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Electrochemical reduction of carbon dioxide to acetic acid on a Cu-Au modified boron-doped diamond electrode with a flow-cell system.

ABSTRACT: Boron-doped diamond (BDD) was modified with copper and gold particles by using an electrodeposition technique to improve its catalytic effect on CO₂ reduction in a flow system. The system was optimized based on the production of formic acid by the electroreduction process. At the optimum applied potential of -1.0 V (vs. Ag/AgCl) and flow rate of 50 mL min^-1, the copper-gold-modified BDD produced formic acid at the highest rate of 4.88 mol m^-2 s^-1 and a concentration of 15.93 ppm, while acetic acid was produced with a rate of 0.11 mol m^-2 s^-1 and a concentration of 0.47 ppm. An advantage of the flow system using the modified BDD was that it was found to accelerate the production rate of acetic acid as well as to decrease the reduction potential of CO₂. Furthermore, better stability of the metal particles was observed when using mixed copper-gold modification on the BDD surface than single modification by either metal. The results indicated that a flow system is suitable to be employed for electroreduction of CO₂ using the bimetal-modified BDD electrodes, especially with copper and gold as the modifying particles.

SUBMITTER: Saprudin MH

PROVIDER: S-EPMC10360371 | biostudies-literature | 2023 Jul

REPOSITORIES: biostudies-literature

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Electrochemical reduction of carbon dioxide to acetic acid on a Cu-Au modified boron-doped diamond electrode with a flow-cell system.

Saprudin Millati H MH Jiwanti Prastika K PK Saprudin Deden D Sanjaya Afiten R AR Putri Yulia M T A YMTA Einaga Yasuaki Y Ivandini Tribidasari A TA

RSC advances 20230721 32

Boron-doped diamond (BDD) was modified with copper and gold particles by using an electrodeposition technique to improve its catalytic effect on CO2 reduction in a flow system. The system was optimized based on the production of formic acid by the electroreduction process. At the optimum applied potential of -1.0 V (vs. Ag/AgCl) and flow rate of 50 mL min-1, the copper-gold-modified BDD produced formic acid at the highest rate of 4.88 mol m-2 s-1</sup ...[more]

PMID: 37483677

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Project description:Fabrication of patterned boron-doped diamond (BDD) in an inexpensive and straightforward way is required for a variety of practical applications, including the development of BDD-based electrochemical sensors. This work describes a simplified and novel bottom-up fabrication approach for BDD-based three-electrode sensor chips utilizing direct inkjet printing of diamond nanoparticles on silicon-based substrates. The whole seeding process, accomplished by a commercial research inkjet printer with piezo-driven drop-on-demand printheads, was systematically examined. Optimized and continuous inkjet-printed features were obtained with glycerol-based diamond ink (0.4% vol/wt), silicon substrates pretreated by exposure to oxygen plasma and subsequently to air, and applying a dot density of 750 drops (volume 9 pL) per inch. Next, the dried micropatterned substrate was subjected to a chemical vapor deposition step to grow uniform thin-film BDD, which satisfied the function of both working and counter electrodes. Silver was inkjet-printed to complete the sensor chip with a reference electrode. Scanning electron micrographs showed a closed BDD layer with a typical polycrystalline structure and sharp and well-defined edges. Very good homogeneity in diamond layer composition and a high boron content (∼2 × 1021 atoms cm-3) was confirmed by Raman spectroscopy. Important electrochemical characteristics, including the width of the potential window (2.5 V) and double-layer capacitance (27 μF cm-2), were evaluated by cyclic voltammetry. Fast electron transfer kinetics was recognized for the [Ru(NH3)6]3+/2+ redox marker due to the high doping level, while somewhat hindered kinetics was observed for the surface-sensitive [Fe(CN)6]3-/4- probe. Furthermore, the ability to electrochemically detect organic compounds of different structural motifs, such as glucose, ascorbic acid, uric acid, tyrosine, and dopamine, was successfully verified and compared with commercially available screen-printed BDD electrodes. The newly developed chip-based manufacture method enables the rapid prototyping of different small-scale electrode designs and BDD microstructures, which can lead to enhanced sensor performance with capability of repeated use.

Project description:Diamond is known as a promising electrode material in the fields of cell stimulation, energy storage (e.g., supercapacitors), (bio)sensing, catalysis, etc. However, engineering its surface and electrochemical properties often requires costly and complex procedures with addition of foreign material (e.g., carbon nanotube or polymer) scaffolds or cleanroom processing. In this work, we demonstrate a novel approach using laser-induced periodic surface structuring (LIPSS) as a scalable, versatile, and cost-effective technique to nanostructure the surface and tune the electrochemical properties of boron-doped diamond (BDD). We study the effect of LIPSS on heavily doped BDD and investigate its application as electrodes for cell stimulation and energy storage. We show that quasi-periodic ripple structures formed on diamond electrodes laser-textured with a laser accumulated fluence of 0.325 kJ/cm2 (800 nm wavelength) displayed a much higher double-layer capacitance of 660 μF/cm2 than the as-grown BDD (20 μF/cm2) and that an increased charge-storage capacity of 1.6 mC/cm2 (>6-fold increase after laser texturing) and a low impedance of 2.74 Ω cm2 turn out to be appreciable properties for cell stimulation. Additional morphological and structural characterization revealed that ripple formation on heavily boron-doped diamond (2.8 atom % [B]) occurs at much lower accumulated fluences than the 2 kJ/cm2 typically reported for lower doping levels and that the process involves stronger graphitization of the BDD surface. Finally, we show that the exposed interface between sp2 and sp3 carbon layers (i.e. the laser-ablated diamond surface) revealed faster kinetics than the untreated BDD in both ferrocyanide and RuHex mediators, which can be used for electrochemical (bio)sensing. Overall, our work demonstrates that LIPSS is a powerful single-step tool for the fabrication of surface-engineered diamond electrodes with tunable material, electrochemical, and charge-storage properties.

Dataset Information

Electrochemical reduction of carbon dioxide to acetic acid on a Cu-Au modified boron-doped diamond electrode with a flow-cell system.

Publications

Electrochemical reduction of carbon dioxide to acetic acid on a Cu-Au modified boron-doped diamond electrode with a flow-cell system.

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