Effect of oxygen terminated surface of boron-doped diamond thin-film electrode on seawater salinity sensing

doi:10.1016/j.jmst.2021.01.028

Abstract

Abstract:

Tremendous demands for highly sensitive and stable seawater salinometers have motivated intensive research on advanced electrode materials. Boron-doped diamond (BDD) is attractive in terms of its high mechanical stability and chemical inertness, but is usually hindered by its low double-layer capacitance (C_dl) for seawater salinity detection. Here, inspired by the principle of oxygen-terminated BDD electrode endowing higher C_dl than hydrogen-terminated surface, we introduce the oxygen terminated surface by oxygen plasma or reactive ion etch (RIE), and the fabricated oxygen terminated BDD electrodes demonstrate high sensitivity and long-term stability in seawater salinity detection comparing with the hydrogen terminated BDD electrodes. Significantly, the as-fabricated O-BDD-RIE electrodes not only show remarkable enhanced response even better than the commercial platinum black electrodes but also display long-time stability which is weekly verified by continuous monitor for 90 days. The outstanding performance of the oxygen terminated BDD electrodes can be ascribed to the enhancement of C-O surface functional group on C_dl. In addition, a comprehensive analysis of effective electroactive surface area (EASA) and C_dl proves that the surface oxygen is the major factor for the improved C_dl. In summary, the excellent oxygen terminated BDD electrodes promise potential application in seawater salinity detection.

Key words: Boron-doped diamond, Capacitance, Oxygen plasma, Reactive ion etch, Seawater salinity

Dan Shi, Lusheng Liu, Zhaofeng Zhai, Bin Chen, Zhigang Lu, Chuyan Zhang, Ziyao Yuan, Meiqi Zhou, Bing Yang, Nan Huang, Xin Jiang. Effect of oxygen terminated surface of boron-doped diamond thin-film electrode on seawater salinity sensing[J]. J. Mater. Sci. Technol., 2021, 86: 1-10.

Figures/Tables 10

Scheme 1. Schematic illustration of the synthesis process for H-BDD, O-BDD, O-BDD-RIE and H-BDD-RIE electrodes.

Fig. 1. FE-SEM images of H-BDD (a), O-BDD (b), O-BDD-RIE (c), H-BDD-RIE (d) electrodes with inset graphs of corresponding contact angles; enlarged surface (e) and cross-sectional (f) FE-SEM images of O-BDD-RIE electrode; Raman spectra (g) and XRD patterns (h) of H-BDD, O-BDD, O-BDD-RIE and H-BDD-RIE electrodes.

Fig. 2. XPS spectra (a) and deconvoluted C1 s XPS spectra (b) of H-BDD, O-BDD, O-BDD-RIE and H-BDD-RIE electrodes.

Table 1 Summary of the survey scans XPS Data for H-BDD, O-BDD, O-BDD-RIE and H-BDD-RIE electrodes (at.%).

	H-BDD	O-BDD	O-BDD-RIE	H-BDD-RIE
C 1 s	95.0	84.9	69.4	91.3
O 1 s	2.0	11.4	20.6	4.5
N 1 s	0.0	1.2	1.5	0.0
B 1 s	2.8	2.2	2.2	3.0
Si 2p	0.2	0.3	6.3	1.2

Table 2 The relative abundance of the components obtained from deconvolution of the C1 s spectra for H-BDD, O-BDD, O-BDD-RIE and H-BDD-RIE electrodes (%).

	H-BDD	O-BDD	O-BDD-RIE	H-BDD-RIE
C-sp²	1.0	0.1	0.2	0.8
C-H	36.0	12.2	12.1	31.1
C-sp³	39.5	42.6	42.6	42.8
C-O	21.4	24.1	32.9	9.4
C=O	2.0	21.0	12.2	15.9

Fig. 3. CVs in 0.1 M H2SO4 (a) and 1 M KCl containing 1 mM [Fe(CN)6]3-/4- (b) based on H-BDD, O-BDD, O-BDD-RIE and H-BDD-RIE electrodes at a scan rate of 100 mV/s and Nyquist plots (c) (inset shows the magnification Nyquist plots of O-BDD and O-BDD-RIE electrodes), Bode representations (d) of electrochemical impedance spectra of H-BDD, O-BDD, O-BDD-RIE and H-BDD-RIE electrodes in 0.1 M H2SO4.

Table 3 Potential Windows (±1 mA/cm2) in 0.1 M H2SO4, ΔEp in 1 M KCl containing 1 mM [Fe(CN)6]3-/4- and double layer capacitances (Cdl, Calculated at 0.2 V) in the standard seawater (S = 40 ‰) based on H-BDD, O-BDD, O-BDD-RIE and H-BDD-RIE electrodes.

	Potential Windows (V)	ΔE_p (mV)	C_dl (μF/cm²)
H-BDD	3.56	68.22	1.01
O-BDD	2.79	74.59	8.83
O-BDD-RIE	3.02	100.92	35.41
H-BDD-RIE	3.34	75.22	2.93

Fig. 4. Current response towards different salinity using electrodes of H-BDD, O-BDD, O-BDD-RIE and H-BDD-RIE (a) and differential capacitance curve based on H-BDD, O-BDD, O-BDD-RIE and H-BDD-RIE electrodes in the standard seawater (S = 40‰). Scan rate = 100 mV/s. (The standard deviations are all below 1.03 × 10-5 A/cm2 (n = 5)).

Fig. 5. Stability evaluation of current response towards different salinity for H-BDD (a), O-BDD (b), O-BDD-RIE (c) and H-BDD-RIE (d) electrodes during 90 days. (The standard deviations are all below 1.76 × 10-5 A/cm2 (n = 5)).

Fig. 6. Current response towards different salinity using O-BDD-RIE electrode in the standard seawater and real seawater (The standard deviations are all below 5.25 × 10-6 A/cm2 (n = 5)).

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