Nickel complexes containing N4 schiff-base macrocycles dereived from diphenylamine-2,2'-dicarboxaldehyde for catalytic CO2 reduction DOI Creative Commons

Methasit Juthathan

Published: Jan. 1, 2022

In this dissertation,�nickel(II) complexes featuring N4-Schiff base macrocycles�derived from diphenylamine-2,2'-dicarboxaldehyde (1-Ni and�2-Ni) with a new crystal structure ([2-Ni]Me)�were synthesized and investigated for electrochemical CO2 reduction (ECR). Cyclic voltammetry (CV) of two nickel complexes, 1-Ni 2-Ni, illustrated the catalytic response whereas one, [2-Ni]Me, virtually remained peak-shaped in presence CO2,�indicating�the feasibility ECR activity these complexes. To develop heterogeneous catalysts aqueous media, all were adhered on N-doped graphene (NG) through non-covalent interaction, obtaining Ni@NG hybrid catalysts. The showed satisfactory faradaic efficiency CO production (FECO) 60-80% at overpotential 0.56 V vs. RHE. catalysts�demonstrated�that necessity N-H functionality ligand is less important system owing to plenty viable hydrogen-bond proton donors water bicarbonate species. Besides, an unexpected formation bearing acridine-based Schiff ([NiLACR]2+) was obtained�via rearrangement diphenylamine-2,2'-dicarboxaldehyde. addition, properties hydrogen evolution reaction preliminary investigated.

Language: Английский

Electrocatalytic CO2 Reduction Coupled with Water Oxidation by bi- and Tetranuclear Copper Complexes Based on di-2-pyridyl Ketone Ligand DOI Creative Commons
Siyuan Yang, Tian Liu, Wenbo Huang

et al.

Molecules, Journal Year: 2025, Volume and Issue: 30(7), P. 1544 - 1544

Published: March 31, 2025

In the field of sustainable energy conversion and storage technologies, copper-based complexes have become a research hotspot due to their efficient stable catalytic performance. The development bifunctional catalysts that can simplify steps, enhance efficiency, reduce catalyst usage has an important area. this study, we successfully synthesized two copper with different geometries utilizing di(2-pyridyl) ketone as ligand, [CuII2L2Cl2]·0.5H2O (1) [Cu4IIL4(OCH3)2](NO3)2 (2) (L = deprotonated methoxy-di-pyridin-2-yl-methanol), which serve homogeneous electrocatalysts for water oxidation CO2 reduction simultaneously. turnover frequency (TOF) 1 2 electrocatalytic are 7.23 s−1 0.31 under almost neutral condition (pH 8.22), respectively. Meanwhile, TOF CO 4.27 8.9 s−1, addition, both remain essentially unchanged during processes, demonstrating good stability. Structural analysis reveals distinct efficiencies originate from geometric configurations: binuclear structure complex facilitates proton-coupled electron transfer oxidation, whereas tetranuclear architecture enhances activation. Complexes represent first molecular capable catalyzing reduction. findings in work open up new avenues advancement artificial photosynthesis simulation

Language: Английский

Citations

0
Influence of the Type of Macrocycle on the Stabilisation of the High Oxidation State of the Manganese Ion and Electrode Processes DOI Creative Commons
Danuta Tomczyk, Sławomira Skrzypek, Piotr Seliger

et al.

Molecules, Journal Year: 2025, Volume and Issue: 30(8), P. 1860 - 1860

Published: April 21, 2025

Dinuclear di-µ-oxo complexes of Mn3+ and Mn4+ ions, mononuclear ions with tetraazamacrocycles ([12]aneN4, [14]aneN4, [15]aneN4) C-substituted derivative (Me6[14]aneN4) as well Mn2+ N-substituted derivatives ((N-Me)2[14]aneN4, (N-Me)4[14]aneN4, (N-Me)Me2py [14]aneN4) oxo2[14]aneN4 were studied. Based on spectroscopic (UV VIS IR) conductometric studies, the types synthesised (cis or trans isomers complexes, oxygen bridges class II according to Robin Day classification for dinuclear complexes) determined. On basis voltammetric spectroelectrochemical trans-cis isomerisation at level ion cis-trans demonstrated ligands free C positions. The oxidise EC mechanism, in which follow-up reaction is a disproportionation reaction. thermodynamic stabilisation was determined by comparing formal potentials (Ef0), constants (k1) formation (βIII). study showed possibility oxidation mononuclear, pseudo-octahedral greatest both monomers dimers N

Language: Английский

Citations

0
Molecularly dispersed nickel complexes on N-doped graphene for electrochemical CO2reduction DOI

Methasit Juthathan,

Teera Chantarojsiri, Kittipong Chainok

et al.

Dalton Transactions, Journal Year: 2023, Volume and Issue: 52(33), P. 11407 - 11418

Published: Jan. 1, 2023

In this work, new hybrid catalysts based on molecularly dispersed nickel complexes N-doped graphene were developed for electrochemical CO2 reduction (ECR). Nickel(II) (1-Ni, 2-Ni), and a crystal structure ([2-Ni]Me), featuring N4-Schiff base macrocycles, synthesized investigated their potential in ECR. Cyclic voltammetry (CV) NBu4PF6/CH3CN solution demonstrated that the bearing N-H groups (1-Ni 2-Ni) showed substantial current enhancement presence of CO2, while absence ([2-Ni]Me) resulted an almost unchanged voltammogram. This indicated necessity functionality towards ECR aprotic media. All three successfully immobilized nitrogen-doped (NG) via non-covalent interactions. Ni@NG exhibited satisfactory CO2-to-CO aqueous NaHCO3 with faradaic efficiency (FE) 60-80% at overpotential 0.56 V vs. RHE. The activity [2-Ni]Me@NG also suggested moiety from ligand is less important heterogeneous system owing to viable hydrogen-bond formation proton donors water bicarbonate ions. finding could pave way understanding effects modifying framework position toward fine tuning reactivity through molecular-level modulation.

Language: Английский

Citations

7
Experimental and Theoretical Investigations on Hydrogen Evolution Reaction (HER) Abilities of Some Salphen and Salen Complexes DOI

Hajar Zaidan Khalaf Alshammari,

Houcine Ghalla, Rayya A. Al-Balushi

et al.

Chemistry Africa, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 30, 2024

Language: Английский

Citations

0
Metalation of a Hierarchical Self-Assembly Consisting of π-Stacked Cubes through Single-Crystal-to-Single-Crystal Transformation DOI Creative Commons
Bin Wang,

Zi‐Ang Nan,

Jin Liu

et al.

Molecules, Journal Year: 2023, Volume and Issue: 28(13), P. 4923 - 4923

Published: June 22, 2023

Single-crystal-to-single-crystal metalation of organic ligands represents a novel method to prepare metal-organic complexes, but remains challenging. Herein, hierarchical self-assembly {(H12L8)·([N(C2H5)4]+)3·(ClO4-)15·(H2O)32} (1) (L = tris(2-benzimidazolylmethyl) amine) consisting π-stacked cubes which are assembled from eight partially protonated L is obtained. By soaking the crystals compound 1 in aqueous solution Co(SCN)2, coordinate with Co2+ ions stoichiometrically and ClO4- exchange SCN- via single-crystal-to-single-crystal transformation, leading {([CoSCNL]+)8·([NC8H20]+)3·(SCN)11·(H2O)13} (2).

Language: Английский

Citations

1
Synthesis and Characterization of Bipyridyl-(Imidazole)n Mn(II) Compounds and Their Evaluation as Potential Precatalysts for Water Oxidation DOI Creative Commons
Ge Mu, Ryan B. Gaynor,

Baylee N. McIntyre

et al.

Molecules, Journal Year: 2023, Volume and Issue: 28(20), P. 7221 - 7221

Published: Oct. 23, 2023

Metalloenzymes make extensive use of manganese centers for oxidative catalysis, including water oxidation; the need to develop improved synthetic catalysts these processes has long motivated development bioinspired complexes. Herein, we report a series bpy-(imidazole)n (n = 1 or 2) (bpy 2,2′-bipyridyl) ligands and their Mn2+ Four complexes are structurally characterized using single-crystal X-ray diffraction, revealing different tridentate tetradentate ligand coordination modes. Cyclic voltammetry is consistent with ligand-centered reductions metal-centered oxidations, UV-vis spectroscopy complemented by TD-DFT calculations shows primarily transitions minor contributions from charge-transfer type at higher energies. In solution, ESI-MS studies provide evidence reorganization, suggesting complex speciation behavior. The oxidation in presence probed cyclic voltammetry, but low stability aqueous solution leads decomposition precludes ultimate application as electrocatalysts. Possible reasons suggestions improvement discussed.

Language: Английский

Citations

0
Nickel complexes containing N4 schiff-base macrocycles dereived from diphenylamine-2,2'-dicarboxaldehyde for catalytic CO2 reduction DOI Creative Commons

Methasit Juthathan

Published: Jan. 1, 2022

In this dissertation,�nickel(II) complexes featuring N4-Schiff base macrocycles�derived from diphenylamine-2,2'-dicarboxaldehyde (1-Ni and�2-Ni) with a new crystal structure ([2-Ni]Me)�were synthesized and investigated for electrochemical CO2 reduction (ECR). Cyclic voltammetry (CV) of two nickel complexes, 1-Ni 2-Ni, illustrated the catalytic response whereas one, [2-Ni]Me, virtually remained peak-shaped in presence CO2,�indicating�the feasibility ECR activity these complexes. To develop heterogeneous catalysts aqueous media, all were adhered on N-doped graphene (NG) through non-covalent interaction, obtaining Ni@NG hybrid catalysts. The showed satisfactory faradaic efficiency CO production (FECO) 60-80% at overpotential 0.56 V vs. RHE. catalysts�demonstrated�that necessity N-H functionality ligand is less important system owing to plenty viable hydrogen-bond proton donors water bicarbonate species. Besides, an unexpected formation bearing acridine-based Schiff ([NiLACR]2+) was obtained�via rearrangement diphenylamine-2,2'-dicarboxaldehyde. addition, properties hydrogen evolution reaction preliminary investigated.

Language: Английский

Citations

0