Huang Hangyu, Wang Weiyun, Yuan Ziyi, Li Sihao, Zhou Can
College of Energy and Environment, Shenyang Aerospace University, Shenyang 110136, China.
College of Energy and Environment, Shenyang Aerospace University, Shenyang 110136, China; Key Laboratory of Clean Energy, Liaoning Province, Shenyang 110136, China.
Int J Biol Macromol. 2025 Jun;311(Pt 3):143942. doi: 10.1016/j.ijbiomac.2025.143942. Epub 2025 May 4.
CO emission from fossil fuel combustion is still the main cause of greenhouse effect, designing CO solid adsorbents with high selective adsorbability remains challenging. In this study, cellulose nanofibers were modified by 3-aminopropyltriethoxysilane (APTES) for revealing the adsorption mechanism of CO by APTES modified cellulose aerogel. Based on Density Function Theory(DFT), it was calculated that the adsorption configurations, adsorption energy, and partial density of states of CO on the pristine and modified surfaces, which revealed at the atomic level the mechanism influenced by the APTES grafting. The results indicate that the CO adsorption properties of cellulose are improved with the increasing APTES loading. The method of GGA-PBE is most suitable for the cellulose unit cell in the DFT calculation; two most stable cellulose surfaces (100) and (001) were selected for the adsorption simulation. It is suggested that the pristine cellulose surfaces have extremely weak adsorption energy to CO, and the adsorption energy is significantly improved after the aminopropyl modification, and the modified (0 0 1) surface has the lowest adsorption energy, which is-1.766 eV. Projected density of state analysis indicates that the C atom on the (0 0 1) surface produces a lower peak with a wider span. The results of adsorption energy and PDOS jointly prove that after APTES modification, the (0 0 1) surface of cellulose has the strongest adsorption property, which enhances the adsorption properties of cellulose materials.
化石燃料燃烧产生的一氧化碳排放仍是温室效应的主要原因，设计具有高选择性吸附能力的一氧化碳固体吸附剂仍然具有挑战性。在本研究中，用3-氨丙基三乙氧基硅烷（APTES）对纤维素纳米纤维进行改性，以揭示APTES改性纤维素气凝胶对一氧化碳的吸附机理。基于密度泛函理论（DFT），计算了一氧化碳在原始表面和改性表面上的吸附构型、吸附能和态密度，从原子水平揭示了APTES接枝影响的机理。结果表明，随着APTES负载量的增加，纤维素对一氧化碳的吸附性能得到改善。GGA-PBE方法最适合DFT计算中的纤维素晶胞；选择两个最稳定的纤维素表面（100）和（001）进行吸附模拟。结果表明，原始纤维素表面对一氧化碳的吸附能极弱，氨基丙基改性后吸附能显著提高，改性后的（0 0 1）表面吸附能最低，为-1.766 eV。态密度投影分析表明，（0 0 1）表面的C原子产生的峰较低且跨度较宽。吸附能和态密度的结果共同证明，APTES改性后，纤维素的（0 0 1）表面具有最强的吸附性能，增强了纤维素材料的吸附性能。
