电荷动力学工程: 量子点诱导的全空间电场协同Ag2S量子点/CoWO4 S型异质结促进光催化析氢

doi:10.1016/S1872-2067(26)65147-9

催化学报 ›› 2026, Vol. 88: 233-246.DOI: 10.1016/S1872-2067(26)65147-9

电荷动力学工程: 量子点诱导的全空间电场协同Ag₂S量子点/CoWO₄ S型异质结促进光催化析氢

马小龙^a^,¹, 吴之强^c^,¹, 姚惠琴^b^,^*(), 刘彬^d, 靳治良^a^,^*(), Paolo Fornasiero^e^,^*()

^a 北方民族大学化学与化学工程学院, 宁夏太阳能化学转化技术重点实验室, 国家民委化工技术基础重点实验室, 宁夏银川 750021, 中国
^b 宁夏医科大学基础医学院, 宁夏银川 750004, 中国
^c 宁夏师范大学化学与化工学院, 宁夏绿色催化材料与技术重点实验室, 宁夏固原 756099, 中国
^d 韶关学院化学与土木工程学院, 广东韶关 512005, 中国
^e 里雅斯特大学化学与制药科学系, 里雅斯特, 意大利

收稿日期:2026-01-05 接受日期:2026-04-14 出版日期:2026-09-18 发布日期:2026-09-05
通讯作者: *电子信箱: yaohq@nxmu.edu.cn (姚惠琴),
zl-jin@nun.edu.cn (靳治良),
pfornasiero@units.it (P. Fornasiero).
基金资助:
宁夏回族自治区自然科学基金(2023AAC02046);北方民族大学研究生创新项目(CYX25251)

Charging dynamics engineering: Quantum dots-induced full-space electric field cooperative Ag₂S QDs/CoWO₄ S-scheme heterojunction boosting photocatalytic hydrogen evolution

Xiaolong Ma^a^,¹, Zhiqiang Wu^c^,¹, Huiqin Yao^b^,^*(), Bin Liu^d, Zhiliang Jin^a^,^*(), Paolo Fornasiero^e^,^*()

^a Ningxia Key Laboratory of Solar Chemical Conversion Technology, Key Laboratory for Chemical Engineering and Technology, State Ethnic Affairs Commission, School of Chemistry and Chemical Engineering, North Minzu University, Yinchuan 750021, Ningxia, China
^b School of Basic Medical Science, Ningxia Medical University, Yinchuan 750004, Ningxia, China
^c Ningxia Key Laboratory of Green Catalytic Materials and Technology, College of Chemistry and Chemical Engineering, Ningxia Normal University, Guyuan 756099, Ningxia, China
^d School of Chemistry and Civil Engineering, Shaoguan University, Shaoguan 512005, Guangdong, China
^e Department of Chemical and Pharmaceutical Sciences, Center for Energy, Environment and Transport Giacomo Ciamiciam, INSTM Trieste Research Unit and ICCOM-CNR Trieste Research Unit, University of Trieste, 34127 Trieste, Italy

Received:2026-01-05 Accepted:2026-04-14 Online:2026-09-18 Published:2026-09-05
About author:First author contact:1 共同第一作者.
1 Contributed equally to this work.
Supported by:
The Ningxia Hui Autonomous Region Natural Science Foundation project(2023AAC02046);The Graduate Innovation Project of North Minzu University(CYX25251)

摘要/Abstract

摘要：

光催化制氢作为一种极具发展潜力的能源转化策略, 光催化剂是其关键组成部分. 过渡金属钨酸盐(如CoWO₄)由于其良好的化学稳定性、环境友好性、且成本低廉而备受关注. 助催化剂不仅能显著提升主催化剂的活性与稳定性, 还可有效抑制光生载流子复合, 从而大幅提升光催化产氢的效率. 量子点因其独特的光电性能已成为光催化领域的新兴材料. Ag₂S量子点兼具了量子点与金属硫化物的双重优势, 在光催化产氢领域中潜力显著. 构建强大的全空间电场(FSEF)是优化电荷动力学, 进而提升光催化产氢效率的关键策略之一. 非中心对称半导体的极化体电场(BEF)可驱动电荷分离, 而S型异质结的界面电场(IEF)能加速电荷转移. 因此, 通过将BEF与IEF进行级联耦合, 得以成功构建出强大的FSEF. 该FSEF能够优化电荷传输动力学并提高载流子分离效率, 进而显著加快光催化析氢反应.
有效调控电荷动力学对于提升光催化析氢活性至关重要. 本文在成功合成的Ag₂S量子点基础上, 通过利用CoWO₄和Ag₂S量子点之间的能带结构和费米能级差异, 合理设计并构建了CoWO₄/Ag₂S S型异质结. 同时, 通过电荷极化策略在Ag₂S量子点修饰的CoWO₄光催化剂上诱导构建出高效的FSEF, 这种高效的FSEF是通过BEF和IEF的级联耦合形成的. 飞秒瞬态吸收光谱、光辅助开尔文探针力显微镜、原位X射线光电子能谱等表征技术以及密度泛函理论计算证实了CoWO₄/Ag₂S S型异质结和FSEF的构建. S型异质结的成功构建有效保留了具有强氧化还原能力的光生空穴和电子, 使其参与反应; 同时, FSEF的建立为析氢反应提供了强大的驱动力, 从而极大提升了电荷的迁移效率. 在这种持续驱动的FSEF与S型异质结的协同作用下, 不仅显著提高了光生载流子的分离效率, 而且使得大量光生电子能够快速地迁移至催化剂表面以参与水的还原反应, 从而极大地提高了光催化产氢效率. 5 h内复合光催化剂CWAS-10的氢气生成速率达到了1546.23 μmol·g^-1·h^-1. 与初始CoWO₄和Ag₂S相比, 其性能分别提高了近2.6倍和4.2倍. 这主要得益于全空间电场与S型异质结对电荷动力学行为的有效优化.
综上, 合理设计构建FSEF协同S型异质结对电荷动力学行为的优化可有效提升光催化剂活性. 本研究为量子点诱导FSEF优化S型异质结中的电荷转移动力学提供了一种新策略, 为能量转换领域的高效光催化剂设计提供了有价值的见解.

关键词: Ag₂S量子点, CoWO₄, S型异质结, 全空间电场, 电荷转移动力学

Abstract:

Quantum dots (QDs) demonstrate significant potential in the field of photocatalytic hydrogen production due to their unique photoelectronic properties. In this study, based on the successful synthesis of Ag₂S QDs, a rationally designed CoWO₄/Ag₂S S-scheme heterojunction was constructed by utilizing the band structure and Fermi level difference between CoWO₄ and Ag₂S QDs. Simultaneously, an efficient full-space electric field was engineered on the Ag₂S QDs-modified CoWO₄ photocatalyst through charge polarization strategy. Specifically, this robust full-space electric field was formed via cascaded coupling of the bulk electric field and the interface electric field. The successful establishment of both the CoWO₄/Ag₂S S-scheme heterojunction and the full-space electric field was confirmed through characterization techniques including femtosecond transient absorption spectra, Kelvin probe force microscopy and in-situ X-ray photoelectron spectroscopy, along with density functional theory calculation results. Under the synergistic effect of the continuously driven full-space electric field and the S-scheme heterojunction, the separation of photogenerated electrons and holes has been significantly enhanced, enabling substantial electron accumulation on the catalyst surface for reaction participation, thereby greatly improving charge utilization efficiency. Meanwhile, it greatly facilitates the participation of highly oxidizing-reducing capable photogenerated electrons and holes in the reaction, providing sufficient driving force for the hydrogen evolution reaction. Ultimately, the hydrogen production rate of CWAS-10 reached 1546.23 μmol·g^-1·h^-1 within 5 h. Compared with the original CoWO₄ and Ag₂S, the performance was improved by nearly 2.6 and 4.2 times, respectively. This study offers a novel strategy for constructing S-scheme heterojunctions via quantum dot modification and synergistically regulating charge dynamics, providing valuable insights for the design of efficient photocatalysts in the field of energy conversion.

Key words: Ag₂S quantum dots, CoWO₄, S-scheme heterojunction, Full-space electric field, Charge transfer kinetics

马小龙, 吴之强, 姚惠琴, 刘彬, 靳治良, Paolo Fornasiero. 电荷动力学工程: 量子点诱导的全空间电场协同Ag₂S量子点/CoWO₄ S型异质结促进光催化析氢[J]. 催化学报, 2026, 88: 233-246.

Xiaolong Ma, Zhiqiang Wu, Huiqin Yao, Bin Liu, Zhiliang Jin, Paolo Fornasiero. Charging dynamics engineering: Quantum dots-induced full-space electric field cooperative Ag₂S QDs/CoWO₄ S-scheme heterojunction boosting photocatalytic hydrogen evolution[J]. Chinese Journal of Catalysis, 2026, 88: 233-246.

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图/表 6

Fig. 1. (a,b) XRD patterns of Ag2S, CoWO4 and CWAS-X. (c-f) High-resolution XPS spectra of Ag 3d, S 2p, Co 2p and W 4f. (g-j) TEM images of CoWO4, Ag2S and CWAS-10. AFM images of CoWO4 (k) and CWAS-10 (l). (m) EDS images of CWAS-10.

Fig. 2. (a) The H2 production amounts of Ag2S, CoWO4 and CWAS-10. (b) The H2 production amount of CWAS-X. (c) The H2 production amounts with different EY additions. (d) The H2 production amounts of different masses of CWAS-10. (e) The H2 production amounts with different volumes of TEOA. (f) Hydrogen production cycle experiment. The surface temperatures of CoWO4 (g), Ag2S (h), and CWAS-10 (i).

Fig. 3. (a) Transient photocurrent response curves of Ag2S, CoWO4 and CWAS-10. (b) EIS of Ag2S, CoWO4 and CWAS-10. (c) LSV of Ag2S, CoWO4 and CWAS-10. (d) Tafel curves of Ag2S, CoWO4 and CWAS-10. (e) Capacitance of CoWO4 and CWAS-10 at different scan rates. (f) UV-visible absorption spectra of CoWO4, Ag2S and CWAS-10. PL and TRPL spectra of CoWO4 (g), Ag2S (h), EY (i) and CWAS-10 (j). (l) Band structure diagrams of CoWO4 and Ag2S.

Fig. 4. Band gap diagrams of CoWO4 (a) and Ag2S (b). DOS of CoWO4 (c) and Ag2S (d). WF of CoWO4 (e) and Ag2S (f). (g,j) Charge difference integral diagrams of CoWO4. (h) The average electrostatic potential electric field map of CoWO4. (i,k) Charge difference integral diagrams of CWAS-10. (l) Electron transfer mechanism diagram of the full space electric field of CWAS-10. Dielectric functions (m), absorption spectra (n), reflection spectra (o), and loss spectra (p) of CoWO4, Ag2S and CWAS-10.

Fig. 5. Two-dimensional pseudo-color TA map of CoWO4 (a) and CWAS-10 (b). Transient absorption spectra of CoWO4 (c) and CWAS-10 (d). Fitting of decay kinetics of CoWO4 (e) and CWAS-10 (f). (g) Carrier transport dynamics of CoWO4 and CWAS-10.

Fig. 6. (a-d) Three-dimensional surface potential distribution of CoWO4 and CWAS-10 under dark and light conditions. KPFM of CoWO4 (e) and CWAS-10 (f). In-situ XPS fine spectra of Ag (g) and Co (h). (i) The reaction mechanism of CWAS-10.

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电荷动力学工程: 量子点诱导的全空间电场协同Ag₂S量子点/CoWO₄ S型异质结促进光催化析氢

Charging dynamics engineering: Quantum dots-induced full-space electric field cooperative Ag₂S QDs/CoWO₄ S-scheme heterojunction boosting photocatalytic hydrogen evolution

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