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Boosting CO2 Conversion with Terminal Alkynes by Molecular Architecture of Graphene Oxide-Supported Ag Nanoparticles
Matter ( IF 17.3 ) Pub Date : 2020-08-05 , DOI: 10.1016/j.matt.2020.07.022
Xiaofei Zhang , Haitao Liu , Yanan Shi , Jianyu Han , Zhongjie Yang , Yin Zhang , Chang Long , Jun Guo , Yanfei Zhu , Xueying Qiu , Guangxin Xue , Lingjuan Zhang , Binghao Zhang , Lin Chang , Zhiyong Tang

Carboxylation of terminal alkynes with CO2 via direct C–H bond activation is a highly appealing way to capture and convert CO2 but faces great challenges and difficulty. Here, we report an efficient catalyst that is prepared simply through introduction of p-tert-butylaniline into graphite oxide powders followed by localized growth of Ag nanoparticles (NPs). The bulky nature of p-tert-butylaniline facilitates the powder exfoliation, giving rise to mass production of uniform modified graphene oxide (tert-GO) nanosheets of 4 nm in thickness. Notably, Ag/tert-GO shows excellent catalytic activity for converting alkynes regardless of containing electron-donating or electron-withdrawing groups under mild reaction conditions. The synergy of the amide linkages on tert-GO nanosheets and the supported small-sized Ag NPs is recognized as the vital role in promoting adsorption of CO2 and subsequent conversion.



中文翻译:

氧化石墨烯负载的Ag纳米粒子的分子结构促进末端炔烃的CO 2转化

末端炔烃通过直接的C–H键活化与CO 2进行羧基化是吸引和转化CO 2的极具吸引力的方法,但面临巨大的挑战和困难。在这里,我们报告说,简单地通过引入制备一种有效的催化剂p --butylaniline成石墨氧化物粉末,随后的Ag纳米颗粒(NP)的局部生长。p-tert的体积大丁基苯胺有助于粉末剥落,从而可大量生产厚度为4 nm的均匀改性氧化石墨烯(tert-GO)纳米片。值得注意的是,无论在温和的反应条件下,Ag / tert-GO都具有出色的催化炔烃转化活性,无论其含有给电子基团或吸电子基团。tert-GO纳米片上的酰胺键与负载的小型Ag NP的协同作用被认为是促进CO 2吸附和后续转化的关键作用。

更新日期:2020-08-05
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