华东理工大学张金龙团队报道了调节原子精确铂位促进甲烷光驱动干重整。相关研究成果于2024年8月12日发表于国际顶尖学术期刊《德国应用化学》。

甲烷的光驱动干重整是一种有前景且温和的方法，可以将两种温室气体转化为有价值的合成气。然而，开发原子精确地调节活性位点并实现平衡稳定的合成气生产的简单策略来仍然具有挑战性。

该文中，研究人员开发了一种空间限制方法来精确控制TiO₂表面上的铂物种，从单原子到纳米簇-。由单原子和亚纳米簇组成的结构会产生明显的电子-金属-载体相互作用，由此产生的界面状态会促使表面电荷重排。

这些原子-团簇组件的独特几何和电子性质有助于CH₄和CO₂的有效活化，加速中间偶联并最大限度地减少副反应。该催化剂表现出34.41 mol gPt^-1 h^-1的出色合成气生成率，具有优异的耐久性，在365 nm处显示出9.1%的表观量子产率和1289 h^-1的周转频率。

该项工作为在原子尺度上探索更多的多分子系统提供了深刻的理解。

附：英文原文

Title: Regulating Atomically-Precise Pt Sites for Boosting Light-Driven Dry Reforming of Methane

Author: Chengxuan He, Qixin Li, Zhicheng Ye, Lijie Wang, Yalin Gong, Songting Li, Jiaxin Wu, Zhaojun Lu, Shiqun Wu, Jinlong Zhang

Issue&Volume: 2024-08-12

Abstract: Light-driven dry reforming of methane is a promising and mild route to convert two greenhouse gas into valuable syngas. However, developing facile strategy to atomically-precise regulate the active sites and realize balanced and stable syngas production is still challenging. Herein, we developed a spatial confinement approach to precisely control over platinum species on TiO2 surfaces, from single atoms to nanoclusters. The configuration comprising single atoms and sub-nanoclusters engenders pronounced electronic metal-support interactions, with resultant interfacial states prompting surface charge rearrangement. The unique geometric and electronic properties of these atom-cluster assemblies facilitate effective activation of CH4 and CO2, accelerating intermediate coupling and minimizing side reactions. Our catalyst exhibits an outstanding syngas generation rate of 34.41 mol gPt-1 h-1 with superior durability, displaying high apparent quantum yield of 9.1% at 365 nm and turnover frequency of 1289 h-1. This work provides insightful understanding for exploring more multi-molecule systems at an atomic scale.

DOI: 10.1002/anie.202412308

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202412308