EDA-assisted synthesis of multifunctional snowflake-Cu2S/CdZnS S-scheme heterojunction for improved the photocatalytic hydrogen evolution

doi:10.1016/j.jmst.2021.11.073

Abstract

Abstract:

The charge separation efficiency is one of the main factors affecting the solar photocatalytic decomposition of water to produce hydrogen. Constructing a unique heterojunction can accelerate the separation and transfer of photo-generated charges, and effectively improve the photocatalytic efficiency, which is considered a potential strategy. Accordingly, the 2%Cu₂S/CZS step-scheme (S-scheme) heterojunction based on morphology and electronic structure was successfully prepared via simple hydrothermal method. Compared with the monomer Cu₂S and CdZnS, the hydrogen evolution rate of 2%Cu₂S/CZS samples is significantly increased. In particular, the 2%Cu₂S/CZS not only shows high hydrogen evolution rate of 5904 μmol g^-1 h^-1 (3.19 times than original CdZnS), but also presents preferable cyclic endurance. According to the characterization, we believe that the introduction of Cu₂S has the following three advantages: (i) The snowflake structure of Cu₂S reduces the agglomeration of granular CdZnS. (ii) The Cu₂S with narrow band gap broadens the light response range of the composite catalyst. (iii) The Cu₂S was introduced into CdZnS to form S-scheme heterojunction, which accelerated the separation and transfer of photo-generated charge. This work broadens the idea of designing efficient photocatalyst of hydrogen evolution.

Key words: S-scheme, Heterojunction, Multifunctional, Snowflake-Cu₂S, Photocatalyst

Guorong Wang, Yongkang Quan, Kaicheng Yang, Zhiliang Jin. EDA-assisted synthesis of multifunctional snowflake-Cu₂S/CdZnS S-scheme heterojunction for improved the photocatalytic hydrogen evolution[J]. J. Mater. Sci. Technol., 2022, 121: 28-39.

Figures/Tables 12

Scheme 1. Schematic diagram of the synthesis of Cu2S/CZS composite catalyst.

Fig. 1. (a, b) XRD patterns of CZS, Cu2S and 2%Cu2S/CZS, (c) XRD spectra of X%Cu2S/CZS (X=1, 2, 3 and 5) composite samples with different Cu2S content, (d) Comparison of XRD patterns of 2%Cu2S/CZS samples before and after hydrogen evolution.

Fig. 2. SEM image of (a, b) CZS, (c) Cu2S, (d) 2%Cu2S/CZS, (e) TEM image of CZS, (f, g) 2%Cu2S/CZS, (h) HRTEM image of the 2%Cu2S/CZS, (i) EDX spectrum of 2%Cu2S/CZS.

Fig. 3. (a) XPS survey spectra, XPS spectra of (b) Cd 3d, (c) Zn 2p, (d) S 2p and (e) Cu 2p.

Fig. 4. The N2 adsorption-desorption isotherm plots of CZS (a), Cu2S (b) and 2%Cu2S/CZS (c).

Table 1. The SBET, pore volume and average pore size of CZS, Cu2S and 2%Cu2S/CZS.

Samples	S_BET (m²/g)^a	Pore volume (cm³/g)^b	Average pore size (nm)^b
CZS	22	0.088	15
Cu₂S	6	0.014	8
2%Cu₂S/CZS	18	0.080	16

Fig. 5. (a) Hydrogen evolution performance of Cu2S, CZS and 2%Cu2S/CZS, (b) Hydrogen evolution performance of X%Cu2S/CZS (X=1, 2, 3 and 5) composite samples with different Cu2S content, (c) Stability test of 2%Cu2S/CZS composite sample, (d) Comparison of hydrogen evolution of 2%Cu2S/CZS composite catalyst under different sacrificial reagents, (e) AQE of 2%Cu2S/CZS, (f) SEM image of 2%Cu2S/CZS after hydrogen evolution.

Fig. 6. (a) The steady-state and (b) transient fluorescence spectra of CZS, Cu2S and 2%Cu2S/CZS.

Table 2. Kinetic analysis of emission decay for samples.

Samples	lifetime, τ (ns)	Rel (%)	<τ> (ns)	χ²
CZS	τ₁=0.97	A₁=41.82	2.00	1.67
	τ₂=5.20	A₂=34.91
	τ₃=130.98	A₃=23.27
Cu₂S	τ₁=0.55	A₁=43.05	1.15	1.73
	τ₂=4.28	A₂=35.72
	τ₃=115.46	A₃=21.24
2%Cu₂S/CZS	τ₁=5.35	A₁=33.37	2.07	1.65
	τ₂=134.52	A₂=24.14
	τ₃=1.01	A₃=42.49

Fig. 7. (a) UV-vis DRS of CZS, Cu2S and 2%Cu2S/CZS, (b) The Eg of CZS.

Fig. 8. (a, b) The Mot-Schottky curves of CZS and Cu2S, (c) the energy band distribution of the two semiconductors, (d-f) IT, EIS, LSV curve of CZS, Cu2S and 2%Cu2S/CZS.

Scheme 2. The possible photocatalytic hydrogen evolution mechanism of 2%Cu2S/CZS.

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EDA-assisted synthesis of multifunctional snowflake-Cu₂S/CdZnS S-scheme heterojunction for improved the photocatalytic hydrogen evolution

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