单层硫化铟锌纳米片锌空位锚定银团簇用于高效双功能光催化

doi:10.1016/S1872-2067(26)65246-1

催化学报 ›› 2027, Vol. 92: 285-299.DOI: 10.1016/S1872-2067(26)65246-1

单层硫化铟锌纳米片锌空位锚定银团簇用于高效双功能光催化

杨利芳^a,1, 张雨格^b,1, 刘勇^c,*, 杨治军^a, 李广慧^a, 周建伟^a, 孟苏刚^b,*, Raf Dewil^c,d

^a新乡学院化学与材料工程学院, 河南新乡 453000, 中国;
^b淮北师范大学化学与化工学院, 绿色精准合成化学与应用教育部重点实验室, 安徽淮北 235000, 中国;
^c荷语鲁汶大学化学工程系, 过程与环境技术实验室, 圣卡特莱娜瓦弗, 比利时;
^d牛津大学工程科学系, 牛津, 英国

收稿日期:2026-05-31 接受日期:2026-07-27 出版日期:2027-01-18 发布日期:2026-10-30
通讯作者: *电子信箱: liuyong0781@outlook.com (刘勇), sgmeng@chnu.edu.cn (孟苏刚).
作者简介:¹共同第一作者.
基金资助:
国家自然科学基金(52002142); 安徽省学科/专业带头人计划(DTR2025015); 绿色和精准合成化学及应用教育部重点实验室自主课题(KLGPSCA202502); 河南省自然科学基金(252300421938, 262300420253); 河南省重点研发专项(252102520006);河南省研究生教育改革与质量提升工程(YJS2025GZZ53).

Zn vacancy-anchored Ag clusters on single-unit-cell ZnIn₂S₄ nanosheets for efficient dual-function photocatalysis

Lifang Yang^a,1, Yuge Zhang^b,1, Yong Liu^c,*, Zhijun Yang^a, Guanghui Li^a, Jianwei Zhou^a, Sugang Meng^b,*, Raf Dewil^c,d

^aSchool of Chemistry and Materials Engineering, Xinxiang University, Xinxiang 453000, Henan, China;
^bKey Laboratory of Green and Precise Synthetic Chemistry and Applications, Ministry of Education; School of Chemistry and Chemical Engineering, Huaibei Normal University, Huaibei 235000, Anhui, China;
^cLaboratory of Chemical and Biochemical Reactor Engineering and Safety, Department of Chemical Engineering, KU Leuven, J. De Nayerlaan 5, 2860 Sint-Katelijne-Waver, Belgium;
^dDepartment of Engineering Science, University of Oxford, Parks Road, Oxford OX1 3PJ, United Kingdom

Received:2026-05-31 Accepted:2026-07-27 Online:2027-01-18 Published:2026-10-30
Contact: *E-mail: liuyong0781@outlook.com (Y. Liu), sgmeng@chnu.edu.cn (S. Meng).
Supported by:
National Natural Science Foundation of China (52002142), the Funding Program for Leading scholar of Anhui Province (DTR2025015), the Foundation of Key Laboratory of Green and Precise Synthetic Chemistry Applications (KLGPSCA202502), the Natural Science Foundation of Henan Province (252300421938, 262300420253), the Key Specialized Research and Development Breakthrough in Henan province (252102520006), and the Postgraduate Education Reform and Quality Improvement Project of Henan Province (YJS2025GZZ53).

摘要/Abstract

摘要： 在大气CO₂浓度持续上升引发全球气候危机的背景下, 开发高效的人工光合成系统以实现碳中和具有重要意义. 传统的CO₂还原或析氢反应往往依赖牺牲剂来消耗空穴, 这不仅造成了光生载流子能量的浪费, 还增加了成本. 相比之下, 将还原半反应与高附加值有机物的选择性氧化耦合, 构建双功能光催化体系, 能同步实现能源转化与精细化学品合成, 展现出极高的经济性和应用前景. 然而, 如何设计能在复杂氧化还原环境中高效分离电荷并驱动多步电子转移的催化剂仍是巨大挑战. 本文通过缺陷工程与金属团簇的协同设计, 为解决光生载流子复合快、表面反应能垒高的问题提供了全新的解决方案.
本文创新性地构筑了具有单胞层厚度(约2.39 nm)的Ag/ZnIn₂S₄-V_zn(Ag/ZIS-V_zn)纳米片, 并阐明了锌空位(V_zn)作为高亲和力位点锚定金属Ag团簇的调控机制. 在设计思路上, 利用水热法制备富含锌空位的单层ZIS, 随后通过简单的静电吸附工艺将Ag团簇精准固载. 表征结果显示, 由于Ag⁺ (115 pm)的离子半径大于Zn²⁺(74 pm), Ag的引入导致了ZIS晶格的膨胀, X-射线衍射峰出现明显左移, 而Raman光谱中233 cm¹处出现的新峰则证实了Ag–S键的形成. 结果表明, 1%Ag/ZIS-V_zn表现出最佳活性: 在苯甲醇氧化耦合析氢体系中, 产氢速率达到33.6 mmol·g^–1·h^–1, 是纯ZIS的5.2倍; 在引入CO₂的体系中, CO产率达15.87 μmol·g^–1·h^–1, 且伴随高收率的苯甲醛和氢化安息香生成. 更显著的是, 该催化剂在18次循环测试中表现出卓越的稳定性, 甚至由于光诱导下的非对称欧姆接触优化, 活性随循环次数增加而稳步提升. 密度泛函理论计算证实, V_zn显著增强了Ag团簇的结合能(从4.18提至7.17 eV), 避免了团簇聚集. 功函数分析显示, Ag (4.26 eV)与ZIS-V_zn (5.22 eV)之间形成了内建电场, 驱动电子从ZIS流向Ag团簇. 瞬态光电流、电化学阻抗谱及时间分辨荧光光谱寿命测试(从0.79延长至0.89 ns)共同证明了这种空间分离机制抑制了电荷复合. 原位X-射线光电子能谱揭示了光照下Zn、In、S能级向高能位移而Ag向低能位移, 直接捕获了电荷定向迁移的信号. 在表面催化动力学上, Ag团簇不仅作为电子陷阱, 还通过协同效应将CO₂还原中生成COOH*中间体的能垒从0.42降至0.10 eV. 同时, 原位漫反射红外光谱捕捉到了CHO*和COOH*等关键中间体, 而电子顺磁共振探测到的DMPO-^•CH(OH)Ph自由基信号则证实了空穴介导的苯甲醇α-H提取过程. 这种多尺度的协同优化, 确保了催化剂在复杂双功能反应中的高效性.
综上, 本研究成功阐明了原子级缺陷与金属团簇之间的相互作用逻辑, 证明了通过界面电场和能垒工程可以精准操控复杂的氧化还原流向, 不仅为构筑单胞层厚度的高性能光催化剂提供了理论支撑, 也为未来设计低成本、高耐用性的太阳能转化系统开辟了新途径, 对推动绿色化学合成与能源可持续发展具有深远影响.

关键词: 光催化, 双功能, 苯甲醇氧化, 制氢, 二氧化碳还原

Abstract: Dual-function photocatalysis coupling reduction reactions with organic selective oxidation offers a sustainable strategy for energy and environmental challenges. Herein, we demonstrate a rational design of ultrathin, one-unit-cell Ag/ZnIn₂S₄-V_Zn (Ag/ZIS-V_Zn) nanosheets, featuring zinc vacancies (V_Zn) as high-affinity anchoring sites for Ag clusters. This unique configuration promotes ohmic contact between Ag clusters and the V_Zn-rich ZnIn₂S₄ substrate. Combined experiments, in situ characterizations, and theoretical studies reveal that this Ag-V_Zn coupling fundamentally reconfigures the charge-carrier dynamics, ensuring efficient spatial decoupling and establishing an optimized landscape for surface catalysis. Consequently, the Ag/ZIS-V_Zn architecture exhibits exceptional bifunctional performance for the selective oxidative valorization of phenylcarbinol into value-added chemicals, concurrently coupled with efficient hydrogen evolution, outperforming the reference benchmarks of ZIS, Ag/ZIS and ZIS-V_Zn. Remarkably, the integration of CO₂ into the photocatalytic system enables a tandem process, coupling phenylcarbinol oxidation with CO₂ photoreduction. This synergy is underpinned by strengthened CO₂ adsorption and a lowered energy barrier for the rate-limiting formation of *COOH intermediate. Furthermore, 1%Ag/ZIS-V_Zn exhibits outstanding durability, retaining performance over 18 cycles. By elucidating the cooperative mechanism between metal vacancies and anchored clusters, this study establishes a design blueprint for high-performance, durable photocatalysts capable of steering complex, multi-component solar-driven transformations.

Key words: Photocatalysis, Dual-function, Phenylcarbinol oxidation, H₂ production, CO₂ reduction

杨利芳, 张雨格, 刘勇, 杨治军, 李广慧, 周建伟, 孟苏刚, Raf Dewil. 单层硫化铟锌纳米片锌空位锚定银团簇用于高效双功能光催化[J]. 催化学报, 2027, 92: 285-299.

Lifang Yang, Yuge Zhang, Yong Liu, Zhijun Yang, Guanghui Li, Jianwei Zhou, Sugang Meng, Raf Dewil. Zn vacancy-anchored Ag clusters on single-unit-cell ZnIn₂S₄ nanosheets for efficient dual-function photocatalysis[J]. Chinese Journal of Catalysis, 2027, 92: 285-299.

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单层硫化铟锌纳米片锌空位锚定银团簇用于高效双功能光催化

Zn vacancy-anchored Ag clusters on single-unit-cell ZnIn₂S₄ nanosheets for efficient dual-function photocatalysis

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单层硫化铟锌纳米片锌空位锚定银团簇用于高效双功能光催化

Zn vacancy-anchored Ag clusters on single-unit-cell ZnIn2S4 nanosheets for efficient dual-function photocatalysis

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Zn vacancy-anchored Ag clusters on single-unit-cell ZnIn₂S₄ nanosheets for efficient dual-function photocatalysis