Mo2N QDs/ZnIn2S4异质结中的等离激元-激子-声子协同作用实现光生电子与空穴的同步高值化利用

doi:10.1016/S1872-2067(26)64967-4

催化学报 ›› 2026, Vol. 83: 219-230.DOI: 10.1016/S1872-2067(26)64967-4

Mo₂N QDs/ZnIn₂S₄异质结中的等离激元-激子-声子协同作用实现光生电子与空穴的同步高值化利用

李金河^a^,¹, 姚霞喜^b^,¹, 于晓慧^a, 周小松^c, 任伟^a, 王乐乐^a, 王伟康^a, 刘芹芹^a^,^*()

^a江苏大学材料科学与工程学院, 江苏镇江 212013
^b苏州工学院材料工程学院, 江苏常熟 215500
^c岭南师范学院化学与化工学院, 广东湛江 524048

收稿日期:2025-08-21 接受日期:2025-11-28 出版日期:2026-04-18 发布日期:2026-03-04
通讯作者: * 电子信箱: qqliu@ujs.edu.cn (刘芹芹).
作者简介:¹共同第一作者.
基金资助:
国家自然科学基金(22472069);国家自然科学基金(22102064);江苏省研究生科研与实践创新计划(KYCX24_3947)

Simultaneous value-added utilization of photogenerated electrons and holes via plasmon-exciton-phonon synergy in Mo₂N QDs/ZnIn₂S₄ heterojunction

Jinhe Li^a^,¹, Xiaxi Yao^b^,¹, Xiaohui Yu^a, Xiaosong Zhou^c, Wei Ren^a, Lele Wang^a, Weikang Wang^a, Qinqin Liu^a^,^*()

^aSchool of Materials Science & Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu, China
^bSchool of Materials Engineering, Suzhou University of Technology, Changshu 215500, Jiangsu, China
^cSchool of Chemistry and Chemical Engineering, Lingnan Normal University, Zhanjiang 524048, Guangdong, China

Received:2025-08-21 Accepted:2025-11-28 Online:2026-04-18 Published:2026-03-04
Contact: * E-mail: qqliu@ujs.edu.cn (Q. Liu).
About author:¹Contributed to this work equally.
Supported by:
National Natural Science Foundation of China(22472069);National Natural Science Foundation of China(22102064);Postgraduate Research & Practice Innovation Program of Jiangsu Province(KYCX24_3947)

摘要/Abstract

摘要：

全球能源需求的持续增长与环境问题的日益严峻, 亟需发展高效的太阳能-化学能转化技术. 传统光催化分解水制氢虽前景广阔, 但其氧化半反应动力学缓慢, 制约了实际应用效率. 虽然牺牲剂可提升电荷分离效率, 但其消耗会导致资源浪费并产生二次污染. 因此, 将析氢反应与可以获得高值化合物的氧化反应相耦合, 不仅可同步实现清洁氢能与高价值化学品的合成, 还能有效提升原子经济性与过程可持续性, 成为当前光催化领域的重要发展方向. 然而, 如何同时促进光生电子与空穴的高效分离与利用, 实现氧化还原反应动力学的协同提升, 仍是该体系面临的关键挑战.
发展高效的光催化氧化还原耦合系统, 关键在于实现高效的载流子分离动力学并设计有效的氧化还原位点. 本文在超薄ZnIn₂S₄纳米片表面构建非金属等离激元Mo₂N量子点, 形成0D/2D Mo₂N/ZnIn₂S₄异质结. 具体制备过程如下: 首先通过水热法合成超薄ZnIn₂S₄纳米片, 随后利用静电自组装将Mo₂N量子点(粒径约6 nm)均匀负载于纳米片表面. 透射电镜结果表明, Mo₂N量子点紧密锚定在ZnIn₂S₄表面. X射线光电子能谱与开尔文探针力显微镜分析表明, 异质结界面形成欧姆接触, 并建立起由Mo₂N指向ZnIn₂S₄的强内建电场. 飞秒瞬态吸收光谱结果表明, 复合催化剂载流子寿命延长至1501.7 ps. 同时Mo₂N量子点的局域表面等离激元共振效应可产生高能热电子, 显著降低表观活化能至4.87 kJ mol^-1. 电化学阻抗测试表明, 异质结界面电荷转移电阻显著降低, 有利于光生电子快速迁移至Mo₂N活性位点. 表面光电压测试进一步证实, 在光照下Mo₂N/ZnIn₂S₄异质结表现出强烈的表面电势响应, 其内建电场强度较纯ZnIn₂S₄提升约3.1倍. 通过原位红外光谱分析, 在光催化过程中监测到4-甲氧基苯甲醇逐步脱氢生成4-甲氧基苯甲醛的关键中间体信号. 利用密度泛函理论计算探究Mo₂N/ZnIn₂S₄异质结的电荷分布与反应路径. 通过调控Mo₂N负载量, 优化后的Mo₂N/ZnIn₂S₄复合催化剂实现高效的析氢与4-甲氧基苯甲醇氧化协同反应, H₂产率达96.3 mmol·h^-1·g^-1, 4-甲氧基苯甲醛产率达38.7 mmol·h^-1·g^-1, 在420 nm处的表观量子效率达13.7%.
综上, 本工作通过在超薄半导体表面构建非金属等离激元量子点, 构筑0D/2D异质结, 利用光子-声子协同效应同时增强载流子分离与反应动力学, 发展了一种可用于太阳能驱动燃料与高值化学品协同生产的高效光催化体系, 为设计多功能耦合光催化系统提供了新策略.

关键词: 光催化, 产氢, 4-甲氧基苯甲醇氧化, 局域表面等离激元共振, 光子-声子协同效应

Abstract:

The persistent challenge impeding photocatalytic advancement lies in achieving simultaneous efficient utilization of photogenerated carriers for dual value-added reactions. This study demonstrates the synergistic interplay of plasmon-exciton-phonon interactions within non-metallic plasmonic Mo₂N quantum dots anchored on ultrathin ZnIn₂S₄ nanosheets (0D/2D Mo₂N/ZnIn₂S₄), which simultaneously enhances photocatalytic hydrogen evolution and selective oxidation of 4-methoxybenzyl alcohol to 4-methoxybenzaldehyde. Integrated experimental, operando spectroscopic, and theoretical analyses reveal triple cooperative mechanisms: localized surface plasmon resonance at Mo₂N sites generates high-energy hot electrons through plasmon-exciton coupling, significantly reducing the apparent activation energy to 4.87 kJ·mol^-1; quantum confinement synergizing with the 0D/2D ohmic-junction concentrates excitons at nanoscale interfaces, enabling prolonged carrier lifetime; meanwhile, directional photon-to-phonon energy conversion induces uniform photothermal heating (ΔT = 55.9 °C), kinetically accelerating dehydrogenation while balancing redox half-reactions. This synergy achieves sacrificial-free co-production rates of 96.3 mmol·h^-1·g^-1 H₂ and 38.7 mmol·h^-1·g^-1 4-methoxybenzaldehyde with 13.7% apparent quantum efficiency at 420 nm, establishing a new paradigm for solar-driven chemical refineries via precision plasmon-phonon engineering.

Key words: Photocatalysis, H₂ evolution, 4-Methoxybenzyl alcohol oxidation, Localized surface plasmon resonance, Photon-phonon cooperativity

李金河, 姚霞喜, 于晓慧, 周小松, 任伟, 王乐乐, 王伟康, 刘芹芹. Mo₂N QDs/ZnIn₂S₄异质结中的等离激元-激子-声子协同作用实现光生电子与空穴的同步高值化利用[J]. 催化学报, 2026, 83: 219-230.

Jinhe Li, Xiaxi Yao, Xiaohui Yu, Xiaosong Zhou, Wei Ren, Lele Wang, Weikang Wang, Qinqin Liu. Simultaneous value-added utilization of photogenerated electrons and holes via plasmon-exciton-phonon synergy in Mo₂N QDs/ZnIn₂S₄ heterojunction[J]. Chinese Journal of Catalysis, 2026, 83: 219-230.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)64967-4

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图/表 7

Fig. 1. (a) Schematic synthesis of Mo2N/ZIS. TEM (b) and HRTEM (c) images of Mo2N. (d) HRTEM image of Mo2N/ZIS. (e) EDX images of Mo2N/ZIS.

Fig. 2. (a) XRD patterns of ZIS and MNZIS-5. In-situ high-resolution XPS spectra of S 2p (b), In 3d (c), Zn 2p (d), Mo 3d (e), and N 1s (f).

Fig. 3. Work functions of ZIS (a) and Mo2N (b). (c) Plane-averaged electron density differences along the Z-direction of Mo2N/ZIS composite. (d) Differential charge density (yellow represents electron accumulation; cyan represents electron dissipation). 2D charge density difference maps (e) and illustration in Mo2N/ZIS (f).

Fig. 4. H2 (a) and 4-MBAL (b) production rates of ZIS and composite with different Mo2N ratios. H2 (c) and 4-MBAL (d) production rates of ZIS and MNZIS-5 under different condition. (e) Comparison of H2 evolution between MNZIS-5 and reported literature. (f) Temperature dependence of 4-MBAL production rate for ZIS and MNZIS-5. Infrared thermograms at different irradiation times (g) and UV-vis DRS (h) of ZIS, Mo2N, and MNZIS-5.

Fig. 5. Surface charge density (a), surface photovoltage (b), IEF strength (c), electrochemical impedance spectroscopy(d), photocurrents (e), PL spectra (f), time-resolved photoluminescence spectra (g), open-circuit potential (h) and electron spin resonance (i) of ZIS and MNZIS-5.

Fig. 6. fs-TA of ZIS (a) and MNZIS-5 (b). Kinetic profiles of ZIS (c) and MNZIS-5 (d). (e) Scheme of the decay pathways of photoinduced electrons and hot-exciton production in ZIS and MNZIS-5.

Fig. 7. (a) In-situ DRIFTS of MNZIS-5. (b) Reaction pathways of 4-MBA oxidation on Mo2N and Mo2N/ZIS by DFT calculation. (c) Schematic illustration of H2 and 4-MBAL production over Mo2N/ZIS.

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Mo₂N QDs/ZnIn₂S₄异质结中的等离激元-激子-声子协同作用实现光生电子与空穴的同步高值化利用

Simultaneous value-added utilization of photogenerated electrons and holes via plasmon-exciton-phonon synergy in Mo₂N QDs/ZnIn₂S₄ heterojunction

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