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| 001 | 631969 | ||
| 005 | 20250715151532.0 | ||
| 024 | 7 | _ | |a 10.1021/acsami.5c09657 |2 doi |
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| 100 | 1 | _ | |a Deka, Dhruba Jyoti |0 P:(DE-H253)PIP1114355 |b 0 |
| 245 | _ | _ | |a Tyrosinase Enzyme-Inspired Cu(I)-Porous Organic Polymer for Selective Oxidation of Biomass-Derived 5-HMF |
| 260 | _ | _ | |a Washington, DC |c 2025 |b Soc. |
| 336 | 7 | _ | |a article |2 DRIVER |
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| 520 | _ | _ | |a In biobased PET, terephthalic acid (TPA) can be replaced with biobase alternatives like bioderived 5-diformylfuran (DFF). In this work, we have selectively synthesized DFF from the oxidation of 5-hydroxymethylfurfural (HMF) using our tyrosinase enzyme-inspired catalysts vicinal V-Cu-POP and nonvicinal NV-Cu-POP, respectively. Motivated by the oxygenated form of tyrosinase, we introduced binuclear copper(I) moieties into a porous organic polymer to create enzyme-inspired heterogeneous catalysts for the selective oxidation of HMF. V-Cu-POP can effectively activate O$_2$ for mild and selective oxidation because the two Cu centers are in close proximity, which is impossible in the case of NV-Cu-POP. For the determination of the coordination environment of the catalytically active site, the X-ray absorption near-edge structure (XANES) studies and the copper(I) state for both the enzyme-inspired catalysts V-Cu-POP and NV-Cu-POP are identified through characteristic features in the absorption spectra. The fitting parameters and EXAFS spectra rule out the formation of the Cu–Cu bond. Further, the key intermediate μ-hydroxy species (Cu (II)–O–O–Cu (II)), which forms during the reaction in the case of the enzyme-inspired catalyst, V-Cu-POP is also confirmed by time-resolved in situ ATR-IR spectroscopy and DFT computational study. This intermediate is not formed in the case of nonvicinal NV-Cu-POP, which is the main reason for lower catalytic activity toward HMF oxidation. NV-Cu-POP still retains the peaks of reactants at the same reaction conditions, which is confirmed by time-resolved in situ ATR-IR spectroscopy. Overall, in this study, we have shown how a tyrosinase enzyme-inspired catalyst exhibits greater catalytic activity toward the oxidation reaction due to the formation of its vicinal conformer compared to the nonvicinal conformer. |
| 536 | _ | _ | |a 632 - Materials – Quantum, Complex and Functional Materials (POF4-632) |0 G:(DE-HGF)POF4-632 |c POF4-632 |f POF IV |x 0 |
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| 700 | 1 | _ | |a Boro, Bishal |0 P:(DE-HGF)0 |b 1 |
| 700 | 1 | _ | |a Chen, Yuping |0 P:(DE-HGF)0 |b 2 |
| 700 | 1 | _ | |a Chahal, Kapil |0 P:(DE-HGF)0 |b 3 |
| 700 | 1 | _ | |a Nandy, Subhajit |0 P:(DE-H253)PIP1108447 |b 4 |u desy |
| 700 | 1 | _ | |a Wang, Caiqi |0 P:(DE-HGF)0 |b 5 |
| 700 | 1 | _ | |a Lin, Hongfei |0 P:(DE-HGF)0 |b 6 |
| 700 | 1 | _ | |a Tang, Qing |0 P:(DE-HGF)0 |b 7 |
| 700 | 1 | _ | |a Mondal, John |0 P:(DE-H253)PIP1114361 |b 8 |e Corresponding author |
| 773 | _ | _ | |a 10.1021/acsami.5c09657 |g Vol. 17, no. 25, p. 36840 - 36854 |0 PERI:(DE-600)2467494-1 |n 25 |p 36840 - 36854 |t ACS applied materials & interfaces |v 17 |y 2025 |x 1944-8244 |
| 856 | 4 | _ | |u https://bib-pubdb1.desy.de/record/631969/files/Tyrosinase%20Enzyme-Inspired%20Cu%28I%29-Porous%20Organic%20Polymer%20for%20Selective%20Oxidation%20of%20Biomass-Derived%205-HMF%2C%20ACS%20Appl.%20Mater.%20%26%20Interfaces%2C%2017%20%2825%29%2C%2036840-36854%2C%20%282025%29.pdf |
| 856 | 4 | _ | |y Published on 2025-06-13. Available in OpenAccess from 2026-06-13. |u https://bib-pubdb1.desy.de/record/631969/files/Supporting%20Information%20for%20Review.pdf |
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| 856 | 4 | _ | |y Published on 2025-06-13. Available in OpenAccess from 2026-06-13. |x pdfa |u https://bib-pubdb1.desy.de/record/631969/files/Supporting%20Information%20for%20Review.pdf?subformat=pdfa |
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