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Solar‐Driven Nitrogen Fixation Catalyzed by Stable Radical‐Containing MOFs: Improved Efficiency Induced by a Structural Transformation
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-08-13 , DOI: 10.1002/anie.202009630 Kong‐Qiu Hu 1 , Peng‐Xiang Qiu 2 , Li‐Wen Zeng 1 , Shu‐Xian Hu 3 , Lei Mei 1 , Shu‐Wen An 1 , Zhi‐Wei Huang 1 , Xiang‐He Kong 1 , Jian‐Hui Lan 1 , Ji‐Pan Yu 1 , Zhi‐Hui Zhang 4 , Zhong‐Fei Xu 3 , John K Gibson 5 , Zhi‐Fang Chai 6 , Yun‐Fei Bu 2 , Wei‐Qun Shi 1
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-08-13 , DOI: 10.1002/anie.202009630 Kong‐Qiu Hu 1 , Peng‐Xiang Qiu 2 , Li‐Wen Zeng 1 , Shu‐Xian Hu 3 , Lei Mei 1 , Shu‐Wen An 1 , Zhi‐Wei Huang 1 , Xiang‐He Kong 1 , Jian‐Hui Lan 1 , Ji‐Pan Yu 1 , Zhi‐Hui Zhang 4 , Zhong‐Fei Xu 3 , John K Gibson 5 , Zhi‐Fang Chai 6 , Yun‐Fei Bu 2 , Wei‐Qun Shi 1
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Herein we present a new viologen‐based radical‐containing metal–organic framework (RMOF) Gd‐IHEP‐7, which upon heating in air undergoes a single‐crystal‐to‐single‐crystal transformation to generate Gd‐IHEP‐8. Both RMOFs exhibit excellent air and water stability as a result of favorable radical‐radical interactions, and their long‐lifetime radicals result in wide spectral absorption in the range 200–2500 nm. Gd‐IHEP‐7 and Gd‐IHEP‐8 show excellent activity toward solar‐driven nitrogen fixation, with ammonia production rates of 128 and 220 μmol h−1 g−1, respectively. Experiments and theoretical calculations indicate that both RMOFs have similar nitrogen fixation pathways. The enhanced catalytic efficiency of Gd‐IHEP‐8 versus Gd‐IHEP‐7 is attributed to intermediates stabilized by enhanced hydrogen bonding.
中文翻译：
稳定的含自由基的MOF催化太阳能驱动的固氮：通过结构转变诱导的效率提高
本文中，我们介绍了一种新的基于紫精的含自由基金属-有机骨架Gd-IHEP-7，它在空气中加热后会经历单晶至单晶转变，从而生成Gd-IHEP-8。由于有利的自由基与自由基的相互作用，两种RMOF均表现出出色的空气和水稳定性，它们的长期自由基可导致200–2500 nm范围内的宽光谱吸收。Gd-IHEP-7和Gd-IHEP-8对太阳能驱动的固氮表现出出色的活性，氨的产生速率分别为128和220μmolh -1 g -1， 分别。实验和理论计算表明，两种RMOF具有相似的固氮途径。Gd-IHEP-8与Gd-IHEP-7相比增强的催化效率归因于通过增强氢键而稳定的中间体。
更新日期：2020-08-13
中文翻译：
稳定的含自由基的MOF催化太阳能驱动的固氮：通过结构转变诱导的效率提高
本文中，我们介绍了一种新的基于紫精的含自由基金属-有机骨架Gd-IHEP-7，它在空气中加热后会经历单晶至单晶转变，从而生成Gd-IHEP-8。由于有利的自由基与自由基的相互作用，两种RMOF均表现出出色的空气和水稳定性，它们的长期自由基可导致200–2500 nm范围内的宽光谱吸收。Gd-IHEP-7和Gd-IHEP-8对太阳能驱动的固氮表现出出色的活性，氨的产生速率分别为128和220μmolh -1 g -1， 分别。实验和理论计算表明，两种RMOF具有相似的固氮途径。Gd-IHEP-8与Gd-IHEP-7相比增强的催化效率归因于通过增强氢键而稳定的中间体。
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