Microwave-Assisted Rapid Synthesis of Well-Shaped MOF-74 (Ni) for CO2 Efficient Capture
Microwave-Assisted Rapid Synthesis of Well-Shaped MOF-74 (Ni) for CO2 Efficient Capture
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微波辅助快速合成形状良好的 MOF-74 (Ni) 以实现 CO2 高效捕获
DOI：
10.1021/acs.inorgchem.8b03271
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发表时间：
2019-02-18
影响因子：
4.6
通讯作者：
He, Chi
中科院分区：
文献类型：
--
作者：
Chen, Changwei;Feng, Xiangbo;He, Chi
在本工作中，分别通过水热（HT）、冷凝回流（CE）和微波辅助（MW）方法制备了一系列具有窄微孔通道和丰富的不饱和金属位点的MOF-74（Ni）材料。通过粉末X射线衍射、N-2吸附、场发射扫描电子显微镜、傅里叶变换红外(FTIR)、热重(TG)/TG-FTIR、X射线光电子能谱、紫外-可见-近红外、NH3/CO2-程序升温脱附等手段对合成材料的理化性质进行了表征。 原位漫反射红外傅立叶变换光谱。通过等温吸附和动态吸附实验评价其CO2/N-2吸附性能。我们发现，MW 是合成具有高效 CO2 捕获能力的 MOF-74 (Ni) 材料的快速简便的方案。通过MW工艺可以在60分钟内获得形状良好的MW-140吸附剂，其在25℃下具有5.22 mmol/g的优异CO2吸附容量，几乎比商业活性炭（0.89 mmol/g）高出6倍。动态吸附实验结果表明，MW-140材料在潮湿条件下（RH = 90%）具有最高的CO2吸附容量，为3.37 mmol/g。重要的是，MW-140具有优异的吸附稳定性和可回收性、优异的CO2捕获选择性（CO2/N-2 = 31）以及适当的CO2吸附等量热（21-38 kJ/mol），使其成为工业CO2捕获的有前途和潜力的材料。表征结果表明，MOF-74（Ni）材料的高捕获能力可归因于丰富的狭窄微孔通道和丰富的五配位Ni2+开放金属位点的协同效应，有利于捕获CO2分子。
In the present work, a series of MOF-74 (Ni) materials with narrow micropore channels and abundant unsaturated metal sites was respectively prepared via hydro thermal (HT), condensation reflux (CE), and microwave assisted (MW) methods. The physicochemical properties of synthesized materials were characterized by powder X-ray diffraction, N-2-sorption, field-emission scanning electron microscopy, Fourier-transform infrared (FTIR), thermogravimetric (TG)/TG-FTIR, X-ray photoelectron spectroscopy, UV-vis-near infrared, NH3/CO2-temperature programmed desorption, and in situ diffuse reflectance infrared Fourier transform spectroscopy. Their CO2/N-2 adsorption performances were evaluated by isotherm adsorption and dynamic adsorption experiments. We found that the MW is a rapid and facile protocol for the synthesis of MOF-74 (Ni) materials with highly efficient CO2 capture capacity. The well-shaped MW-140 adsorbent with superior CO2 adsorption capacity of 5.22 mmol/g at 25 degrees C can be obtained within 60 min by the MW process, almost 6 times higher than that of the commercial activated carbon (0.89 mmol/g). Results of dynamic adsorption experiments showed that the MW-140 material possesses the highest CO2 adsorption capacity of 3.37 mmol/g under humid conditions (RH = 90%). Importantly, MW-140 has excellent adsorption stability and recyclability, superior CO2 capture selectivity (CO2/N-2 = 31), and appropriate isosteric heat in CO2 adsorption (21-38 kJ/mol), making it a promising and potential material for industrial CO2 capture. Characterization results demonstrated that the high capture capability of MOF-74 (Ni) materials can be attributed to the synergistic effect of abundant narrow micropore channels and rich five-coordinated Ni2+ open metal sites which are beneficial for the trapping of CO2 molecules.