Defect-induced efficient dry reforming of methane over two-dimensional Ni/h-boron nitride nanosheet catalysts
Defect-induced efficient dry reforming of methane over two-dimensional Ni/h-boron nitride nanosheet catalysts
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DOI：
10.1016/j.apcatb.2018.07.001
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发表时间：
2018-12-15
影响因子：
22.1
通讯作者：
Zhang, Dengsong
中科院分区：
文献类型：
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作者：
Cao, Yang;Maitarad, Phornphimon;Zhang, Dengsong
有效提高催化剂的稳定性和抗焦性是甲烷干法重整的一个重要方面。在这里，我们报道了嵌入在六方氮化硼纳米片空位缺陷上的镍纳米颗粒(Ni/h-BNNS)可以通过抑制二维(2D)界面电子效应来优化催化性能。实验结果和密度泛函理论计算表明，Ni/h-BNNS催化剂缺陷的表面工程能通过电子给体/受体机制强烈影响金属-载体相互作用，有利于CH4和CO2的吸附和催化活化。在120h的耐久性试验中，Ni/h-BNNS催化剂表现出了优异的催化性能。此外，原位技术进一步揭示了活性镍中心的可能回收机理，证实了Ni/h-BNNS催化剂的催化活性得到了提高。这项工作突出了缺陷修饰界面的促进机理，同样适用于热化学稳定性催化剂的设计。
Efficient enhancement of catalytic stability and coke-resistance is a crucial aspect for dry reforming of methane. Here, we report Ni nanoparticles embedded on vacancy defects of hexagonal boron nitride nanosheets (Ni/h-BNNS) can optimize catalytic performance by taming two-dimensional (2D) interfacial electronic effects. Experimental results and density functional theory calculations indicate that surface engineering on defects of Ni/h-BNNS catalyst can strongly influence metal-support interaction via electron donor/acceptor mechanisms and favor the adsorption and catalytic activation of CH4 and CO2. The Ni/h-BNNS catalyst exhibits superior catalytic performance during a 120 h durability test. Furthermore, in situ techniques further reveal possible recovery mechanism of the active Ni sites, identifying the enhanced catalytic activities of the Ni/h-BNNS catalyst. This work highlights promotional mechanism of defect-modified interface and should be equally applicable for design of thermochemically stable catalysts.