Magnetically Assembled Photonic Crystal Gels with Wide Thermochromic Range and High Sensitivity.

Thermochromic poly(N-isopropyl acrylamide) (PNIPAM) photonic crystal gels based on 1D magnetically assembling colloidal nanocrystal clusters have attracted much attention due to its convenient preparation process, striking color response, and good mechanical strength. However, there remain challenges to broaden the thermochromic range and improve the sensitivity for their iridescent color display. Here, a PNIPAM photonic gel with wide thermochromic range and high sensitivity is prepared by using four-arm star poly(ethylene glycol) acrylamide (PEGAAm) as cross-linker at appropriately reduced magnetic field strength as well as cross-linker content. PEGAAm improves the homogeneity of the microstructure in PNIPAM photonic gel and thus maintains the structure colors at a wide temperature range from room temperature to 44 °C. The reduced magnetic field strength of 70 Gs and low cross-linker content (the molar ratio of monomer to cross-linker of 300:1) lead to a large initial lattice spacing of the photonic gel and thus wide diffraction wavelength migration of 194 nm. This optimized PNIPAM gel exhibits vivid iridescent colors from orange-red to indigo blue as temperature increases from 20 to 44 °C with satisfactory repeatability. Therefore, it may be an ideal candidate for temperature sensors and displays with utility and accuracy such as low-temperature burns.

Implanting Atomic Dispersed Ru in PtNi Colloidal Nanocrystal Clusters for Efficient Catalytic Performance in Electro-oxidation of Liquid Fuels.

Although PtRu alloy nanocatalysts have been certified to possess excellent electrocatalytic performance and CO-poisoning tolerance toward formic acid and methanol electro-oxidation, the unaffordable usages of ruthenium (Ru) and platinum (Pt) have greatly limited their widespread adoption. Here, a facile one-pot method is reported for implanting atomic dispersed Ru in PtNi colloidal nanocrystal clusters with different Ru/Pt/Ni molar ratios, greatly reducing the dosages of Pt and Ru, and further improving the catalytic performances for the electro-oxidation of formic acid and methanol. Through simple control of the amount of Ni(acac)2 precursor, trimetallic Ru0.3 Pt70.5 Ni29.2 , Ru0.6 Pt55.9 Ni43.5 , Ru0.2 Pt77.3 Ni22.5 , and Ru0.9 Pt27.3 Ni71.8 colloidal nanocrystal clusters (CNCs) are obtained. In particular, the Ru0.3 Pt70.5 Ni29.2 CNCs exhibit excellent specific activities for formic acid and methanol electro-oxidation, that is, 14.2 and 15.3 times higher, respectively, than those of the Pt/C catalyst. Moreover, the Ru0.3 Pt70.5 Ni29.2 CNCs also possess better anti-CO-poisoning properties and diffusion ability than the other RuPtNi CNCs. The excellent formic acid and methanol electro-oxidation activities of RuPtNi CNCs are ascribed to the optimal ligand effects derived from the Pt, Ni, and atomic dispersed Ru atoms, which can improve the OH adsorption ability and further the anti-CO-poisoning capability. This research opens a new door for increasing the electro-oxidation properties of liquid fuels by using lower dosages of noble metals in Pt-based catalysts.

Libraries of Uniform Magnetic Multicore Nanoparticles with Tunable Dimensions for Biomedical and Photonic Applications.

Multicore iron oxide nanoparticles, also known as colloidal nanocrystal clusters, are magnetic materials with diverse applications in biomedicine and photonics. Here, we examine how both of their characteristic dimensional features, the primary particle and sub-micron colloid diameters, influence their magnetic properties and performance in two different applications. The characterization of these basic size-dependent properties is enabled by a synthetic strategy that provides independent control over both the primary nanocrystal and cluster dimensions. Over a wide range of conditions, electron microscopy and X-ray diffraction reveal that the oriented attachment of smaller nanocrystals results in their crystallographic alignment throughout the entire superstructure. We apply a sulfonated polymer with high charge density to prevent cluster aggregation and conjugate molecular dyes to particle surfaces so as to visualize their collection using handheld magnets. These libraries of colloidal clusters, indexed both by primary nanocrystal dimension (dp) and overall cluster diameter (Dc), form magnetic photonic crystals with relatively weak size-dependent properties. In contrast, their performance as MRI T2 contrast agents is highly sensitive to cluster diameter, not primary particle size, and is optimized for materials of 50 nm diameter (r2 = 364 mM-1 s-1). These results exemplify the relevance of dimensional control in developing applications for these versatile materials.

One-pot synthesis of magnetic colloidal nanocrystal clusters coated with chitosan for selective enrichment of glycopeptides.

Selective enrichment of glycopeptides prior to the mass spectrometry (MS) analysis is essential due to ion suppression effect during ionization caused by the co-presence of non-glycosylated peptides. Among the enrichment approaches, hydrophilic interaction liquid chromatography (HILIC) based on magnetic separation has become a popular method in recent years. As the conventional synthesis procedures of these materials are tedious and time-consuming with at least four steps. Herein, magnetic colloidal nanocrystal clusters coated with chitosan (Fe3O4@CS MCNCs) have been successfully prepared by a simple one-pot method. The resulting Fe3O4@CS MCNCs demonstrated an excellent ability for glycopeptide enrichment with high selectivity, low detection limit and high binding capacity. Furthermore, in the analysis of real complicated biological sample, 283 unique N-glycosylation sites corresponding to 175 glycosylated proteins were identified in three replicate analyses of 45µg protein sample extracted from HeLa cells, indicating the great potential in detection and identification of low abundant glycopeptides in glycoproteome analysis.