The covalent attachment of molecules to 2D materials is an emerging area as strong covalent chemistry offers new hybrid properties and greater mechanical stability compared with nanoparticles. A nickel bis-aminothiophenol catalyst was grafted onto a range of 2D carbon nitrides (C₃N_xH_y) to form noble metal-free photocatalysts for H₂ production. The hybrids produce H₂ beyond 8 days with turnover numbers reaching 1360 based on nickel, a more than 3 fold higher durability than reported molecular catalyst-carbon nitride mixtures, and under longer wavelengths (>475 nm). Time-resolved spectroscopy reveals sub-microsecond electron transfer to the grafted catalyst, six orders of magnitude faster compared with similar reports of non-grafted catalysts. The photoelectrons on the catalyst have a ca. 1000 times longer half-time (7 ms) compared with bare carbon nitride (10 μs). The grafting strategy operates across a range of molecular catalyst-carbon nitride combinations, thus paving the way for robust efficient photocatalysts based on low-cost tunable components.

中文翻译：

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在C3NxHy上共价接枝分子催化剂，将其作为可靠，高效且定义明确的光催化剂，用于太阳能燃料合成

分子与2D材料的共价连接是一个新兴领域，因为与纳米粒子相比，强大的共价化学提供了新的杂化特性和更高的机械稳定性。将镍双氨基氨基苯酚催化剂接枝到一系列2D碳氮化物（C ₃ N _x H _y）上，以形成用于H ₂生产的不含贵金属的光催化剂。杂种产生H ₂超过8天，基于镍的营业额达到1360，比报道的分子催化剂-氮化碳混合物的耐久性高3倍以上，并且波长更长（> 475 nm）。时间分辨光谱显示亚微秒电子转移至接枝催化剂，与非接枝催化剂的类似报道相比，转移速度快了六个数量级。催化剂上的光电子具有约1 。半衰期（7 ms）的时间是裸氮化碳（10μs）的1000倍。接枝策略适用于各种分子催化剂-碳氮化合物的组合，从而为基于低成本可调组分的坚固高效的光催化剂铺平了道路。