ZnxCd1-xS quantum dot with enhanced photocatalytic H2-production performance

doi:10.1016/S1872-2067(20)63614-2

Abstract

Abstract:

H₂ is an important energy carrier for replacing fossil fuel in the future due to its high energy density and environmental friendliness. As a sustainable H₂-generation method, photocatalytic H₂ production by water splitting has attracted much interest. Here, oil-soluble Zn_xCd_1-_xS quantum dot (ZCS QD) with a uniform particle size distribution were prepared by a hot-injection method. However, no photocatalytic H₂-production activity was observed for the oil-soluble ZCS QD due to its hydrophobicity. Thus, the oil-soluble ZCS QD was converted into a water-soluble ZCS QD by a ligand-exchange method. The water-soluble ZCS QD exhibited excellent photocatalytic H₂-production performance in the presence of glycerin and Ni²⁺, with an apparent quantum efficiency of 15.9% under irradiation of 420 nm light. Further, the photocatalytic H₂-generation activity of the ZCS QD was ~10.7 times higher than that of the Zn_xCd_1-_xS relative samples prepared by the conventional co-precipitation method. This work will inspire the design and fabrication of other semiconductor QD photocatalysts because QD exhibits excellent separation efficiency for photogenerated electron-hole pairs due to its small crystallite size.

Key words: ZnxCd1-xS, Solid-solution photocatalyst, Photocatalytic H2 production, Oil-soluble quantum dot, Water-oil soluble quantum dot

Rongrong Gao, Bei Cheng, Jiajie Fan, Jiaguo Yu, Wingkei Ho. Zn_xCd_1-_xS quantum dot with enhanced photocatalytic H₂-production performance[J]. Chinese Journal of Catalysis, 2021, 42(1): 15-24.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63614-2

https://www.cjcatal.com/EN/Y2021/V42/I1/15

Figures/Tables 10

Fig. 1. The schematic illustration of the ligand-exchange process for ZCS QD.

Fig. 2. The XRD patterns of ZCS QD and ZCS RS.

Fig. 3. The TEM (a,c) and high-resolution TEM (b,d) images of ZCS QD (a,b) and ZCS RS (c,d).

Fig. 4. (a) UV-vis diffuse reflection spectra, (b) Kubelka-Munk function vs. photon energy curves, and Mott-Schottky plots of ZCS QD (c) and ZCS RS (d).

Fig. 5. (a) The survey spectra, (b) Zn 2p, (c) Cd 3d, (d) S 2p high-resolution XPS spectra of the ZCS QD and ZCS RS.

Fig. 6. (a) Steady-state photoluminescence (PL), (b) time-resolved PL spectra, (c) transient photocurrent responses, and (d) electrochemical impedance spectroscopy (EIS) spectra of the ZCS QD and ZCS RS.

Table 1 Fitted parameters obtained from the decay curves of the samples.

Samples	τ₁(ns) (Rel. %)	τ₂(ns) (Rel. %)	τ₃(ns) (Rel. %)	τ_a(ns)
ZCS QD	0.26 (29.24%)	4.22 (24.03%)	16.61 (46.73%)	8.9
ZCS RS	0.24 (65.38%)	3.02 (21.88%)	13.46 (12.74%)	2.5

Fig. 7. (a) Photocatalytic H2-production rates of ZCS RS, RS-1% Ni, QD, and QD-1% Ni. (b) Photocatalytic H2 production over time for the ZCS QD and RS with 1% Ni.

Table 2 Comparisons of the photocatalytic H2-production performance of various ZnxCd1-xS-based photocatalysts.

Photocatalysts	Sacrifice agent	Light	Yield (μmol g^-1 h^-1)	Ref.
Zn_xCd_1-_xS-1% Ni	Glycerol	300 W Xe lamp	2253	This work
RGO/Zn_0.5Cd_0.5S	Na₂S-Na₂SO₃	300 W Xe lamp	770	[59]
SiC/Zn_0.5Cd_0.5S	Na₂S-Na₂SO₃	586 mW/cm² Xe lamp	894	[60]
P-Zn_0.5Cd_0.5S	HMF	30 × 3W LED	419	[61]
Cu₂S/Zn_0.71Cd_0.29S	Na₂S-Na₂SO₃	100 mW/cm² Xe lamp	1202	[62]
Ni₃C/Zn_0.3Cd_0.7S	Na₂S-Na₂SO₃	300 W Xe lamp	3310.1	[63]
Hierarchical Zn_0.64Cd_0.36S	Na₂S-Na₂SO₃	300 W Xe lamp	815	[64]
GO/Zn_0.5Cd_0.5S	Na₂S-Na₂SO₃	150 W Xe lamp	1060	[65]
RGO/Zn_0.8Cd_0.2S	Na₂S-Na₂SO₃	100 mW/cm² Xe lamp	1824	[57]
CoPt₃/Zn_0.5Cd_0.5S	Na₂S-Na₂SO₃	300 W	2830	[66]

Fig. 8. (a) Proposed mechanism of photocatalytic H2 production. (b) The schematic illustration of the difference in transfer distance of carriers for ZCS QD and RS.

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Zn_xCd_1-_xS quantum dot with enhanced photocatalytic H₂-production performance

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