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Article ; Online: Dynamics of the Oral Microbiome During Initial Military Training at Fort Benning, Georgia.

Zudock, Kristina K / Player, Robert / Ernlund, Amanda / Timm, Collin M / English, Caroline E / Ellis, Michael W / Tribble, David R / Merrell, D Scott / Bennett, Jason W / Millar, Eugene V

Military medicine

2024

Abstract: Introduction: Military trainees are at increased risk for infectious disease outbreaks because of the unique circumstances of the training environment (e.g., close proximity areas and physiologic/psychologic stress). Standard medical countermeasures in ... ...

Abstract	Introduction: Military trainees are at increased risk for infectious disease outbreaks because of the unique circumstances of the training environment (e.g., close proximity areas and physiologic/psychologic stress). Standard medical countermeasures in military training settings include routine immunization (e.g., influenza and adenovirus) as well as chemoprophylaxis [e.g., benzathine penicillin G (Bicillin) for the prevention of group A streptococcal disease] for pathogens associated with outbreaks in these settings. In a population of U.S. Army Infantry trainees, we evaluated changes in the oral microbiome during a 14-week military training cycle. Materials and methods: Trainees were enrolled in an observational cohort study in 2015-2016. In 2015, Bicillin was administered to trainees to ameliorate the risk of group A Streptococcus outbreaks, whereas in 2016, trainees did not receive a Bicillin inoculation. Oropharyngeal swabs were collected from participants at days 0, 7, 14, 28, 56, and 90 of training. Swabs were collected, flash frozen, and stored. DNA was extracted from swabs, and amplicon sequencing of the 16s rRNA gene was performed. Microbiome dynamics were evaluated using the QIIME 2 workflow along with DADA2, SINA with SILVA, and an additional processing in R. Results: We observed that microbiome samples from the baseline (day 0) visit were distinct from one another, whereas samples collected on day 14 exhibited significant microbiome convergence. Day 14 convergence was coincident with an increase in DNA sequences associated with Streptococcus, though there was not a significant difference between Streptococcus abundance over time between 2015 and 2016 (P = .07), suggesting that Bicillin prophylaxis did not significantly impact overall Streptococcus abundance. Conclusions: The temporary convergence of microbiomes is coincident with a rise in communicable infections in this population. The dynamic response of microbiomes during initial military training supports similar observations in the literature of transient convergence of the human microbiome under cohabitation in the time frame including in this experiment. This population and the associated longitudinal studies allow for controlled studies of human microbiome under diverse conditions.
Language	English
Publishing date	2024-01-02
Publishing country	England
Document type	Journal Article
ZDB-ID	391061-1
ISSN	1930-613X ; 0026-4075
ISSN (online)	1930-613X
ISSN	0026-4075
DOI	10.1093/milmed/usad488
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Article ; Online: Nasal microbiota evolution within the congregate setting imposed by military training.

Blum, Faith C / Whitmire, Jeannette M / Bennett, Jason W / Carey, Patrick M / Ellis, Michael W / English, Caroline E / Law, Natasha N / Tribble, David R / Millar, Eugene V / Merrell, D Scott

Scientific reports

2022 Volume 12, Issue 1, Page(s) 11492

Abstract: The human microbiome is comprised of a complex and diverse community of organisms that is subject to dynamic changes over time. As such, cross-sectional studies of the microbiome provide a multitude of information for a specific body site at a particular ...

Abstract	The human microbiome is comprised of a complex and diverse community of organisms that is subject to dynamic changes over time. As such, cross-sectional studies of the microbiome provide a multitude of information for a specific body site at a particular time, but they fail to account for temporal changes in microbial constituents resulting from various factors. To address this shortcoming, longitudinal research studies of the human microbiome investigate the influence of various factors on the microbiome of individuals within a group or community setting. These studies are vital to address the effects of host and/or environmental factors on microbiome composition as well as the potential contribution of microbiome members during the course of an infection. The relationship between microbial constituents and disease development has been previously explored for skin and soft tissue infections (SSTIs) within congregate military trainees. Accordingly, approximately 25% of the population carries Staphylococcus aureus within their nasal cavity, and these colonized individuals are known to be at increased risk for SSTIs. To examine the evolution of the nasal microbiota of U.S. Army Infantry trainees, individuals were sampled longitudinally from their arrival at Fort Benning, Georgia, until completion of their training 90 days later. These samples were then processed to determine S. aureus colonization status and to profile the nasal microbiota using 16S rRNA gene-based methods. Microbiota stability differed dramatically among the individual trainees; some subjects exhibited great stability, some subjects showed gradual temporal changes and some subjects displayed a dramatic shift in nasal microbiota composition. Further analysis utilizing the available trainee metadata suggests that the major drivers of nasal microbiota stability may be S. aureus colonization status and geographic origin of the trainees. Nasal microbiota evolution within the congregate setting imposed by military training is a complex process that appears to be affected by numerous factors. This finding may indicate that future campaigns to prevent S. aureus colonization and future SSTIs among high-risk military trainees may require a 'personalized' approach.
MeSH term(s)	Cross-Sectional Studies ; Disease Susceptibility ; Georgia ; Humans ; Longitudinal Studies ; Microbiota/genetics ; Military Personnel/education ; Nasal Cavity/microbiology ; RNA, Ribosomal, 16S/genetics ; Risk Factors ; Soft Tissue Infections/microbiology ; Staphylococcal Skin Infections/microbiology ; Staphylococcus aureus/genetics ; Staphylococcus aureus/isolation & purification
Chemical Substances	RNA, Ribosomal, 16S
Language	English
Publishing date	2022-07-07
Publishing country	England
Document type	Journal Article ; Research Support, Non-U.S. Gov't ; Research Support, N.I.H., Extramural ; Research Support, U.S. Gov't, Non-P.H.S.
ZDB-ID	2615211-3
ISSN	2045-2322 ; 2045-2322
ISSN (online)	2045-2322
ISSN	2045-2322
DOI	10.1038/s41598-022-15059-z
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Article: Molecular Electronic Effects on the Thermal Grafting of Aryl Iodides to TiO2 Surfaces

English, Caroline R / Hamers Robert J

The Journal of Physical Chemistry C. 2015 Dec. 17, v. 119, no. 50

2015

Abstract: Recent studies have shown that aromatic iodides can readily graft to hydroxylated surfaces of TiO₂ and other metal oxides, forming a convenient route to molecular functionalization of metal oxides. While these reactions appear similar to the Williamson ... ...

Abstract	Recent studies have shown that aromatic iodides can readily graft to hydroxylated surfaces of TiO₂ and other metal oxides, forming a convenient route to molecular functionalization of metal oxides. While these reactions appear similar to the Williamson ether synthesis of organic chemistry, the SN2 mechanism typically invoked in solution phase reactions is less accessible on surfaces, and the mechanism of the surface reactions is poorly understood. We have undertaken a combined experimental and computational study in an effort to understand how the molecular electronic structure impacts the surface reactivity. Computational studies of reaction enthalpies were compared were used to generate Hammett plots that were then compared to experimental measurements of surface grafting rate for molecules with different substituent groups. Our results show that there is poor correlation between Hammett parameters and surface reactivity. Additional experiments were conducted to evaluate the impact of molecular hydrophobic character on reaction rate. Our results suggest that radical reactions or other pathways are likely responsible for controlling reactivity of aromatic halides with TiO₂ surfaces.
Keywords	enthalpy ; hydrophobicity ; hydroxylation ; iodides ; organic chemistry ; organoiodine compounds ; physical chemistry ; titanium dioxide
Language	English
Dates of publication	2015-1217
Size	p. 27972-27981.
Publishing place	American Chemical Society
Document type	Article
ISSN	1932-7455
DOI	10.1021%2Facs.jpcc.5b08333
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Evolution of chemical-specific adjustment factors (CSAF) based on recent international experience; increasing utility and facilitating regulatory acceptance.

Bhat, Virunya S / Meek, M E Bette / Valcke, Mathieu / English, Caroline / Boobis, Alan / Brown, Richard

Critical reviews in toxicology

2017 Volume 47, Issue 9, Page(s) 729–749

Abstract: The application of chemical-specific toxicokinetic or toxicodynamic data to address interspecies differences and human variability in the quantification of hazard has potential to reduce uncertainty and better characterize variability compared with the ... ...

Abstract	The application of chemical-specific toxicokinetic or toxicodynamic data to address interspecies differences and human variability in the quantification of hazard has potential to reduce uncertainty and better characterize variability compared with the use of traditional default or categorically-based uncertainty factors. The present review summarizes the state-of-the-science since the introduction of the World Health Organization/International Programme on Chemical Safety (WHO/IPCS) guidance on chemical-specific adjustment factors (CSAF) in 2005 and the availability of recent applicable guidance including the WHO/IPCS guidance on physiologically-based pharmacokinetic (PBPK) modeling in 2010 as well as the U.S. EPA guidance on data-derived extrapolation factors in 2014. A summary of lessons learned from an analysis of more than 100 case studies from global regulators or published literature illustrates the utility and evolution of CSAF in regulatory decisions. Challenges in CSAF development related to the adequacy of, or confidence in, the supporting data, including verification or validation of PBPK models. The analysis also identified issues related to adequacy of CSAF documentation, such as inconsistent terminology and often limited and/or inconsistent reporting, of both supporting data and/or risk assessment context. Based on this analysis, recommendations for standardized terminology, documentation and relevant interdisciplinary research and engagement are included to facilitate the continuing evolution of CSAF development and guidance.
MeSH term(s)	Chemical Safety/legislation & jurisprudence ; Chemical Safety/trends ; Humans ; International Cooperation ; Research/standards ; Research/trends ; Risk Assessment/trends ; Uncertainty ; United States ; United States Environmental Protection Agency ; World Health Organization
Language	English
Publishing date	2017-10
Publishing country	England
Document type	Journal Article ; Review
ZDB-ID	1097071-x
ISSN	1547-6898 ; 1040-8444
ISSN (online)	1547-6898
ISSN	1040-8444
DOI	10.1080/10408444.2017.1303818
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Article ; Online: SARS-CoV-2 infection is associated with self-reported post-acute neuropsychological symptoms within six months of follow-up.

Andronescu, Liana R / Richard, Stephanie A / Scher, Ann I / Lindholm, David A / Mende, Katrin / Ganesan, Anuradha / Huprikar, Nikhil / Lalani, Tahaniyat / Smith, Alfred / Mody, Rupal M / Jones, Milissa U / Bazan, Samantha E / Colombo, Rhonda E / Colombo, Christopher J / Ewers, Evan / Larson, Derek T / Maves, Ryan C / Berjohn, Catherine M / Maldonado, Carlos J /

English, Caroline / Sanchez Edwards, Margaret / Rozman, Julia S / Rusiecki, Jennifer / Byrne, Celia / Simons, Mark P / Tribble, David / Burgess, Timothy H / Pollett, Simon D / Agan, Brian K

PloS one

2024 Volume 19, Issue 4, Page(s) e0297481

Abstract: Background: Chronic neuropsychological sequelae following SARS-CoV-2 infection, including depression, anxiety, fatigue, and general cognitive difficulties, are a major public health concern. Given the potential impact of long-term neuropsychological ... ...

Abstract	Background: Chronic neuropsychological sequelae following SARS-CoV-2 infection, including depression, anxiety, fatigue, and general cognitive difficulties, are a major public health concern. Given the potential impact of long-term neuropsychological impairment, it is important to characterize the frequency and predictors of this post-infection phenotype. Methods: The Epidemiology, Immunology, and Clinical Characteristics of Emerging Infectious Diseases with Pandemic Potential (EPICC) study is a longitudinal study assessing the impact of SARS-CoV-2 infection in U.S. Military Healthcare System (MHS) beneficiaries, i.e. those eligible for care in the MHS including active duty servicemembers, dependents, and retirees. Four broad areas of neuropsychological symptoms were assessed cross-sectionally among subjects 1-6 months post-infection/enrollment, including: depression (Patient Health Questionnaire-9), anxiety (General Anxiety Disorder-7), fatigue (PROMIS® Fatigue 7a), and cognitive function (PROMIS® Cognitive Function 8a and PROMIS® Cognitive Function abilities 8a). Multivariable Poisson regression models compared participants with and without SARS-CoV-2 infection history on these measures, adjusting for sex, ethnicity, active-duty status, age, and months post-first positive or enrollment of questionnaire completion (MPFP/E); models for fatigue and cognitive function were also adjusted for depression and anxiety scores. Results: The study population included 2383 participants who completed all five instruments within six MPFP/E, of whom 687 (28.8%) had at least one positive SARS-CoV-2 test. Compared to those who had never tested positive for SARS-CoV-2, the positive group was more likely to meet instrument-based criteria for depression (15.4% vs 10.3%, p<0.001), fatigue (20.1% vs 8.0%, p<0.001), impaired cognitive function (15.7% vs 8.6%, p<0.001), and impaired cognitive function abilities (24.3% vs 16.3%, p<0.001). In multivariable models, SARS-CoV-2 positive participants, assessed at an average of 2.7 months after infection, had increased risk of moderate to severe depression (RR: 1.44, 95% CI 1.12-1.84), fatigue (RR: 2.07, 95% CI 1.62-2.65), impaired cognitive function (RR: 1.64, 95% CI 1.27-2.11), and impaired cognitive function abilities (RR: 1.41, 95% CI 1.15-1.71); MPFP/E was not significant. Conclusions: Participants with a history of SARS-CoV-2 infection were up to twice as likely to report cognitive impairment and fatigue as the group without prior SARS-CoV-2 infection. These findings underscore the continued importance of preventing SARS-CoV-2 infection and while time since infection/enrollment was not significant through 6 months of follow-up, this highlights the need for additional research into the long-term impacts of COVID-19 to mitigate and reverse these neuropsychological outcomes.
MeSH term(s)	Humans ; Self Report ; COVID-19/complications ; COVID-19/epidemiology ; SARS-CoV-2 ; Follow-Up Studies ; Longitudinal Studies ; Fatigue/epidemiology ; Fatigue/etiology ; Anxiety Disorders
Language	English
Publishing date	2024-04-16
Publishing country	United States
Document type	Journal Article
ZDB-ID	2267670-3
ISSN	1932-6203 ; 1932-6203
ISSN (online)	1932-6203
ISSN	1932-6203
DOI	10.1371/journal.pone.0297481
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Article ; Online: Safety, immunogenicity, and efficacy of NDV-3A against Staphylococcus aureus colonization: A phase 2 vaccine trial among US Army Infantry trainees.

Millar, Eugene V / Bennett, Jason W / Barin, Burc / Carey, Patrick M / Law, Natasha N / English, Caroline E / Schwartz, Michael M / Cochrane, Terrence / Ellis, Michael W / Tribble, David R / Timothy Cooke, M / Hennessey, John P

Vaccine

2021 Volume 39, Issue 23, Page(s) 3179–3188

Abstract: Background: Military trainees are at increased risk for Staphylococcus aureus colonization and infection. Disease prevention strategies are needed, but a S. aureus vaccine does not currently exist.: Methods: We enrolled US Army Infantry trainees ( ... ...

Abstract	Background: Military trainees are at increased risk for Staphylococcus aureus colonization and infection. Disease prevention strategies are needed, but a S. aureus vaccine does not currently exist. Methods: We enrolled US Army Infantry trainees (Fort Benning, GA) in a phase 2, randomized, double-blind, placebo-controlled trial of NDV-3A, a vaccine containing a recombinant adhesin/invasion protein of Candida albicans that has structural similarity to the S. aureus protein clumping factor A. Study participants received one intramuscular dose of NDV-3A or placebo (adjuvant alone) within 72 h of arrival on base. Longitudinal nasal and oral (throat) swabs were collected throughout the 14-week Infantry training cycle. Safety, immunogenicity, and efficacy of NDV-3A against S. aureus nasal / oral acquisition were the endpoints. Results: The NDV-3A candidate had minimal reactogenicity and elicited robust antigen-specific B- and T-cell responses. During the 56-day post-vaccination period, there was no difference in the incidence of S. aureus nasal acquisition between those who were randomized to receive NDV-3A vs. placebo (25.6% vs. 29.1%; vaccine efficacy [VE]: 12.1%; p = 0.31). In time-to-event analysis, there was no difference between study groups with respect to the S. aureus colonization-free interval (VE: 13%; p = 0.29). Similarly, the efficacy of NDV-3A against S. aureus oral acquisition was poor (VE: 2.4%; p = 0.52). Conclusions: A single dose of NDV-3A did not prevent nasal nor oral acquisition of S. aureus in a population of military trainees at high risk for colonization.
MeSH term(s)	Humans ; Immunogenicity, Vaccine ; Military Personnel ; Staphylococcal Infections/prevention & control ; Staphylococcal Vaccines/adverse effects ; Staphylococcus aureus ; Vaccines
Chemical Substances	Staphylococcal Vaccines ; Vaccines
Language	English
Publishing date	2021-05-04
Publishing country	Netherlands
Document type	Clinical Trial, Phase II ; Journal Article ; Randomized Controlled Trial ; Research Support, U.S. Gov't, Non-P.H.S.
ZDB-ID	605674-x
ISSN	1873-2518 ; 0264-410X
ISSN (online)	1873-2518
ISSN	0264-410X
DOI	10.1016/j.vaccine.2021.04.031
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Article: Safety, immunogenicity, and efficacy of NDV-3A against Staphylococcus aureus colonization: A phase 2 vaccine trial among US Army Infantry trainees

Elsevier Ltd Vaccine. 2021 May 27, v. 39, no. 23

2021

Abstract: Military trainees are at increased risk for Staphylococcus aureus colonization and infection. Disease prevention strategies are needed, but a S. aureus vaccine does not currently exist.We enrolled US Army Infantry trainees (Fort Benning, GA) in a phase 2, ...

Abstract	Military trainees are at increased risk for Staphylococcus aureus colonization and infection. Disease prevention strategies are needed, but a S. aureus vaccine does not currently exist.We enrolled US Army Infantry trainees (Fort Benning, GA) in a phase 2, randomized, double-blind, placebo-controlled trial of NDV-3A, a vaccine containing a recombinant adhesin/invasion protein of Candida albicans that has structural similarity to the S. aureus protein clumping factor A. Study participants received one intramuscular dose of NDV-3A or placebo (adjuvant alone) within 72 h of arrival on base. Longitudinal nasal and oral (throat) swabs were collected throughout the 14-week Infantry training cycle. Safety, immunogenicity, and efficacy of NDV-3A against S. aureus nasal / oral acquisition were the endpoints.The NDV-3A candidate had minimal reactogenicity and elicited robust antigen-specific B- and T-cell responses. During the 56-day post-vaccination period, there was no difference in the incidence of S. aureus nasal acquisition between those who were randomized to receive NDV-3A vs. placebo (25.6% vs. 29.1%; vaccine efficacy [VE]: 12.1%; p = 0.31). In time-to-event analysis, there was no difference between study groups with respect to the S. aureus colonization-free interval (VE: 13%; p = 0.29). Similarly, the efficacy of NDV-3A against S. aureus oral acquisition was poor (VE: 2.4%; p = 0.52).A single dose of NDV-3A did not prevent nasal nor oral acquisition of S. aureus in a population of military trainees at high risk for colonization.
Keywords	Candida albicans ; Staphylococcus aureus ; T-lymphocytes ; adhesins ; adjuvants ; disease prevention ; immunogenicity ; nose ; placebos ; risk ; throat ; vaccines
Language	English
Dates of publication	2021-0527
Size	p. 3179-3188.
Publishing place	Elsevier Ltd
Document type	Article
Note	NAL-AP-2-clean
ZDB-ID	605674-x
ISSN	1873-2518 ; 0264-410X
ISSN (online)	1873-2518
ISSN	0264-410X
DOI	10.1016/j.vaccine.2021.04.031
Database	NAL-Catalogue (AGRICOLA)

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Journal: Conversion of tris (8-quinolinolato-N1, O8) aluminium to 8-hydroxyquinoline and activity in bacterial reverse mutation assays

English, Caroline J.

Mutation Research. Genetic Toxicology and Environmental Mutagenesis : International Journal on Mutagenesis, Chromosome Breakage and Related Subjects

2005 Volume 582, Page(s) S. 95–104

Language	English
Document type	Journal
Database	OPAC and Environmental database (ULIDAT) of The Federal Environment Agency (UBA)

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Article ; Online: Persistent COVID-19 Symptoms at 6 Months After Onset and the Role of Vaccination Before or After SARS-CoV-2 Infection.

Richard, Stephanie A / Pollett, Simon D / Fries, Anthony C / Berjohn, Catherine M / Maves, Ryan C / Lalani, Tahaniyat / Smith, Alfred G / Mody, Rupal M / Ganesan, Anuradha / Colombo, Rhonda E / Lindholm, David A / Morris, Michael J / Huprikar, Nikhil / Colombo, Christopher J / Madar, Cristian / Jones, Milissa / Larson, Derek T / Bazan, Samantha E / Mende, Katrin /

Saunders, David / Livezey, Jeffrey / Lanteri, Charlotte A / Scher, Ann I / Byrne, Celia / Rusiecki, Jennifer / Ewers, Evan / Epsi, Nusrat J / Rozman, Julia S / English, Caroline / Simons, Mark P / Tribble, David R / Agan, Brian K / Burgess, Timothy H

JAMA network open

2023 Volume 6, Issue 1, Page(s) e2251360

Abstract: Importance: Understanding the factors associated with post-COVID conditions is important for prevention.: Objective: To identify characteristics associated with persistent post-COVID-19 symptoms and to describe post-COVID-19 medical encounters.: ... ...

Abstract	Importance: Understanding the factors associated with post-COVID conditions is important for prevention. Objective: To identify characteristics associated with persistent post-COVID-19 symptoms and to describe post-COVID-19 medical encounters. Design, setting, and participants: This cohort study used data from the Epidemiology, Immunology, and Clinical Characteristics of Emerging Infectious Diseases With Pandemic Potential (EPICC) study implemented in the US military health system (MHS); MHS beneficiaries aged 18 years or older who tested positive for SARS-CoV-2 from February 28, 2020, through December 31, 2021, were analyzed, with 1-year follow-up. Exposures: SARS-CoV-2 infection. Main outcomes and measures: The outcomes analyzed included survey-reported symptoms through 6 months after SARS-CoV-2 infection and International Statistical Classification of Diseases and Related Health Problems, Tenth Revision diagnosis categories reported in medical records 6 months following SARS-CoV-2 infection vs 3 months before infection. Results: More than half of the 1832 participants in these analyses were aged 18 to 44 years (1226 [66.9%]; mean [SD] age, 40.5 [13.7] years), were male (1118 [61.0%]), were unvaccinated at the time of their infection (1413 [77.1%]), and had no comorbidities (1290 [70.4%]). A total of 728 participants (39.7%) had illness that lasted 28 days or longer (28-89 days: 364 [19.9%]; ≥90 days: 364 [19.9%]). Participants who were unvaccinated prior to infection (risk ratio [RR], 1.39; 95% CI, 1.04-1.85), reported moderate (RR, 1.80; 95% CI, 1.47-2.22) or severe (RR, 2.25; 95% CI, 1.80-2.81) initial illnesses, had more hospitalized days (RR per each day of hospitalization, 1.02; 95% CI, 1.00-1.03), and had a Charlson Comorbidity Index score of 5 or greater (RR, 1.55; 95% CI, 1.01-2.37) were more likely to report 28 or more days of symptoms. Among unvaccinated participants, postinfection vaccination was associated with a 41% lower risk of reporting symptoms at 6 months (RR, 0.59; 95% CI, 0.40-0.89). Participants had higher risk of pulmonary (RR, 2.00; 95% CI, 1.40-2.84), diabetes (RR, 1.46; 95% CI, 1.00-2.13), neurological (RR, 1.29; 95% CI, 1.02-1.64), and mental health-related medical encounters (RR, 1.28; 95% CI, 1.01-1.62) at 6 months after symptom onset than at baseline (before SARS-CoV-2 infection). Conclusions and relevance: In this cohort study, more severe acute illness, a higher Charlson Comorbidity Index score, and being unvaccinated were associated with a higher risk of reporting COVID-19 symptoms lasting 28 days or more. Participants with COVID-19 were more likely to seek medical care for diabetes, pulmonary, neurological, and mental health-related illness for at least 6 months after onset compared with their pre-COVID baseline health care use patterns. These findings may inform the risk-benefit ratio of COVID-19 vaccination policy.
MeSH term(s)	Humans ; Male ; Adult ; Female ; COVID-19/epidemiology ; COVID-19/prevention & control ; SARS-CoV-2 ; COVID-19 Vaccines ; Cohort Studies ; Post-Acute COVID-19 Syndrome
Chemical Substances	COVID-19 Vaccines
Language	English
Publishing date	2023-01-03
Publishing country	United States
Document type	Journal Article ; Research Support, U.S. Gov't, Non-P.H.S. ; Research Support, N.I.H., Extramural
ISSN	2574-3805
ISSN (online)	2574-3805
DOI	10.1001/jamanetworkopen.2022.51360
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Article ; Online: Formation of self-assembled monolayers of π-conjugated molecules on TiO2 surfaces by thermal grafting of aryl and benzyl halides.

English, Caroline R / Bishop, Lee M / Chen, Jixin / Hamers, Robert J

Langmuir : the ACS journal of surfaces and colloids

2012 Volume 28, Issue 17, Page(s) 6866–6876

Abstract: We demonstrate the formation of molecular monolayers of π-conjugated organic molecules on nanocrystalline TiO(2) surfaces through the thermal grafting of benzyl and aryl halides. X-ray photoelectron spectroscopy and Fourier-transform infrared ... ...

Abstract	We demonstrate the formation of molecular monolayers of π-conjugated organic molecules on nanocrystalline TiO(2) surfaces through the thermal grafting of benzyl and aryl halides. X-ray photoelectron spectroscopy and Fourier-transform infrared spectroscopy were used to characterize the reactivity of aryl and benzyl chlorides, bromides, and iodides with TiO(2) surfaces, along with controls consisting of nonhalogenated compounds. Our results show that benzyl and aryl halides follow a similar reactivity trend (I > Br > Cl >> H). While the ability to graft benzyl halides is consistent with the well-known Williamson ether synthesis, the grafting of aryl halides has no similar precedent. The unique reactivity of the TiO(2) surface is demonstrated using nuclear magnetic resonance spectroscopy to compare the surface reactions with the liquid-phase interactions of benzyl and aryl iodides with tert-butanol and -butoxide anion. While the aryl iodides show no detectable reactivity with a tert-butanol/tert-butoxide mixture, they react with TiO(2) within 2 h at 50 °C. Atomic force microscopy studies show that grafting of 4-iodo-1-(trifluoromethyl)benzene onto the rutile TiO(2)(110) surface leads to a very uniform, homogeneous molecular layer with a thickness of ∼0.45 nm, demonstrating formation of a self-terminating molecular monolayer. Thermal grafting of aryl iodides provides a facile route to link π-conjugated molecules to TiO(2) surfaces with the shortest possible linkage between the conjugated electron system and the TiO(2).
Language	English
Publishing date	2012-05-01
Publishing country	United States
Document type	Journal Article
ZDB-ID	2005937-1
ISSN	1520-5827 ; 0743-7463
ISSN (online)	1520-5827
ISSN	0743-7463
DOI	10.1021/la300271h
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