直接Z-scheme光催化复合体系: 金属有机卟啉笼负载于g-C3N4中以增强光解水产氢活性

doi:10.1016/S1872-2067(22)64109-3

催化学报 ›› 2022, Vol. 43 ›› Issue (8): 2249-2258.DOI: 10.1016/S1872-2067(22)64109-3

直接Z-scheme光催化复合体系: 金属有机卟啉笼负载于g-C₃N₄中以增强光解水产氢活性

雷洋, 黄剑锋, 李鑫奥, 吕楚滢, 侯超苹, 刘军民()

中山大学材料科学与工程学院, 低碳化学与能量存储广东省重点实验室, 广东广州510275

收稿日期:2022-02-23 接受日期:2022-04-15 出版日期:2022-08-18 发布日期:2022-06-20
通讯作者: 刘军民
基金资助:
国家自然科学基金(21975291);国家自然科学基金(21572280);广东省自然科学基金(2019A1515011640);广东省自然科学基金(2022A1515011949);广东省自然科学基金(2020A1515110474);广东省自然科学基金(2018A030313479)

Direct Z-scheme photochemical hybrid systems: Loading porphyrin-based metal-organic cages on graphitic-C₃N₄ to dramatically enhance photocatalytic hydrogen evolution

Yang Lei, Jian-Feng Huang, Xin-Ao Li, Chu-Ying Lv, Chao-Ping Hou, Jun-Min Liu()

The Key Laboratory of Low-Carbon Chemistry & Energy Conservation of Guangdong Province, School of Materials Science and Engineering, Sun Yat-sen University, Guangzhou 510275, Guangdong, China

Received:2022-02-23 Accepted:2022-04-15 Online:2022-08-18 Published:2022-06-20
Contact: Jun-Min Liu
Supported by:
National Natural Science Foundation of China(21975291);National Natural Science Foundation of China(21572280);Natural Science Foundation of Guangdong Province(2019A1515011640);Natural Science Foundation of Guangdong Province(2022A1515011949);Natural Science Foundation of Guangdong Province(2020A1515110474);Natural Science Foundation of Guangdong Province(2018A030313479)

摘要/Abstract

摘要：

氢能作为一种环境友好、可再生和无碳的能源一直受到广泛关注. 光催化技术将太阳能转换为氢能, 成为了实现太阳能转化的有效方式, 而决定其转化效率的关键是光催化剂. 目前为止, 多种光催化剂已被用于光催化制氢. 金属有机笼(MOCs)是一种由有机配体和金属离子组成的离散配合物, 在诸多领域得到了广泛的研究, 但是其在光催化制氢方面受到的关注相对较少. 光敏性MOCs可将多种有机生色团和催化活性金属中心通过配位作用自组装形成笼状结构, 实现激发态电子从配体向催化中心的快速转移, 从而可用作光化学分子器件(PMDs). 一个完整的光催化制氢系统一般由质子还原催化剂、进行光捕获的光敏剂和电子供体三个部分组成. 而基于卟啉的光敏剂, 因其在可见光区域的优异光吸收能力、较强电子转移能力以及通过改变中心配位金属以调控光电性质等特点, 在光催化制氢方面引起了众多兴趣. 因此, 基于卟啉光敏剂的MOCs在光催化制氢方面具有较好的应用前景, 但是目前报道较少. 在均相催化过程中, 大多数基于MOC的光催化剂容易失活, 难以回收, 在水中稳定性差. 本文通过将MOC固定于半导体g-C₃N₄中, 制备了新型Z-scheme异质结构光催化剂, 提高了复合材料光生载流子的分离效率, 同时使材料整体有较高的氧化还原效率, 进而提高光催化活性.

通过金属卟啉M-TPyP分子与Pd²⁺催化中心的自组装, 合成了一系列Pd₆L₃型超分子笼MOC-Py-M (M = H, Cu, Zn), 通过核磁和质谱对其结构进行了表征, 并将其用于光催化分解水产氢. 在卟啉基光敏MOC中, 卟啉配体直接与Pd催化中心相连, 在光激发下可以实现光敏剂的光生电子向催化中心的快速转移. 通过将金属有机笼MOC-Py-M与g-C₃N₄结合, 制备成复合材料MOC-Py-M/g-C₃N₄ (M = H, Cu, Zn), 抑制了均相催化过程中常出现的MOC催化剂的失活和降解. 此外, g-C₃N₄, MOC-Py-M (M = H, Cu, Zn)与相应复合材料的红外吸收光谱测试表明, 在复合材料中g-C₃N₄和相应的MOC-Py-M (M = H, Cu, Zn)之间存在较强的π-π相互作用. 在可见光照射下(λ > 420 nm), MOC-Py-Zn/g-C₃N₄的制氢速率(10348 μmol g^‒1 h^‒1)最高, 分别是MOC-Py-H/g-C₃N₄和MOC-Py-Cu/g-C₃N₄光解水制氢速率的27.1倍和9.4倍, 这可归因于MOC-Py-Zn有更好的可见光吸收性能. 另外, 在相同的测试条件下, g-C₃N₄, MOC-Py-Zn和ZnTPyP-Pd-g-C₃N₄均展现了更低的催化活性. 在100 h长期稳定产氢测试中, MOC-Py-M/g-C₃N₄复合材料基于分子笼摩尔数的TON_MOC-Py-Zn = 32616, 远高于均相催化剂MOC-Py-Zn的TON_MOC-Py-Zn = 507. 这说明相比于纯分子笼, 复合材料表现出更高的制氢活性和稳定性. 研究表明, g-C₃N₄除了可分散MOC, 使其在反应过程中不易聚集; 同时可保护MOC, 防止其在光催化中结构坍塌, 从而提高了其稳定性; 另外, g-C₃N₄还起着电子给体的作用, 利用Z-scheme电子转移机制, 可将其光生电子注入到MOC中, 从而抑制了光生电子和空穴的复合, 拓展了材料的可见光响应范围, 进而提升了其光催化性能.

根据MOC-Py-M (M = H, Cu, Zn)和g-C₃N₄的电位结构, 理论上存在两种类型的异质结构, 即type II和Z-scheme. 为了验证Z-scheme构型的电子转移机制, 通过稳态光致发光光谱进行羟基自由基(•OH)定量实验, 以比较羟基自由基浓度的变化. 使用TA作为•OH捕获剂, TA遇到•OH后会生成一种强荧光物质—羟基对苯二甲酸TA-OH. 稳态光致发光光谱表明, 复合材料为Z-scheme电子传递机理: 在可见光激发下, 复合材料中各组分的电子转移方向为g-C₃N₄的光生电子转移到了MOC-Py-M (M = H, Cu, Zn). 各组分的稳态荧光和时间分辨荧光衰减光谱进一步证明, MOC-Py-M (M = H, Cu, Zn)已成功地与g-C₃N₄复合, 光生电荷的快速分离是MOC-Py-M/g-C₃N₄复合材料光催化活性增强的主要原因之一. 综上, 本文为设计合成高效稳定的光催化剂提供了一种新思路.

关键词: 卟啉金属有机笼, g-C₃N₄, 光化学分子器件, 直接Z-scheme异质结构, 光催化水制氢

Abstract:

The rational design of photochemical molecular device (PMD) and its hybrid system has great potential in improving the activity of photocatalytic hydrogen production. A series of Pd₆L₃type metal-organic cages, denoted as MOC-Py-M (M = H, Cu, and Zn), are designed for PMDs by combining metalloporphyrin-based ligands with catalytically active Pd²⁺ centers. These metal-organic cages (MOCs) are first successfully hybridized with graphitic carbon nitride (g-C₃N₄) to form direct Z-scheme heterogeneous MOC-Py-M/g-C₃N₄ (M = H, Cu, and Zn) photocatalysts via π-π interactions. Benefiting from its better light absorption ability, the MOC-Py-Zn/g-C₃N₄ catalyst exhibits high H₂ production activity under visible light (10348 μmol g^-1 h^-1), far superior to MOC-Py-H/g-C₃N₄ and MOC-Py-Cu/g-C₃N₄. Moreover, the MOC-Py-Zn/g-C₃N₄ system obtains an enhanced turn over number (TON) value of 32616 within 100 h, outperforming the homogenous MOC-Py-Zn (TON of 507 within 100 h), which is one of the highest photochemical hybrid systems based on MOC for visible-light-driven hydrogen generation. This confirms the direct Z-scheme heterostructure can promote effective charge transfer, expand the visible light absorption region, and protect the cages from decomposition in MOC-Py-Zn/g-C₃N₄. This work presents a creative example that direct Z-scheme PMD-based systems for effective and persistent hydrogen generation from water under visible light are obtained by heterogenization approach using homogeneous porphyrin-based MOCs and g-C₃N₄ semiconductors.

Key words: Porphyrin-based metal-organic cage, g-C3N4, Photochemical molecular device, Direct Z-scheme heterostructure, Photocatalytic hydrogen evolution, from water

雷洋, 黄剑锋, 李鑫奥, 吕楚滢, 侯超苹, 刘军民. 直接Z-scheme光催化复合体系: 金属有机卟啉笼负载于g-C₃N₄中以增强光解水产氢活性[J]. 催化学报, 2022, 43(8): 2249-2258.

Yang Lei, Jian-Feng Huang, Xin-Ao Li, Chu-Ying Lv, Chao-Ping Hou, Jun-Min Liu. Direct Z-scheme photochemical hybrid systems: Loading porphyrin-based metal-organic cages on graphitic-C₃N₄ to dramatically enhance photocatalytic hydrogen evolution[J]. Chinese Journal of Catalysis, 2022, 43(8): 2249-2258.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(22)64109-3

https://www.cjcatal.com/CN/Y2022/V43/I8/2249

图/表 10

Scheme 1. The chemical structure of TPyP and the construction of Pd-based cage MOC-Py-M (M = H, Cu, and Zn).

Fig. 1. The PXRD patterns of g-C3N4, MOC-Py-M/g-C3N4 and MOC-Py-M (M = H, Cu, and Zn).

Fig. 2. (a,b) SEM and TEM for g-C3N4. (c,d) SEM and TEM for MOC-Py-Zn/g-C3N4. (e) TEM elemental mapping images for MOC-Py-Zn/g-C3N4.

Fig. 3. (a) UV-vis absorption spectra of MOC-Py-M in ethanol solution. (b) UV-vis diffusion reflectance absorption spectra of MOC-Py-M/g-C3N4 (M = H, Cu, and Zn).

Fig. 4. H2 production curves of g-C3N4, MOC-Py-M, and MOC-Py-M/g-C3N4 (M = H, Cu, and Zn) (a), and g-C3N4, Pd/g-C3N4, ZnTPyP/g-C3N4, and ZnTPyP-Pd/g-C3N4 (b) in 100 mL H2O/TEOA (9:1, v/v) irradiated by a 300 W Xe lamp with a cut-off filter (λ > 420 nm).

Fig. 5. Photocurrent responses (a) and EIS Nyquist plots (b) of g-C3N4 and MOC-Py-M/g-C3N4 (M = Cu and Zn) with 0.2 V bias vs. Ag/AgCl under visible light illumination.

Fig. 6. (a) H2 production curves of MOC-Py-Zn and MOC-Py-Zn/g-C3N4 in 100 mL H2O/TEOA (9:1, v/v) under visible light irradiation (λ > 420 nm). (b) accumulated TONs and TOFs based on MOC-Py-Zn of MOC-Py-Zn and MOC-Py-Zn/g-C3N4 in 100 h.

Fig. 7. Schematic illustration for the separation and transfer of photoproduced charges in the MOC-Py-Zn/g-C3N4.

Fig. 8. (a) The Z-scheme electron transfer route for •OH generation of MOC-Py-Zn/g-C3N4. (b) PL spectra at 315 nm excitation for TA-OH produced by MOC-Py-Zn, g-C3N4, and MOC-Py-Zn/g-C3N4 in the presence of TA under visible light.

Fig. 9. PL spectra (a) and time-resolved PL decay curves (b) of g-C3N4, MOC-Py-Zn, and MOC-Py-Zn/g-C3N4 composites at 360 nm excitation.

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直接Z-scheme光催化复合体系: 金属有机卟啉笼负载于g-C₃N₄中以增强光解水产氢活性

Direct Z-scheme photochemical hybrid systems: Loading porphyrin-based metal-organic cages on graphitic-C₃N₄ to dramatically enhance photocatalytic hydrogen evolution

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