Experimental and DFT collaborative investigation on CO2 adsorption mechanism and interfacial chemical interactions of UiO-66-NH2/GO composite

作者：Lili Jiang, Xin Guo, Y. Zhang, Jingyu Zhang, Wei Zhang, Wenfeng Lu, Meng Liu, Zhengbiao Hu, Jianfa Jing, Fuling Tang, Haitao Yu · 发表于：Chemical Engineering Journal · 年份：2025 · DOI：10.1016/j.cej.2025.165488 · 被引用次数：11 · 研究领域：Carbon Dioxide Capture Technologies、Metal-Organic Frameworks: Synthesis and Applications、Covalent Organic Framework Applications

With the escalating severity of global climate change, developing efficient CO₂ adsorption materials has become a pivotal advancement in achieving the “dual carbon” targets. In the present investigation, a graphene oxide (GO)-enhanced metal-organic framework composite (UiO-66-NH 2 /GO) was synthesised via an in-situ method. The influence on CO 2 adsorption performance was comprehensively assessed, alongside exploring the adsorption mechanism and interfacial chemical interactions. Experimental outcomes revealed that at a GO loading of 3 wt%, the UiO-66-NH 2 /GO composite exhibited a CO 2 adsorption capacity of 64.38 cm 3 /g at 298 K, denoting a 53.46% enhancement relative to pure UiO-66-NH 2 (41.95 cm 3 /g) and 1.91 times the benchmark for industrial adsorbents (33.60 cm 3 /g). Following seven adsorption-desorption cycles, the retention rate of the composite's adsorption capacity remained at 98%, indicating excellent potential for CO 2 capture. Furthermore, density functional theory calculations were employed to elucidate the structural configuration of UiO-66-NH 2 /GO and to interpret the CO 2 adsorption mechanism. The results demonstrate that Zr O clusters and GO established strong electronic coupling (energy transfer of 6.98 eV) at the interface, generating multiple adsorption sites. The primary adsorption site I (Zr cluster site) demonstrated a CO 2 adsorption energy of −0.77 eV, whereas the secondary adsorption site II (–NH 2 group site) exhibited an energy of −0.54 eV, s...