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1. Light-Addressable Electrochemical Sensing with Electrodeposited n‑Silicon/Gold Nanoparticle Schottky Junctions

   Terrero Rodríguez, Irina M.; Borrill, Alexandra J.; Schaffer, Katherine J.; Hernandez, Jocelyn B.; O’Neil, Glen D. (July 2020, Analytical chemistry)

   null (Ed.)

   Light-addressable electrochemical sensors (LAESs) are a class of sensors that use light to activate an electrochemical reaction on the surface of a semiconducting photoelectrode. Here, we investigate semiconductor/metal (Schottky) junctions formed between n-type Si and Au nanoparticles as lightaddressable electrochemical sensors. To demonstrate this concept, we prepared n-Si/Au nanoparticle Schottky junctions by electrodeposition and characterized them using scanning electron microscopy, cyclic voltammetry, and electrochemical impedance spectroscopy. We found that the sensors behaved almost identically to Au disk electrodes for the oxidation of an outer-sphere redox couple (ferrocene methanol) and two inner-sphere redox couples (potassium ferrocyanide and dopamine). In buffered dopamine solutions, we observed broad linear ranges and submicromolar detection limits. We then used local illumination to generate a virtual array of electrochemical sensors for dopamine as a strategy for circumventing sensor fouling, which is a persistent problem for electrochemical dopamine sensors. By locally illuminating a small portion of the photoelectrode, many measurements of fouling analytes can be made on a single sensor with a single electrical connection by moving the light beam to a fresh area of the sensor. Altogether, these results pave the way for Schottky junction light-addressable electrochemical sensors to be useful for a number of interesting future applications in chemical and biological sensing. 

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2. Development of Novel Carbon Fiber based Electrodes for Lithium-ion Batteries

   Kaynan, Ozge; Raj, Ayush; Carrola, Mia; Castaneda, Homero; Asadi, Amir (September 2023, American Society for Composites-DESTech publications)

   Carbon fiber-based structural lithium-ion batteries are attracting significant attention in the automotive and aerospace industries due to their dual capability of energy storage and mechanical load-bearing, leading to weight reduction. These batteries utilize lightweight carbon fiber (CF) composites, which offer excellent stiffness, strength-to-weight ratios, and electrical conductivity. Polyacrylonitrile-based CFs, comprising graphitic and amorphous carbon, are particularly suitable for Li-ion battery applications as they allow the storage of lithium ions. However, integrating lithium iron phosphate (LFP) into CFs poses challenges due to complex lab-scale processes and the use of toxic dispersants, hindering large-scale industrial compatibility. To address this, we investigate the development of water-based LFP-integrated CF structural Li-ion batteries. Homogeneous suspensions are created using cellulose nanocrystals (CNCs) to form hybrid structures. The battery system employs LFP-modified CF as the cathode, unsized CF as the anode, and a water-based electrolyte. The LFP-CNC-graphene nanoplatelet (GNP) hybrids are coated onto CFs through immersion coating. Scanning electron microscopy (SEM) images confirm the well-dispersed and well-adhered LFP-CNC-GNP structures on the CF surface, contributing to their mechanical interlocking and electrochemical performance. The batteries demonstrate a specific energy density of 62.67 Wh/kg and a specific capacity of 72.7 mAh/g. Furthermore, the cyclic voltammetry experiments reveal the stability of the LFP-CNC-GNP-coated CF batteries over 200 cycles without degradation. This research enables the engineering of hybrid nanostructured battery laminates using novel LFP-CNC-GNP-coated CFs, opening avenues for the development of innovative Li-ion structural batteries. 

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3. Integrated dual-modality microfluidic sensor for biomarker detection using lithographic plasmonic crystal

   https://doi.org/10.1039/c7lc01211j  

   Ali, Md. Azahar; Tabassum, Shawana; Wang, Qiugu; Wang, Yifei; Kumar, Ratnesh; Dong, Liang (January 2018, Lab on a Chip)

   This paper reports an integrated dual-modality microfluidic sensor chip, consisting of a patterned periodic array of nanoposts coated with gold (Au) and graphene oxide (GO), to detect target biomarker molecules in a limited sample volume. The device generates both electrochemical and surface plasmon resonance (SPR) signals from a single sensing area of Au–GO nanoposts. The Au–GO nanoposts are functionalized with specific receptor molecules, serving as a spatially well-defined nanostructured working electrode for electrochemical sensing, as well as a nanostructured plasmonic crystal for SPR-based sensing via the excitation of surface plasmon polaritons. High sensitivity of the electrochemical measurement originates from the presence of the nanoposts on the surface of the working electrode where radial diffusion of redox species occurs. Complementarily, the SPR detection allows convenient tracking of dynamic antigen–antibody interactions, to describe the association and dissociation phases occurring at the sensor surface. The soft-lithographically formed nanoposts provide high reproducibility of the sensor response to epidermal growth factor receptor ( ErbB2 ) molecules even at a femtomolar level. Sensitivities of the electrochemical measurements to ErbB2 are found to be 20.47 μA μM −1 cm −2 in a range from 1 fM to 0.1 μM, and those of the SPR measurements to be 1.35 nm μM −1 in a range from 10 pM to 1 nM, and 0.80 nm μM −1 in a range from 1 nM to 0.1 μM. The integrated dual-modality sensor offers higher sensitivity (through higher surface area and diffusions from nanoposts for electrochemical measurements), as well as the dynamic measurements of antigen–antibody bindings (through the SPR measurement), while operating simultaneously in a same sensing area using the same sample volume. 

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4. Bioinspired, Mechanically Robust Chemiresistor for Inline Volatile Organic Compounds Sensing

   https://doi.org/10.1002/admt.202000440  

   Xu, Weiheng; Ravichandran, Dharneedar; Jambhulkar, Sayli; Franklin, Rahul; Zhu, Yuxiang; Song, Kenan (August 2020, Advanced Materials Technologies)

   Abstract There are advantages to polymer/nanoparticle composite‐based volatile organic compounds (VOCs) sensors, such as high chemical and physical stability, operability under extreme conditions, flexible use in manufacturing, and low cost. Nevertheless, their lower limit of detection due to thickness‐dependent diffusion has constrained their application. Inspired by the metaxylem in vascular plants and its vertical conduits and horizontal pits that enable efficient transpiration, a polymer/nanoparticle composite‐based sensor is fabricated with a controllable, spontaneously formed, hollow core for inline VOCs transportation, and porous microstructure for radial direction diffusion. The hollow core is surrounded by an inner porous layer (thermoplastic polyurethane (TPU)), a middle sensing layer (TPU/graphene nanoplatelets/multiwalled carbon nanotubes), and an outer mechanically durable layer (TPU). This multilayered structure shows a 600% higher response rate compared to a single‐layered composite fiber sensor, with a low limit of detection (e.g., ≈15 ppm for xylene) and high selectivity based on the Flory–Huggins interaction parameter. This flexible and stretchable sensor also demonstrates a dual parameter sensing capability from VOC concentrations and uniaxial strain deformation. Via a one‐step fiber spinning procedure, this self‐induced hollow fiber offers a unique method of microstructural design, which enables the detection of low‐concentration VOCs by polymer/nanoparticle‐based sensors. 

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5. Informing rational design of graphene oxide through surface chemistry manipulations: properties governing electrochemical and biological activities

   https://doi.org/10.1039/C7GC00159B  

   Wang, Yan; Gilbertson, Leanne M. (January 2017, Green Chemistry)

   It is increasingly realized that rational design is critical to advance potential applications and proactively preclude adverse consequences of carbon nanomaterials (CNMs). Central to this approach is the establishment of parametric relationships that correlate material properties to both their functional performance and inherent hazard. This work aims to decouple the causative mechanisms of material structure and surface chemistry as it relates to the electrochemical and biological activities of graphene oxide (GO). The results are evaluated in the context of established relationships between surface chemistry and oxygen functionalized multi-walled carbon nanotubes (O-MWCNTs), a carbon allotrope. Systematic manipulation of GO surface chemistry is achieved through thermal annealing (under inert conditions, 200–900 °C). To further elucidate the contribution of several properties, chemical reduction was also used as an approach to differentially modify the surface chemistry. Physicochemical properties of GO and reduced GO (rGO) samples were comprehensively characterized using multiple techniques (AFM, TGA, XPS, ATR-FTIR, Raman, and DLS). The results indicate that surface chemistry is a viable design handle to control both activities. Rather than a single direct property ( i.e. , relative presence of carbonyl-containing moieties), it is a balance of multiple consequential properties, (extent of dispersion, defect density, and electrical conductivity) in combination with the relative presence of carbonyl moieties that synergistically contribute to electrochemical and biological activities. The identification of these governing physicochemical properties aims to inform the establishment of design parameters to guide the rational and safe design of CNMs. 

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