Suppressing Jahn-Teller distortion of MnO2 via B-Ni dual single-atoms integration for methane catalytic combustion

IF 15.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Huayu Gu, Fanyu Wang, Sai Chen, Jintong Lan, Jun Wang, Chunlei Pei, Xiao Liu, Jinlong Gong
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引用次数: 0

Abstract

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 MnO2 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 MnO2. 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 MnO2-based materials.

Abstract Image

B-Ni双单原子集成抑制甲烷催化燃烧MnO2的Jahn-Teller畸变
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,为解决围绕宿主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B-Ni双单原子在MnO2通道内的集成,作为电子储层来指导甲烷催化燃烧过程中的电子转移路线。综合分析发现,B原子通过与晶格氧原子形成键来减弱O和Mn原子之间的相互作用。同时,Ni原子促进电子转移,实现MnO2活性的提高。B-Ni双位取代Mn (IV)可以容纳反应过程中产生的多余电子,抑制高自旋Mn (III)的形成,从而阻碍了Jahn-Teller畸变,保持了催化剂的稳定性。这项工作证明了一种有效的改性策略,可以大大延长二氧化锰基材料的使用寿命。
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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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