Li Jian, Han Xu, Wang Dongmei, Zhu Lei, Ha-Thi Minh-Huong, Pino Thomas, Arbiol Jordi, Wu Li-Zhu, Nawfal Ghazzal Mohamed
Université Paris-Saclay, UMR 8000 CNRS, Institut de Chimie Physique, 91405, Orsay, France.
Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST, Campus UAB, Bellaterra, 08193 Barcelona, Catalonia, Spain.
Angew Chem Int Ed Engl. 2022 Oct 24;61(43):e202210242. doi: 10.1002/anie.202210242. Epub 2022 Sep 7.
With a direct band gap, superior charge carrier mobility, and uniformly distributed pores, graphdiyne (GDY) has stimulated tremendous interest from the scientific community. However, its broad application is greatly limited by the complicated multistep synthesis process including complex deprotection of hexakis-[(trimethylsilyl)ethynyl]benzene (HEB-TMS) and peeling of GDY from the substrates. Here, we describe a deprotection-free strategy to prepare GDY powder by directly using HEB-TMS as the monomer. When CuCl was used as the catalysts in DMF solvent, the yield of GDY powder reached ≈100 %. More interestingly, uniformly dispersed CuO nanoparticles with an average diameter of ≈2.9 nm were in situ formed on GDY after the reaction. The prepared CuO/GDY was demonstrated an excellent co-catalyst for photocatalytic hydrogen evolution, comparable to the state-of-art Pt co-catalyst. The deprotection-free approach will widen the use of GDY and facilitate its scaling up to industrial level.
由于具有直接带隙、优异的电荷载流子迁移率和均匀分布的孔隙，石墨炔（GDY）引起了科学界的极大兴趣。然而，其广泛应用受到复杂的多步合成过程的极大限制，该过程包括六（三甲基硅乙炔基）苯（HEB-TMS）的复杂脱保护以及从底物上剥离GDY。在此，我们描述了一种无需脱保护的策略，即直接使用HEB-TMS作为单体来制备GDY粉末。当在DMF溶剂中使用CuCl作为催化剂时，GDY粉末的产率达到约100%。更有趣的是，反应后在GDY上原位形成了平均直径约为2.9nm的均匀分散的CuO纳米颗粒。所制备的CuO/GDY被证明是一种用于光催化析氢的优异助催化剂，与目前最先进的Pt助催化剂相当。这种无需脱保护的方法将拓宽GDY的应用范围，并促进其扩大到工业规模。
