Negative inductive effect enhances charge transfer driving in sulfonic acid functionalized graphitic carbon nitride with efficient visible-light photocatalytic performance
Negative inductive effect enhances charge transfer driving in sulfonic acid functionalized graphitic carbon nitride with efficient visible-light photocatalytic performance
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负感应效应增强磺酸功能化石墨碳氮化物中的电荷转移驱动，具有高效的可见光光催化性能
DOI：
10.1016/s1872-2067(21)63872-x
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发表时间：
2022-02
影响因子：
16.5
通讯作者：
Xing Yan
中科院分区：
文献类型：
--
作者：
Zhang Min;Li Yunfeng;Chang Wei;Zhu Wei;Zhang Luohong;Jin Renxi;Xing Yan
有效的光生载流子迁移/分离是提高g-C3 N4光催化性能的关键。本文合成了磺酸基功能化的g-C3 N4（SACN），并通过g-C3 N4与氨基磺酸的简单固相热反应实现了SACN的同步增强。氨基磺酸作为一种固体强酸，在热处理的辅助下，可以实现对g-C3 N4表面的酸蚀，使其比表面积增大，表面催化反应位点增多。 更重要的是, 理论计算与实验表征结果表明, 磺酸基团的吸电子诱导效应所产生的电荷驱动力可极大改善g-C3N4的电荷转移动力学, 有效抑制了它们的再结合.此外，负诱导效应还可以诱导电荷再分布，降低g-C3 N4的导带电位，从而增强光生电子的还原能力。结果表明，SACN-400在420 ± 15 nm波长处表现出良好的光催化产氢性能，表观量子效率为11.03%，对有机污染物有较好的光催化降解率.
Efficient photogenerated carrier migration/separation plays a critical role in increasing the photocatalytic performance of g-C_3N_4. Herein, sulfonic acid group-functionalized g-C_3N_4(SACN) was synthesized and then synchronously strengthened by a facile-solid-state thermal reaction of g-C_3N_4 and sulfamic acid. As a solid strong acid, sulfamic acid can be used to achieve acid etching on the surface of g-C_3N_4 with the assistance of thermal treatment, leading to an enlarged specific surface area and increased surface catalytic reaction sites. More importantly, our experiments and density functional theory calculations indicate that the driving force generated by the negative inductive effect of sulfonic acid groups significantly improves the charge transfer dynamics and effectively inhibits their recombination. Moreover, the negative inductive effect can induce charge redistribution, which reduces the conduction band potential of g-C_3N_4 to enhance the reduction ability of photo-induced electrons. As a result, the SACN-400 sample showed excellent photocatalytic performance in H2 generation with an apparent quantum efficiency of 11.03% at 420 ± 15 nm, as well as an efficient photodegradation rate for organic pollutants.
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