Tuning the organic ligands to optimize the nitrogen reduction performance of Co(<scp>ii</scp>) or Ni(<scp>ii</scp>)-based MOFs

Qin, Ling; Zhao, Ying-Xin; Liu, Qiang; An, Jin-Long; Wang, Han-Xi; Zhang, Mao-Feng; Shi, Cheng-Wu; Zheng, He-Gen

doi:10.1039/d4qm00418c

Mater. Chem. Front.

2024

DOI: 10.1039/d4qm00418c

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Tuning the organic ligands to optimize the nitrogen reduction performance of Co(ii) or Ni(ii)-based MOFs

Ling Qin,

Ying-Xin Zhao,

Qiang Liu

et al.

Abstract: Electrocatalytic nitrogen reduction to ammonia reaction (eNRR) can use clean energy and catalyst materials to convert N2 to NH3 under relatively mild reaction conditions, but how to design and establish...

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The Effects of Ligands with Different Electron Donation on the Nitrogen Reduction Performance of Constructed Co‐MOFs: NH₃ or N₂H₄?

Qin,

Zhao,

Wang

et al. 2024

Small Methods

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Four cobalt‐based metal‐organic frameworks (Co‐MOFs) based on different ligands with varying electron‐donating properties (dpt = 2,5‐di(pyridin‐4‐yl)‐1,3,4‐thiadiazole, NH₂bdc = 5‐aminoisophthalic acid, OHbdc = 5‐hydroxyisophthalic acid, H₂tdc = thiophene‐2,5‐dicarboxylic acid, and hfipbb = 4,4′‐(hexafluoropropane‐2,2‐diyl)bisbenzoic acid) are synthesized. Among them, Co‐dpt‐NH₂bdc demonstrates the highest nitrogen reduction reaction activity, achieving an ammonia (NH3) yield of 68.61 µg·h⁻¹·mgcat⁻¹ and Faraday efficiency (FE) of 6.75 %. The enhanced performance is attributed to stronger electronic interactions and improved charge transfer capabilities facilitated by the electron‐donating properties of NH₂bdc. Additionally, Co‐dpt‐NH₂bdc can produce hydrazine (N₂H₄), achieving N₂H₄ yield of 90.62 µg·h⁻¹·mgcat⁻¹ and FE of 65.67 %, as a byproduct caused from the interaction between the generated NH₃ and the amino group on the NH₂bdc ligand. This work highlights the potential of molecular engineering in tuning the electronic states of catalytic sites to enhance electrocatalytic activity and provides insights into the production of N₂H₄ through ligand modulation.

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The Effects of Ligands with Different Electron Donation on the Nitrogen Reduction Performance of Constructed Co‐MOFs: NH₃ or N₂H₄?

Qin,

Zhao,

Wang

et al. 2024

Small Methods

View full text Add to dashboard Cite

show abstract

Adjusting the Structure–Activity Relationship of MOFs to Obtain Electrocatalysts with Higher Hydrogen Evolution and Urea Oxidation Performance by Introducing Different Linkers

Zhou,

Liu,

et al. 2024

Inorg. Chem.

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Three kinds of metal−organic frameworks possessing analogous structures were prepared by regulating the structure units of organic linkers. MOF/nickel foam electrocatalysts were formed by in situ hydrothermal growth of MOFs on a clean supported substrate nickel foam (NF), and the corresponding composites were prepared. We phosphatated them and obtained the heterojunction catalyst. Different structure units in the ligand have significant influences on the phosphating, resulting in heterogeneous materials that are not quite the same. Among them, heterogeneous materials with Co 2 P and NiP have the best catalytic performance. We also studied the urea oxidation reaction (UOR) properties of the materials and proved that it is feasible to improve the UOR performance of MOF/NF composites by regulating the structure units in the organic linkers. The results provided an idea for the reasonable selection of organic ligands to construct MOFs to regulate the electrocatalytic performance.

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Tuning the organic ligands to optimize the nitrogen reduction performance of Co(ii) or Ni(ii)-based MOFs

Abstract: Electrocatalytic nitrogen reduction to ammonia reaction (eNRR) can use clean energy and catalyst materials to convert N2 to NH3 under relatively mild reaction conditions, but how to design and establish...

Cited by 2 publications

References 45 publications

The Effects of Ligands with Different Electron Donation on the Nitrogen Reduction Performance of Constructed Co‐MOFs: NH₃ or N₂H₄?

The Effects of Ligands with Different Electron Donation on the Nitrogen Reduction Performance of Constructed Co‐MOFs: NH₃ or N₂H₄?

Adjusting the Structure–Activity Relationship of MOFs to Obtain Electrocatalysts with Higher Hydrogen Evolution and Urea Oxidation Performance by Introducing Different Linkers

Contact Info

Product

Resources

About

Tuning the organic ligands to optimize the nitrogen reduction performance of Co(ii) or Ni(ii)-based MOFs

Abstract: Electrocatalytic nitrogen reduction to ammonia reaction (eNRR) can use clean energy and catalyst materials to convert N2 to NH3 under relatively mild reaction conditions, but how to design and establish...

Cited by 2 publications

References 45 publications

The Effects of Ligands with Different Electron Donation on the Nitrogen Reduction Performance of Constructed Co‐MOFs: NH3 or N2H4?

The Effects of Ligands with Different Electron Donation on the Nitrogen Reduction Performance of Constructed Co‐MOFs: NH3 or N2H4?

Adjusting the Structure–Activity Relationship of MOFs to Obtain Electrocatalysts with Higher Hydrogen Evolution and Urea Oxidation Performance by Introducing Different Linkers

Contact Info

Product

Resources

About

The Effects of Ligands with Different Electron Donation on the Nitrogen Reduction Performance of Constructed Co‐MOFs: NH₃ or N₂H₄?

The Effects of Ligands with Different Electron Donation on the Nitrogen Reduction Performance of Constructed Co‐MOFs: NH₃ or N₂H₄?