酞菁铁纳米片在染料敏化光催化体系中实现高效、高选择性CO2转化

doi:10.1016/S1872-2067(26)65061-9

催化学报 ›› 2026, Vol. 86: 350-362.DOI: 10.1016/S1872-2067(26)65061-9

酞菁铁纳米片在染料敏化光催化体系中实现高效、高选择性CO₂转化

高华^a, 朱勇^a, 温志兵^a, 赵冉^a, 陈治^a, 王思瑶^a, 何双霖^a, 彭况^a, 唐逸文^a, 孙立成^a^,^b, 李斐^a^,^*()

^a 大连理工大学化工学院, 精细化工全国重点实验室, 辽宁大连 116024
^b 西湖大学理学院, 人工光合作用与太阳能燃料中心, 浙江杭州 310024

收稿日期:2025-11-06 接受日期:2025-12-25 出版日期:2026-07-05 发布日期:2026-06-12
通讯作者: ^*电子信箱: lifei@dlut.edu.cn (李斐).
基金资助:
国家重点研发计划项目(2022YFA0911904);国家自然科学基金(22572015);国家自然科学基金(22302028);中央高校基本科研业务费(DUT23LAB611);中央高校基本科研业务费(DUT25Z2704);中央高校基本科研业务费(DUT24BS047);辽宁省自然科学基金计划博士科研启动项目(2023-BSBA-067)

Efficient and selective photocatalytic CO₂ conversion enabled by FePc nanosheets in a dye-sensitized system

Hua Gao^a, Yong Zhu^a, Zhibing Wen^a, Ran Zhao^a, Zhi Chen^a, Siyao Wang^a, Shuanglin He^a, Kuang Peng^a, Yiwen Tang^a, Licheng Sun^a^,^b, Fei Li^a^,^*()

^a State Key Laboratory of Fine Chemicals, Frontier Science Center for Smart Material, Dalian University of Technology, Dalian 116024, Liaoning, China
^b Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, Hangzhou 310024, Zhejiang, China

Received:2025-11-06 Accepted:2025-12-25 Online:2026-07-05 Published:2026-06-12
Supported by:
National Key R&D Program of China(2022YFA0911904);National Natural Science Foundation of China(22572015);National Natural Science Foundation of China(22302028);Fundamental Research Funds for the Central Universities(DUT23LAB611);Fundamental Research Funds for the Central Universities(DUT25Z2704);Fundamental Research Funds for the Central Universities(DUT24BS047);Liaoning Provincial Natural Science Foundation Joint Fund (Doctoral Research Start-up Project)(2023-BSBA-067)

摘要/Abstract

摘要：

光催化CO₂还原利用太阳能将温室气体转化为高附加值燃料和化学品, 是实现碳中和目标的重要途径. 金属酞菁(MPc)材料凭借其明确的M-N₄活性中心和可调的电子结构, 在CO₂还原反应中展现出良好潜力. 然而, 传统块体MPc由于强烈的π-π堆积作用, 导致活性位点可及性低、电子传输效率受限, 制约了其在分散体系中的实际应用. 受自然光合作用中光捕获与催化中心精确空间组织的启发, 构建仿生异质界面成为提升光催化性能的有效策略.

本研究设计并构建了一种三元复合光催化体系RuP-TiO₂-FePc NSs. 首先通过液相超声剥离法制备了超薄酞菁铁纳米片(FePc NSs), 该二维结构显著增加了活性位点暴露并促进了传质过程. 采用两步组装策略: 通过静电作用将FePc NSs负载于TiO₂表面, 随后通过磷酸基团的强配位作用将三联吡啶钌染料(RuP)锚定在TiO₂上, 构筑界面紧密结合、电子传输高效的三元复合光催化剂. 透射电镜、原子力显微镜、X-射线光电子能谱、紫外-可见光光谱等表征结果证实了FePc NSs的成功剥离及其在TiO₂表面的均匀分散, 同时Fe-N₄活性中心的结构完整性得以保持. 光催化性能测试结果表明, 在优化反应条件下, 含1 wt% FePc NSs的RuP-TiO₂-FePc NSs复合材料表现出卓越的CO₂还原性能: CO生成速率达到27.3 mmol g^-1 h^-1, CO选择性超过98%并且在40 h连续光照下活性保持稳定; 经过10次循环(总计100 h)测试后, CO周转数(TON)达到1363, 展现出优异的稳定性. 控制实验及¹³CO₂同位素示踪实验证实产物CO完全来源于CO₂还原. 机理研究揭示了TiO₂在该体系中的双重功能: 既作为分子支架空间组织光敏剂与催化剂以缩短电子传输距离, 又作为半导体桥梁提供高效半导体电荷传输通道. 时间分辨荧光光谱表明电子转移遵循氧化淬灭机制, 存在RuP*→TiO₂→FePc NSs与RuP*→FePc NSs两种并行路径. 原位傅里叶变换红外光谱监测到了关键反应中间体*COOH的特征吸收峰, 结合氘代同位素效应实验, 表明*COOH的质子耦合电子转移过程在反应的决速阶段中发挥了重要作用. 基于上述结果, 提出了完整的催化循环机理: 光激发RuP产生RuP*, 通过氧化淬灭路径将电子传递至FePc NSs; 富电子的FePc NSs活化CO₂, 经*COOH中间体通过多步质子耦合电子转移最终生成CO; 氧化的RuP⁺被BIH还原再生, 完成催化循环.

综上, 本研究通过整合二维材料剥离与界面异质化策略, 成功构建了高效、稳定、高选择性的染料敏化光催化CO₂还原体系. 该工作不仅阐明了多组分异质体系中的协同增强机制, 而且为设计开发高性能人工光合系统提供了新思路, 对推动太阳能驱动CO₂资源化利用的实际应用具有重要参考价值.

关键词: 二氧化碳还原, 酞菁铁纳米片, 染料敏化光催化, 电子转移, 人工光合成

Abstract:

Solar-driven photocatalytic CO₂ conversion offers a sustainable solution for greenhouse gas mitigation and renewable energy storage. While metal phthalocyanines (MPc) exhibit excellent CO₂ reduction capabilities, their practical application in dispersed photocatalytic systems faces limitations of the stacking of MPc molecules that reduces active site accessibility, and inefficient electron transfer limited by diffusive mass transport. To address these challenges, we developed a bioinspired dye-sensitized RuP-TiO₂-FePc nanosheets (NSs) hybrid system, where ultrathin FePc NSs obtained by liquid-phase ultrasonic exfoliation enhance active site exposure and mass transfer, while TiO₂ serves as a mediator to facilitate electron transfer between the photosensitizer and FePc NSs. Time-resolved spectroscopic studies demonstrate that TiO₂ plays a dual role: it spatially organizes functional components to enable surface electron transfer by shortening intermolecular distances, while also functioning as a semiconductor bridge to facilitate charge transport. This synergistic design achieves a remarkable CO production rate of 27.3 mmol g^-1 h^-1 (> 98% selectivity) and exceptional stability (TON_CO = 1363 over 100 h), outperforming many noble-metal-based systems. Our work demonstrates a robust strategy for optimizing bulk catalysts through 2D exfoliation and controlled heterogenization, offering a versatile platform for efficient and durable artificial photosynthesis.

Key words: CO₂ reduction, FePc nanosheets, Dye-sensitized photocatalysis, Electron transfer, Artificial photosynthesis

高华, 朱勇, 温志兵, 赵冉, 陈治, 王思瑶, 何双霖, 彭况, 唐逸文, 孙立成, 李斐. 酞菁铁纳米片在染料敏化光催化体系中实现高效、高选择性CO₂转化[J]. 催化学报, 2026, 86: 350-362.

Hua Gao, Yong Zhu, Zhibing Wen, Ran Zhao, Zhi Chen, Siyao Wang, Shuanglin He, Kuang Peng, Yiwen Tang, Licheng Sun, Fei Li. Efficient and selective photocatalytic CO₂ conversion enabled by FePc nanosheets in a dye-sensitized system[J]. Chinese Journal of Catalysis, 2026, 86: 350-362.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65061-9

https://www.cjcatal.com/CN/Y2026/V86/I7/350

图/表 9

Scheme 1. Evolution of photocatalytic systems from natural photosynthesis to artificial interfaces. The schematic illustrates the progression from natural photosynthetic systems to "soft interface" vesicle systems and then to "hard interface" TiO2 systems, highlighting the key advantages of the latter. SED stands for sacrificial electron donor.

Scheme 2. Schematic illustration of photocatalytic CO2 reduction over RuP-TiO2-FePc NSs under light irradiation.

Fig. 1. TEM images of multi-layer stacked B-FePc (a) and FePc NSs (b). (c) Tyndall effect observed in a colloidal solution of FePc NSs. (d) HAADF-STEM image and corresponding EDS elemental mapping of FePc NSs. (e) AFM image of FePc NSs. UV-vis spectra (f), FT-IR spectra (g), and Raman spectra (h) of B-FePc and FePc NSs.

Fig. 2. (a) TEM and HRTEM images of TiO2-FePc NSs. (b) The corresponding EDS mapping of TiO2-FePc NSs. UV-vis spectra (c), FT-IR spectra (d), and Raman spectra (e) of TiO2 and TiO2-FePc NSs.

Fig. 3. (a) XPS survey spectra of TiO2-FePc NSs. (b) Fe 2p of FePc and TiO2-FePc NSs. C 1s (c), N 1s (d), O 1s (e), and Ti 2p (f) spectra of TiO2-FePc NSs.

Fig. 4. Photocatalytic CO2 reduction performance under illumination (λLED = 450 nm, 5 mg samples, 25 mmol L-1 BIH, 0.1 mol L-1 phenol). (a) RuP-TiO2-FePc NSs (1 wt%) with different H+. (b) Time dependent products yield of CO2 reduction with different systems: heterogeneous (Hete) system of RuP-TiO2-FePc NSs (1 wt%) and semi-homogeneous (Homo) system of [Ru(bpy)3]Cl2·6H2O and FePc NSs with the same molar amounts as Hete. CO2 reduction performance of RuP-TiO2-FePc NSs (1 wt%) under both long-term continuous (c) and multiple cycling illumination (d) conditions.

Fig. 5. Transient photocurrent response (a) and EIS Nyquist plots (b) of RuP-TiO2 and RuP-TiO2-FePc NSs. TRPL lifetime spectra in DMF of RuP-Al2O3, RuP-TiO2, RuP-TiO2-FePc NSs, RuP-TiO2-FePc NSs + BIH (c) and RuP-Al2O3, RuP-Al2O3-FePc NSs (d). Transient absorption spectroscopy measurements of ground-state bleach recovery kinetics for RuP monitored at 450 nm in DMF: RuP-TiO2-FePc NSs (e), and RuP-TiO2-FePc NSs + BIH (f). The transient traces were analyzed using a triple-exponential decay model (Table S5, τ = ∑ Biτi2/∑ Biτi).

Fig. 6. In-situ FT-IR spectra of RuP-TiO2-FePc NSs during photocatalytic CO2 reduction.

Scheme 3. Schematic illustration of possible mechanism for CO2-to-CO conversion in a ternary hybrid system (RuP-TiO2-FePc NSs).

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酞菁铁纳米片在染料敏化光催化体系中实现高效、高选择性CO₂转化

Efficient and selective photocatalytic CO₂ conversion enabled by FePc nanosheets in a dye-sensitized system

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