Liu Wentao, Wang Qiu, Liu Zhi, Ding Guixiang
Faculty of Chemistry and Chemical Engineering, Liaoning Normal University, Dalian 116029, P.R. China.
Department of Chemistry, College of Science, Shantou University, Shantou 515063, P.R. China.
J Colloid Interface Sci. 2022 Sep 15;622:21-30. doi: 10.1016/j.jcis.2022.04.102. Epub 2022 Apr 22.
A series of treble NiAl-LDH/g-CN/carbon quantum dots (LDH/CN/CQDs) photocatalysts is successfully prepared for the photoreduction of CO to CO via a facile hydrothermal pathway. In the 3D flower-like LDH/CN/CQDs, CQDs not only achieve the efficient inhibition of charge recombination but also act as the unhindered "electronic bridges" to synergistically construct a classical type-Ⅱ charge transfer configuration, which synchronously permits the effluence of photogenerated electrons from CN to LDH and holes from LDH to CN, and promotes ultraviolet-visible irradiation respondence. The sample of LDH/CN/CQDs-6 is the optimal one amongst the LDH/CN/CQDs with a larger special surface area (98.43 mg) and an appropriate content of CQDs (66.9 wt%), exhibiting the highest CO evolution rate (5.2 μmol·g·h) under visible light irradiation without any sacrificial agent or photosensitizer in water. This is 26.8- and 20.9-fold higher than those of the pristine LDH, pure CN, and their binary counterparts, respectively, and also outperforms most reported LDH-based photocatalysts. As unhindered electron conduction bridges, the highly dispersed CQDs in the LDH/CN heterojunction significantly increase utilization efficiency of light energy and separation efficiency of photogenerated electron-hole pairs. This work provides a beneficial attempt to integrate CQDs with LDH/CN for the positive synergetic effect on both photoelectric properties and electron transfer to obtain highly enhanced photocatalytic activity of CO into CO, and expected to be extended towards broader photocatalytic applications.
通过简便的水热法成功制备了一系列用于将CO光还原为CO的三重NiAl-LDH/g-CN/碳量子点(LDH/CN/CQDs)光催化剂。在三维花状的LDH/CN/CQDs中,碳量子点不仅实现了对电荷复合的有效抑制,还作为畅通无阻的“电子桥”协同构建了经典的Ⅱ型电荷转移构型,同步允许光生电子从CN流向LDH,空穴从LDH流向CN,并促进紫外-可见光响应。LDH/CN/CQDs-6样品是LDH/CN/CQDs中最优的,具有较大的比表面积(98.43 mg)和适当的碳量子点含量(66.9 wt%),在可见光照射下,在水中无需任何牺牲剂或光敏剂,表现出最高的CO析出速率(5.2 μmol·g·h)。这分别比原始LDH、纯CN及其二元对应物高26.8倍和20.9倍,也优于大多数报道的基于LDH的光催化剂。作为畅通无阻的电子传导桥,LDH/CN异质结中高度分散的碳量子点显著提高了光能利用效率和光生电子-空穴对的分离效率。这项工作为将碳量子点与LDH/CN整合以在光电性能和电子转移方面产生积极协同效应,从而获得将CO高效光催化转化为CO的活性提供了有益尝试,并有望扩展到更广泛的光催化应用。