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氨基取代石墨烯负载单原子金催化剂促进甲酸脱氢的第二球效应
作者:小柯机器人 发布时间:2023/1/26 14:58:53

南方科技大学段乐乐团队报道了氨基取代石墨烯负载单原子金催化剂促进甲酸脱氢的第二球效应。相关研究成果于2023年1月18日发表于国际顶尖学术期刊《德国应用化学》。

调节均相分子催化剂的第二球是提高其催化活性的一种常见而有效的方法,而由于在其第二球中安装官能团存在合成挑战,很少对非均相单原子催化剂的第二球效进行应研究。

受益于石墨炔(GDY)定义明确且易于调整的结构,在氨基取代的GDY上构建了Au单原子催化剂,其中氨基位于Au中心的第二个球体中。氨基修饰的GDY上的Au原子与未官能化的GDY相比显示出优异的甲酸脱氢活性。实验研究,特别是质子盘点研究和理论计算表明,与Au原子相邻的氨基可以充当质子中继站,从而促进中间AuH的质子化以生成H2

该研究为在单原子催化剂上精确构建功能第二球体铺平了道路。

附:英文原文

Title: Second Sphere Effects Promote Formic Acid Dehydrogenation by a Single-Atom Gold Catalyst Supported on Amino-Substituted Graphdiyne

Author: Hong Liu, Zou Haiyuan, Dan Wang, Chuancheng Wang, Fan Li, Hao Dai, Mei Wang, Yong-fei Ji, Lele Duan

Issue&Volume: 2023-01-18

Abstract: Regulating the second sphere of homogeneous molecular catalysts is a common and effective method to boost their catalytic activities, while the second sphere effects have rarely been investigated for heterogeneous single-atom catalysts primarily due to the synthetic challenge for installing functional groups in their second spheres. Benefiting from the well-defined and readily tailorable structure of graphdiyne (GDY), an Au single-atom catalyst on amino-substituted GDY is constructed, where the amino group is located in the second sphere of the Au center. The Au atoms on amino-decorated GDY displayed superior activity for formic acid dehydrogenation compared with those on unfunctionalized GDY. The experimental studies, particularly the proton inventory studies, and theoretical calculations revealed that the amino groups adjacent to an Au atom could serve as proton relays and thus facilitate the protonation of an intermediate AuH to generate H2. Our study paves the way to precisely constructing the functional second sphere on single-atom catalysts.

DOI: 10.1002/anie.202216739

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202216739

期刊信息

Angewandte Chemie:《德国应用化学》,创刊于1887年。隶属于德国化学会,最新IF:16.823
官方网址:https://onlinelibrary.wiley.com/journal/15213773
投稿链接:https://www.editorialmanager.com/anie/default.aspx

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