近日，浙江大学谢鹏飞团队报道了非对称双原子Ru锚定在氮化硼纳米层引发稳定干重整的机制转变。相关论文于2026年4月8日发表在《美国化学会志》上。

甲烷干重整是一种有望减少温室气体排放并将天然气转化为高附加值产品的技术途径。然而，该过程在低温下受到反应活性有限和严重积碳的挑战。

研究组报道了一种锚定在氮化硼纳米层中的双原子钌催化剂。钌原子对空间上差异化的配位环境使其活性中心具有不对称的电荷分布。Ru双原子的协同效应使其在650 °C下分别实现了69%和76%的CH₄与CO₂转化率，接近热力学平衡值，同时在600 °C下保持了1000小时的优异稳定性，且积碳可忽略不计。机理研究表明，缺电子的Ru位点通过增强的极化效应促进CH₄中的C–H键断裂，而另一个富电子的Ru位点则通过双齿吸附构型促进CO₂的活化。

此外，这种独特的双原子Ru结构使得反应遵循Langmuir-Hinshelwood路径，降低了CH₄与CO₂偶联反应生成*CH₂O中间体并产生合成气的能垒，从而避免了过度的C–C键形成和积碳。这项工作为设计多功能催化剂以解决甲烷干重整中反应活性与稳定性之间的跷跷板问题提供了新策略。

附：英文原文

Title: Asymmetric Dual-Atom Ru Anchored in Boron Nitride Nanolayer Triggers Mechanism Transition for Stable Dry Reforming

Author: Yani Zhang, Huibin Wang, Mingjia Zhang, Ning Cao, Ke Wang, Mi Yan, Xingwang Zhang, Pengfei Xie

Issue&Volume: April 8, 2026

Abstract: Methane dry reforming represents a promising approach to reduce greenhouse gas emissions and to utilize natural gas for value-added products. However, this process is challenged by limited reactivity and severe coking at low temperatures. Here, we report a dual-atom ruthenium catalyst anchored in a boron nitride nanolayer. The spatially distinct coordination of the Ru atomic pair gives rise to the asymmetric charge distribution of the active center. The synergy effect of Ru dimer achieves the CH4 and CO2 conversions of 69% and 76% at 650 °C, respectively, which are near thermodynamic equilibrium, while maintaining an exceptional stability of 1000 h at 600 °C with negligible coking. Mechanism studies reveal that an electron-deficient Ru site facilitates the C–H cleavage in CH4 via an enhanced polarization effect, while another electron-rich Ru site promotes CO2 activation with a bidentate adsorption configuration. Furthermore, this unique dual-atom Ru structure enables a Langmuir–Hinshelwood pathway with a reduced barrier of the coupling reaction between CH4 and CO2 to form *CH2O intermediate and produce syngas rather than excessive C–C binding and coke deposition. This work provides a strategy for designing multifunctional catalysts to solve the seesaw issue of reactivity and stability for methane dry reforming.

DOI: 10.1021/jacs.5c19260

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.5c19260