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Thermal Activation of a Copper-Loaded Covalent Organic Framework for Near-Ambient Temperature Hydrogen Storage and Delivery
ACS Materials Letters ( IF 9.6 ) Pub Date : 2020-02-07 , DOI: 10.1021/acsmaterialslett.9b00413 Wade A. Braunecker 1, 2 , Sarah Shulda 1 , Madison B. Martinez 1, 2 , Katherine E. Hurst 1 , Joshua T. Koubek 2 , Sarah Zaccarine 2 , Rachel E. Mow 1, 2 , Svitlana Pylypenko 1, 2 , Alan Sellinger 1, 2 , Thomas Gennett 1, 2 , Justin C. Johnson 1, 2
ACS Materials Letters ( IF 9.6 ) Pub Date : 2020-02-07 , DOI: 10.1021/acsmaterialslett.9b00413 Wade A. Braunecker 1, 2 , Sarah Shulda 1 , Madison B. Martinez 1, 2 , Katherine E. Hurst 1 , Joshua T. Koubek 2 , Sarah Zaccarine 2 , Rachel E. Mow 1, 2 , Svitlana Pylypenko 1, 2 , Alan Sellinger 1, 2 , Thomas Gennett 1, 2 , Justin C. Johnson 1, 2
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Copper(II) formate is efficiently incorporated into the pores of a 2D imine-based covalent organic framework (COF) via coordination with the phenol and imine groups. The coordinated metal ion is then reduced to Cu(I) with a thermal treatment that evolves CO2. After loading with hydrogen gas, the majority of H2 desorbs from the coordinatively saturated Cu(II) COF at temperatures < −100 °C. However, the activated Cu(I) COF retains adsorbed H2 above room temperature. Adsorption/desorption of H2 was highly reversible. Diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) strongly supports a molecular hydrogen interaction with Cu(I). A Kissinger analysis of variable ramp rate desorption experiments estimates the enthalpy of H2 desorption from Cu(I) at 15 kJ mol–1. The results represent an advance toward practical H2 storage and delivery in a lightweight, stable, and highly versatile material.
中文翻译：
铜负载共价有机骨架的热活化，用于近室温氢气的储存和输送
通过与苯酚和亚胺基团的配位，甲酸铜（II）被有效地掺入基于2D亚胺的共价有机骨架（COF）的孔中。然后通过产生CO 2的热处理将配位的金属离子还原为Cu（I）。充满氢气后，大多数H 2在<-100°C的温度下从配位饱和的Cu（II）COF中解吸。但是，活化的Cu（I）COF在室温以上会保留吸附的H 2。H 2的吸附/解吸是高度可逆的。漫反射红外傅里叶变换光谱（DRIFTS）强烈支持分子氢与Cu（I）的相互作用。对可变斜率解吸实验的基辛格分析估计了15 kJ mol –1时H 2从Cu（I）解吸的焓。结果表明，以轻便，稳定且用途广泛的材料向实用的H 2储存和输送迈进了一步。
更新日期：2020-02-07
中文翻译：
铜负载共价有机骨架的热活化，用于近室温氢气的储存和输送
通过与苯酚和亚胺基团的配位，甲酸铜（II）被有效地掺入基于2D亚胺的共价有机骨架（COF）的孔中。然后通过产生CO 2的热处理将配位的金属离子还原为Cu（I）。充满氢气后，大多数H 2在<-100°C的温度下从配位饱和的Cu（II）COF中解吸。但是，活化的Cu（I）COF在室温以上会保留吸附的H 2。H 2的吸附/解吸是高度可逆的。漫反射红外傅里叶变换光谱（DRIFTS）强烈支持分子氢与Cu（I）的相互作用。对可变斜率解吸实验的基辛格分析估计了15 kJ mol –1时H 2从Cu（I）解吸的焓。结果表明，以轻便，稳定且用途广泛的材料向实用的H 2储存和输送迈进了一步。
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