Investigation of hydrogen adsorption sites in ferrocene-based hypercrosslinked polymers by DFT calculations
Herein, two types of Fc-based hypercrosslinked polymers (HHCP and DHCP) with high BET surface area (953.9 and 1062.7 m2 g−1) were prepared by direct one-step phenolic polycondensation aiming at high uptake capacity towards H2. As expected, the hydrogen uptake values of HHCP and DHCP were notably hig...
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| Format: | Article |
| Language: | English |
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Elsevier
2023-05-01
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| Series: | Journal of Materials Research and Technology |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S2238785423009973 |
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| author | Qi Peng Hongwei Zhao Qilin Yang Guang Chen Xinxiu Cao Shaohui Xiong Anguo Xiao Gen Li Bo Liu Qingquan Liu |
| author_facet | Qi Peng Hongwei Zhao Qilin Yang Guang Chen Xinxiu Cao Shaohui Xiong Anguo Xiao Gen Li Bo Liu Qingquan Liu |
| author_sort | Qi Peng |
| collection | DOAJ |
| description | Herein, two types of Fc-based hypercrosslinked polymers (HHCP and DHCP) with high BET surface area (953.9 and 1062.7 m2 g−1) were prepared by direct one-step phenolic polycondensation aiming at high uptake capacity towards H2. As expected, the hydrogen uptake values of HHCP and DHCP were notably higher than those of porous polymers with a higher surface area under the same conditions. The maximum H2 uptake of HCPs at 77 K/1.0 bar are determined to be 2.51 wt % for HHCP and 2.74 wt % for DHCP, respectively. Despite the pore structure playing a determinant role in hydrogen adsorption, the adsorption sites in the polymer framework can be another essential factor to influence the hydrogen adsorption capacity. The interactions between the Fc building block and H2 are revealed by DFT calculation to fully illustrate the role of Fc in H2 adsorption. The results indicate that both iron atoms and benzene rings in Fc-based HCPs contribute to the adsorption of hydrogen. Moreover, it is interesting to find that the most stable adsorption site around the Fc building unit is the position directly above the Cp ring. The results in this work may more reasonably explain the phenomenon that the introduction of Fc units could enhance the adsorption of H2 in many studies, which also provides possible insights into the application of metallocene compounds in H2 adsorption. |
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| issn | 2238-7854 |
| language | English |
| last_indexed | 2024-03-13T04:07:58Z |
| publishDate | 2023-05-01 |
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| spelling | doaj.art-0811678908984c50bae04b27012863a22023-06-21T06:57:29ZengElsevierJournal of Materials Research and Technology2238-78542023-05-012471897197Investigation of hydrogen adsorption sites in ferrocene-based hypercrosslinked polymers by DFT calculationsQi Peng0Hongwei Zhao1Qilin Yang2Guang Chen3Xinxiu Cao4Shaohui Xiong5Anguo Xiao6Gen Li7Bo Liu8Qingquan Liu9School of Material Science and Engineering, Hunan Provincial Key Laboratory of Advanced Materials for New Energy Storage and Conversion, Hunan University of Science and Technology, Xiangtan, 411201, ChinaSchool of Material Science and Engineering, Hunan Provincial Key Laboratory of Advanced Materials for New Energy Storage and Conversion, Hunan University of Science and Technology, Xiangtan, 411201, China; Corresponding author.School of Material Science and Engineering, Hunan Provincial Key Laboratory of Advanced Materials for New Energy Storage and Conversion, Hunan University of Science and Technology, Xiangtan, 411201, ChinaSchool of Material Science and Engineering, Hunan Provincial Key Laboratory of Advanced Materials for New Energy Storage and Conversion, Hunan University of Science and Technology, Xiangtan, 411201, ChinaSchool of Material Science and Engineering, Hunan Provincial Key Laboratory of Advanced Materials for New Energy Storage and Conversion, Hunan University of Science and Technology, Xiangtan, 411201, ChinaSchool of Material Science and Engineering, Hunan Provincial Key Laboratory of Advanced Materials for New Energy Storage and Conversion, Hunan University of Science and Technology, Xiangtan, 411201, ChinaSchool of Material Science and Engineering, Hunan Provincial Key Laboratory of Advanced Materials for New Energy Storage and Conversion, Hunan University of Science and Technology, Xiangtan, 411201, China; Hunan Provincial Key Laboratory of Water Treatment Functional Materials, Hunan University of Arts and Science, Changde, 415000, China; Corresponding author. Hunan Provincial Key Laboratory of Water Treatment Functional Materials, Hunan University of Arts and Science, Changde 415000, China.School of Material Science and Engineering, Hunan Provincial Key Laboratory of Advanced Materials for New Energy Storage and Conversion, Hunan University of Science and Technology, Xiangtan, 411201, ChinaSchool of Material Science and Engineering, Hunan Provincial Key Laboratory of Advanced Materials for New Energy Storage and Conversion, Hunan University of Science and Technology, Xiangtan, 411201, China; Hunan Provincial Key Laboratory of Water Treatment Functional Materials, Hunan University of Arts and Science, Changde, 415000, ChinaSchool of Material Science and Engineering, Hunan Provincial Key Laboratory of Advanced Materials for New Energy Storage and Conversion, Hunan University of Science and Technology, Xiangtan, 411201, China; Corresponding author.Herein, two types of Fc-based hypercrosslinked polymers (HHCP and DHCP) with high BET surface area (953.9 and 1062.7 m2 g−1) were prepared by direct one-step phenolic polycondensation aiming at high uptake capacity towards H2. As expected, the hydrogen uptake values of HHCP and DHCP were notably higher than those of porous polymers with a higher surface area under the same conditions. The maximum H2 uptake of HCPs at 77 K/1.0 bar are determined to be 2.51 wt % for HHCP and 2.74 wt % for DHCP, respectively. Despite the pore structure playing a determinant role in hydrogen adsorption, the adsorption sites in the polymer framework can be another essential factor to influence the hydrogen adsorption capacity. The interactions between the Fc building block and H2 are revealed by DFT calculation to fully illustrate the role of Fc in H2 adsorption. The results indicate that both iron atoms and benzene rings in Fc-based HCPs contribute to the adsorption of hydrogen. Moreover, it is interesting to find that the most stable adsorption site around the Fc building unit is the position directly above the Cp ring. The results in this work may more reasonably explain the phenomenon that the introduction of Fc units could enhance the adsorption of H2 in many studies, which also provides possible insights into the application of metallocene compounds in H2 adsorption.http://www.sciencedirect.com/science/article/pii/S2238785423009973H2 uptakeAdsorption sitesDFT calculation |
| spellingShingle | Qi Peng Hongwei Zhao Qilin Yang Guang Chen Xinxiu Cao Shaohui Xiong Anguo Xiao Gen Li Bo Liu Qingquan Liu Investigation of hydrogen adsorption sites in ferrocene-based hypercrosslinked polymers by DFT calculations Journal of Materials Research and Technology H2 uptake Adsorption sites DFT calculation |
| title | Investigation of hydrogen adsorption sites in ferrocene-based hypercrosslinked polymers by DFT calculations |
| title_full | Investigation of hydrogen adsorption sites in ferrocene-based hypercrosslinked polymers by DFT calculations |
| title_fullStr | Investigation of hydrogen adsorption sites in ferrocene-based hypercrosslinked polymers by DFT calculations |
| title_full_unstemmed | Investigation of hydrogen adsorption sites in ferrocene-based hypercrosslinked polymers by DFT calculations |
| title_short | Investigation of hydrogen adsorption sites in ferrocene-based hypercrosslinked polymers by DFT calculations |
| title_sort | investigation of hydrogen adsorption sites in ferrocene based hypercrosslinked polymers by dft calculations |
| topic | H2 uptake Adsorption sites DFT calculation |
| url | http://www.sciencedirect.com/science/article/pii/S2238785423009973 |
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