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2. Synthesis of Chiral 1,2-Amino Alcohol-Containing Compounds Utilizing Ruthenium-Catalyzed Asymmetric Transfer Hydrogenation of Unprotected α‑Ketoamines.

Author

Mangunuru, Hari P. R., Terrab, Leila, Janganati, Venumadhav, Kalikinidi, Nageswara Rao, Tenneti, Srinivasarao, Natarajan, Vasudevan, Shada, Arun D. R., Naini, Santhosh Reddy, Gajula, Praveen, Lee, Daniel, Samankumara, Lalith P., Mamunooru, Manasa, Jayaraman, Aravindan, Sahani, Rajkumar Lalji, Yin, Jinya, Hewa-Rahinduwage, Chathuranga C., Gangu, Aravind, Chen, Anji, Wang, Zhirui, and Desai, Bimbisar

Published
2024
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3. Design and Discovery of Water-Soluble Benzooxaphosphole-Based Ligands for Hindered Suzuki–Miyaura Coupling Reactions with Low Catalyst Load.

Author

Shada, Arun D. R., Mangunuru, Hari P. R., Terrab, Leila, Tenneti, Srinivasarao, Kalikinidi, Nageswara Rao, Naini, Santhosh Reddy, Gajula, Praveen, Crull, Emily B., Janganati, Venumadhav, Kovvuri, Raghavendra, Natarajan, Vasudevan, Lee, Daniel, Yin, Jinya, Samankumara, Lalith, Mahar, Rohit, Zhang, Xueyi, Chen, Anji, Hewa-Rahinduwage, Chathuranga C., Wang, Zhirui, and Mamunooru, Manasa

Published
2024
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4. Design and Discovery of Water-Soluble Benzooxaphosphole-Based Ligands for Hindered Suzuki–Miyaura Coupling Reactions with Low Catalyst Load

Author

Shada, Arun D. R., primary, Mangunuru, Hari P. R., additional, Terrab, Leila, additional, Tenneti, Srinivasarao, additional, Kalikinidi, Nageswara Rao, additional, Naini, Santhosh Reddy, additional, Gajula, Praveen, additional, Crull, Emily B., additional, Janganati, Venumadhav, additional, Kovvuri, Raghavendra, additional, Natarajan, Vasudevan, additional, Lee, Daniel, additional, Yin, Jinya, additional, Samankumara, Lalith, additional, Mahar, Rohit, additional, Zhang, Xueyi, additional, Chen, Anji, additional, Hewa-Rahinduwage, Chathuranga C., additional, Wang, Zhirui, additional, Mamunooru, Manasa, additional, Rana, Jagruti, additional, Wannere, Chaitanya S., additional, Armstrong, Joseph D., additional, Williamson, R. Thomas, additional, Sirasani, Gopal, additional, Qu, Bo, additional, and Senanayake, Chris H., additional

Published
2023
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5. Synthesis of Chiral 1,2-Amino Alcohol-Containing Compounds Utilizing Ruthenium-Catalyzed Asymmetric Transfer Hydrogenation of Unprotected a-Ketoamines

Author

Mangunuru, Hari P. R., Terrab, Leila, Janganati, Venumadhav, Kalikinidi, Nageswara Rao, Tenneti, Srinivasarao, Natarajan, Vasudevan, Shada, Arun D. R., Naini, Santhosh Reddy, Gajula, Praveen, Lee, Daniel, Samankumara, Lalith P., Mamunooru, Manasa, Jayaraman, Aravindan, Sahani, Rajkumar Lalji, Yin, Jinya, Hewa-Rahinduwage, Chathuranga C., Gangu, Aravind, Chen, Anji, Wang, Zhirui, Desai, Bimbisar, Yue, Tai Y., Wannere, Chaitanya S., Armstrong, Joseph D., Donsbach, Kai O., Sirasani, Gopal, Gupton, B. Frank, Qu, Bo, and Senanayake, Chris H.

Abstract

Herein, we disclose a facile synthetic strategy to access an important class of drug molecules that contain chiral 1,2-amino alcohol functionality utilizing highly effective ruthenium-catalyzed asymmetric transfer hydrogenation of unprotected a-ketoamines. Recently, the COVID-19 pandemic has caused a crisis of shortage of many important drugs, especially norepinephrine and epinephrine, for the treatment of anaphylaxis and hypotension because of the increased demand. Unfortunately, the existing technologies are not fulfilling the worldwide requirement due to the existing lengthy synthetic protocols that require additional protection and deprotection steps. We identified a facile synthetic protocol via a highly enantioselective one-step process for epinephrine and a two-step process for norepinephrine starting from unprotected a-ketoamines 1band 1a, respectively. This newly developed enantioselective ruthenium-catalyzed asymmetric transfer hydrogenation was extended to the synthesis of many 1,2-amino alcohol-containing drug molecules such as phenylephrine, denopamine, norbudrine, and levisoprenaline, with enantioselectivities of >99% ee and high isolated yields.

Published
2024
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8. Sex-Specific Effects of Plastic Caging in Murine Viral Myocarditis

Author

Bruno, Katelyn A., primary, Macomb, Logan P., additional, Morales-Lara, A. Carolina, additional, Mathews, Jessica E., additional, Frisancho, J. Augusto, additional, Yang, Alex L., additional, Di Florio, Damian N., additional, Edenfield, Brandy H., additional, Whelan, Emily R., additional, Salomon, Gary R., additional, Hill, Anneliese R., additional, Hewa-Rahinduwage, Chathuranga C., additional, Scott, Ashley J., additional, Greyner, Henry D., additional, Molina, Frank A., additional, Greenaway, Merci S., additional, Cooper, George M., additional, and Fairweather, DeLisa, additional

Published
2021
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11. Evaluation of the Long-Term Storage Stability of the Cyanide Antidote: Dimethyl Trisulfide and Degradation Product Identification

Author

Warnakula, Indika K., primary, Ebrahimpour, Afshin, additional, Li, Sun Yi, additional, Gaspe Ralalage, Ramesha D., additional, Hewa-Rahinduwage, Chathuranga C., additional, Kiss, Márton, additional, Rios, Christian T., additional, Kelley, Kyler D., additional, Whiteman, Ashley C., additional, Thompson, David E., additional, Rockwood, Gary A., additional, and Petrikovics, Ilona, additional

Published
2020
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15. Atomically dispersed Pb ionic sites in PbCdSe quantum dot gels enhance room-temperature NO2 sensing.

Author

Geng, Xin, Li, Shuwei, Mawella-Vithanage, Lalani, Ma, Tao, Kilani, Mohamed, Wang, Bingwen, Ma, Lu, Hewa-Rahinduwage, Chathuranga C., Shafikova, Alina, Nikolla, Eranda, Mao, Guangzhao, Brock, Stephanie L., Zhang, Liang, and Luo, Long

Subjects
QUANTUM dots, P-type semiconductors, HUMAN ecology, DETECTION limit, METAL ions, BINDING sites
Abstract

Atmospheric NO2 is of great concern due to its adverse effects on human health and the environment, motivating research on NO2 detection and remediation. Existing low-cost room-temperature NO2 sensors often suffer from low sensitivity at the ppb level or long recovery times, reflecting the trade-off between sensor response and recovery time. Here, we report an atomically dispersed metal ion strategy to address it. We discover that bimetallic PbCdSe quantum dot (QD) gels containing atomically dispersed Pb ionic sites achieve the optimal combination of strong sensor response and fast recovery, leading to a high-performance room-temperature p-type semiconductor NO2 sensor as characterized by a combination of ultra–low limit of detection, high sensitivity and stability, fast response and recovery. With the help of theoretical calculations, we reveal the high performance of the PbCdSe QD gel arises from the unique tuning effects of Pb ionic sites on NO2 binding at their neighboring Cd sites. Quantum dot-based NO2 sensors often suffer from low sensitivity or long recovery times. Here, the authors report that bimetallic PbCdSe quantum dot gels containing atomically dispersed Pb ionic sites enable ultra-sensitive and fast NO2 sensing. [ABSTRACT FROM AUTHOR]

Published
2021
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16. Quantum Dot Assembly Driven by Electrochemically Generated Metal-Ion Crosslinkers

Author

Hewa-Rahinduwage, Chathuranga C., Silva, Karunamuni L., Brock, Stephanie L., and Luo, Long

Abstract

Control of nanoparticle assembly is a critical enabler for fabricating nanostructures capable of complex, system-level functionality. Here, we report a facile electrochemical method for assembling quantum dots (QDs) into mesoporous gels directly onto an electrode surface using localized, in situ generated metal ion crosslinkers (Ni2+, Co2+, Ag+, or Zn2+) within a colloidal solution of metal chalcogenide nanoparticles capped with ligands featuring pendant carboxylate groups. A mechanistic study reveals a critical stoichiometry of 0.5 metal ions: 1 QD in solution is required to trigger metal ion-mediated electrogelation (ME-gelation), representing a much lower concentration of metal ions than is needed for initiating crosslinking throughout an entire volume of solution (>26 metal ions: 1 QD in solution). The application of the ME gelation approach for the fabrication of QD-based electronic devices is demonstrated by electrochemical patterning of QD gels onto a printed circuit board chip.

Published
2021
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17. Photoexcited NO 2 Enables Accelerated Response and Recovery Kinetics in Light-Activated NO 2 Gas Sensing.

Author

Geng X, Liu X, Mawella-Vithanage L, Hewa-Rahinduwage CC, Zhang L, Brock SL, Tan T, and Luo L

Subjects
Gases, Kinetics, Temperature, Nitrogen Dioxide, Quantum Dots
Abstract

Slow response and recovery kinetics is a major challenge for practical room-temperature NO 2 gas sensing. Here, we report the use of visible light illumination to significantly shorten the response and recovery times of a PbSe quantum dot (QD) gel sensor by 21% (to 27 s) and 63% (to 102 s), respectively. When combined with its high response (0.04%/ppb) and ultralow limit of detection (3 ppb), the reduction in response and recovery time makes the PbSe QD gel sensor among the best p-type room-temperature NO 2 sensors reported to date. A combined experimental and theoretical investigation reveals that the accelerated response and recovery time is primarily due to photoexcitation of NO 2 gaseous molecules and adsorbed NO 2 on the gel surface, rather than the excitation of the semiconductor sensing material, as suggested by the currently prevailing light-activated gas-sensing theory. Furthermore, we find that the extent of improvement attained in the recovery speed also depends on the distribution of excited electrons in the adsorbed NO 2 /QD gel system. This work suggests that the design of light-activated sensor platforms may benefit from a careful assessment of the photophysics of the analyte in the gas phase and when adsorbed onto the semiconductor surface.

Published
2021
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