Efficiently electrochemical CO2 reduction on molybdenum-nitrogen-carbon catalysts with optimized p-block axial ligands

Liu, Yingnan; Wang, Dashuai; Yang, Boguang; Li, Zhongjian; Peng, Xianyun; Liu, Zhibin; Zeng, Libin; Zhang, Tao; Rodriguez, Raúl D.; Lei, Lecheng; Hou, Yang

doi:10.1016/j.ces.2023.118638

Cited by 5 publications

(4 citation statements)

References 59 publications

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“…Conversely, the selectivity of Ni–N 4 /Gra SAC is weakened by most axial ligands. Liu et al [ 181 ] have systematically studied more than 20 p-block elements as axial ligands to tailor the Mo–N 4 structure for CO 2 RR. Theoretical calculations revealed the possibility of using p-block elements as axial ligands to improve the performance of the catalyst for two-electron CO 2 RR.…”

Section: Axial Coordination Design Of Sacs In Energy Electrocatalysis...mentioning

confidence: 99%

Advances on Axial Coordination Design of Single-Atom Catalysts for Energy Electrocatalysis: A Review

Zhang,

Jin,

Yang

et al. 2023

Nano-Micro Lett.

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Single-atom catalysts (SACs) have garnered increasingly growing attention in renewable energy scenarios, especially in electrocatalysis due to their unique high efficiency of atom utilization and flexible electronic structure adjustability. The intensive efforts towards the rational design and synthesis of SACs with versatile local configurations have significantly accelerated the development of efficient and sustainable electrocatalysts for a wide range of electrochemical applications. As an emergent coordination avenue, intentionally breaking the planar symmetry of SACs by adding ligands in the axial direction of metal single atoms offers a novel approach for the tuning of both geometric and electronic structures, thereby enhancing electrocatalytic performance at active sites. In this review, we briefly outline the burgeoning research topic of axially coordinated SACs and provide a comprehensive summary of the recent advances in their synthetic strategies and electrocatalytic applications. Besides, the challenges and outlooks in this research field have also been emphasized. The present review provides an in-depth and comprehensive understanding of the axial coordination design of SACs, which could bring new perspectives and solutions for fine regulation of the electronic structures of SACs catering to high-performing energy electrocatalysis.

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Section: Axial Coordination Design Of Sacs In Energy Electrocatalysis...mentioning

confidence: 99%

Advances on Axial Coordination Design of Single-Atom Catalysts for Energy Electrocatalysis: A Review

Zhang,

Jin,

Yang

et al. 2023

Nano-Micro Lett.

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“…To address this problem, various strategies have been employed to overcome the potential variations of CO over non-noble metal catalysts, including doping modification, 18 oxidation state regulation, 19 defect regulation, 20 surface hydrophobicity regulation, 21 bimetallic synergies, 22 and particle size, etc . 23 Introducing p-block elements is an effective strategy to optimize the surface structure of catalysts, which can effectively withstand potential fluctuation in electrocatalytic CO 2 reduction to CO. 24,25 Dopants induce electronic modulation in active sites and exhibit a significantly low free energy of *COOH formation. 26 To date, metal catalysts modified via non-metallic heteroatom ( e.g.…”

Section: Introductionmentioning

confidence: 99%

p–d Orbital hybrid Ni–Al NC catalyst withstanding potential variations in highly selective electro-reduction of CO₂ to CO

Wang,

Zhang,

Luo

et al. 2024

New J. Chem.

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“…41 The adsorption energy of COOH* can be regulated by modifying the coordination environment of metal sites, which can be achieved by modifying the coordination number, 42,43 heteroatoms, 44,45 and introducing axial ligands. 46,47 Specifically, the two types of d−band centers of Fe−N 4 and Ni−N 4 led to different adsorption strengths of the intermediates. The Fe centers easily adsorb CO 2 and strongly bond with the intermediates, whereas the Ni centers weakly adsorb carbon oxides.…”

Section: ■ Introductionmentioning

confidence: 99%

“…For Fe–N 4 and Ni–N 4 SACs, the volcanic relationship between the adsorption energy of COOH* and the limiting potential of CO 2 RR to CO has been found in recent research . The adsorption energy of COOH* can be regulated by modifying the coordination environment of metal sites, which can be achieved by modifying the coordination number, , doping heteroatoms, , and introducing axial ligands. , Specifically, the two types of d–band centers of Fe–N 4 and Ni–N 4 led to different adsorption strengths of the intermediates. The Fe centers easily adsorb CO 2 and strongly bond with the intermediates, whereas the Ni centers weakly adsorb carbon oxides. − Previous research has focused on d–band center engineering to decrease the d-band of Fe and increase that of Ni. − …”

Section: Introductionmentioning

confidence: 99%

Regulating Adsorption of Intermediates via the Sulfur Modulating Dual-Atomic Sites for Boosting CO₂RR

Huang,

Li,

et al. 2024

ACS Catal.

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The formation of dual-atom catalysts or heteroatom ligand modulation is the most promising strategy for optimizing single−atom catalysts (SACs) for the more efficient conversion of CO 2 to valuable chemicals. However, heteroatom ligands introduced into the dual-atomic sites are expected but still under-explored. In this study, a dual-atom Fe−Ni pair electrocatalyst with N− and S−coordination in porous carbon nanosheets was conceptually predicted for electrocatalytic CO 2 reduction to CO (CO 2 RR). In contrast to SACs and traditional diatomic catalysts (DACs), joined S−coordination can balance the cooperative activities of Fe and Ni sites, making the CO 2 adsorption configuration bidentate at both Fe−Ni sites. This regulation leads to a substantial change in CO* adsorption from Fe to Ni sites, facilitating CO desorption and boosting the electrocatalytic CO 2 RR. Experimental results demonstrate that the obtained FeNi−NSC catalyst achieves high selectivity with the Faradaic efficiencies for CO of 96.1%, and a remarkable activity with the turnover frequency of 6526.9 h −1 at −1.0 V, which were over 4.5 and 2.5 times of those from the single Fe or Ni sites. This work gives us insight into designing highly effective catalysts guided by theoretical calculation.

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Efficiently electrochemical CO2 reduction on molybdenum-nitrogen-carbon catalysts with optimized p-block axial ligands

Cited by 5 publications

References 59 publications

Advances on Axial Coordination Design of Single-Atom Catalysts for Energy Electrocatalysis: A Review

Advances on Axial Coordination Design of Single-Atom Catalysts for Energy Electrocatalysis: A Review

p–d Orbital hybrid Ni–Al NC catalyst withstanding potential variations in highly selective electro-reduction of CO₂ to CO

Regulating Adsorption of Intermediates via the Sulfur Modulating Dual-Atomic Sites for Boosting CO₂RR

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Efficiently electrochemical CO2 reduction on molybdenum-nitrogen-carbon catalysts with optimized p-block axial ligands

Cited by 5 publications

References 59 publications

Advances on Axial Coordination Design of Single-Atom Catalysts for Energy Electrocatalysis: A Review

Advances on Axial Coordination Design of Single-Atom Catalysts for Energy Electrocatalysis: A Review

p–d Orbital hybrid Ni–Al NC catalyst withstanding potential variations in highly selective electro-reduction of CO2 to CO

Regulating Adsorption of Intermediates via the Sulfur Modulating Dual-Atomic Sites for Boosting CO2RR

Contact Info

Product

Resources

About

p–d Orbital hybrid Ni–Al NC catalyst withstanding potential variations in highly selective electro-reduction of CO₂ to CO

Regulating Adsorption of Intermediates via the Sulfur Modulating Dual-Atomic Sites for Boosting CO₂RR