Gu Huayu, Wang Fanyu, Chen Sai, Lan Jintong, Wang Jun, Pei Chunlei, Liu Xiao, Gong Jinlong
Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, 430079, China.
School of Chemical Engineering and Technology, Key Laboratory for Green Chemical Technology of Ministry of Education, Tianjin University, Tianjin, 300072, China.
Nat Commun. 2025 Jan 25;16(1):1008. doi: 10.1038/s41467-025-56281-3.
Precisely managing electron transfer pathways throughout the catalytic reaction is paramount for bolstering both the efficacy and endurance of catalysts, offering a pivotal solution to addressing concerns surrounding host structure destabilization and cycling life degradation. This paper describes the integration of B-Ni dual single-atoms within MnO channels to serve as an electronic reservoir to direct the electron transfer route during methane catalytic combustion. Comprehensive analysis discovers that B atoms weaken the interaction between O and Mn atoms by forming bonds with lattice oxygen atoms. Meanwhile, Ni atoms facilitate electron transfer to achieve the heightened activity of MnO. The B-Ni dual-sites instead of Mn (IV) could accommodate excess electrons generated during the reaction to inhibit the formation of high spin Mn (III) species, thereby hindering the Jahn-Teller distortion and maintaining the catalyst stability. This work demonstrates an effective modification strategy to substantially prolong the service life of MnO-based materials.
在整个催化反应过程中精确管理电子转移途径对于提高催化剂的效率和耐久性至关重要，这为解决围绕主体结构不稳定和循环寿命退化的问题提供了关键解决方案。本文描述了将B-Ni双单原子整合到MnO通道中，作为电子库以在甲烷催化燃烧过程中引导电子转移路径。综合分析发现，B原子通过与晶格氧原子形成键来削弱O和Mn原子之间的相互作用。同时，Ni原子促进电子转移以实现MnO活性的提高。B-Ni双位点而非Mn(IV)可以容纳反应过程中产生的过量电子，以抑制高自旋Mn(III)物种的形成，从而阻碍 Jahn-Teller 畸变并保持催化剂稳定性。这项工作展示了一种有效的改性策略，可大幅延长MnO基材料的使用寿命。
