Reversible Emulsions from Polyoxometalate-Polymer: A Robust Strategy to Cyclic Emulsion Catalysis and High-Internal-Phase Emulsion Materials.

Reversible Pickering emulsions, achieved by switchable, interfacially active colloidal particles, that enable on-demand emulsification/demulsification or phase inversion, hold substantial promise for biphasic catalysis, emulsion polymerization, cutting fluids, and crude oil pipeline transportation. However, particles with such a responsive behavior usually require complex chemical syntheses and surface modifications, limiting their extensive use. Herein, we report a simple route to generate emulsions that can be controlled and reversibly undergo phase inversion. The emulsions are prepared and stabilized by the interfacial assembly of polyoxometalate (POM)-polymer, where their electrostatic interaction at the interface is dynamic. The wettability of the POMs that dictates the emulsion type can be readily regulated by tuning the number of polymer chains bound to POMs, which, in turn, can be controlled by varying the concentrations of both components and the water/oil ratio. In addition, the number of polymer chains anchored to the POMs can be varied by controlling the number of negative charges on the POMs through an in situ redox reaction. As such, a reversible inversion of the emulsions can be triggered by switching between exposure to ultraviolet light and the introduction of oxygen. Combining the functions of POM itself, a cyclic interfacial catalysis system was realized. Inversion of the emulsion also affords a pathway to high-internal-phase emulsions. The diversity of the POMs, the polymers, and the responsive switching groups open numerous new, simple strategies for designing a wide range of responsive soft matter for cargo loading, controlled release, and delivery in biomedical and engineering applications without time-consuming particle syntheses.

Recent progress in emulsion gels: from fundamentals to applications.

Emulsion gels, also known as gelled emulsions or emulgels, have garnered great attention both in fundamental research and practical applications due to their superior stability, tunable morphology and microstructure, and promising mechanical and functional properties. From an application perspective, attention in this area has been, historically, mainly focused on food industries, e.g., engineering emulsion gels as fat substitutes or delivery systems for bioactive food ingredients. However, a growing body of studies has, in recent years, begun to demonstrate the full potential of emulsion gels as soft templates for designing advanced functional materials widely applied in a variety of fields, spanning chemical engineering, pharmaceutics, and materials science. Herein, a concise and comprehensive overview of emulsion gels is presented, from fundamentals to applications, highlighting significant recent progress and open questions, to scout for and deepen their potential applications in more fields.

Serum NFL discriminates Parkinson disease from essential tremor and reflect motor and cognition severity.

OBJECTIVE: To investigate the diagnostic value of serum neurofilament light chain (NFL) for discriminating Parkinson disease (PD) from Essential tremor (ET) and healthy controls, and to evaluate its correlation with some clinical features of PD patients. METHODS: This cross-sectional study measured NFL levels with electrochemiluminescence immunoassay in serum of 146 PD patients, 82 ET patients and 60 age-matched healthy controls. We used multivariate regression analyses to examine whether NFL contributes to PD biomarkers. Disease severity were assessed by Unified Parkinson's Disease Rating Scale part III (UPDRS III), Hoehn & Yahr (H-Y) stage and Mini-Mental State Examination (MMSE). RESULTS: Serum NFL levels were significantly higher in PD than in ET and healthy controls (16.6 ± 3.5, 12.2 ± 2.4 and 11.8 ± 2.4 pg/mL, respectively, p < 0.001). In patients with PD, serum NFL were markedly increased in patients with advanced H-Y stage and patients with dementia (both p < 0.001). The correlation analysis revealed that serum NFL was positively associated with UPDRS III score (r = 0.79, p < 0.001) and H-Y stage (r = 0.86, p < 0.001), and negatively correlated with MMSE scores (r = - 0.70, p < 0.001). Further multivariate regression analyses showed that serum NFL was an independent contributor to motor symptom and cognition severity in PD patients (all p < 0.01). CONCLUSIONS: Serum NFL levels were markedly elevated may be a useful clinical biomarker for discriminating PD patients from ET and controls. Serum NFL may serve as a potential blood biomarker for motor and cognition severity of PD.

Recent Progress toward Physical Stimuli-Responsive Emulsions.

Emulsion as a fine dispersion of immiscible liquids has involved widespread applications in industry, pharmaceuticals, agriculture, and personal care. Stimuli-responsive emulsions capable of on-demand demulsification or changing their properties are required in many cases such as controllable release cargo, oil recovery, emulsifier recycling, and product separation, great progress is achieved in these areas. Among these various triggers, much effort is made to develop physical stimuli, due to the noninvasive and environmentally friendly characteristics. Physical stimuli-responsive emulsions provide plenty of valuable practical applications in the fields of sustainable industry, biomedical reaction, drug delivery. Here, the recent development in the field of emulsions in response to physical stimuli consisting of temperature, light, magnetic fields, electrical fields, etc., is summarized. The preparation methods and mechanisms of physical stimuli-responsive emulsions and their applications of catalysis reaction, drug delivery, and oil recovery are highlighted in this review. The future directions and outstanding problems of the physical stimuli-responsive emulsions are also discussed.

Inflammation/coagulopathy/fibrinolysis: Dynamic indicators of COVID-19 progression in patients with moderate COVID-19 in Wenzhou, China.

BACKGROUND: The majority of the coronavirus disease 2019 (COVID-19) non-survivors meet the criteria for disseminated intravascular coagulation (DIC). Although timely monitoring of clotting hemorrhagic development during the natural course of COVID-19 is critical for understanding pathogenesis, diagnosis, and treatment of the disease, however, limited data are available on the dynamic processes of inflammation/coagulopathy/fibrinolysis (ICF). METHODS: We monitored the dynamic progression of ICF in patients with moderate COVID-19. Out of 694 COVID-19 inpatients from 10 hospitals in Wenzhou, China, we selected 293 adult patients without comorbidities. These patients were divided into different daily cohorts according to the COVID-19 onset-time. Furthermore, data of 223 COVID-19 patients with comorbidities and 22 critical cases were analyzed. Retrospective data were extracted from electronic medical records. RESULTS: The virus-induced damages to pre-hospitalization patients triggered two ICF fluctuations during the 14-day course of the disease. C-reactive protein (CRP), fibrinogen, and D-dimer levels increased and peaked at day 5 (D) 5 and D9 during the 1st and 2nd fluctuations, respectively. The ICF activities were higher during the 2nd fluctuation. Although 12-day medication returned high CRP concentrations to normal and blocked fibrinogen increase, the D-dimer levels remained high on days 17 ±â€¯2 and 23 ±â€¯2 days of the COVID-19 course. Notably, although the oxygenation index, prothrombin time and activated partial thromboplastin time were within the normal range in critical COVID-19 patients at administration, 86% of these patients had a D-dimer level > 500 µg/L. CONCLUSION: COVID-19 is linked with chronic DIC, which could be responsible for the progression of the disease. Understanding and monitoring ICF progression during COVID-19 can help clinicians in identifying the stage of the disease quickly and accurately and administering suitable treatment.

Unexpected Elasticity in Assemblies of Glassy Supra-Nanoparticle Clusters.

Granular materials, composed of densely packed particles, are known to possess unique mechanical properties that are highly dependent on the surface structure of the particles. A microscopic understanding of the structure-property relationship in these systems remains unclear. Here, supra-nanoparticle clusters (SNPCs) with precise structures are developed as model systems to elucidate the unexpected elastic behaviors. SNPCs are prepared by coordination-driven assembly of polyhedral oligomeric silsesquioxane (POSS) with metal-organic polyhedron (MOP). Due to the disparity in sizes, the POSS-MOP assemblies, like their classic nanoparticles counterparts, ordering is suppressed, and the POSS-MOP mixtures will vitrify or jam as a function of decreasing temperature. An unexpected elasticity is observed for the SNPC assemblies with a high modulus that is maintained at temperatures far beyond the glass transition temperature. From studies on the dynamics of the hierarchical structures of SNPCs and molecular dynamic simulation, the elasticity has its origins in the interpenetration of POSS-ended arms. The physical molecular interpenetration and inter-locking phenomenon favors the convenient solution or pressing processing of the novel cluster-based elastomers.

The Interfacial Assembly of Polyoxometalate Nanoparticle Surfactants.

Polyoxometalates (POMs) using {Mo72V30} as an example, dissolved in water, can interact with amine-terminated polydimethylsiloxane (PDMS-NH2) dissolved in toluene at the water/toluene interface to form POM-surfactants that significantly lower the interfacial tension and can be used to stabilize liquids via interfacial elasticity. The jamming of the POM-surfactants at the water/oil interface with consequent wrinkling occurs with a decrease in the interfacial area. The packing density of the POM-surfactants at the interface can be tuned by varying the strength of screening with the addition of cations with differing hydrated radii.

The Microscopic Structure-Property Relationship of Metal-Organic Polyhedron Nanocomposites.

Monodispersed hairy nanocomposites with typical 2 nm (isophthalic acid)24 Cu24 metal-organic polyhedra (MOP) as a core protected by 24 polymer chains with controlled narrow molecular weight distribution has been probed by imaging and scattering studies for the heterogeneity of polymers in the nanocomposites and the confinement effect the MOPs imposing on anchored polymers. Typical confined-extending surrounded by one entanglement area is proposed to describe the physical states of the polymer chains. This model dictates the counterintuitive thermal and rheological properties and prohibited solvent exchange properties of the nanocomposites, whilst those polymer chain states are tunable and deterministic based on their component inputs. From the relationship between the structure and behavior of the MOP nanocomposites, a MOP-composited thermoplastic elastomer was obtained, providing practical solutions to improve mechanical/rheological performances and processabilities of inorganic MOPs.

Coordination-Supported Imidazolate Networks: Water- and Heat-Stable Mesoporous Polymers for Catalysis.

The poor water stability of most porous coordination polymers (PCPs) or metal-organic frameworks (MOFs) is widely recognized as a barrier hampering their practical applications. Here, a facile and scalable route to prepare metal-containing polymers with a good stability in boiling water (100 °C, 24 h) and air (up to 390 °C) is presented. The bifunctional 1-vinylimidazole (VIm) with a coordinating site and a polymerizable organic group is introduced as the building block. This core strategy includes the synthesis of a rigid monomer with four VIm branches through a coordination process at room temperature, followed by a radical polymerization. We refer to this material as coordination-supported imidazolate networks (CINs). Interestingly, CINs are composed of rich mesopores from 2-15 nm, as characterized by low-energy (60 kV) STEM-HAADF images. In particular, the stable CINs illustrate a high turnover frequency (TOF) of 779 h-1 in the catalytic oxidation of phenol with H2 O as the green solvent.

Self-Regulated Nanoparticle Assembly at Liquid/Liquid Interfaces: A Route to Adaptive Structuring of Liquids.

The controlled structuring of liquids into arbitrary shapes can be achieved in biphasic liquid media using the interfacial assemblies of nanoparticle surfactants (NP-surfactants), that consist of a polar nanoparticle "head group" bound to one or more hydrophobic polymer "tails". The nonequilibrium shapes of the suspended liquid phase can be rendered permanent by the jamming of the NP-surfactants formed and assembled at the interface between the liquids as the system attempts to minimize the interfacial area between the liquids. While critical to the structuring process, little is known of the dynamic mechanical properties of the NP-surfactant monolayer at the interface as it is dictated by the characteristics of the component, including NP size and concentration and the molecular weight and concentration of polymers bound to the NPs. Here we provide the first comprehensive understanding of the dynamic mechanical character of two-dimensional NP-surfactant assemblies at liquid/liquid interfaces. Our results indicate that the dynamics of NP-polymer interactions are self-regulated across multiple time scales and are associated with specific mesoscale interactions between self-similar and cross-complementary components. Furthermore, the mechanical properties of the NP-surfactant monolayer are tunable over a broad range and deterministic on the basis of those component inputs. This control is key to tailoring the functional attributes of the reconfigurable structured liquids to suit specific applications.

Dynamic Electrostatic Interfacial Engineering for Block Copolymer Microparticles with Reversible Structures.

Responsive nanoparticle surfactants (NPSs) can dynamically and reversibly modulate the interfacial interactions between incompatible components, which are essential in the interfacial catalysis, corrosion, and self-assembly of block copolymers (BCPs). However, NPSs with stimuli-responsive behavior often involve tedious chemical synthesis and surface modifications. Herein, we propose a strategy to in situ construct a kind of dynamic and reversible NPSs by the interfacial electrostatic interaction between the negatively charged nanoparticles (NPs) and the positively charged homopolymers. The NPSs assembled at the oil/water interface reduce the interfacial tension and direct the confined assembly of BCP. Meanwhile, the dynamic NPSs can be disassembled by increasing the pH value or introducing competitive electrostatic attractions, which can dynamically and reversibly change the interfacial properties as well as the alignment of polymer chains, enabling BCP microparticles with reversibly switchable lamellar and cylindrical structures. Furthermore, by the introduction of aggregation-induced emission luminogens as tails to the NPSs, the reversible transformation of BCP microparticles can be visualized by fluorescence emission, which is dependent on the nanostructures of microparticles. This work establishes a concept for dynamically manipulating interfacial interactions and reversibly switching BCP microparticles without time-consuming NPS synthesis, showing promising applications in the fabrication of smart materials with switchable structures and properties.

Electric, magnetic, and shear field-directed assembly of inorganic nanoparticles.

Ordered assemblies of inorganic nanoparticles (NPs) have shown tremendous potential for wide applications due to their unique collective properties, which differ from those of individual NPs. Various assembly methods, such as external field-directed assembly, interfacial assembly, template assembly, biomolecular recognition-mediated assembly, confined assembly, and others, have been employed to generate ordered inorganic NP assemblies with hierarchical structures. Among them, the external field-directed assembly method is particularly fascinating, as it can remotely assemble NPs into well-ordered superstructures. Moreover, external fields (e.g., electric, magnetic, and shear fields) can introduce a local and/or global field intensity gradient, resulting in an additional force on NPs to drive their rotation and/or translation. Therefore, the external field-directed assembly of NPs becomes a robust method to fabricate well-defined functional materials with the desired optical, electronic, and magnetic properties, which have various applications in catalysis, sensing, disease diagnosis, energy conversion/storage, photonics, nano-floating-gate memory, and others. In this review, the effects of an electric field, magnetic field, and shear field on the organization of inorganic NPs are highlighted. The methods for controlling the well-ordered organization of inorganic NPs at different scales and their advantages are reviewed. Finally, future challenges and perspectives in this field are discussed.

Preparation of Janus Droplets and Hydrogels with Controllable Morphologies by an Aqueous Two-Phase System on the Superamphiphobic Surface.

Janus particles, having the property integration of each component, have attracted increasing attention due to their considerable potential in the field of material engineering applications. However, organic solvents or sophisticated equipment during the fabrication processes is generally inevitable. Here, we report a facile route to prepare Janus droplets and hydrogels via aqueous two-phase systems (ATPS). Simply merging two polymers, i.e., polyethylene glycol (PEG) and dextran (DEX), as aqueous droplets on a superamphiphobic surface leads to phase separation, provided that their concentrations exceed the threshold in the mixed aqueous droplets, thus generating a Janus structure. Various morphologies of such Janus droplets can be well controlled by manipulating the locations of these two polymers' concentration on the phase diagram, and the evolution of the mixed droplets are deterministic on the basis of the kinetics of their phase separation and the degree of hydrophobicity of the substrate. Introducing monomers and/or nanoparticles, further, into a certain phase of the ATPS droplet followed by photopolymerizing enables Janus hydrogel particles with diverse functionalities to be obtained. The ease and green techniques with which the Janus balance and curvature between two phases of the Janus droplet can be finely tuned point to new directions in designing Janus particles and hold great promises in biological engineering.

Serum BDNF discriminates Parkinson's disease patients with depression from without depression and reflect motor severity and gender differences.

OBJECTIVE: To evaluate the diagnostic value of serum Brain-derived neurotrophic factor (BDNF) levels for discriminating PD with depression from without depression, and to investigate whether serum BDNF levels were associated with motor severity and gender in depressed PD patients. METHODS: Demographic and clinical data were collected from 122 PD patients with depression, 137 without depression and 110 healthy controls. All participants' serum BDNF concentrations were measured. Their motor abilities and activity were assessed by the Unified PD Rating Scale Part III (UPDRS III) score and the Hoehn and Yahr (H-Y) stage. Depression was scored using the 17-item Hamilton Rating Scale for Depression (HAMD-17). Associations were analyzed with multivariate regression. RESULTS: The serum BDNF levels were lower in depressed PD patients compared to non-depressed PD patients and controls (p < 0.001). The BDNF levels were negatively correlated with UPDRS III score (r = - 0.54, p < 0.001) and H-Y stage (r = - 0.45, p < 0.001). Decreased BDNF levels were associated with women only among depressed PD patients (r = 0.45, p < 0.001). The HAMD-17 score was negatively correlated with BDNF levels (r = - 0.59, p < 0.001), and positively associated with UPDRS III score (r = 0.51, p < 0.001). Multiple regression analysis demonstrated that in the depressed PD patients, female, H-Y stage and UPDRS III score were independent contributors to the BDNF levels (p < 0.001; p = 0.006; p = 0.03, respectively), BDNF and UPDRS III score were independent contributors to HAMD-17 score (p < 0.001, p = 0.01, respectively). CONCLUSIONS: Decreased serum BDNF levels may be a useful clinical biomarker of depression in PD patients. Serum BDNF may serve as a potential biomarker for motor severity of PD patients with depression, especially in female.

Association of Decreased Serum BDNF With Restless Legs Syndrome in Parkinson's Disease Patients.

Objective: To objective of the study was to investigate whether serum brain-derived neurotrophic factor (BDNF) levels are associated with the severity of restless legs syndrome (RLS) in Parkinson's disease (PD). Methods: A total of 249 PD patients with (n = 53) and without RLS (n = 196) and 326 age-matched controls were included in this study. All the serum BDNF levels of the participants were measured. The International Restless Legs Syndrome Study Group Rating Scale (IRLSSG-RS) was administered for the severity of RLS. The severity of PD patients were assessed by the Unified PD Rating Scale (UPDRS) and the Hoehn and Yahr (H-Y) stage. Results: The prevalence of RLS was significantly higher in PD patients (21.3%) than in the controls group (7.4%) (p < 0.05). The IRLSSG-RS score in PD patients with RLS (16.25 ± 5.24) was significantly increased than in controls with RLS (12.08 ± 3.99) (p < 0.01). The serum BDNF levels were significantly decreased in PD patients with RLS than in PD patients without RLS, controls without RLS, and controls with RLS (p < 0.001). BDNF levels were negatively associated with IRLSSG-RS in both PD patients with RLS and controls with RLS group (both p < 0.01). Multiple regression analysis confirmed that in either PD with RLS or controls with RLS group, BDNF was an independent contributor to IRLSSG-RS (both p < 0.01). Conclusions: Decreased serum BDNF levels may be involved in the pathophysiology of RLS in PD, suggesting that it may serve as a potential blood biomarker of diagnostic value for RLS in PD.

Peripheral BDNF/TrkB protein expression is decreased in Parkinson's disease but not in Essential tremor.

BDNF-to-TrkB signaling pathways plays an important role in the long-term maintenance of the nigrostriatal system and that its deficiency may contribute to the onset and progression of Parkinson's disease (PD). To our knowledge this is the first study to investigate the expression of the brain-derived neurotrophic factor (BDNF) and phosphorylation status of TrkB in peripheral blood lymphocytes of 28 PD and 28 Essential tremor (ET) patients and 28 healthy controls using western blot analysis. Compared with controls, no significant difference of BDNF and total and phosphorylated TrkB levels were observed in ET, whereas BDNF and phosphorylated TrkB levels were significantly decreased in the PD groups (p < 0.001). Interestingly, BDNF and phosphorylated TrkB levels were positively correlated with disease duration, UPDRS score, Hoehn-Yahr staging, as well as L-DOPA medication in PD patients. These results suggest that the decreased peripheral alteration of BDNF/TrkB levels found in patients with PD is directly related to the dopaminergic neurons neurodegeneration and that decreased expression of BDNF/TrkB may lead to the development of innovative biomarkers of PD, whereas the increased level of BDNF and phosphorylated TrkB at advanced stages may due to L-DOPA medication.

Hydrophilic Porous Poly(l-Lactic Acid) Nanomembranes: Self-Assembly, and Anti-Biofouling and Anti-Thrombosis Effects.

Hydrophilic PEGylated porous self-assembled nanomembranes (PSANMs) with average thickness and pore diameter of ca. 10 and 20-24 nm were successfully prepared by an emulsification-induced programmable self-assembly strategy. The hydrophilicity, anti-biofouling, and anti-thrombosis properties of PEGylated PSANMs were largely improved in comparison with the nonfunctionalized PSANMs, which could transform into hydrophilic (PEGylated PSANMs, minimum water contact angle: 38.8°) from hydrophobic units (PSANMs, maximum water contact angle: 137.5°) with increasing PEG density and length. The total protein adsorption of PEGylated PSANMs was about six times lower than that of the PSANMs, while the thrombosis of the PEGylated PSANMs (maximum R-time: 5.37 min) was also greatly relieved in comparison with the PSANMs (minimum R-time: 2.93 min). Such PEG-modified PSANMs may have applications in drug delivery and tissue and organ repair in vivo.

Folate Receptor-Mediated Renal-Targeting Nanoplatform for the Specific Delivery of Triptolide to Treat Renal Ischemia/Reperfusion Injury.

Triptolide (TP) has been widely used in clinical medicine; however, it has created a dilemma due to its toxicity and nonspecificity. Here, we reported a biocompatible and high-efficiency renal-targeting nanoplatform for renal ischemia/reperfusion injury (IRI) therapy, in which the toxic drug of TP was encapsulated into folate (FA)-modified Pluronic F127/P123 nanoparticles (FPNPs). The TP-loaded FPNPs (TP-FPNPs) had good stability and could effectively reduce the cytotoxicity of TP. Compared with the Pluronic nanoparticles (PNPs) group, cellular uptake ability of FPNPs significantly improved because of folate receptor-mediated endocytosis effect. Ex vivo organ imaging and pharmacokinetic results indicated that FPNPs possessed high kidney selectivity and long retention time. The therapeutic effect of TP-FPNPs on renal IRI was more superior to that of free TP, such as lower acute tubular injury index (2.9-fold), renal function indexes of serum creatinine (4.3-fold), urea nitrogen (2.0-fold), and Western blotting (2.4-fold). Systemic toxicity assay suggested that TP-FPNPs had much lower nephrotoxicity, hepatotoxicity, and genital system toxicity than free TP. Thus, renal-targeting FPNPs will be a potential delivery platform of hydrophobic drugs for treatment of renal diseases.

Kidney-targeted triptolide-encapsulated mesoscale nanoparticles for high-efficiency treatment of kidney injury.

Bad water solubility and undesired toxicity of triptolide (TP) still restrict its clinical applications in renal diseases. In this work, well-defined, monodispersed, and uniform-sized TP-encapsulated mesoscale nanoparticles (TP-MNPs) were fabricated through a nanoprecipitation method, which possesses special kidney-targeting capacity, slow-release property, and high-efficiency treatment for renal ischaemia-reperfusion injury (IRI). The TP-MNPs had good cytocompatibility in wide TP concentration (0-500 ng ml-1) and time ranges (6-24 h). Ex vivo organ fluorescence imaging and pharmacokinetic analysis suggested that TP-MNPs possessed excellent kidney-targeting capability with long retention time (7 days). The TP-MNPs with a very low dose of TP (0.01 mg kg-1) could effectively protect the kidney against IRI, while 0.01 mg kg-1 TP was completely ineffective. After treatment with TP-MNPs, the serum creatine, blood urea nitrogen, expression of C3 complement, and phospho-extracellular signal-regulated kinase of renal IRI mice were estimated to be 5.9-, 2.0-, 5.4-, and 2.8-fold lower than those of the mice treated with TP, respectively. Compared with TP, the TP-MNPs exhibited ignorable hepatotoxicity, reproductive toxicity, and immunotoxicity, such as lower alanine aminotransferase (0.5 fold) and aspartate aminotransferase (0.2 fold), and a higher ratio of CD4+/CD8+ (2.2 fold). Thus, the monodispersed and uniform-sized TP-MNPs with special kidney-targeting and slow-release property may pave an avenue for designing a new therapeutic strategy for renal diseases.

Guiding kinetic trajectories between jammed and unjammed states in 2D colloidal nanocrystal-polymer assemblies with zwitterionic ligands.

Mesostructured matter composed of colloidal nanocrystals in solidified architectures abounds with broadly tunable catalytic, magnetic, optoelectronic, and energy storing properties. Less common are liquid-like assemblies of colloidal nanocrystals in a condensed phase, which may have different energy transduction behaviors owing to their dynamic character. Limiting investigations into dynamic colloidal nanocrystal architectures is the lack of schemes to control or redirect the tendency of the system to solidify. We show how to solidify and subsequently reconfigure colloidal nanocrystal assemblies dimensionally confined to a liquid-liquid interface. Our success in this regard hinged on the development of competitive chemistries anchoring or releasing the nanocrystals to or from the interface. With these chemistries, it was possible to control the kinetic trajectory between quasi-two-dimensional jammed (solid-like) and unjammed (liquid-like) states. In future schemes, it may be possible to leverage this control to direct the formation or destruction of explicit physical pathways for energy carriers to migrate in the system in response to an external field.