Hybrid Microgels with Confined Needle-like Lanthanide Phosphate Nanocrystals
Bibliographic record
Abstract
We describe the room-temperature synthesis and characterization of needle-like lanthanide phosphate (LnPO 4 ) nanocrystals in water, based on in situ precipitation of LnPO 4 using functional aqueous microgels as a soft nanoreactor. The poly(NIPAm/VCL/MAA) microgels were prepared by the copolymerization of N -isopropylacrylamide, N -vinylcaprolactam, and methacrylic acid. Our goal was to prepare Ln-encoded microgels suitable for bead-based biological assays employing mass cytometry. The low solubility of nanocrystalline LnPO 4 avoids the problem of Ln ion leakage from the microgels. The main challenge was to find appropriate conditions to confine the LnPO 4 precipitate to the interior of the microgels. Various sources of phosphate ions led to precipitation of LnPO 4 on the exterior of the microgels. One approach worked. It involved three steps: neutralization of the MAA groups in the microgels with NaOH, ion exchange with a lanthanide salt, followed by treatment with a large excess of PBS buffer at pH 7.4. In this way, we obtained microgels containing ca. 10 7 Ln atoms per microgel (Ln = La, Nd, Eu, Tb, Ho, Tm). The microgels were shown to be uniform in size by dynamic light scattering and transmission electron microscopy. The LnPO 4 -containing microgels showed much higher stability against leakage of metals to acidic buffers compared to the LnF 3 -containing microgels reported previously [ Lin, W.; Langmuir 2011, 27, 7265]. Small-angle X-ray scattering measurements and selected area electron diffraction data showed striking differences in the internal structure of hybrid microgels containing TbPO 4 from those containing TbF 3 . The TbF 3 -containing microgels had a core–shell structure with an amorphous TbF 3 core, whereas the TbPO 4 microgels contained needle-like nanocrystals (width ca. 2 nm, lengths on the order of 80 nm) distributed throughout the structure. These microgels are very promising materials for biological assays based on mass cytometry.
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How this classification was reachedexpand
Full frame machine prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.
Distilled classifier scores by category (both heads)
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.001 | 0.000 |
Machine scores (provisional)
The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.
Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one source (direct Gemma or distilled Codex), not a consensus.
How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".