A Self-Sufficient Photocatalytic CO2 Reduction over Ionic Liquid-Modified Three-Dimensional-Printed Pt Single-Atom TiO2 Nanosheets

IF 7.1 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Chemistry of Materials Pub Date : 2026-10-13 Epub Date: 2026-09-23 DOI:10.1021/acs.chemmater.6c01235

Hamza Majeed Ansari, Kaleem Ullah, Sana Karamat, Yu-Peng Han, Dhandapani Kuzhandaivel, Zul Qarnain, Sohail Mumtaz, Ateeq Ur Rehman Baloch, Amir Said

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引用次数: 0

Abstract

The photocatalytic carbon dioxide reduction reaction (CO₂RR) offers a promising route to convert waste CO₂ into valuable synthetic fuels and chemicals using solar energy. However, practical application is hindered by insufficient charge separation, weak CO₂ activation, and poor catalyst recoverability. Herein, we systematically synthesized a self-sufficient photocatalyst comprising ionic liquid (IL)-modified Pt single atoms on TiO₂ nanosheets, fabricated in both powder (IL-Pt/TiO₂) and 3D-printed monolithic (3D-IL-Pt/TiO₂) forms. In the photocatalytic CO₂RR, the 3D-IL-Pt/TiO₂ exhibits a significantly enhanced CO evolution rate of 2051.46 μmol g^–1 h^–1, significantly higher than that of the powder sample (1598.79 μmol g^–1 h^–1) and far exceeding the sum of the individual constituents without additional cocatalysts. The spectroscopic analysis reveals that while the IL alone does not perturb the TiO₂ lattice, its combination with atomically dispersed Pt induces a strong interfacial electronic redistribution. This synergistic interaction of IL and Pt atoms stabilizes surface Ti³⁺ species and electron-rich Pt sites and modifies the surface oxygen environment without degrading the bulk structure of TiO₂. Notably, the system functions most effectively without external photosensitizers, which otherwise compete for light absorption and promote charge recombination. Long-term stability tests reveal that the 3D-printed monolith retained stable performance over extended cycling, whereas the powder material gradually deactivated. These findings demonstrate that optimized interfacial electronic regulation, rather than extreme band-edge position, governs photocatalytic efficiency, offering a strategy for scalable solar-driven CO₂ conversion.

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离子液体修饰的三维印刷Pt单原子tio2纳米片上的自光催化CO2还原

光催化二氧化碳还原反应（CO2RR）为利用太阳能将二氧化碳转化为有价值的合成燃料和化学品提供了一条有前途的途径。然而，由于电荷分离不充分、CO2活化弱、催化剂可恢复性差，阻碍了其实际应用。本文中，我们系统地合成了一种自给自足的光催化剂，包括离子液体（IL）修饰的Pt单原子在TiO2纳米片上，以粉末（IL-Pt/TiO2）和3d打印的单片（3D-IL-Pt/TiO2）形式制备。在光催化CO2RR中，3D-IL-Pt/TiO2的CO析出速率为2051.46 μmol g-1 h-1，显著高于粉末样品（1598.79 μmol g-1 h-1），且远高于未添加辅助催化剂的单个组分的总和。光谱分析表明，虽然单独的IL不会扰乱TiO2晶格，但它与原子分散的Pt的结合诱导了强烈的界面电子重分布。IL和Pt原子的协同作用稳定了表面Ti3+物质和富电子Pt位，改变了表面氧环境，而不降低TiO2的整体结构。值得注意的是，该系统在没有外部光敏剂的情况下最有效地工作，否则会竞争光吸收并促进电荷重组。长期稳定性测试表明，3d打印的单体在长时间循环中保持稳定的性能，而粉末材料逐渐失活。这些发现表明，优化的界面电子调节，而不是极端的带边位置，控制光催化效率，为可扩展的太阳能驱动的二氧化碳转换提供了一种策略。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Chemistry of Materials 工程技术-材料科学：综合

CiteScore

14.10

自引率

5.80%

发文量

929

审稿时长

1.5 months

期刊介绍： The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.