Synergistically boosted photocatalytic production of hydrogen peroxide via protonation and oxygen doping on graphitic carbon nitride
Synergistically boosted photocatalytic production of hydrogen peroxide via protonation and oxygen doping on graphitic carbon nitride
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DOI：
10.1016/j.nanoen.2023.108917
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发表时间：
2023-09
期刊：
影响因子：
17.6
通讯作者：
D. Wen;Yaorong Su;Junyu Fang;Dan Zheng;Yangsen Xu;Shuang Zhou;Aiyun Meng;Peigang Han
中科院分区：
文献类型：
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作者：
D. Wen;Yaorong Su;Junyu Fang;Dan Zheng;Yangsen Xu;Shuang Zhou;Aiyun Meng;Peigang Han
改性石墨氮化碳（g-C3N4）光催化合成过氧化氢（H2O2）已被公认为一种有前途的绿色可持续发展工艺。但g- c3n4改性对光催化表面反应表面性质的影响仍需进一步探索。在这项工作中，我们设计并合成了质子化诱导的氧掺杂g-C3N4(pCN1)，在微观水平上显示出独特的卷曲纳米片结构。在可见光照射下，pCN1的光催化h2o2产率达到707 μmol g−1h−1，约为原始g- c3n4的8倍。增强的光催化性能是由于质子化和氧掺杂的协同作用，不仅极大地促进了氧分子的吸附和h2o2产物的解吸，而且促进了电荷的分离。此外，质子化过程提供的更丰富的质子可以与催化剂表面邻近的氧原子结合，从而促进OOH*中间体的形成，提高h2o2产率。本研究为制备高效改性g- c3n4光催化剂提供了一种简单有效的方法，可用于清洁、方便地合成H2O2。
Photocatalytic synthesis of hydrogen peroxide (H2O2) using modified graphitic carbon nitride (g-C3N4) has been recognized as a promising green and sustainable process. However, the effect of g-C3N4modification on the surface properties of photocatalytic surface reactions still needs extended exploration. In this work, we design and synthesize a protonation induced oxygen doping in g-C3N4(pCN1), which shows uniquely curled nanosheet structures in microscopic level. Under visible light irradiation, the photocatalytic H2O2production rate of pCN1 reaches 707 μmol g−1h−1, which is approximately eight times higher than that of primitive g-C3N4. The enhanced photocatalytic performance is attributed to the synergistic effect of protonation and oxygen doping, which not only dramatically facilitates the adsorption of oxygen molecules and the desorption of H2O2product, but also promotes the charge separation. In addition, more abundant protons supplied via protonation process can combine with the adjacent oxygen atoms on catalyst surface, thus promoting the formation of OOH* intermediate and improving the H2O2yield. This work provides a facile and effective strategy to prepare highly-efficient modified g-C3N4photocatalyst for the clean and convenient synthesis of H2O2.