Progress 01/15/25 to 01/14/26
Outputs
Target Audience:Research results have been prestented in national and international conferences and the audiences are researchers in environmental chemistry, environmental science, and environmental engineering in academia. Changes/Problems:
Nothing Reported
What opportunities for training and professional development has the project provided?The project has trained two Ph.D. students in environmental engineering. How have the results been disseminated to communities of interest?We have presented our work in national and international conferences. What do you plan to do during the next reporting period to accomplish the goals?We will continue with evaluating the stability of Co-based SACs, espeically their performance with the presence of natural organic matter (NOM). We aim to understand how NOM can potentially foul the catalysts and change the reaction mechanisms and pathways of activating peroxymonosulfate. We also hope to understand how NOM will be degraded by reactive oxygen species (produced through peroxymonosulfate activation).
Impacts
What was accomplished under these goals?
We have developed different types of SACs and DACs. Some SACs and DACs are Fe and Fe-Mn loaded on nitrogen-doped carbon, and they are able to activate oxygen gas to produce hydroxyl radicals for effective viral pathogen disinfection. Other SACs are Co loaded on graphitic carbon nitride nanosheets, and they are able to activate peroxymonosulfate for contaminant transformation. For viral pathogen control, both non-enveloped and enveloped viruses have been tested, and biomolecular damage (e.g., protein, lipid, and genome) has been found and viral lifecycle (i.e., binding to host cells and internalization into host cells) has been interrupted after SACs/DACs disinfection. For Co-based SACs, they selectively produce singlet oxygen by activatingperoxymonosulfate, and the steady-state singlet oxygen concentration is 100-1,000 times higher than that of hydroxyl radicals and sulfate radicals.
Publications
- Type:
Conference Papers and Presentations
Status:
Accepted
Year Published:
2025
Citation:
Fu, J., Shuai, D. Sustainable Activation of Oxygen Gas using Artificial Enzymes for Viral Pathogen Disinfection. ACS Fall Meeting, 08/2025. ORAL
- Type:
Conference Papers and Presentations
Status:
Accepted
Year Published:
2025
Citation:
Fu, J., Shuai, D. Sustainable Activation of Oxygen Gas using Artificial Enzymes for Viral Pathogen Disinfection. 2025 AEESP Conference, 05/2025. ORAL
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Progress 01/15/24 to 01/14/25
Outputs
Target Audience:
Nothing Reported
Changes/Problems:
Nothing Reported
What opportunities for training and professional development has the project provided?The project has trained two Ph.D. students in STEM. How have the results been disseminated to communities of interest?
Nothing Reported
What do you plan to do during the next reporting period to accomplish the goals?We will continue with the current plan and apply developed SACs for degrading a broad spectrum of agrochemicals in agricultural wastewater and evaluate catalyst performance. We will especially focus on the selectivity for degradaing contaminants in complex wastewater matrices.
Impacts
What was accomplished under these goals?
We have developed SACs with a high metal loading on graphitic carbon nitride through two different approaches. One was loading CoCl2 onto graphitic carbon nitride and subsequent two-step annealing processes to avoid the agglomeration of Co and the formation of nanoparticles. The other one was mixing CoCl2 with formamide under elevated temperature, forming precipitates, and annealing. The two approaches produced Co-SACs that can active peroxymonosulfate rapidly, but show distinct selectivity. One catalyst produced hydroxyl radicals as the dominant reactive species, whereas the others produced sulfate radicals as the dominant reactive species. This unique selectivity can find broad engineering applications for treating agricultural wastewater, espeically the ones with complex matrices. In particular, sulfate radicals are more selective in complex wastewater matrices and they can degrade agrochemicals more easily. The other part of the project was developing artificial enzymes for eliminating pathogens in agricultural wastewater and promoting water reuse. Artificial enzymes such as oxidase-mimicking catalysts stand out for their unique ability to function without external energy or chemical inputs, in contrast to conventional disinfection methods. In our study, we developed a zeolitic imidazolate framework-based SAC co-doped with Fe and Mn to mimic oxidase activity for viral pathogen inactivation. Aberration-corrected high-angle-annular-dark-field scanning transmission electron microscopy and extended X-ray absorption fine structure confirm the atomic dispersion of Fe and Mn. The catalyst oxidized 3,3',5,5'-tetramethylbenzidine with the presence of oxygen gas but not in an inert environment with nitrogen, confirming the indispensability of oxygen for catalytic oxidation. Probe chemical tests and electron paramagnetic resonance spectroscopy elucidated that hydroxyl radicals, one of the most potent reactive oxygen species, were generated under ambient conditions, promising for virus disinfection. Both murine norovirus (MNV) and murine coronavirus (MHV) were selected as non-enveloped and enveloped human virus surrogates, highlighting the broad-spectrum effectiveness of our artificial enzyme for disinfecting viral pathogens. The catalyst inactivated 2 log?? of MNV within 60 minutes, and it was more efficient in disinfecting MHV. Gene damage was observed in disinfection, possibly along with the damage of other viral biomolecules such as proteins and lipids. Key viral lifecycle was also disrupted, such as binding to and internalization into host cells. The impairment of viral biomolecules and lifecycle elucidated the mechanism of virus disinfection in catalysis. Owing to the excellent performance through sustainable activation of oxygen gas, our oxidase-mimicking catalyst shows promise for wastewater reuse.This research advances the field of environmental catalysis and environmental pathogen control and paves the avenue for developing efficient, sustainable, and multipurpose solutions to address global health and environmental challenges.
Publications
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Progress 01/15/23 to 01/14/24
Outputs
Target Audience:We have published a paper on Environ. Sci. Technol., and the readers of that journal are our target audiences. We have also presented our work in national and international conferences and the conference attendees are our target audiences. Changes/Problems:
Nothing Reported
What opportunities for training and professional development has the project provided?The project has trained one Ph.D. student in STEM from underrepresented groups (female). The Ph.D. student has already obtained the degree and is now pursueing her postdoctoral studies in the Medical School at Yale University. How have the results been disseminated to communities of interest?The research outcomes have been published on Environ. Sci. Technol., and have been presented in national and international conferences. What do you plan to do during the next reporting period to accomplish the goals?We are planning to increase the metal loadings on catalysts to improve catalytic performance. One major bottleneck of using single and double atom catalysts for agricultural wastewater treatment is the limited metal loading on catalyst supports. We are currently optimizing our catalyst synthesis procedures and will significantly improve the metal loading from less than 1% to 10%. By doing so, we aim to increase the catalyst performance by at least 10 times.
Impacts
What was accomplished under these goals?
We have successfully synthesized single- and double-atom catalysts with enhanced performance for activating peroxides (peroxoymonosulfate, PMS) and inactivating coronaviruses as environmental pathogens. In particular, the Fe−Fe double-atom catalyst supported on sulfur-doped graphitic carbon nitride outperformed other catalysts for oxidation, and it activated PMS likely through a nonradical route of catalyst-mediated electron transfer. This Fe−Fe double-atom catalyst enhanced PMS disinfection kinetics for inactivating murine coronaviruses (i.e., murine hepatitis virus strain A59 (MHV-A59)) by 2.17−4.60 times when compared to PMS treatment alone in diverse environmental media including simulated saliva and freshwater. The molecular-level mechanism of MHV-A59 inactivation was also elucidated. Fe−Fe double-atom catalysis promoted the damage of not only viral proteins and genomes but also internalization, a key step of virus lifecycle in host cells, for enhancing the potency of PMS disinfection. For the first time, our study advances double-atom catalysis for environmental pathogen control and provides fundamental insights of murine coronavirus disinfection. Our work paves a new avenue of leveraging advanced materials for improving disinfection, sanitation, and hygiene practices and protecting public health.
Publications
- Type:
Journal Articles
Status:
Published
Year Published:
2023
Citation:
Zhe Zhou, Mengqiao Li, Yuxin Zhang, Lingchen Kong, Virginia F Smith, Mengyang Zhang, Anders J Gulbrandson, Gordon H Waller, Feng Lin, Xitong Liu, David P Durkin, Hanning Chen, Danmeng Shuai, FeFe Double-Atom Catalysts for Murine Coronavirus Disinfection: Nonradical Activation of Peroxides and Mechanisms of Virus Inactivation, Environ. Sci. Technol. 2023, 57, 9, 38043816
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Progress 01/15/22 to 01/14/23
Outputs
Target Audience:The research outcomes have been presented in the ACS and AEESP conferences. The target audiences include undergraduate and graduate students and professionals in chemistry, catalysis, environmental chemistry, and environmental engineering. Changes/Problems:
Nothing Reported
What opportunities for training and professional development has the project provided?The project has trained one graduate student from underreprented group in STEM. How have the results been disseminated to communities of interest?The results have been disseminated to undergraduate and graduate students and professionals in chemistry, catalysis, environmental chemistry, and environmental engineers in two national and international conferences. What do you plan to do during the next reporting period to accomplish the goals?We will synthesize new single and double atom catalysts with improved features and performance for degrading persistent organic micropollutants, especially the ones that are relevant to the agrochemicals. We will also identify the mechanism of catalyst activation and pollutant transformation.
Impacts
What was accomplished under these goals?
We have successfully synthesized singe and double atom catalysts with Fe loaded on S-doped graphitic carbon nitride, and we have characterized these catalysts with advanced microscopic and spectroscopic tools, evaluated their performance for degrading organic micropollutants and inactivating pathogens. We have also identified key reactive processes and steps for peroxide activation and contaminant/pathogen removal. In particular, S-dopant and Fe-Fe dimer were able to promote the catalytic performance through electron donating/withdrawing and activating peroxymonosulfate, the catalyst mediated electron transfer instead radical-driven oxidation was dominating the contaminant degradation and pathogen inactivation, and the catalyst showed excellent performance for inactiving murine coronaviruses in diverse environmental matrices. The mechanism of virus disinfection was also identified, and the oxidiation damaged viral proteins and genomes but not lipids, and the oxidation compromised virus internalization but not binding in the virus's lifecycle assessment.
Publications
- Type:
Conference Papers and Presentations
Status:
Accepted
Year Published:
2022
Citation:
Fe-Based Double-Atom Catalysts Boosting Electron-Transfer for Disinfecting Coronaviruses (AEESP conference)
- Type:
Conference Papers and Presentations
Status:
Accepted
Year Published:
2022
Citation:
Fe-Based Double-Atom Catalysts Boosting Electron-Transfer for Disinfecting Coronaviruses (ASM Microbe Conference)
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