MXene (Ti3C2) Vacancy Confined Single-Atom Catalyst for Efficient Functionalization of CO2,Journal of the American Chemical Society

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MXene (Ti3C2) Vacancy Confined Single-Atom Catalyst for Efficient Functionalization of CO2
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2019-01-30 , DOI: 10.1021/jacs.8b13579
Di Zhao ₁ , Zheng Chen ₁ , Wenjuan Yang ₁ , Shoujie Liu _{1,

2} , Xun Zhang ₃ , Yi Yu ₃ , Weng-Chon Cheong ₁ , Lirong Zheng ₄ , Fuqiang Ren ₅ , Guobing Ying ₆ , Xing Cao ₁ , Dingsheng Wang ₁ , Qing Peng ₁ , Guoxiu Wang ₇ , Chen Chen ₁

Affiliation

A central topic in single-atom catalysis is building strong interactions between single atoms and the support for stabilization. Herein we report the preparation of stabilized single-atom catalysts via a simultaneous self-reduction stabilization process at room temperature using ultrathin two-dimensional Ti3- xC2T yMXene nanosheets characterized by abundant Ti-deficit vacancy defects and a high reducing capability. The single atoms therein form strong metal-carbon bonds with the Ti3- xC2T y support and are therefore stabilized onto the sites previously occupied by Ti. Pt-based single-atom catalyst (SAC) Pt1/Ti3- xC2T y offers a green route to utilizing greenhouse gas CO2, via the formylation of amines, as a C1 source in organic synthesis. DFT calculations reveal that, compared to Pt nanoparticles, the single Pt atoms on Ti3- xC2T y support feature partial positive charges and atomic dispersion, which helps to significantly decrease the adsorption energy and activation energy of silane, CO2, and aniline, thereby boosting catalytic performance. We believe that these results would open up new opportunities for the fabrication of SACs and the applications of MXenes in organic synthesis.

中文翻译：

MXene (Ti3C2) 空位限制单原子催化剂，用于 CO2 的有效功能化

单原子催化的一个中心主题是在单原子和稳定支持之间建立强相互作用。在此，我们报告了使用超薄二维 Ti3-xC2T yMXene 纳米片在室温下通过同步自还原稳定过程制备稳定的单原子催化剂，该纳米片具有丰富的缺钛空位缺陷和高还原能力。其中的单个原子与 Ti3-xC2T y 载体形成牢固的金属-碳键，因此稳定在先前由 Ti 占据的位置上。Pt 基单原子催化剂 (SAC) Pt1/Ti3-xC2T y 为利用温室气体 CO2 提供了一条绿色途径，通过胺的甲酰化，作为有机合成中的 C1 来源。DFT 计算表明，与 Pt 纳米粒子相比，Ti3-xC2T y 载体上的单个 Pt 原子带有部分正电荷和原子分散，有助于显着降低硅烷、CO2 和苯胺的吸附能和活化能，从而提高催化性能。我们相信这些结果将为 SAC 的制造和 MXenes 在有机合成中的应用开辟新的机会。

更新日期：2019-01-30

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