期刊
FUEL
卷 327, 期 -, 页码 -出版社
ELSEVIER SCI LTD
DOI: 10.1016/j.fuel.2022.125085
关键词
Competitive coordination-removal strategy; Benzoic acid modification; Defective MOFs; Catalytic transfer hydrogenation; Furfural
资金
- Natural Science Foundation of China [21975284, 22005342]
- Fundamental Research Funds for the Central Universities [20CX02217A]
- Opening Fund of State Key Laboratory of Heavy Oil Processing
- Shandong Provincial Natural Science Foundation [ZR2020QE058]
- QLUT Special Funding for Distinguished Scholars [2419010420]
By using a competitive coordination-removal strategy with benzoic acid as a modulator, this study synthesized defective MOF-808 (D-x-MOF-808) for the highly efficient production of furfuryl alcohol from furfural. The addition of HBC can control ligand deficiency and the number of exposed Zr sites, leading to excellent catalytic performance.
The highly efficient production of furfuryl alcohol (FFA) from biomass-derived furfural (FFR) is attracting increasing attention due to its wide application in the production of value-added chemicals. Zr-based MOF-808 is promising for liquid catalytic transfer hydrogenation (CTH) of FFR to FFA in terms of possessing a great number of Lewis-acid sites. Herein, a series of defective MOF-808 (D-x-MOF-808) samples were prepared via a competitive coordination-removal strategy by modulating with benzoic acid (HBC). HBC was introduced as the temporary ligand for competing with formal ligand 1,3,5-benzenetricarboxylic acid (H3BTC) to coordinate with metal clusters and then it was removed with methanol to obtain the D-x-MOF-808. The results showed that HBC serves not only as a temporary ligand participating in the synthesis of MOF-808 to obtain defective structure but also as a modulator controlling the particle size by terminating the growth of crystals. By changing the amount of HBC addition, the degree of ligand deficiency and the number of exposed Zr sites can be well regulated. Especially, excellent performance of FFR conversion (99%), FFA selectivity (94.4%) and FFA formation rate (48.6 mmol.g(-1).h(-1)) was achieved over D-40-MOF-808 sample with 2-propanol as a hydrogen donor under mild conditions (90 degrees C, 2 h), ranking it the best among the reported catalysts. Detailed characterizations proved that the high activity of D-40-MOF-808 was jointly influenced by the high surface area, the high content of exposed Zr metal sites and ligand deficiency.
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