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Abstract We report the exfoliation process optimization, physicochemical characterizations, and comparative aggregation behavior of the inorganic 2D nanomaterial hexagonal Boron Nitride (h-BN) produced from two repetitive sonication-centrifugation processes with varying centrifugation speeds and recycle frequency: Continuous and Segmented protocols. Enhancing exfoliation efficiency and understanding aqueous stability are essential for sustainable design and environmental applications. Results showed that the Segmented protocol outperformed the Continuous protocol by having a six-fold increase in the exfoliated h-BN nanosheet yield by reusing the unexfoliated bulk h-BN and decreasing centrifugation speeds. Centrifugation speeds of 1880 and 950 rpm produced nanosheets of similar sizes due to the slight difference in the centrifugal force generated in both protocols. Moreover, nanosheets from both protocols had enhanced polarity due to the higher amounts of −OH bonds attached to the exposed edges of the nanosheets. However, the hydroxylation percentage of the nanosheets decreased with centrifugation speed. Both protocols produced h-BN nanosheets that were stable in DI water dispersion. The comparatively lower initial aggregation rate at all centrifugation speeds supported the fact that the Segmented protocol nanosheets were more stable than the Continuous ones. The Segmented protocol h-BN nanosheets showed better overall stability at lower speeds than the other centrifugation speeds. Segmented protocol nanosheets from 3750 rpm had the lowest aggregation rate than the other centrifugation speed. These findings assist in finding the balance between exfoliation protocol, environmental application, and implication of h-BN nanosheets. 

Despite the emergence of eco-friendly solvents and scalable methods for polymeric membrane fabrication, studies on the impacts of solvent synthesis and manufacturing scale-up have not been conducted. To this end, a life cycle assessment (LCA) was developed with the goal of determining the global environmental and health impacts of producing polysulfone (PSf) membranes with the solvents PolarClean and γ-valerolactone (GVL) via doctor blade extrusion (DBE) and slot die coating (SDC). Along with PolarClean and GVL, dimethylacetamide (DMAc) and N-methyl-2-pyyrolidone (NMP) were included in the LCA as conventional solvents for comparison. The dope solution viscosity had a major influence on the material inventories; to produce a normalized membrane unit on a surface area basis, a larger quantity of PSf-PolarClean-GVL materials was required due to its high viscosity. The life cycle impact assessment found electricity and PolarClean to be major contributing parameters to multiple impact categories during membrane fabrication. The commercial synthesis route of PolarClean selected in this study required hazardous materials derived from petrochemicals, which increased its impact on membrane fabrication. Due to more materials being required to fabricate membranes via SDC to account for tool fluid priming, the PSf-PolarClean-GVL membrane fabricated via SDC exhibited the highest impacts. The amount of electricity and concentration of PolarClean were the most sensitive parameters according to Spearman’s rank coefficient analysis. A scenario analysis in which the regional energy grid was substituted found that using the Swedish grid, which comprises far more renewable technologies than the global and US energy grids, significantly lowered impacts in most categories. Despite the reported eco-friendly benefits of using PolarClean and GVL as alternatives to conventional organic solvents, the results in this study provide a wider perspective of membrane fabrication process impacts, highlighting that upstream impacts can counterbalance the beneficial properties of alternative materials. 

The removal of small molecular weight charged compounds from aqueous solutions using membrane remains a challenge. In this study, polysulfone (PSf)- and sulfonated polyether ether ketone (SPEEK)-based membranes were fabricated via non-solvent induced phase separation process (NIPS) using N-Methyl-2-Pyrrolidone (NMP) as solvent and water as non-solvent. Membranes were characterized structurally and morphologically, followed by toxicity assessment conducted before and after filtration, both with and without annealing at various pH values to evaluate potential leaching of trapped solvent from the membrane pores. Additionally, membrane performance was characterized using binary mixtures of cationic and anionic dyes. The results demonstrated selective filtration behavior, with cationic dyes being preferentially rejected due to size exclusion and electrostatic interactions. Additionally, a key focus of this work was the investigation of solvent leaching, framed within a Safe(r)-by-Design (SbD) approach aimed at enhancing functional performance while minimizing environmental toxicity. Toxicity assessments using a model organism, a nematode Caenorhabditis elegans, revealed that annealing reduced solvent leaching and thus permeate toxicity, particularly at neutral pH values, by facilitating trapped solvent release prior to membrane use. These findings provide insights for the importance of including an SbD approach during membrane casting to fabricate membranes with desirable properties while minimizing toxicity. 

Biosensors often combine biological recognition elements with nanomaterials of varying compositions and dimensions to facilitate or enhance the operating mechanism of the device. While incorporating nanomaterials is beneficial to developing high-performance biosensors, at the stages of scale-up and disposal, it may lead to the unmanaged release of toxic nanomaterials. Here we attempt to foster connections between the domains of biosensors development and human and environmental toxicology to encourage a holistic approach to the development and scale-up of biosensors. We begin by exploring the toxicity of nanomaterials commonly used in biosensor design. From our analysis, we introduce five factors with a role in nanotoxicity that should be considered at the biosensor development stages to better manage toxicity. Finally, we contextualize the discussion by presenting the relevant stages and routes of exposure in the biosensor life cycle. Our review found little consensus on how the factors presented govern nanomaterial toxicity, especially in composite and alloyed nanomaterials. To bridge the current gap in understanding and mitigate the risks of uncontrolled nanomaterial release, we advocate for greater collaboration through a precautionary One Health approach to future development and a movement towards a circular approach to biosensor use and disposal.