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Modular assembly of electron transfer pathways in bimetallic MOFs for photocatalytic ammonia synthesis

机译:光催化氨合成的双金属MOF中电子转移途径的模块化组装

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It is a long-term pursuit to implement the green and sustainable photocatalytic production of ammonia via the conversion of water and nitrogen under mild conditions. Due to the rapid recombination of photoexcited carriers and competitive reaction of hydrogen evolution, how to effectively utilize the electrons in the photocatalytic procedure becomes a key issue to achieve high photocatalytic N2 reduction. In this study, electron pathway engineering (EPE) is proposed to regulate the electron transfer and utilization by using the stable amino-functionalized UiO-66 with bimetallic Ce–Hf nodes (NU6(Ce–Hf)) as the photocatalysts. The photocatalytic results confirm that the sample with the Ce : Hf molar ratio exhibits optimal performance (158.4 μmol g−1 h−1), which is ascribed to the electron transfer efficiency promoted by the electron buffering effect of Ce species and the selective adsorption ability of Hf species for nitrogen molecules. In addition, the selectivity of the nitrogen fixation reaction is approximately up to 100%, which is attributed to the inhibition of hydrogen evolution reaction by Hf species. This study may offer some inspirations to realize the effective transfer and utilization of electrons for photocatalytic materials.
机译:这是长期的追求,可以通过在轻度条件下的水和氮来实施氨的绿色和可持续的光催化生产。由于光激发载体的快速重组和氢进化的竞争反应,如何有效利用电子在光催化程序中成为实现高光催化N2还原的关键问题。在这项研究中,提出了电子通路工程(EPE),以通过使用Bimetallic CE-HF节点(NU6(CE – HF))作为光催化剂来调节电子传输和利用。光催化结果证实,具有CE:HF摩尔比的样品表现出最佳性能(158.4μmolG -1 H -1),这归因于CE物种的电子缓冲效应和选择性吸附能力的电子传递效率促进的电子传递效率用于氮分子的HF物种。另外,氮固定反应的选择性大约为100%,这归因于HF物种抑制氢进化反应。这项研究可能会提供一些灵感,以实现电子对光催化材料的有效传输和利用。

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