Unraveling the Synergy Mechanism between Photocatalysis and Peroxymonosulfate Activation on a Co/Fe Bimetal-Doped Carbon Nitride,ACS Catalysis

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Unraveling the Synergy Mechanism between Photocatalysis and Peroxymonosulfate Activation on a Co/Fe Bimetal-Doped Carbon Nitride
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-06-21 , DOI: 10.1021/acscatal.3c01496
Heng Shi _{1,

2} , Yi He _{1,

2,

3} , Yubin Li ₄ , Pingya Luo _{1,

2}

Affiliation

Fenton-like catalysis based on peroxymonosulfate (PMS) activation has shown great potential in the treatment of organic wastewater. Heterogeneous Fenton-like catalysts containing transition metal active sites are highly efficient for PMS activation. However, the reduction of oxidized metal active sites was usually not prompt due to the sluggish reaction kinetics, which caused the insufficient redox cycle of the metal active sites and further hampered the catalysis efficiency. Recent studies have shown that the synergy effect between photocatalysis and PMS activation may address the above obstacle and boost overall efficiency. However, a deeper understanding of this synergy effect is still missing, making it difficult to be rationally controlled; thus, a poor synergy effect is frequently reported. Herein, a Co/Fe bimetal-doped graphitic carbon nitride (g-C₃N₄) was designed representatively through systematical characterization and theoretical calculation, the synergy effect was revealed to be profoundly determined by the competitive role of a hole in the system and the adsorbed metastable PMS* on the catalyst surface, and furthermore, the synergy effect can be rationally manipulated; when the Co/Fe doping ratio is 2.5:2.5, the as-prepared g-C₃N₄ with a moderate valence band position can endow the catalyst with an optimized photo-Fenton-like synergistic effect and the highest catalytic degradation performance. This work sheds light on the rational design of highly efficient photo-Fenton-like catalysts.

中文翻译：

揭示 Co/Fe 双金属掺杂碳氮化物上光催化和过一硫酸盐活化之间的协同机制

基于过一硫酸盐（PMS）活化的类芬顿催化在有机废水处理方面显示出巨大的潜力。含有过渡金属活性位点的非均相类芬顿催化剂对于 PMS 活化非常有效。然而，由于反应动力学缓慢，氧化金属活性位点的还原通常不及时，导致金属活性位点的氧化还原循环不足，进一步阻碍了催化效率。最近的研究表明，光催化和 PMS 激活之间的协同效应可以解决上述障碍并提高整体效率。但目前对这种协同效应还缺乏更深入的认识，难以合理调控；因此，经常有报道称协同效应较差。在此处，₃ N ₄）通过系统表征和理论计算进行了代表性设计，揭示了协同效应是由系统中空穴与催化剂表面吸附的亚稳态PMS*的竞争作用深刻决定的，而且协同效应可以合理地操纵；当Co/Fe掺杂比为2.5:2.5时，所制备的具有中等价带位置的gC ₃ N ₄可以赋予催化剂最佳的类光芬顿协同效应和最高的催化降解性能。这项工作揭示了高效光芬顿类催化剂的合理设计。

更新日期：2023-06-21

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