Issue 16, 2024

Electrostatic [FeFe]-hydrogenase–carbon nitride assemblies for efficient solar hydrogen production


The assembly of semiconductors as light absorbers and enzymes as redox catalysts offers a promising approach for sustainable chemical synthesis driven by light. However, achieving the rational design of such semi-artificial systems requires a comprehensive understanding of the abiotic–biotic interface, which poses significant challenges. In this study, we demonstrate an electrostatic interaction strategy to interface negatively charged cyanamide modified graphitic carbon nitride (NCNCNX) with an [FeFe]-hydrogenase possessing a positive surface charge around the distal FeS cluster responsible for electron uptake into the enzyme. The strong electrostatic attraction enables efficient solar hydrogen (H2) production via direct interfacial electron transfer (DET), achieving a turnover frequency (TOF) of 18 669 h−1 (4 h) and a turnover number (TON) of 198 125 (24 h). Interfacial characterizations, including quartz crystal microbalance (QCM), photoelectrochemical impedance spectroscopy (PEIS), intensity-modulated photovoltage spectroscopy (IMVS), and transient photocurrent spectroscopy (TPC) have been conducted on the semi-artificial carbon nitride-enzyme system to provide a comprehensive understanding for the future development of photocatalytic hybrid assemblies.

Graphical abstract: Electrostatic [FeFe]-hydrogenase–carbon nitride assemblies for efficient solar hydrogen production

Supplementary files

Article information

Article type
Edge Article
26 Jan 2024
13 Mar 2024
First published
13 Mar 2024
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2024,15, 6088-6094

Electrostatic [FeFe]-hydrogenase–carbon nitride assemblies for efficient solar hydrogen production

Y. Liu, C. Pulignani, S. Webb, S. J. Cobb, S. Rodríguez-Jiménez, D. Kim, R. D. Milton and E. Reisner, Chem. Sci., 2024, 15, 6088 DOI: 10.1039/D4SC00640B

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