Review
Biochemical Research Methods
Wenjiao Fan, Wei Ren, Chenghui Liu
Summary: This article reviews the applications of optical counting and imaging of micro/nano-sized single entities in biomolecular analysis. Compared to conventional ensemble measurement-based assays, single-entity assays offer ultrahigh sensitivity and the ability to detect heterogeneity among individual target molecules.
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Nicholas B. Williams, Aaron Nash, Nobuyuki Yamamoto, Margaret Patrick, Ich C. Tran, Jing Gu
Summary: This study investigates the activity and electrolytic decomposition pathways of an iron-based catalyst attached to a silicon interface, demonstrating that surface modification can inhibit the formation of native SiO2 and improve hydrogen production efficiency.
ADVANCED MATERIALS INTERFACES
(2021)
Article
Materials Science, Multidisciplinary
Niloufar Afzali, Reza Keshavarzi, Shahram Tangestaninejad, Sixto Gimenez, Valiollah Mirkhani, Majid Moghadam, Iraj Mohammadpoor-Baltork
Summary: Metal-Organic Frameworks (MOFs) are a group of compounds with high porosity and diverse capabilities in photoelectrochemistry, however, they still face challenges due to bulk and surface recombination issues. This study introduced a dual strategy to enhance charge separation and catalytic activity by using mesoporous TiO2 to minimize bulk recombination and a CoPi co-catalyst to increase MOF catalytic activity. The results showed significant improvement in photocurrent density for PEC water oxidation, validating the effectiveness of the developed strategy for further applications in photocatalysis and photoelectrochemistry.
APPLIED MATERIALS TODAY
(2021)
Article
Materials Science, Multidisciplinary
Pranati Nayak, Minjun Yang, Zhiwei Wang, Xiuting Li, Ruiyang Miao, Richard G. G. Compton
Summary: We quantified the inherent electro-oxidation behavior of a single Ti(3)C(2)T(x)MXene particle using Single-Entity Electrochemistry. MXene undergoes irreversible oxidation at potentials greater than 0.3 V (vs. SCE), and the extent of oxidation is dependent on the applied potential. A close correlation is observed with ensembles of drop-cast particles with submonolayer coverage.
APPLIED MATERIALS TODAY
(2022)
Review
Chemistry, Physical
Hang Ren, Martin A. Edwards
Summary: Most electrochemical processes exhibit stochastic and discrete behavior, especially when the number of entities measured is limited. However, utilizing probabilistic and statistical interpretation can provide insights that match or exceed those from macroscopic measurements.
CURRENT OPINION IN ELECTROCHEMISTRY
(2021)
Review
Chemistry, Physical
Hao-Wei Wang, Si-Min Lu, Mengjie Chen, Yi-Tao Long
Summary: Single-entity electrochemistry, focusing on transient electrochemical processes at the confined interface, has become a promising field due to advancements in optical techniques. Recent progress in optical-electrochemical measurements has provided detailed information on precise localization, dynamic behavior tracking, and confinement-controlled electrochemistry.
CURRENT OPINION IN ELECTROCHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Nesrine Aissaoui, Josephine Lai-Kee-Him, Allan Mills, Nathalie Declerck, Zakia Morichaud, Konstantin Brodolin, Sonia Baconnais, Eric Le Cam, Jean Baptiste Charbonnier, Remy Sounier, Sebastien Granier, Virginie Ropars, Patrick Bron, Gaetan Bellot
Summary: Technological breakthroughs in electron microscopy have made it possible to study biological macromolecular complexes with novel challenges, such as sample preparation and heterogeneous macromolecular assemblies. In this study, a V-shaped DNA origami template was used to position proteins, demonstrating a new approach for characterizing mechanosensitive proteins and expanding the range of potential targets for single-particle EM investigation. Validation with RNAP protein showed compatibility with cryo-EM sample preparation.
Article
Chemistry, Multidisciplinary
So Dam Kim, Joon Ho Park, Hyokyum Ahn, Jeeho Lee, Chan-Ho Shin, Woo-Dong Jang, Byung-Kwon Kim, Hyun S. Ahn
Summary: This study extends the single-entity analysis to Pickering emulsions for the first time, revealing their similar hydrodynamic behavior to other nano-objects and elucidating the electron-transport mechanism. This research contributes to electrochemical nanomaterial synthesis.
Article
Chemistry, Physical
Si-Min Lu, Meng-Yin Li, Yi-Tao Long
Summary: Single-entity electrochemistry allows for the measurement of single cells, particles, and molecules at the nanoscale using well-defined interfaces. The characteristics of the nanoconfined electrode interface have a significant impact on the assay limitation and selectivity of single-entity measurement, which is controlled by the dynamic chemistry interactions between the target and the electrode interface.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Si-Min Lu, Meng-Yin Li, Yi-Tao Long
Summary: This article discusses the use of single-entity electrochemistry to measure single cells, particles, and molecules at the nanoscale, and how nanoconfined electrode interfaces enhance measurement characteristics. Stochastic single-entity collision electrochemistry and nanopore electrochemistry are explored as examples of how interactions affect charge transfer and mass transport.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Kai Mundsinger, Bryan T. Tuten, Lily Wang, Kira Neubauer, Christian Kropf, Megan L. O'Mara, Christopher Barner-Kowollik
Summary: We present a single-chain nanoparticle (SCNP) system that exhibits three times higher catalytic efficiency for the photooxidation of nonpolar alkenes compared to an equivalent concentration of small-molecule photosensitizer. The SCNP is constructed using poly(ethylene glycol) methyl ether methacrylate and glycidyl methacrylate, compacted through multifunctional thiol-epoxide ligation, and functionalized with Rose Bengal (RB). The confined RB within the SCNP achieves enhanced photocatalysis for nonpolar alkenes due to spatial proximity in the hydrophobic region.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Analytical
Jee Woo Kim, Gowrisankar Aruchamy, Byung-Kwon Kim
Summary: This review provides an overview of the recent developments and applications of single-entity electrochemistry (SEE) in the field of analytical/electroanalytical chemistry, with a focus on single metal nanoparticles, emulsion nanodroplets, and bio-entities.
TRAC-TRENDS IN ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Na Kong, Jin He, Wenrong Yang
Summary: Controlling and understanding the chemistry of molecular junctions is important in various fields. Stochastic single-entity collision electrochemistry (SECE) provides powerful tools to study single entities at the nanoscale. Molecular junctions formed by SECE collision have potential applications in monitoring molecular dynamics with high spatial and temporal resolution.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Richard G. Compton, Yuanyuan Lu, Xiuting Li
Summary: The electrocatalytic properties of multiwalled carbon nanotubes (MWCNTs) on the oxygen reduction reaction (ORR) in aqueous base have been studied at the single entity level. It has been shown that the electroactive surface functionality facilitates significant electrocatalysis, resulting in the formation of peroxide at lower potentials compared to bare carbon macroelectrodes and carbon nanotube modified electrodes.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Shan Chen, Congcong Yin, Zongxiong Huang, Junyan Chen, Yuhao Zheng, Jinghu Chen, Shuangli Yang, Yuwen Su, Yimin Fang
Summary: Graphene exhibits the ability to undergo oxygen evolution reaction and form oxygen nanobubbles at negative potential, acting as a mimic of superoxide dismutase (SOD). Catalytic sites are distributed at the edge and bulk of graphene, rather than on metal oxide residues. Metal oxide nanoparticles on the graphene sheet play an important role in promoting the catalysis by increasing the concentration of superoxide through an electrocatalyzed Fenton reaction.
Article
Chemistry, Physical
Zach N. Nilsson, Lacey M. Beck, Justin B. Sambur
Summary: Energy transfer measurements are used to measure distances between donors and acceptors in heterogeneous environments. The study explores if ensemble-level spectroscopy can quantify the distance between donor defect sites in NC and acceptor molecules. It was found that the emissive defect sites are on average separated by 0.5 nm from the A555 acceptor molecules, predominantly located at or near the surface of large NCs.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
Christina Cashen, R. Colby Evans, Zach N. Nilsson, Justin B. Sambur
Summary: By using a correlated optical-TEM technique, we were able to simultaneously measure the electrochemical behavior of multiple particles without the need to make electrical contacts to individual particles on the TEM grid. Our measurements revealed significant heterogeneity in electrochemical activity among particles.
FRONTIERS IN CHEMISTRY
(2021)
Article
Nanoscience & Nanotechnology
Michael Van Erdewyk, Justin B. Sambur
Summary: This study reveals the limiting effect of doping heterogeneity on the photoelectrochemical performance of TMD nanoflake and demonstrates the equal efficiency of n-type and p-type regions in natural MoS2 nanoflakes. The findings open up the possibility of synthesizing efficient TMD nanoflake photocatalysts with well-defined lateral p- and n-type domains.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Iman Naseri, Morteza Ziaee, Zach N. Nilsson, Danielle R. Lustig, Mostafa Yourdkhani
Summary: In this study, nanostructured heaters based on laser-induced graphene (LIG) were developed by direct writing on nonuniform and porous aramid woven fabric. The synthesized graphene exhibited good electrical properties, and the produced heaters showed high electrothermal efficiency with steady-state temperatures up to 170 degrees C. The LIG-aramid fabric heaters also demonstrated easy impregnation with thermosetting resins, allowing the development of flexible and stiff composites. The results showed consistent electrothermal performance of the flexible composite heater under various conditions and excellent de-icing capability of the LIG-aramid fabric heater for ice melting.
Article
Electrochemistry
Michael Van Erdewyk, Justin B. Sambur
Summary: Research has found that in TMD nanoflakes, photogenerated holes in hidden p-type domains can travel micron-scale distances and preferentially react with iodide, affecting the overall efficiency. The efficiency of the entire nanoflake is determined by the size, efficiency, and location of n- and p-type domains.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Steven Marquez, Travis Varra, Cami Christensen, Om Rajasekharan, Carter Dojan, Janelle Hobbs, Abigail Otten, Luke Salzer, Jennifer D. Schuttlefield Christus, Justin B. Sambur
Summary: Scanning probe-based microscopes (SPMs) are widely used in various scientific fields to manipulate and image matter on the nanoscale. However, due to the lack of availability and affordability of SPM tools, many students are unable to learn and contribute to this important imaging technique. In this study, we introduce an affordable scanning laser-based imaging system to educate students and enable them to conduct independent research in solar energy and other SPM techniques.
JOURNAL OF CHEMICAL EDUCATION
(2023)
Review
Chemistry, Physical
Michael Van Erdewyk, Dakota B. Lorenz, Justin B. Sambur
Summary: In the late 1970s and early 1980s, researchers found that smooth crystals were necessary for high-efficiency photoelectrochemical solar cells based on TMDS. However, anecdotal observations hinted at performance variation among apparently smooth crystals. This mini-review article explores how spatially resolved photoelectrochemical techniques are solving the mystery of performance variation.
CURRENT OPINION IN ELECTROCHEMISTRY
(2023)
Article
Chemistry, Physical
Luke D. Salzer, Brian Diamond, Kelly Nieto, R. Colby Evans, Amy L. Prieto, Justin B. Sambur
Summary: In this study, the influence of structure and composition on the performance of Niobium tungsten oxide, an anode material for Li-ion batteries, was systematically investigated. The results show that Li-ion diffusivity increases with block size, but capacity loss also increases. Additionally, the slope of the charge-discharge profile increases with increasing block size, which hinders the use of larger block sizes for constant power applications.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Multidisciplinary Sciences
Rachelle Austin, Yusef R. Farah, Thomas Sayer, Bradley M. Luther, Andres Montoya-Castillo, Amber T. Krummel, Justin B. Sambur
Summary: We demonstrate ultrafast hot exciton and free carrier extraction in a proof-of-concept photoelectrochemical solar cell made from inexpensive monolayer MoS2. Our approach allows for ultrathin charge transport distances and has potential applications in thin photovoltaic and solar fuel systems. This work provides valuable insights for future design strategies of 2D semiconductors.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Editorial Material
Chemistry, Physical
Justin Sambur, Jakoah Brgoch
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Danielle R. Lustig, Enes Buz, Justin T. Mulvey, Joseph P. Patterson, Kevin R. Kittilstved, Justin B. Sambur
Summary: Poly(ethylene glycol) (PEG) ligands can inhibit biomolecule adhesion to surfaces and are suitable for nanocrystal drug carriers. A FRET-based spectroscopy approach was used to assess the permeability of molecules through PEG-coated zinc oxide nanocrystals (NCs), revealing a porous or patchy morphology of the PEG ligand shell.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Multidisciplinary
Steven Marquez, Travis Varra, Cami Christensen, Om Rajasekharan, Carter Dojan, Janelle Hobbs, Abigail Otten, Luke Salzer, Jennifer D. Schuttlefield Christus, Justin B. Sambur
Summary: Scanning probe-based microscopes (SPMs) are widely used in various fields to manipulate and image matter at the nanoscale. However, their availability in high schools and universities is limited, hindering students' education in this important technique. To address this issue, we present an affordable scanning laser-based imaging system to introduce students to the underlying image formation process of SPM. With this system, students can learn and apply their knowledge to research projects and other SPM techniques.
JOURNAL OF CHEMICAL EDUCATION
(2023)
Article
Nanoscience & Nanotechnology
R. Colby Evans, Rachelle Austin, Rebecca C. Miller, Alexander Preston, Zach N. Nilsson, Kaka Ma, Justin B. Sambur
Summary: The influence of nanoparticle surface facets on the electrochromic properties of hexagonal WO3 nanorod thin films was explored in this study. It was found that different surface facets exhibited distinct electrochemical and optical properties, affecting the optical switching and stability differently. This suggests that surface facet and particle morphology engineering can be viable strategies to enhance the performance and stability of electrochromic thin films for smart window applications.
ACS APPLIED NANO MATERIALS
(2021)