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

Nature Communications Pub Date : 2025-07-01 DOI:10.1038/s41467-025-60954-4

Yilin Jiang, Ruonan Xi, Jinlin Yin, Chen Sun, Yukong Li, Chao Wu, Chi Zhang, Honghan Fei

{"title":"A layered lead halide framework intercalated with Ru(bpy)3 for efficient CO2 photoreduction.","authors":"Yilin Jiang, Ruonan Xi, Jinlin Yin, Chen Sun, Yukong Li, Chao Wu, Chi Zhang, Honghan Fei","doi":"10.1038/s41467-025-60954-4","DOIUrl":null,"url":null,"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.","PeriodicalId":19066,"journal":{"name":"Nature Communications","volume":"16 1","pages":"5910"},"PeriodicalIF":14.7000,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12219702/pdf/","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Communications","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1038/s41467-025-60954-4","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}

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.

查看原文本刊更多论文

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。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

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.