Abstract

Artificial photosynthesis is the imitation of natural photosynthesis, which promises an efficient way to use solar energy to synthesize organic matters, in which the key step is the coenzyme regeneration (NADH/NADPH). To achieve an efficient regeneration rate, various photocatalysts have been developed, such as g-C3N4 and mesoporous carbon nitride (mpg-C3N4). Generally, efficiency determination of different photocatalysts requires laborious experiments, high consumption of reagents, and a considerable amount of time. Here, based on the one-step artificial photosystem I method, we processed the analytical experiment in a very simple PDMS well (20 μL, a drop) to achieve a rapid screening of photocatalysts. For comparison, we used two types of graphitic carbon nitrides, few-layer g-C3N4 and mpg-C3N4. Compared with the slurry systems, firstly, the regeneration rate of mpg-C3N4 drop-reactor system is 4.3 times and 7.1 times those of the few-layer g-C3N4-slurry system and mpg-C3N4-slurry system, respectively. Secondly, this one-drop method reduces the typical verification time from 90 min to 5 min and lowers the liquid volume from 20 mL to 20 μL. Thirdly, this operation is a pump-free and soft lithography technique-free process. The miniaturization of the photocatalytic reaction in the PDMS well improves the regeneration rates, saves samples, and achieves high-throughput screening of multiple photocatalysts.

Highlights

  • The discovery of efficient photocatalysts is of vital importance for artificial photosynthesis [1–12]

  • The efficiency test requires numerous experiments, which consumes large volumes of reagents and takes a long time. This laborious and time consuming nature imposes a technical limit to the quick development of the artificial photosynthesis based coenzyme regeneration

  • Rapid screening has not attracted the due attention to the field of artificial-photosynthesis-based coenzyme regeneration

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Summary

Introduction

The discovery of efficient photocatalysts is of vital importance for artificial photosynthesis [1–12]. The efficiency test requires numerous experiments, which consumes large volumes of reagents and takes a long time This laborious and time consuming nature imposes a technical limit to the quick development of the artificial photosynthesis based coenzyme regeneration. Pentamethylcyclopentadienylrhodium(III) chloride dimer (CAS Number: 12354-85-7), 2,2 -Bipyridyl (CAS Number 366-18-7), ethanol (CAS Number: 64-17-5), cyanamide (CAS Number: 420-04-2), NH4HF2 (CAS Number: 1341-49-7) and other chemicals were purchased from Sigma-Aldrich Co. Ludox-HS 40 colloidal silica suspension (LUDOX® HS-40 colloidal silica 40 wt % suspension in H2O, CAS Number 7631-86-9) was purchased from Sigma-Aldrich Co. The schematic illustration of the process is shown in Figure 1B as follows: (1) mixing Pentamethylcyclopentadienylrhodium(III) chloride dimer, 2,2 -Bipyridyl and photocatalyst (e.g., mpg-C3N4) together in ethanol (solvent). The reaction between Pentamethylcyclopentadienylrhodium(III) chloride dimer and 2,2 -Bipyridyl in ethanol formed compound M {[Cp*Rh(bpy)Cl]Cl}, a kind of electron mediator. After the addition of the reaction solution, a thin glass slide was covered on the well to avoid evaporation

Synthesis of mpg-C3N4 and Few-Layer g-C3N4
Material Characterization
NADH Photoregeneration
PDMS Well Fabrication and Drop-Reactor Method
Discussion
Conclusions
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