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Boron-doped diamond semiconductor electrodes: Efficient photoelectrochemical CO₂ reduction through surface modification.

ABSTRACT: Competitive hydrogen evolution and multiple proton-coupled electron transfer reactions limit photoelectrochemical CO₂ reduction in aqueous electrolyte. Here, oxygen-terminated lightly boron-doped diamond (BDD_L) thin films were synthesized as a semiconductor electron source to accelerate CO₂ reduction. However, BDD_L alone could not stabilize the intermediates of CO₂ reduction, yielding a negligible amount of reduction products. Silver nanoparticles were then deposited on BDD_L because of their selective electrochemical CO₂ reduction ability. Excellent selectivity (estimated CO:H₂ mass ratio of 318:1) and recyclability (stable for five cycles of 3 h each) for photoelectrochemical CO₂ reduction were obtained for the optimum silver nanoparticle-modified BDD_L electrode at -1.1 V vs. RHE under 222-nm irradiation. The high efficiency and stability of this catalyst are ascribed to the in situ photoactivation of the BDD_L surface during the photoelectrochemical reaction. The present work reveals the potential of BDD_L as a high-energy electron source for use with co-catalysts in photochemical conversion.

SUBMITTER: Roy N

PROVIDER: S-EPMC5125091 | biostudies-literature | 2016 Nov

REPOSITORIES: biostudies-literature

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Boron-doped diamond semiconductor electrodes: Efficient photoelectrochemical CO2 reduction through surface modification.

Roy Nitish N Hirano Yuiri Y Kuriyama Haruo H Sudhagar Pitchaimuthu P Suzuki Norihiro N Katsumata Ken-Ichi KI Nakata Kazuya K Kondo Takeshi T Yuasa Makoto M Serizawa Izumi I Takayama Tomoaki T Kudo Akihiko A Fujishima Akira A Terashima Chiaki C

Scientific reports 20161128

Competitive hydrogen evolution and multiple proton-coupled electron transfer reactions limit photoelectrochemical CO2 reduction in aqueous electrolyte. Here, oxygen-terminated lightly boron-doped diamond (BDDL) thin films were synthesized as a semiconductor electron source to accelerate CO2 reduction. However, BDDL alone could not stabilize the intermediates of CO2 reduction, yielding a negligible amount of reduction products. Silver nanopar ...[more]

PMID: 27892544

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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.

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Boron-doped diamond semiconductor electrodes: Efficient photoelectrochemical CO₂ reduction through surface modification.

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Boron-doped diamond semiconductor electrodes: Efficient photoelectrochemical CO<sub>2</sub> reduction through surface modification.

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