1D/2D TiO2/ZnIn2S4 S型异质结光催化剂及其高效制氢性能

doi:10.1016/S1872-2067(21)63875-5

催化学报 ›› 2022, Vol. 43 ›› Issue (2): 339-349.DOI: 10.1016/S1872-2067(21)63875-5

1D/2D TiO₂/ZnIn₂S₄ S型异质结光催化剂及其高效制氢性能

李金懋^a^,^b, 吴聪聪^a, 李矜^a^,^$(), 董兵海^a, 赵丽^a^,^*(), 王世敏^a^,^#()

^a湖北大学材料科学与工程学院, 有机化工新材料省部共建协同创新中心, 功能材料绿色制备与应用教育部重点实验室, 湖北武汉 430062
^b湖北师范大学化学化工学院, 污染物分析与资源化技术湖北省重点实验室,湖北黄石 435002

收稿日期:2021-05-02 接受日期:2021-06-10 出版日期:2022-02-18 发布日期:2021-07-02
通讯作者: 李矜,赵丽,王世敏
基金资助:
国家重点研发计划政府间国际科技创新合作重点专项(2019YFE0107100);国家自然科学基金(52002121);国家自然科学基金(62004064)

1D/2D TiO₂/ZnIn₂S₄ S-scheme heterojunction photocatalyst for efficient hydrogen evolution

Jinmao Li^a^,^b, Congcong Wu^a, Jin Li^a^,^$(), Binghai Dong^a, Li Zhao^a^,^*(), Shimin Wang^a^,^#()

^aCollaborative Innovation Center for Advanced Organic Chemical Materials Co-constructed by the Province and Ministry, Ministry-of-Education Key Laboratory for the Green Preparation and Application of Functional Materials, School of Materials Science and Engineering, Hubei University, Wuhan 430062, Hubei, China
^bHubei Key Laboratory of Pollutant Analysis and Reuse Technology, College of Chemistry and Chemical Engineering, Hubei Normal University, Huangshi 435002, Hubei, China

Received:2021-05-02 Accepted:2021-06-10 Online:2022-02-18 Published:2021-07-02
Contact: Jin Li, Li Zhao, Shimin Wang
Supported by:
This work was supported by Key Program for Intergovernmental S&T Innovation Cooperation Projects of National Key R&D Program of China(2019YFE0107100);the National Natural Science Foundation of China(52002121);the National Natural Science Foundation of China(62004064)

摘要/Abstract

摘要：

通过半导体催化剂利用太阳能分解水制氢被认为是解决人类面临的环境问题和能源危机的有效途径. 在众多的半导体光催化剂中, TiO₂由于其良好的光化学稳定性、无毒性、丰富的形貌以及低廉的价格, 在光催化制氢领域备受关注. 然而TiO₂的内在缺陷, 如较宽的带隙、较窄的光响应范围, 光生电子空穴对的快速复合, 极大限制了其太阳能制氢效率. 构建异质结结构被认为是解决以上问题的一个有效方法, 通过将TiO₂与另一个半导体复合可以提升催化剂对太阳光的吸收范围, 也可降低光生电子空穴对的复合速率. 但构建一个成功的异质结结构不仅要满足上述的要求, 还需要保留异质结催化剂体系中光生电子和空穴的氧化还原能力.
研究表明, S型异质结是将两个具有合适能带结构的半导体进行耦合, 由于费米能级的差异, 两个半导体间将发生电子转移, 从而引起能带弯曲并形成内建电场. 光照条件下, 具有较弱还原能力的光生电子在内建电场和能带弯曲的作用下与较弱氧化能力的光生空穴复合, 实现异质结催化剂体系中各个半导体内部光生载流子有效分离的目标, 同时保留了异质结催化剂体系中较强氧化能力和较强还原能力的光生电子和空穴, 进而实现光催化活性的提高.
本文采用水热合成方法, 将具有更强还原能力和可见光响应特性的半导体(ZnIn₂S₄)原位生长在TiO₂纳米纤维表面, 构建了1D/2D TiO₂/ZnIn₂S₄ S型异质结光催化剂. 最优比例的TiO₂/ZnIn₂S₄复合材料表现出优越的光催化制氢活性(6.03 mmol/h/g), 分别是纯TiO₂和纯ZnIn₂S₄制氢活性的3.7倍和2倍. TiO₂/ZnIn₂S₄复合材料光催化活性的提高可以归因于紧密的异质结界面、光生载流子的有效分离、丰富的反应活性位点以及增强的光吸收能力. 通过原位XPS和DFT计算研究了异质结内部光生电子的转移机制. 结果表明, 在光照条件下电子由TiO₂向ZnIn₂S₄迁移, 遵循了S型异质结内部电子的转移机制, 实现了TiO₂和ZnIn₂S₄内部光生载流子的有效分离, 同时保留了具有较强还原能力的ZnIn₂S₄价带电子和较强氧化能力的TiO₂导带空穴, 从而显著提升光催化制氢效率. 综上, 本文制备的TiO₂/ZnIn₂S₄ S型异质结光催化剂很好地克服了TiO₂在光催化制氢领域所面临的诸多障碍, 为设计和制备高效异质结光催化剂提供了新的思路.

关键词: S型异质结, TiO₂, ZnIn₂S₄, 1D/2D, 光催化产氢

Abstract:

TiO₂ is a promising photocatalyst with limited use in practical applications owing to its wide bandgap, narrow light response range, and rapid recombination of photoexcited carriers. To address these limitations, a novel 1D/2D TiO₂/ZnIn₂S₄ heterostructure was designed according to the principles of the S-scheme heterojunction. The TiO₂/ZnIn₂S₄ (TZISx) hybrids prepared via a hydrothermal method afforded significant improvement in photocatalytic hydrogen evolution (PHE) in comparison to pristine TiO₂ and ZnIn₂S₄. In particular, the optimal TZIS2 sample (mass ratio of ZnIn₂S₄ to TiO₂ was 0.4) exhibited the highest PHE activity (6.03 mmol/h/g), which was approximately 3.7 and 2.0 times higher than those of pristine TiO₂ and ZnIn₂S₄, respectively. This improvement in the PHE of the TZIS2 sample could be attributed to the formation of an intimate heterojunction interface, high-efficiency separation of charge carriers, abundant reactive sites, and enhanced light absorption capacity. Notably, theoretical and experimental results demonstrated that the S-scheme mechanism of interfacial electron transfer in the TZISx composites facilitated the transfer and separation of photoexcited charge carriers, resulting in more isolated photoexcited electrons for the PHE reaction.

Key words: S-scheme heterojunction, TiO₂, ZnIn₂S₄, 1D/2D, Photocatalytic hydrogen evolution

李金懋, 吴聪聪, 李矜, 董兵海, 赵丽, 王世敏. 1D/2D TiO₂/ZnIn₂S₄ S型异质结光催化剂及其高效制氢性能[J]. 催化学报, 2022, 43(2): 339-349.

Jinmao Li, Congcong Wu, Jin Li, Binghai Dong, Li Zhao, Shimin Wang. 1D/2D TiO₂/ZnIn₂S₄ S-scheme heterojunction photocatalyst for efficient hydrogen evolution[J]. Chinese Journal of Catalysis, 2022, 43(2): 339-349.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(21)63875-5

https://www.cjcatal.com/CN/Y2022/V43/I2/339

图/表 10

Fig. 1. (a) Schematic of the synthesis of TZISx composites; (b) Zeta potential of TiO2 in ethanol aqueous solution (volume ratio of water to ethanol is 2:1).

Fig. 2. (a) XRD data, (b) nitrogen adsorption-desorption isotherms, (c) pore-size distributions, and (d) UV-vis diffuse reflectance spectra of TiO2, ZnIn2S4, and TZISx composites.

Fig. 3. (a) XPS survey data of TiO2, ZnIn2S4, and TZIS2; Ti 2p (b) andO 1s (c) high-resolution XPS data of TiO2 and TZIS2 in dark or under light irradiation; Zn 2p (d), In 3d (e), and S 2p (f) XPS data of ZnIn2S4 and TZIS2 in dark and under light irradiation.

Table 1 Physical properties of the as-prepared photocatalysts.

Sample	S_BET (m²/g)	Pore size (nm)	Pore volume (cm³/g)
TiO₂	23.6	15.5	0.09
TZIS1	26.6	14.5	0.10
TZIS2	58.3	11.9	0.17
TZIS3	81.5	10.9	0.22
ZnIn₂S₄	146.3	9.1	0.33

Fig. 4. FESEM images of TiO2 (a), ZnIn2S4 (b), and TZIS2 (c); TEM (d) and HRTEM (e) images of TZIS2; (f) Energy-dispersive X-ray mapping images of TZIS2.

Fig. 5. (a) PHE activities of the as-prepared samples in TEOA solution; (b) PHE activity of TZIS2 using different sacrificial reagents; (c) AQE of TZIS2 using different sacrificial reagents; (d) Cyclic PHE experiments of TZIS2 in TEOA aqueous solution; (e) XRD data of TZIS2 before and after reaction.

Table 2 Comparison of H2 evolution rate using representative photocatalysts.

Photocatalyst	Light source	Electron donor	H₂ evolution rate (mmol/h/g)	Ref.
ZnIn₂S₄/TiO_2‒_x	LED lamp (420 nm)	Na₂S/Na₂SO₃	0.53	[14]
ZnIn₂S₄@SiO₂@TiO₂	300 W Xe lamp	TEOA	0.62	[16]
rGO/TiO₂/ZIS	300 W Xe lamp	Na₂S/Na₂SO₃	0.46	[38]
TiO₂@ZnIn₂S₄	300 W Xe lamp	Lactic acid	1.24	[40]
Ti₃C₂@TiO₂/ZIS	300 W Xe lamp	Na₂S/Na₂SO₃	1.19	[50]
TiO₂ nanobelt/ZnIn₂S₄	300 W Xe lamp	Na₂S/Na₂SO₃	0.35	[60]
TiO₂ nanofiber/ZnIn₂S₄	300 W Xe lamp	TEOA Lactic acid Methanol Na₂S/Na₂SO₃	6.03 2.32 1.92 1.56	This work

Fig. 6. (a) PL spectra of the as-prepared samples; (b) TRPL of TiO2 and TZIS2; Transient photocurrent (c) and EIS plots (d) of TiO2, ZnIn2S4, and TZIS2.

Fig. 7. XPS valence band spectra (a) and Tauc plots (b) of TiO2 and ZnIn2S4; Calculated electrostatic potentials of TiO2 (c) and ZnIn2S4 (d).

Fig. 8. Schematic showing the S-scheme electron transfer between TiO2 and ZnIn2S4.

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1D/2D TiO₂/ZnIn₂S₄ S型异质结光催化剂及其高效制氢性能

1D/2D TiO₂/ZnIn₂S₄ S-scheme heterojunction photocatalyst for efficient hydrogen evolution

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