Ultrathin 3D radial tandem-junction photocathode with a high onset potential of 1.15 V for solar hydrogen production

doi:10.1016/S1872-2067(21)64046-9

Abstract

Abstract:

Combining a progressive tandem junction design with a unique Si nanowire (SiNW) framework paves the way for the development of high-onset-potential photocathodes and enhancement of solar hydrogen production. Herein, a radial tandem junction (RTJ) thin film water-splitting photocathode has been demonstrated experimentally for the first time. The photocathode is directly fabricated on vapor-liquid-solid-grown SiNWs and consists of two radially stacked p-i-n junctions, featuring hydrogenated amorphous silicon (a-Si:H) as the outer absorber layer, which absorbs short wavelengths, and hydrogenated amorphous silicon germanium (a-SiGe:H) as the inner layer, which absorbs long wavelengths. The randomly distributed SiNW framework enables highly efficient light-trapping, which facilitates the use of very thin absorber layers of a-Si:H (~50 nm) and a-SiGe:H (~40 nm). In a neutral electrolyte (pH = 7), the three-dimensional (3D) RTJ photocathode delivers a high photocurrent onset of 1.15 V vs. the reversible hydrogen electrode (RHE), accompanied by a photocurrent of 2.98 mA/cm² at 0 V vs. RHE, and an overall applied-bias photon-to-current efficiency of 1.72%. These results emphasize the promising role of 3D radial tandem technology in developing a new generation of durable, low-cost, high-onset-potential photocathodes capable of large-scale implementation.

Key words: Solar hydrogen production, 3D radial tandem junction, Amorphous silicon photocathode, Very thin absorber, High onset potential

Shaobo Zhang, Huiting Huang, Zhijie Zhang, Jianyong Feng, Zongguang Liu, Junzhuan Wang, Jun Xu, Zhaosheng Li, Linwei Yu, Kunji Chen, Zhigang Zou. Ultrathin 3D radial tandem-junction photocathode with a high onset potential of 1.15 V for solar hydrogen production[J]. Chinese Journal of Catalysis, 2022, 43(7): 1842-1850.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)64046-9

https://www.cjcatal.com/EN/Y2022/V43/I7/1842

Figures/Tables 7

Fig. 1. (a-d) Schematic illustration of the fabrication procedures of RTJs. SEM images of H2-plasma-treated Sn catalyst droplets (e) and VLS-grown p-type SiNWs (f). Top view of RTJ without ITO (g) and with ITO/Pt (h). Side view without ITO (k) and with ITO/Pt catalyst (l). (i) Final fabricated RTJ configuration. (j) Photograph of the RTJ photocathode. (m) Cross-section SEM image of the RTJ unit. (n) Absorption curves of radial junction and planar junction. Scale bar in (e) is 300 nm, while the others are 200 nm.

Fig. 2. (a) EDS spectra measured on the RTJ photocathode at Ep values of 3, 5, and 11 keV (without ITO layer); the detected position is indicated by a green cross in the top-right inset image, in which the scale bar represents 200 nm. (b) Different effective Lp of the EDS analysis at different probing energies.

Fig. 3. TEM image (a) and EDS elemental mapping images (b-f) (In, blue; Sn, green; Si, pink; Ge, golden; Pt, orange). All scale bars are 200 nm.

Fig. 4. (a) Schematic drawing of the PEC device under operation with the RTJ photocathode, with hydrogen evolution occurring at the RTJ photocathode. (b) Corresponding band diagram of the RTJ photocathode. (c) COMSOL-simulated light absorption patterns of cross-sections (at 1/4 height) and vertical sections (in the y-plane) of the RTJs at different incident wavelengths.

Fig. 5. (a) Photograph of the RTJ photocathode working in 0.1 mol/L KPi electrolyte (pH 7). J-V (b) and ABPE (c) curves for the RTJ photocathodes with different thicknesses of the Pt catalyst. (d) Extracted values of Vonset, Jph (at 0 V vs. RHE), and ABPE with different nominal thicknesses of the Pt catalyst.

Fig. 6. Schematic diagram (a) and a photograph (b) of the test condition. (c) J-V curves of the RTJ solar cells with different thicknesses of the Pt catalyst. Values of Voc and Vonset (d) and Jsc and Jph (at 0 V vs. RHE) (e) of the RTJ solar cells and photocathodes for different thicknesses of the Pt catalyst. (f) Transmission spectra of the catalysts with different Pt thicknesses, with photographs of the Pt catalysts deposited on quartz. To remove the effect of the quartz, a baseline was obtained by placing quartz at the measuring location.

Fig. 7. EIS Nyquist plots of RTJ photocathodes with different thicknesses of the Pt catalyst at 1 V vs. RHE (a) and 0.7 V vs. RHE (b). (c) Chronoamperometric stability test of the RTJ photocathode with the 2.5 nm Pt catalyst at the fixed potential of 0 V vs. RHE. (d) Measured and calculated amounts of H2 and O2 generated by the RTJ photocathode with the 2.5 nm Pt catalyst at 0 V vs. RHE.

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