Size-Dependent Microwave Heating and Catalytic Activity of Fine Iron Particles in the Deep Dehydrogenation of Hexadecane.
Size-Dependent Microwave Heating and Catalytic Activity of Fine Iron Particles in the Deep Dehydrogenation of Hexadecane.
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DOI：
10.1021/acs.chemmater.2c00630
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发表时间：
2022-05-24
影响因子：
8.6
通讯作者：
Edwards, Peter P.
中科院分区：
文献类型：
--
作者：
Jie, Xiangyu;Chen, Roujia;Biddle, Tara;Slocombe, Daniel R.;Dilworth, Jonathan Robin;Xiao, Tiancun;Edwards, Peter P.
了解电磁微波辐射与固体物质的相互作用及其在活性催化部位的作用机理，将有助于更深入地了解微波引发的化学作用和过程，并将进一步优化这类多相催化。在这里，我们研究了微波辐射与固体铁催化剂相互作用以及模型烃十六烷深度脱氢的基本机理。我们发现，在这些非均相过程中，颗粒金属Fe电子从微波“反射体”到微波“吸收体”的尺寸相关电子跃迁是高效金属催化的核心。因此，用于高效微波引发脱氢反应的Fe金属催化剂的最佳粒径约为80-120 nm，其催化性能强烈依赖于工作频率下Fe粒子的平均半径与微波表面深度(r/δ)的比值。重要的是，所选择的铁催化剂的粒度最终将影响催化剂的基本加热性质，并决定性地影响其在微波引发下的催化性能。此外，我们还发现，当两种或两种以上的材料--以机械混合物的形式存在--同时暴露在微波辐射下时，每种组成材料都将独立地对微波做出反应。因此，两种材料之间的相互作用被发现具有协同效应，随后有助于加热和改善整体催化性能。
Knowledge of the electromagnetic microwave radiation–solid matter interaction and ensuing mechanisms at active catalytic sites will enable a deeper understanding of microwave-initiated chemical interactions and processes, and will lead to further optimization of this class of heterogeneous catalysis. Here, we study the fundamental mechanism of the interaction between microwave radiation and solid Fe catalysts and the deep dehydrogenation of a model hydrocarbon, hexadecane. We find that the size-dependent electronic transition of particulate Fe metal from a microwave “reflector” to a microwave “absorber” lies at the heart of efficient metal catalysis in these heterogeneous processes. In this regard, the optimal particle size of a Fe metal catalyst for highly effective microwave-initiated dehydrogenation reactions is approximately 80–120 nm, and the catalytic performance is strongly dependent on the ratio of the mean radius of Fe particles to the microwave skin depth (r/δ) at the operating frequency. Importantly, the particle size of selected Fe catalysts will ultimately affect the basic heating properties of the catalysts and decisively influence their catalytic performance under microwave initiation. In addition, we have found that when two or more materials—present as a mechanical mixture—are simultaneously exposed to microwave irradiation, each constituent material will respond to the microwaves independently. Thus, the interaction between the two materials has been found to have synergistic effects, subsequently contributing to heating and improving the overall catalytic performance.
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影响因子：
16.6
作者：
Liu B;Slocombe DR;Wang J;Aldawsari A;Gonzalez-Cortes S;Arden J;Kuznetsov VL;AlMegren H;AlKinany M;Xiao T;Edwards PP
通讯作者：
Edwards PP
影响因子：
37.8
作者：
Jie, Xiangyu;Li, Weisong;Edwards, Peter
通讯作者：
Edwards, Peter
影响因子：
4.6
作者：
Gonzalez-Cortes, S.;Slocombe, D. R.;Edwards, P. P.
通讯作者：
Edwards, P. P.
影响因子：
3.2
作者：
Han, Mangui;Tang, Wei;Deng, Longjiang
通讯作者：
Deng, Longjiang
影响因子：
1.8
作者：
NIMTZ, G;MARQUARDT, P;GLEITER, H
通讯作者：
GLEITER, H