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首页> 外文期刊>Catalysis science & technology >Visible-light-driven sonophotocatalysis for enhanced Cr() reduction over mixed-linker zirconium-porphyrin MOFs
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Visible-light-driven sonophotocatalysis for enhanced Cr() reduction over mixed-linker zirconium-porphyrin MOFs

机译：可见光驱动的超声心催化，可增强混合链锆 - 卟啉MOF的Cr（）还原（）降低

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摘要

In this study, we synthesized and characterized two mixed-linker zirconium-porphyrin metal–organic frameworks, PCN-134 and PCN-138, constructed from tetratopic light harvesting TCPP ligands and tritopic BTB/TBTB ligands (TCPP = trakis(4-carboxyphenyl)porphyrin), BTB = benzene tribenzoate, TBTB = 4,4′,4′′-(2,4,6-trimethylbenzene-1,3,5-triyl)tribenzoate). In consideration of good chemical stability, ligand-based photogenerated charge generation and broad visible light absorption, PCN-134 and PCN-138 were employed as catalysts for reducing Cr(vi) to Cr(iii) in an established sonophotocatalytic system. The average reaction rates of Cr(vi) reduction in sonophotocatalysis (20 kHz, 120 W) were 0.237 mg L−1 min−1 and 0.266 mg L−1 min−1 for PCN-134 and PCN-138, respectively. By comparison, the average reaction rates of Cr(vi) reduction in photocatalysis were 0.074 mg L−1 min−1 and 0.115 mg L−1 min−1 for PCN-134 and PCN-138. In addition, there are no catalytic activities over the synthesized MOFs in sonocatalytic Cr(vi) reduction. The two mixed-linker MOFs in the sonophotocatalytic Cr(vi) reduction system exhibited 2–3 times higher reactivity than that in the individual photocatalysis. Notably, no electron sacrificial agents were used in the established sonophotocatalytic process. A mechanism study demonstrated that the synergistic effect of sonocatalysis and photocatalysis promoted the photoinduced electron transfer from the MOFs to Cr(vi) and enhanced the catalytic activity. This work might provide a novel strategy for improving the efficiency of MOF-based photocatalytic systems.
机译：In this study, we synthesized and characterized two mixed-linker zirconium-porphyrin metal–organic frameworks, PCN-134 and PCN-138, constructed from tetratopic light harvesting TCPP ligands and tritopic BTB/TBTB ligands (TCPP = trakis(4-carboxyphenyl)卟啉），btb =苯三生酸盐，tbtb = 4,4'，4'' - （2,4,6-三甲基苯苯基1,3,5-三甲基）tribenzoate）。考虑到良好的化学稳定性，基于配体的光生电荷产生和广泛的可见光吸收，PCN-134和PCN-138被用作将CR（VI）降低至CR（III）的催化剂。对于PCN-134和PCN-138，Sonophotocatalysis（20 kHz，120 W）的Cr（VI）降低的平均反应速率分别为0.237 mg l-1 min-1和0.266 mg l-1 min-1。相比之下，光催化中Cr（VI）降低的平均反应速率为0.074 mg l-1 min-1，对于PCN-134和PCN-138而言，PCN-134和0.115 mg L-1 min-1。另外，在超声催化CR（VI）还原中，没有合成的MOF的催化活性。超声催化性CR（VI）还原系统中的两个混合链链链球MOF的反应性比单个光催化中的反应性高2-3倍。值得注意的是，在已建立的超声催化过程中没有使用电子牺牲剂。一项机制研究表明，声催化和光催化的协同作用促进了光诱导的电子从MOF到CR（VI）的转移，并增强了催化活性。这项工作可能提供了提高基于MOF的光催化系统效率的新型策略。

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