Scientia Sinica Chimica, Journal Year: 2024, Volume and Issue: 54(10), P. 1689 - 1699
Published: July 16, 2024
Advanced Materials, Journal Year: 2024, Volume and Issue: 36(38)
Published: Aug. 3, 2024
Abstract Multinuclear metal clusters are ideal candidates to catalyze small molecule activation reactions involving the transfer of multiple electrons. However, synthesizing active is a big challenge. Herein, on constructing an unparalleled Co 4 (SO ) cluster within porphyrin‐based metal–organic frameworks (MOFs) and electrocatalytic features such for oxygen evolution reaction (OER) reduction (ORR) reported. The II sulfate complexes tetrakis(4‐pyridyl)porphyrin under solvothermal conditions afforded ‐M‐MOFs (M═Co, Cu, Zn). Crystallographic studies revealed that these have same framework structure, having connected by metalloporphyrin units through Co─N pyridyl bonds. In cluster, four ions chemically symmetrically equivalent each coordinated with O atoms give distorted cube‐like structure. Electrocatalytic showed all OER ORR. Importantly, regulating activity units, it confirmed electrocatalysis. With use porphyrins as connecting ‐Co‐MOF displays highest in this series MOFs showing 10 mA cm −2 current density at 357 mV overpotential ORR half‐wave potential 0.83 V versus reversible hydrogen electrode (RHE). Theoretical synergistic effect two proximal facilitating formation O─O This work fundamental significance present construction structures electrocatalysis demonstrate cooperation between during bond process.
Language: Английский
Citations
9
Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown
Published: Nov. 7, 2024
Abstract Metal‐coordinated N‐doped carbon (M‐N‐C) materials with highly curved structures have become a promising class of electrocatalysts for the oxygen reduction reaction (ORR). However, stability these remains problem due to traditional post‐metal loading strategy. Herein, single‐atomic Co‐N‐C active sites anchored on helical carbonaceous nanotubes (HCNTs) are prepared (Co‐N‐C@HCNT) by pyrolyzing Co porphyrins and polypyrroles (PPys) mixtures at high‐temperature one‐step method. Aberration‐corrected high‐angle annular dark‐field scanning transmission electron microscopy (HAADF‐STEM) X‐ray absorption fine structure (XAFS) measurements confirm Co‐N 4 coordination Co‐N‐C@HCNT. The optimized Co‐N‐C@HCNT exhibits excellent catalytic ORR activity half‐wave potential ( E 1/2 ) 0.86 V versus reversible hydrogen electrode (vs RHE) compared Co‐N‐C@CNT without = 0.81 vs measured in 0.1 m KOH. also displays slight current decrease (4%) after running 10 h featuring tightly HCNTs electrostatic interactions between metal PPys. Theoretical calculations indicate that can increase charge d‐band center site, which enhances electrocatalytic activity. This work provides simple but effective strategy construct M‐N‐C materials.
Language: Английский
Citations
9
Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 511, P. 215869 - 215869
Published: April 18, 2024
Language: Английский
Citations
8
ChemPhysChem, Journal Year: 2024, Volume and Issue: 25(7)
Published: Feb. 7, 2024
Abstract Using functionalized supporting materials for the immobilization of molecular catalysts is an appealing strategy to improve efficiency electrocatalysis. Herein, we report covalent tethering cobalt porphyrins on phenolic resins ( PR ) improved electrocatalytic oxygen reduction reaction (ORR) and evolution (OER). A porphyrin bearing alkyl bromide substituent was covalently tethered resins, through substitution bromides with hydroxyl groups, afford molecule‐engineered Co‐PR ). The resulted efficient ORR OER by displaying half‐wave potential E 1/2 =0.78 V versus RHE overpotential 420 mV get 10 mA/cm 2 current density. We propose that many residual groups will surround Co play critical roles in facilitating proton electron transfers. Importantly, outperformed unmodified loaded simple physical adsorption (termed Co@PR zinc‐air battery assembled using displayed a performance comparable Pt/C+Ir/C. This work significant present as material support electrocatalysts demonstrate electrocatalysis use resin residues.
Language: Английский
Citations
6
International Journal of Hydrogen Energy, Journal Year: 2024, Volume and Issue: 71, P. 1342 - 1350
Published: May 26, 2024
Language: Английский
Citations
4
ACS Catalysis, Journal Year: 2024, Volume and Issue: unknown, P. 14350 - 14355
Published: Sept. 13, 2024
Language: Английский
Citations
4
Electrochimica Acta, Journal Year: 2025, Volume and Issue: unknown, P. 145986 - 145986
Published: March 1, 2025
Language: Английский
Citations
0
Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown
Published: April 15, 2025
Abstract Electrocatalytic nitrite (NO 2 − ) reduction RR) to ammonia (NH 3 is a promising green technology for producing NH with high efficiency. Cobalt macrocyclic complexes have attracted great interest because of their ability selectively convert NO , but suffer from low yields. Herein, cobalt porphyrin conjugated polymer on carbon nanotubes (CoPCOP@CNT) reported display exceptional RR performance large yield 133.39 mg h −1 CoP at −1.0 V and Faradaic efficiency (FE) 98.0% −0.8 V. Utilizing CoPCOP@CNT as the catalyst cathode, Zn‐NO battery exhibits remarkable power density (5.34 mW cm −2 ), open‐circuit voltage (≈1.45 V), FE (94.6%), (29.15 ). The active intermediates reaction pathways CoPCOP in process are revealed by differential electrochemical mass spectroscopy theory calculations. This work highlights potential electrocatalysts based metal porphyrins conversion nitrogenous pollutant into .
Language: Английский
Citations
0
Chemical Society Reviews, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 1, 2025
Recent progress made in Co-based electrocatalysts for selective four-electron (4e − ) and two-electron (2e electrocatalytic oxygen reduction reactions is reviewed.
Language: Английский
Citations
0
Diamond and Related Materials, Journal Year: 2025, Volume and Issue: unknown, P. 112368 - 112368
Published: April 1, 2025
Language: Английский
Citations
0