Lee Jang Mee, Yang Jae-Hun, Kwon Nam Hee, Jo Yun Kyung, Choy Jin-Ho, Hwang Seong-Ju
Center for Hybrid Interfacial Chemical Structure (CICS), Department of Chemistry and Nanoscience, College of Natural Sciences, Ewha Womans University, Seoul 03760, Korea.
Dalton Trans. 2018 Feb 27;47(9):2949-2955. doi: 10.1039/c7dt03466k.
Efficient visible light active hybrid photocatalysts for H production can be synthesized by the intercalative hybridization of Zn-Cr-layered double hydroxide (Zn-Cr-LDH) with a mesoporous g-CN lattice. Small Zn-Cr-LDH nanocrystals with a size of ∼6 nm are immobilized in the mesopores of g-CN. Beyond an optimal LDH/g-CN molar ratio of 0.3, a further increase in the LDH content leads to the surface deposition of LDH crystals on the g-CN material as well as the intercalative immobilization of LDH into its mesopores, indicating the controllability of the LDH deposition site. The Zn-Cr-LDH-g-CN nanohybrids exhibit smaller surface areas than the pristine g-CN, confirming the intercalative stabilization of Zn-Cr-LDH nanocrystals in the mesopore of g-CN. The hybridization between Zn-Cr-LDH and g-CN is effective in enhancing visible light absorptivity and also in depressing electron-hole recombination, which is attributable to an efficient electronic coupling between both the hybridized components. The present Zn-Cr-LDH-g-CN nanohybrid exhibits promising photocatalytic activities for visible light-induced H production at a rate of 155.7 μmol g h, which is much superior to that of the pristine g-CN (21.7 μmol g h). The present study underscores that the intercalative immobilization of Zn-Cr-LDH crystals in the limited space of a mesopore is quite useful in improving the visible light active photocatalyst functionality of mesoporous carbon nitride.
通过将锌 - 铬层状双氢氧化物(Zn - Cr - LDH)与介孔石墨相氮化碳(g - CN)晶格进行插层杂化,可以合成用于制氢的高效可见光活性混合光催化剂。尺寸约为6纳米的小尺寸Zn - Cr - LDH纳米晶体被固定在g - CN的介孔中。当LDH/g - CN摩尔比超过最佳值0.3时,LDH含量的进一步增加会导致LDH晶体在g - CN材料表面沉积,同时LDH也会插层固定在其介孔中,这表明了LDH沉积位点的可控性。Zn - Cr - LDH - g - CN纳米杂化物的表面积比原始g - CN小,这证实了Zn - Cr - LDH纳米晶体在g - CN介孔中的插层稳定作用。Zn - Cr - LDH与g - CN之间的杂化有效地增强了可见光吸收能力,同时也抑制了电子 - 空穴复合,这归因于两种杂化组分之间的有效电子耦合。目前制备的Zn - Cr - LDH - g - CN纳米杂化物在可见光诱导制氢方面表现出有前景的光催化活性,产氢速率为155.7 μmol g⁻¹ h⁻¹,远优于原始g - CN(21.7 μmol g⁻¹ h⁻¹)。本研究强调,将Zn - Cr - LDH晶体插层固定在介孔的有限空间中对于提高介孔氮化碳的可见光活性光催化剂功能非常有用。