by non‐metal ionic liquid precursors due to the lower free energy of the key intermediate *COOH and the stronger adsorption energy.

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Constructing single Cu–N₃ sites for CO₂ electrochemical reduction over a wide potential range

Abstract: Cu-N-doped carbon nanotube with unsaturated coordination Cu atom (Cu-N3) was fabricated and exhibited over 90% CO faradaic efficiency (FE) in a wide potential range from -0.42 to -0.92 V. The...

Cited by 27 publications

References 44 publications

Sustainable Synthesis of Dual Single‐Atom Catalyst of PdN₄/CuN₄ for Partial Oxidation of Ethylene Glycol

Sustainable Synthesis of Dual Single‐Atom Catalyst of PdN₄/CuN₄ for Partial Oxidation of Ethylene Glycol

Theoretical exploration on the activity of copper single-atom catalysts for electrocatalytic reduction of CO₂

Low‐Coordinated Single‐Atom Catalysts Modulated by Metal Ionic Liquids for Efficient CO₂ Electroreduction

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Constructing single Cu–N3 sites for CO2 electrochemical reduction over a wide potential range

Abstract: Cu-N-doped carbon nanotube with unsaturated coordination Cu atom (Cu-N3) was fabricated and exhibited over 90% CO faradaic efficiency (FE) in a wide potential range from -0.42 to -0.92 V. The...

Cited by 27 publications

References 44 publications

Sustainable Synthesis of Dual Single‐Atom Catalyst of PdN4/CuN4 for Partial Oxidation of Ethylene Glycol

Sustainable Synthesis of Dual Single‐Atom Catalyst of PdN4/CuN4 for Partial Oxidation of Ethylene Glycol

Theoretical exploration on the activity of copper single-atom catalysts for electrocatalytic reduction of CO2

Low‐Coordinated Single‐Atom Catalysts Modulated by Metal Ionic Liquids for Efficient CO2 Electroreduction

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Constructing single Cu–N₃ sites for CO₂ electrochemical reduction over a wide potential range

Sustainable Synthesis of Dual Single‐Atom Catalyst of PdN₄/CuN₄ for Partial Oxidation of Ethylene Glycol

Sustainable Synthesis of Dual Single‐Atom Catalyst of PdN₄/CuN₄ for Partial Oxidation of Ethylene Glycol

Theoretical exploration on the activity of copper single-atom catalysts for electrocatalytic reduction of CO₂

Low‐Coordinated Single‐Atom Catalysts Modulated by Metal Ionic Liquids for Efficient CO₂ Electroreduction