Graphitic carbon nitride, as an excellent metal-free catalyst, is a promising candidate for cataluminescence (CTL) sensing of H₂S owing to its high sulfur tolerance, environmental friendliness and low cost. Herein, in view of inner chemical inertness and low special surface area of g-C₃N₄, fluorine with strong electronegativity was employed to adjust the electron density of g-C₃N₄ to obtain fluorine functionalized graphitic carbon nitride (F-g-C₃N₄) for H₂S sensing. As expected, the CTL response of F-g-C₃N₄ exhibits more than 30 times higher towards H₂S by contrast with that of g-C₃N₄. Results demonstrated that F-g-C₃N₄ was more conducive to the adsorption of O₂ and H₂S due to the enlarged special surface area, the easier formation of hydrogen bond and the changed electronic structure, which was also supported by density functional theory calculations. Additionally, the F-g-C₃N₄-based sensor exhibits as high sensitivity as that of metal catalyst-based sensors but a longer lifetime. Meanwhile, the F-g-C₃N₄-based sensor has much higher CTL responses in the range of 1.27∼64.00 μg mL⁻¹, lower detection limit of 0.07 μg mL⁻¹ when comparing with previously reported metal-free catalyst-based sensors. Undoubtedly, this work not only opened up a novel approach to improve the sensing performance of g-C₃N₄, but also proposed an efficient strategy for obtaining satisfying catalytic performance of other metal-free layered materials.

石墨质氮化碳是一种优异的无金属催化剂，由于其高耐硫性，环境友好性和低成本，因此是用于H ₂ S催化发光（CTL）传感的有前途的候选者。在此，鉴于gC ₃ N ₄的内部化学惰性和低比表面积，使用具有强电负性的氟来调节gC ₃ N ₄的电子密度，以获得用于H的氟官能化石墨碳氮化物（FgC ₃ N ₄）。₂ S感应。不出所料，FgC ₃ N ₄的CTL响应对H _2的表现高出30倍以上相比之下，S与gC ₃ N _4相比。结果表明，FgC ₃ N _4的比表面积增大，氢键的形成更容易，电子结构的变化更有利于O ₂和H ₂ S的吸附，这也得到密度泛函理论计算的支持。另外，基于FgC ₃ N ₄的传感器表现出与基于金属催化剂的传感器一样高的灵敏度，但是使用寿命更长。同时，基于FgC ₃ N ₄的传感器在1.27〜64.00μgmL ^-1范围内具有更高的CTL响应。与先前报道的不含金属的基于催化剂的传感器相比，检测限较低，为0.07μgmL ^-1。无疑，这项工作不仅为提高gC ₃ N ₄的感测性能开辟了新途径，而且提出了一种获得其他无金属层状材料令人满意的催化性能的有效策略。