Electron Hopping by Interfacing Semiconducting Graphdiyne Nanosheets and Redox Molecules for Selective...

Area of Science:

• Materials Science
• Electrochemistry
• Nanotechnology

Background:

• Electrocatalyst selectivity depends on active sites and electronic coupling through matrices.
• Designing efficient electron transport pathways is crucial for targeted catalytic activity.

Purpose of the Study:

• To demonstrate a strategy for achieving catalytic specificity by interfacing methylene green (MG) with graphdiyne (GDY).
• To investigate the formation of MG dimers within GDY and their impact on electron transfer dynamics.

Main Methods:

• Utilized optical spectroscopy, electrochemistry, and computational simulations.
• Fabricated and characterized graphdiyne (GDY) nanosheets intercalated with methylene green (MG).

Main Results:

• Observed the formation of MG dimers within the interlayer space of GDY nanosheets.
• Demonstrated distinct electron transfer pathways: electron hopping via MG dimers and electron tunneling through GDY.
• Achieved accelerated oxidation of dihydronicotinamide adenine dinucleotide (7.06 × 10^-2 cm·s^-1) and decelerated oxidation of ascorbic acid (6.60 × 10^-5 cm·s^-1).

Conclusions:

• The MG-GDY interface enables tunable electron transfer, leading to high selectivity in mediated bioelectrocatalysis.
• This approach provides a universal strategy for modulating electrochemical properties of low-dimensional materials.