TY - JOUR
T1 - Heavily boron-doped diamond grown on scalable heteroepitaxial quasi-substrates
T2 - A promising single crystal material for electrochemical sensing applications
AU - Liu, Zhichao
AU - Baluchová, Simona
AU - Sartori, André F.
AU - Li, Ziyu
AU - Gonzalez-Garcia, Yaiza
AU - Schreck, Matthias
AU - Buijnsters, Josephus G.
PY - 2023
Y1 - 2023
N2 - In this work, three distinct heteroepitaxial single-crystal boron-doped diamond (SC-BDD) electrodes were fabricated and subjected to detailed surface analysis and electrochemical characterization. Specifically, the heteroepitaxy approach allowed to synthesize large-area (1 cm2) and heavily-doped (100)-oriented SC-BDD electrodes. Their single-crystal nature and crystal orientation were confirmed by X-ray diffraction, while scanning electron and atomic force microscopies revealed marked variations in surface morphology resulting from their growth on respective on-axis and off-axis substrates. Further, absence of sp2 impurities along with heavy boron doping (>1021 cm−3) was demonstrated by Raman spectroscopy and Mott-Schottky analysis, respectively. Cyclic voltammetry (CV) in a 0.1 M KNO3 solution revealed wide potential windows (∼3.3 V) and low double-layer capacitance (<4 μF cm−2) of the SC-BDD electrodes. Their highly conductive, ‘metal-like’ nature was confirmed by CV with [Ru(NH3)6]3+/2+ probe manifesting near-reversible redox response with ΔEp approaching 0.059 V. The same probe was used to record scanning electrochemical micrographs, which clearly demonstrated homogeneously distributed electrochemical activity of the heteroepitaxial SC-BDD electrodes. Minor differences in their electrochemical performance, presumably resulting from the somewhat different morphological features, were only unveiled during CV with surface sensitive compounds [Fe(CN)6]3−/4− and dopamine. The latter was also used to show the possibility of applying herein developed heteroepitaxial SC-BDD electrodes for electrochemical sensing, whereas experiments with anthraquinone-2,6-disulfonate revealed their enhanced resistance to fouling. All in all, heteroepitaxial SC-BDD represents a highly attractive electrode material which can, owing to the fabrication strategy, easily overcome size limitation, currently preventing broader use of single crystal diamond electrodes in electrochemical applications.
AB - In this work, three distinct heteroepitaxial single-crystal boron-doped diamond (SC-BDD) electrodes were fabricated and subjected to detailed surface analysis and electrochemical characterization. Specifically, the heteroepitaxy approach allowed to synthesize large-area (1 cm2) and heavily-doped (100)-oriented SC-BDD electrodes. Their single-crystal nature and crystal orientation were confirmed by X-ray diffraction, while scanning electron and atomic force microscopies revealed marked variations in surface morphology resulting from their growth on respective on-axis and off-axis substrates. Further, absence of sp2 impurities along with heavy boron doping (>1021 cm−3) was demonstrated by Raman spectroscopy and Mott-Schottky analysis, respectively. Cyclic voltammetry (CV) in a 0.1 M KNO3 solution revealed wide potential windows (∼3.3 V) and low double-layer capacitance (<4 μF cm−2) of the SC-BDD electrodes. Their highly conductive, ‘metal-like’ nature was confirmed by CV with [Ru(NH3)6]3+/2+ probe manifesting near-reversible redox response with ΔEp approaching 0.059 V. The same probe was used to record scanning electrochemical micrographs, which clearly demonstrated homogeneously distributed electrochemical activity of the heteroepitaxial SC-BDD electrodes. Minor differences in their electrochemical performance, presumably resulting from the somewhat different morphological features, were only unveiled during CV with surface sensitive compounds [Fe(CN)6]3−/4− and dopamine. The latter was also used to show the possibility of applying herein developed heteroepitaxial SC-BDD electrodes for electrochemical sensing, whereas experiments with anthraquinone-2,6-disulfonate revealed their enhanced resistance to fouling. All in all, heteroepitaxial SC-BDD represents a highly attractive electrode material which can, owing to the fabrication strategy, easily overcome size limitation, currently preventing broader use of single crystal diamond electrodes in electrochemical applications.
KW - Electrochemical performance
KW - Heavy boron doping
KW - Heteroepitaxial growth
KW - Large-area electrodes
KW - Single-crystal diamond
KW - Surface analysis
UR - http://www.scopus.com/inward/record.url?scp=85143802963&partnerID=8YFLogxK
U2 - 10.1016/j.carbon.2022.10.023
DO - 10.1016/j.carbon.2022.10.023
M3 - Article
AN - SCOPUS:85143802963
VL - 201
SP - 1229
EP - 1240
JO - Carbon
JF - Carbon
SN - 0008-6223
ER -