Two Birds with One Stone: Concurrent Ligand Removal and Carbon Encapsulation Decipher Thickness-Dependent Catalytic Activity.
Two Birds with One Stone: Concurrent Ligand Removal and Carbon Encapsulation Decipher Thickness-Dependent Catalytic Activity.
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DOI：
10.1021/acs.nanolett.2c03181
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发表时间：
2022-11-09
期刊：
影响因子：
10.8
通讯作者：
Lu, Xing
中科院分区：
文献类型：
--
作者：
Guo, Kun;Chang, Litao;Li, Ning;Bao, Lipiao;Shubeita, Samir de Moraes;Baidak, Aliaksandr;Yu, Zhixin;Lu, Xing
碳壳包覆过渡金属基核已成为一种有趣的催化剂结构类型，但壳厚度对包埋组分的催化性能的影响尚不清楚。在这里，我们提出了一个概念验证的研究，揭示了通过碳化的各向同性和均匀的油胺（OAM）配体，覆盖胶体二硫化钼的厚度效应。热处理将OAm变成均匀的碳壳，而MoS2单层的大小保持不变。当针对酸性析氢反应进行评价时，煅烧的MoS2催化剂提供取决于煅烧温度的火山型活性趋势。卢瑟福背散射光谱和深度剖析X射线光电子能谱始终提供了一个准确的量化碳壳厚度。同样的变化模式的催化活性和碳壳厚度，动力学研究的帮助下，然后令人信服地证明了火山曲线的两个分支上的电子和质子电导率的各自的限制。
A carbon shell encapsulating a transition metal-based core has emerged as an intriguing type of catalyst structure, but the effect of the shell thickness on the catalytic properties of the buried components is not well known. Here, we present a proof-of-concept study to reveal the thickness effect by carbonizing the isotropic and homogeneous oleylamine (OAm) ligands that cover colloidal MoS2. A thermal treatment turns OAm into a uniform carbon shell, while the size of MoS2 monolayers remains identical. When evaluated toward an acidic hydrogen evolution reaction, the calcined MoS2 catalysts deliver a volcano-type activity trend that depends on the calcination temperature. Rutherford backscattering spectrometry and depth-profiling X-ray photoelectron spectroscopy consistently provide an accurate quantification of the carbon shell thickness. The same variation pattern of catalytic activity and carbon shell thickness, aided by kinetic studies, is then persuasively justified by the respective limitations of electron and proton conductivities on the two branches of the volcano curve.
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