Merging Single-Atom-Dispersed Silver and Carbon Nitride to a Joint Electronic System via Copolymerization with Silver Tricyanomethanide
Merging Single-Atom-Dispersed Silver and Carbon Nitride to a Joint Electronic System via Copolymerization with Silver Tricyanomethanide
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DOI：
10.1021/acsnano.5b04210
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发表时间：
2016-03-01
期刊：
影响因子：
17.1
通讯作者：
Dontsova, Dariya
中科院分区：
文献类型：
--
作者：
Chen, Zupeng;Pronkin, Sergey;Dontsova, Dariya
在此，我们提出了一种方法来创建单原子分散的银和氮化碳聚合物之间的混合物。三氰基甲烷银（AgTCM）在模板化氮化碳合成过程中用作反应性共聚单体，以将负电荷和银原子/离子引入系统。通过光致发光测量、X射线光电子能谱研究和表面4-电位测量，证明了在离域联合电子系统的形成下成功地引入了额外的电子密度。同时，固态核磁共振谱和电化学阻抗谱分析表明，氮化碳网络的主要结构没有受到干扰。合成还导致可见光吸收的改善和最终产品中更高表面积的发展。原子分散的AgTCM掺杂的氮化碳在炔的选择性氢化中显示出增强的性能，与通过喷雾沉积和碳化还原方法制备的其它常规Ag基材料的性能相比，在此以1-己炔为例。
Herein, we present an approach to create a hybrid between single-atom-dispersed silver and a carbon nitride polymer. Silver tricyanomethanide (AgTCM) is used as a reactive comonomer during templated carbon nitride synthesis to introduce both negative charges and silver atoms/ions to the system. The successful introduction of the extra electron density under the formation of a delocalized joint electronic system is proven by photoluminescence measurements, X-ray photoelectron spectroscopy investigations, and measurements of surface 4-potential. At the same time, the principal structure of the carbon nitride network is not disturbed, as shown by solid-state nuclear magnetic resonance spectroscopy and electrochemical impedance spectroscopy analysis. The synthesis also results in an improvement of the visible light absorption and the development of higher surface area in the final products. The atom-dispersed AgTCM-doped carbon nitride shows an enhanced performance in the selective hydrogenation of alkynes in comparison with the performance of other conventional Ag-based materials prepared by spray deposition and impregnation-reduction methods, here exemplified with 1-hexyne.