A layered lead halide framework intercalated with Ru(bpy)3 for efficient CO2 photoreduction.

IF 14.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Yilin Jiang, Ruonan Xi, Jinlin Yin, Chen Sun, Yukong Li, Chao Wu, Chi Zhang, Honghan Fei
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引用次数: 0

Abstract

Three-dimensional lead halide hybrids exhibit excellent photophysical properties but suffer from inherent instability. In contrast, two-dimensional layered lead halides offer enhanced environmental stability, yet their strongly bound excitons restrict efficient charge transport. Here we present a covalent intercalation strategy involving the benchmark photosensitizer [Ru(bpy)3]2+ into a layered lead halide framework, featuring cationic [Pb23X42]4+ (X- = Cl- or Br-) layers pillared by [Ru(bpy)3]2+ ligands via Pb2+-carboxylate coordination. This hybrid material achieves nearly full visible-light absorption and efficient photoinduced charge transfer from [Ru(bpy)3]2+ to the lead halide layers. This affords efficient CO2-to-CO photoreduction with an apparent quantum efficiency of ~3.0% at 500 nm, exceeding the performance of all previously reported organolead halide photocatalysts. Mechanistic studies indicate that the [Ru(bpy)3]2+ ligands enhance charge transport to Pb2+ sites, facilitating CO2 activation and reducing the reaction barrier for the *COOH intermediate. This work establishes a paradigm for intercalation chemistry in robust layered lead halide hybrids.

一种嵌入Ru(bpy)3的层状卤化铅框架,用于有效的CO2光还原。
三维卤化铅杂化物具有优异的光物理性能,但存在固有的不稳定性。相比之下,二维层状卤化铅提供了增强的环境稳定性,但它们的强束缚激子限制了有效的电荷传输。在这里,我们提出了一种共价插层策略,将基准光敏剂[Ru(bpy)3]2+插入到层状卤化铅框架中,其特征是阳离子[Pb23X42]4+ (X- = Cl-或Br-)层,由[Ru(bpy)3]2+配体通过Pb2+-羧酸盐配位支撑。该杂化材料实现了几乎完全的可见光吸收和高效的光诱导电荷从[Ru(bpy)3]2+转移到卤化铅层。这提供了有效的CO2-to-CO光还原,在500 nm处的表观量子效率为~3.0%,超过了所有先前报道的有机卤化铅光催化剂的性能。机理研究表明,[Ru(bpy)3]2+配体增强了电荷向Pb2+位点的传输,促进了CO2活化,降低了*COOH中间体的反应势垒。这项工作为坚固层状卤化铅杂化物的插层化学建立了一个范例。
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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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