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Interstitial carbon-platinum electronic metal-support interaction structure boost synergistic removal of O3 and CH3SH via surface atomic oxygen
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2023-03-05 , DOI: 10.1016/j.apcatb.2023.122578
Dingren Ma , Jing Cao , Kairui Liu , Yexing Zhang , Qiwen Liang , Yajing Huang , Xinyi Guan , Lingling Hu , Chun He , Dehua Xia

Carbon atoms in the interstitial sites of metal nanoparticles have strong influence on heterogeneous catalysis via electronic metal-support interactions (EMSI). Here, the Pt catalysts with interstitial C-Pt EMSI structures were first developed and identified to boost the removal of ozone (O3) and methyl mercaptan (CH3SH). Experimental results showed that the intrinsic activity of the catalysts with low Pt loading (wt%, 0.95 %) was 186 times higher than that of commercial MnO2. This excellent catalytic performance was attributed to dual-site catalytic structures to promote the adsorption/activation of O3 at interstitial C and capture/oxidation of CH3SH at Pt simultaneously. More importantly, the interstitial C sites retained surface atomic oxygen (*O) with excellent reactivity and lowered the energy barrier of Csingle bondS bond breakage, thus achieving efficient decomposition of CH3SH into CO2/SO42-. This work provides high-performance catalysts and new mechanistic insights for the synergistic control of O3 and CH3SH.



中文翻译:

间隙碳-铂电子金属-载体相互作用结构促进表面原子氧协同去除O3和CH3SH

金属纳米粒子间隙位点中的碳原子通过电子金属-载体相互作用 (EMSI) 对多相催化产生强烈影响。在这里,首先开发并鉴定了具有间隙 C-Pt EMSI 结构的 Pt 催化剂,以促进臭氧 (O 3 ) 和甲硫醇 (CH 3 SH)的去除。实验结果表明,低Pt负载量(wt%,0.95%)催化剂的本征活性是商业MnO 2的186倍。这种优异的催化性能归因于双中心催化结构,以促进O 3在间隙C处的吸附/活化和CH 3的捕获/氧化同时在 Pt 的 SH。单键更重要的是,间隙C位保留了具有优异反应活性的表面原子氧(*O),降低了C -S键断裂的能垒,从而实现了CH 3 SH高效分解为CO 2 /SO 4 2-这项工作为 O 3和 CH 3 SH的协同控制提供了高性能催化剂和新的机理见解。

更新日期:2023-03-07
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