Photocatalytic reactive oxygen species (ROS)-induced reactions provide an appealing method to solve the environmental and energy issues, whereas the current oxidation reaction generally suffered from low efficiency and poor selectivity due to uncontrollable O₂ activation process. In view of the existence of competitive electron and energy transfer pathway, we propose that highly efficient superoxide radical anion (·O₂⁻) generation can be achieved by optimizing the order degree of the photocatalyst. Herein, by taking carbon nitride polymer as an example, we optimized the crystallization process of carbon nitride polymer by selecting precursors of different polymerization degrees with a molten salt method. Benefiting from the high crystallinity, extended π-conjugated system and strong van der-Waals interactions between interlayers, the modified carbon nitride polymer exhibited accelerated charge transport and enhancement in electron induced molecular oxygen activation reactions under visible light. Consequently, the CCN-P exhibits about 1.5 times higher conversion rate in hydroxylation of phenylboronic acid and over 6-fold faster degradation rate in Rh B organic pollutants photodegradation with respect to pristine carbon nitride. This study provides an in-depth understanding on the optimization of the O₂ activation process and the design of advanced photocatalysts.

光催化活性氧（ROS）诱导的反应为解决环境和能源问题提供了一种有吸引力的方法，而当前的氧化反应由于O ₂活化过程不可控而通常效率低下且选择性差。鉴于有竞争力的电子和能量传递路径的存在，我们建议，高效超氧阴离子自由基（·O2 ₂ ^-可以通过优化光催化剂的有序度来实现。本文以氮化碳聚合物为例，通过熔盐法选择聚合度不同的前驱体，优化了氮化碳聚合物的结晶工艺。得益于高结晶度，扩展的π共轭体系和中间层之间的强范德华相互作用，改性的氮化碳聚合物在可见光下显示出加速的电荷传输和电子诱导的分子氧活化反应的增强。因此，相对于原始碳氮化物，CCN-P在苯基硼酸的羟基化反应中具有约1.5倍的高转化率，在Rh B有机污染物的光降解中具有约6倍的降解速度。₂活化过程和高级光催化剂的设计。