Issue 8, 2024

Unveiling the role of a ground state charge transfer complex in carbon nanoparticles for highly efficient metal-free solar hydrogen production

Abstract

Carbon-based nanoparticles (CNPs) are exciting metal-free photocatalysts for solar hydrogen production. However, significant challenges remain in elucidating their complex structures and identifying the potential catalytic sites. Herein, we report a specific ground-state charge-transfer complex between nitrogen, phosphorus-co-functionalized carbon-based nanoparticles (N, P-CNPs) and a sacrificial electron donor (SED) namely triethanolamine (TEOA), defined as N, P-CNPs (TEOA). Optical and surface analytical investigations show the initial snapshot of the ground-state charge-transfer complex, which is further clarified through femtosecond transient absorption spectroscopy, electrochemical study, and computational analysis. Results suggest the crucial role of phosphorus functionalization in establishing the ground-state charge-transfer complex. The long-lived free carriers in the N, P-CNP (TEOA) charge transfer state stimulate highly efficient photocatalytic solar hydrogen production rates of 1.02 mmol g−1 h−1 and 651 μmol g−1 h−1 from normal (mili-Q) and natural sea water, respectively, without any metal co-catalyst. Notably, TEOA plays a dual role; it forms a unique ground-state charge-transfer state with N, P-CNPs, and the excess TEOA molecules act as a potential hole-scavenger to boost the photocatalytic hydrogen generation process.

Graphical abstract: Unveiling the role of a ground state charge transfer complex in carbon nanoparticles for highly efficient metal-free solar hydrogen production

Supplementary files

Article information

Article type
Paper
Submitted
20 Dec 2023
Accepted
15 Jan 2024
First published
16 Jan 2024
This article is Open Access
Creative Commons BY-NC license

J. Mater. Chem. A, 2024,12, 4712-4726

Unveiling the role of a ground state charge transfer complex in carbon nanoparticles for highly efficient metal-free solar hydrogen production

S. Kar, A. Kumar, R. Mandal, S. Chawla, S. G. Patra, A. K. De and S. Bhattacharyya, J. Mater. Chem. A, 2024, 12, 4712 DOI: 10.1039/D3TA07895G

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