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A Themed Issue in Honor of Professor George Whitesides on...
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A Themed Issue in Honor of Professor George Whitesides on the Occasion of His 85th Birthday Anniversary

A special issue of Chemistry (ISSN 2624-8549).

Deadline for manuscript submissions: 15 December 2024 | Viewed by 4885

Special Issue Editors

Prof. Dr. Valentine Vullev

E-Mail Website
Guest Editor
Department of Bioengineering, University of California, 900 University Ave., Riverside, CA 92521, USA
Interests: biophysics; microfluidics; charge transfer
Prof. Dr. Igor Alabugin

E-Mail Website
Guest Editor
Department of Chemistry and Biochemistry, Florida State University, Tallahassee, FL 32306, USA
Interests: organic reaction mechanisms; stereoelectronic effects; organic photochemistry; DNA photocleavage; carbon-rich materials; chemistry of alkynes; radical chemistry; cyclizations; cycloaromatizations; electron upconversion; hole catalysis; high energy functional groups
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

We are delighted to announce a Special Issue dedicated to celebrating the remarkable contributions of Professor George M. Whitesides in the broad field of chemical science. As a pioneer, inventor, and visionary, Professor Whitesides has left an indelible mark on multiple disciplines, bridging the gap between fundamental research and practical applications.

Professor Whitesides has consistently pushed the boundaries of scientific exploration. His work spans chemistry, materials science, and biophysics: from self-assembled monolayers to soft robotics, its impact resonates across diverse domains. When his work attracts others to a field, he often transitions to a new research area looking for new and interesting problems to solve. In fact, his perpetual quest for intriguing problems often creates new fields.

We invite original research articles, reviews, and perspectives that align with Professor Whitesides’ areas of expertise.

Topics of interest include, but are not limited to, the following:

  • Soft lithography and microfluidics: exploring advancements in microfabrication techniques, surface patterning, optofluidics, and lab-on-a-chip.
  • Complexity/emergence and simplicity: investigating emergent phenomena, complexity theory, and the science of simplicity, along with their importance for addressing pending problems.
  • Physical and organic chemistry, materials, and infochemistry: organometallic chemistry, NMR spectroscopy, polymer science, photophysics, and information storage.
  • Biophysics and origin of life: the role of water, cell surfaces and polyvalency in biomolecular recognition, rational drug design, and entropy and life.
  • Catalysis and sustainable chemistry: highlighting innovations in catalysis, green chemistry, energy production and conservation, and the quest for sustainable solutions.
  • Health science for developing economies: sharing insights on affordable diagnostics, point-of-care devices, and global health challenges.
  • Surface science, micro- and nanotechnology: discussing surface modification, interfacial charge transport, molecular electronics, nanomaterials, and mesoscopic and macroscopic self-assembly.

Manuscripts should be submitted through our online submission system.

Please indicate that your submission is intended for the “George Whitesides Special Issue.”

All submissions will be published and will be taken into account for the printed version of the Special Issue if they pass rigorous peer review.

Prof. Dr. Valentine Vullev
Prof. Dr. Igor Alabugin
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Chemistry is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 1800 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • nanotechnology
  • physical organic chemistry
  • microfluidics
  • soft lithography
  • surface science
  • complexity
  • origin of life
  • catalysis
  • sustainable chemistry

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Further information on MDPI's Special Issue polices can be found here.

Published Papers (5 papers)

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Research

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19 pages, 45939 KiB  
Article
Design and Rapid Prototyping of 3D-Printed Microfluidic Systems for Multiphase Flow
by Bastian Oldach, Robin Fortmann, Theo Pleie, Philip Timm and Norbert Kockmann
Chemistry 2024, 6(6), 1458-1476; https://doi.org/10.3390/chemistry6060088 - 21 Nov 2024
Viewed by 285
Abstract
Since the emergence of microfluidic devices, subtractive manufacturing techniques have dominated their production. Although the conventional manufacturing processes are well established, they come along with some disadvantages that limit the accessibility and hinder the further development of microfluidics. With the rise of additive [...] Read more.
Since the emergence of microfluidic devices, subtractive manufacturing techniques have dominated their production. Although the conventional manufacturing processes are well established, they come along with some disadvantages that limit the accessibility and hinder the further development of microfluidics. With the rise of additive manufacturing, researchers are focused on developing alternative fabrication methods to promote affordability and accessibility. This paper presents the opportunities and challenges of laser-based stereolithography printers for the fabrication of microfluidic equipment. Emphasis is put on the design and iterative prototyping process from the initial design idea to the final device. To print with adequate and sufficient geometrical accuracy and suitable material, the optimization of the printer’s performance is discussed. Regarding the design of multiphase microfluidics and its complex fluid behavior, suitable surface treatments, including an appropriate cleaning protocol, and coating strategies to make the printed channels either hydrophilic or hydrophobic are presented to ensure applicability. With these fundamentals of additive manufacturing in microfluidic fabrication at hand, the second focus of this contribution is on the application of a modular co-flow device and a monolithic flow-focusing device to generate droplets and slugs in different multiphase flow applications. The presented co-flow setup features a tapered capillary that affects the droplet and slug sizes due to differing diameters, with larger diameters leading to larger droplets and slugs and vice versa. Several design parameters for the flow-focusing device were evaluated to determine the influence of device design on multiphase flow formation. It was found that the diameter of the inlet for the dispersed phase has the greatest effect on the size of the resulting droplets and slugs and covers the largest range of adjustable sizes. Full article
(This article belongs to the Special Issue A Themed Issue in Honor of Professor George Whitesides on the Occasion of His 85th Birthday Anniversary)
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12 pages, 2868 KiB  
Article
Dynamic Magnetic Control of Lanthanide Metal–Organic Framework Crystals and Their Polarized Emissions
by Bojun Shi, Hao Jia, Lingfang Chen, Shuchun Zhang, Yu Zhang, Baipeng Yin, Shuming Bai and Chuang Zhang
Chemistry 2024, 6(6), 1415-1426; https://doi.org/10.3390/chemistry6060084 - 14 Nov 2024
Viewed by 397
Abstract
Traditional barcode encoding methods are constrained by the inability to dynamically control crystal orientations, thereby limiting their applications. In this work, we investigate the dynamic magnetic control of lanthanide metal–organic framework crystals and their potential for advancing photonic barcode technology. A paramagnetic fluorescent [...] Read more.
Traditional barcode encoding methods are constrained by the inability to dynamically control crystal orientations, thereby limiting their applications. In this work, we investigate the dynamic magnetic control of lanthanide metal–organic framework crystals and their potential for advancing photonic barcode technology. A paramagnetic fluorescent Eu-MOF microcrystal with sizes ranging from 30 to 40 μm in length and 5 to 10 μm in width was synthesized, and its magnetic orientation and polarized emission were systematically investigated. Eu-MOF crystallizes in an orthorhombic space group, growing along the crystallographic b-axis and ultimately forming an anisotropic cuboid shape. Eu-MOF microcrystals exhibit significant magnetic anisotropy, causing the crystallographic c-axis of the crystal to align with the magnetic field when a uniaxial magnetic field of ~10 mT is applied. Furthermore, the Eu-MOF microcrystal exhibited characteristic Eu emissions with peaks at 594 nm, 616 nm, and 695 nm, and showed a high degree of polarization (DOP), reaching 0.904 at 616 nm. Therefore, the utilization of a rotating magnetic field not only enables precise and dynamic control over the crystal orientations but also results in a significant variation in the luminescence intensity. This capability enabled us to propose an innovative encryption barcode scheme in which the emission intensities of different luminescence peaks are converted into barcode widths, with the sequence of magnetic field directions serving as the encryption key. This approach presents a novel method for data storage and anti-counterfeiting, significantly enhancing the versatility and capacity of photonic barcodes. Full article
(This article belongs to the Special Issue A Themed Issue in Honor of Professor George Whitesides on the Occasion of His 85th Birthday Anniversary)
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14 pages, 2075 KiB  
Article
Controlled Assembly of Lipid Molecules via Regulating Transient Spatial Confinement
by Yuqi Huang, Umit Celik, Ziqian Xu, Daniel Speer, Dario Ossola, Roland Faller, Atul N. Parikh and Gang-Yu Liu
Chemistry 2024, 6(5), 1287-1300; https://doi.org/10.3390/chemistry6050074 - 19 Oct 2024
Viewed by 901
Abstract
The constructs of lipid molecules follow self-assembly, driven by intermolecular interactions, forming stacking of lipid bilayer films. Achieving designed geometry at nano- to micro-levels with packing deviating from the near-equilibrium structure is difficult to achieve due to the strong tendency of lipid molecules [...] Read more.
The constructs of lipid molecules follow self-assembly, driven by intermolecular interactions, forming stacking of lipid bilayer films. Achieving designed geometry at nano- to micro-levels with packing deviating from the near-equilibrium structure is difficult to achieve due to the strong tendency of lipid molecules to self-assemble. Using ultrasmall (<fL) droplets containing designed molecules, our prior work has demonstrated that molecular assembly, in principle, is governed mainly by transient inter-molecular interactions under their dynamic spatial confinement, i.e., tri-phase boundaries during drying. As a result, the assemblies can deviate, sometimes significantly, from the near-equilibrium structures of self-assembly. The present work applies the approach and concept to lipid molecules using 1-palmitoyl-2-oleoyl-sn-glycero-3-phosphocholine (POPC). Taking advantage of the high spatial precision and the minute size of the delivery probe in our combined atomic force microscopy and microfluidic delivery, the transient shape of each liquid droplet is regulated. In doing so, the final geometry of the POPC assemblies has been regulated to the designed geometry with nanometer precision. The results extend the concept of controlled assembly of molecules to amphiphilic systems. The outcomes exhibit high potential in lipid-based biomaterial science and biodevice engineering. Full article
(This article belongs to the Special Issue A Themed Issue in Honor of Professor George Whitesides on the Occasion of His 85th Birthday Anniversary)
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11 pages, 1853 KiB  
Article
Lactone-Terminated Self-Assembled Monolayers for Mimicking Nanoscale Polyester Surfaces
by Pooria Tajalli, Jennifer M. Hernandez Rivera, Mina Omidiyan, Jong Moon Lee, Hung-Vu Tran and T. Randall Lee
Chemistry 2024, 6(4), 666-676; https://doi.org/10.3390/chemistry6040039 - 31 Jul 2024
Viewed by 976
Abstract
Two series of lactone-terminated alkanethiol adsorbates with five- and six-membered lactone groups, γ-COCnSH and δ-COCnSH (n = 11, 12), were synthesized and employed to create nanoscale self-assembled monolayers (SAMs) on gold substrates to mimic the properties of commercially available poly(lactic-co-glycolic acid) (PLGA) and [...] Read more.
Two series of lactone-terminated alkanethiol adsorbates with five- and six-membered lactone groups, γ-COCnSH and δ-COCnSH (n = 11, 12), were synthesized and employed to create nanoscale self-assembled monolayers (SAMs) on gold substrates to mimic the properties of commercially available poly(lactic-co-glycolic acid) (PLGA) and poly(glycolic acid) (PGA) surfaces. 1H and 13C nuclear magnetic resonance (NMR) were employed to characterize the adsorbate molecules. The thicknesses of the corresponding self-assembled monolayers (SAMs) were evaluated by ellipsometry. The conformational characteristics of the SAMs were analyzed using polarization modulation infrared reflection adsorption spectroscopy (PM-IRRAS), with a focus on the C-H antisymmetric stretching vibrations of the alkyl spacers. To evaluate the packing densities of the monolayers, X-ray photoelectron spectroscopy (XPS) measurements were performed. Separately, contact angle measurements provided insights into the wettability of the surfaces. Remarkably, the contact angle data across a broad range of probe liquids for the γ-COC11SH and γ-COC12SH SAMs were consistently similar to each other and to the contact angle values of the PLGA surface, rather than to PGA. This finding suggests that the lactone-terminated SAMs investigated in this study effectively mimic nanoscale polyester surfaces, enabling the exploration of interfacial properties of polyesters in the absence of swelling and/or surface reconstruction phenomena. Full article
(This article belongs to the Special Issue A Themed Issue in Honor of Professor George Whitesides on the Occasion of His 85th Birthday Anniversary)
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Review

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24 pages, 5133 KiB  
Review
Advancements in Microfluidic Platforms for Glioblastoma Research
by Rachana Raman, Vijendra Prabhu, Praveen Kumar and Naresh Kumar Mani
Chemistry 2024, 6(5), 1039-1062; https://doi.org/10.3390/chemistry6050060 - 15 Sep 2024
Viewed by 1021
Abstract
Glioblastoma (GBM) is a malignant cancer affecting the brain. As per the WHO classifications, it is a grade IV glioma and is characterized by heterogenous histopathology, high recurrence rates, and a high median age of diagnosis. Most individuals diagnosed with GBM are aged [...] Read more.
Glioblastoma (GBM) is a malignant cancer affecting the brain. As per the WHO classifications, it is a grade IV glioma and is characterized by heterogenous histopathology, high recurrence rates, and a high median age of diagnosis. Most individuals diagnosed with GBM are aged between 50 and 64 years, and the prognosis is often poor. Untreated GBM patients have a median survival of 3 months, while treatments with Temozolomide (TMZ) and radiotherapy can improve the survival to 10–14 months. Tumor recurrence is common, owing to the inefficiency of surgical resection in removing microscopic tumor formations in the brain. A crucial component of GBM-related research is understanding the tumor microenvironment (TME) and its characteristics. The various cellular interactions in the TME contribute to the higher occurrence of malignancy, resistance to treatments, and difficulty in tumor resection and preventative care. Incomplete pictures of the TME have been obtained in 2D cultures, which fail to incorporate the ECM and other crucial components. Identifying the hallmarks of the TME and developing ex vivo and in vitro models can help study patient-specific symptoms, assess challenges, and develop courses of treatment in a timely manner which is more efficient than the current methods. Microfluidic models, which incorporate 3D cultures and co-culture models with various channel patterns, are capable of stimulating tumor conditions accurately and provide better responses to therapeutics as would be seen in the patient. This facilitates a more refined understanding of the potential treatment delivery systems, resistance mechanisms, and metastatic pathways. This review collates information on the application of such microfluidics-based systems to analyze the GBM TME and highlights the use of such systems in improving patient care and treatment options. Full article
(This article belongs to the Special Issue A Themed Issue in Honor of Professor George Whitesides on the Occasion of His 85th Birthday Anniversary)
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Planned Papers

The below list represents only planned manuscripts. Some of these manuscripts have not been received by the Editorial Office yet. Papers submitted to MDPI journals are subject to peer-review.

Title: Design and Rapid Prototyping of 3D-Printed Microfluidic Systems for Multiphase Flow
Author: Kockmann
Highlights: Microstructured devices; Microfluidics; Additive manufacturing; Stereolithography; Droplets; Design Thinking; Rapid Prototyping

Title: Packed bed microreactors for sustainable chemistry and process development
Author: Yue
Highlights: • Packed bed microreactors open many opportunities for the efficient heterogeneous catalysis. • Application areas include catalyst screening, kinetic/chemistry study and reaction optimization. • Microreactor performance is related to the improved catalytic chemistry and process intensification.

Title: Advancements of Microfluidics in Glioblastoma Cancer
Author: Mani
Highlights: •“Glioblastoma” a unique tumor microenvironment is immunosuppressive and highly malignant. •Development of microfluidic systems for organ-on-a-chip studies serve as a promising tool to understand their pathogenesis. •The use of microfluidic systems can eliminate several obstacles in drug development processes, single-cell studies and TME stimulations to identify potential therapeutic targets.

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