Jiawei Zhang, Jingjing Ma, Chen Liu, Qi Wang, Yiling Xu, Long Fang, Kai Xia, Deshuai Sun
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引用次数: 0
摘要
环境友好和高吸附容量是二氧化碳吸附剂的重要特性。生物基金属有机框架(bioMOFs)材料在捕获二氧化碳方面具有显著优势。氨基酸如 l-谷氨酸(Glu)和 L-天冬氨酸(Asp)被用作配体,用于合成生物MOFs、Asp-Cu 和 Glu-Cu。表征结果证实,Asp-Cu 和 Glu-Cu 分别具有叔胺和仲胺结构。在 1 bar CO2 压力下,Glu-Cu 和 Asp-Cu 的吸附容量分别达到 253 mg-g-1 和 277 mg-g-1;在 0.15 bar CO2 压力下,Glu-Cu 和 Asp-Cu 的吸附容量分别达到 190 mg-g-1 和 223 mg-g-1。在温度、含水量、二氧化硫浓度和其他成分等不同条件下,对生物MOFs 的二氧化碳吸附性能进行了全面评估。吸附数据与伪一阶动力学和 Weber-Morris 粒子内扩散模型拟合良好。动力学研究表明,少量的水会明显加快伪一阶动力学常数,而过量的水蒸气则会极大地阻碍 CO2 的内扩散常数。由于二氧化硫与 MOF 表面的活性位点发生了快速反应,二氧化硫的存在导致这两种 MOF 的吸附能力下降。此外,这些生物 MOF 易于回收和再生,至少可循环使用 20 次。主要的二氧化碳吸附机制涉及 Asp-Cu 上的催化水化反应,而化学吸附则发生在 Glu-Cu 上。这两种机制都伴随着物理吸附。
Bio-base Metal Organic Frameworks as Potential CO2 Adsorbents
Environmental friendliness and high adsorption capacity are important properties of CO2 adsorbents. Bio-based metal–organic framework (bioMOFs) materials offer notable benefits for CO2 capture. Amino acids like l-glutamic acid (Glu) and L-aspartate (Asp) are employed as ligands for the synthesis of bioMOFs, Asp-Cu and Glu-Cu. Characterization results confirmed that Asp-Cu and Glu-Cu possessed tertiary amine and secondary amine structures, respectively. The adsorption capacities of Glu-Cu and Asp-Cu were up to 253 mg·g−1 and 277 mg·g−1 at 1 bar CO2 pressure and 190 mg·g−1 and 223 mg·g−1 at 0.15 bar CO2 pressure. The CO2 adsorption properties of bioMOFs were comprehensively evaluated under various conditions, including temperature, water content, SO2 concentration, and other compositions. Adsorption data were fitted well with the pseudo-first-order kinetics and Weber-Morris intraparticle diffusion model. The kinetic studies revealed that a small amount of water significantly accelerated the pseudo-first-order kinetic constants, whereas excess water vapor greatly hindered the intra-diffusion constants of CO2. The presence of SO2 led to a decrease in the adsorption capacity of both MOFs due to rapid reactions occurring with active sites on the MOF surface. Furthermore, these bioMOFs were easily recovered and regenerated for at least 20 cycles. The primary CO2 adsorption mechanism involved catalytic hydration reactions on Asp-Cu, while chemical adsorption occurred on Glu-Cu. Both mechanisms were accompanied by physical adsorption.
期刊介绍:
The Korean Journal of Chemical Engineering provides a global forum for the dissemination of research in chemical engineering. The Journal publishes significant research results obtained in the Asia-Pacific region, and simultaneously introduces recent technical progress made in other areas of the world to this region. Submitted research papers must be of potential industrial significance and specifically concerned with chemical engineering. The editors will give preference to papers having a clearly stated practical scope and applicability in the areas of chemical engineering, and to those where new theoretical concepts are supported by new experimental details. The Journal also regularly publishes featured reviews on emerging and industrially important subjects of chemical engineering as well as selected papers presented at international conferences on the subjects.