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Single-Photon-Induced Post-Ionization to Boost Ion Yields in MALDI Mass Spectrometry Imaging**

Angewandte Chemie 2022年第34期134卷

作者： Dr. Christoph Bookmeyer Ulrich Röhling Prof. Dr. Klaus Dreisewerd Dr. Jens Soltwisch Institute of Hygiene University of Münster Robert-Koch-Str. 41 48149 Münster Germany Metabolomics Interdisciplinary Laboratory University of Tarragona Avinguda Països Catalans 26 43007 Tarragona (Spain) Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (equal) Visualization (lead) Writing - original draft (lead) Writing - review & editing (equal) Institute of Medical Physics and Biophysics University of Münster Robert-Koch-Str. 31 48149 Münster Germany Deceased (2021) Contribution: Conceptualization (supporting) Investigation (lead) Resources (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (equal) Funding acquisition (equal) Methodology (supporting) Supervision (equal) Writing - original draft (supporting) Writing - review & editing (equal) Contribution: Conceptualization (lead) Data curation (supporting) Formal analysis (supporting) Funding acquisition (equal) Investigation (supporting) Methodology (equal) Supervision (lead) Writing - original draft (lead) Writing - review & editing (equal)

Matrix-assisted laser desorption/ionization mass spectrometry imaging (MALDI-MSI) is a rapidly growing method in the life sciences. However, for many analyte classes, its sensitivity is limited due to poor ionization efficiencies. To mitigate this problem, we here introduce a novel post-ionization scheme based on single-photon induced chemical ionization using pulsed RF-Kr lamps. The fine-vacuum conditions of a dual ion-funnel ion source effectively thermalize the evolving MALDI plume and enable ample gas-phase reactions. Injected chemical dopants crucially support fragment-less ionization to [ M +H] + /[ M −H] − species. Based on this interplay, numerous glycerophospho-, sphingo-, and further lipids, registered from mammalian tissue sections, were boosted by up to three orders of magnitude, similar to results obtained with laser-based post-ionization (MALDI-2). Experiments with deuterated matrix and dopant, however, indicated complex chemical ionization pathways different from MALDI-2.

关键词： Analytical Methods Lipidomics MALDI-MS Imaging Mass Spectrometry Post-Ionization

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Hydrophobicity Directed Chiral Self-Assembly and Aggregation-Induced Emission: Diacetylene-Cored Pseudopeptide Chiral Dopants

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Angewandte Chemie 2022年第42期134卷

作者： Govind P. Maurya Deepak Verma Aloka Sinha Luc Brunsveld V. Haridas Department of Chemistry Indian Institute of Technology Delhi Hauz Khas New Delhi- 110016 India Contribution: Conceptualization (lead) Investigation (lead) Writing - original draft (equal) Writing - review & editing (supporting) Department of Physics Indian Institute of Technology Delhi Hauz Khas New Delhi- 110016 India Contribution: Investigation (supporting) Contribution: Investigation (supporting) Resources (supporting) Department of Biomedical Engineering Laboratory of Chemical Biology and Institute for Complex Molecular Systems Eindhoven University of Technology P.O. Box 513 5600 MB Eindhoven The Netherlands Contribution: Formal analysis (supporting) Validation (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (lead) Data curation (supporting) Formal analysis (equal) Funding acquisition (lead) Investigation (supporting) Methodology (equal) Project administration (lead) Resources (lead) Software (equal) Supervision (lead) Validation (equal) Visualization (equal) Writing - original draft (lead) Writing - review & editing (lead)

Here we delineate simple and tunable hydrophobically driven chiral functional assemblies of diacetylene cored pseudopeptides. These amino acid appended, rigid core dialkynes constitute promising chiral supramolecular building blocks for materials properties engineering. The chiral appended amino acid elements allow for simple tuning of solubility and interaction properties as well as governing chirality, while the central dialkyne core can impart hydrophobically driven assembly and Aggregation Induced Emission (AIE) properties. The self-assembly of these rod-like dialkynes can be regulated by tuning the solvent environment, with for example self-assembly into vesicles in acetonitrile and into helical organization with AIE in a H 2 O/DMSO mixture. Of additional high interest, these supramolecular materials, themselves devoid of liquid crystal (LC) properties, can induce chirality into non-chiral LC matrices with high helical twisting power.

关键词： Aggregation-Induced Emission Liquid Crystal Pseudopeptides Self-Assembly Supramolecular Helix

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Fostering resilience during the COVID-19 pandemic via a digital mental health intervention—A pilot study

Mental Health Science

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Mental Health Science 2023年第3期1卷

作者： Jennifer K. Kulke Barbara Nacke Corinna Jacobi TUM Department of Sport and Health Sciences SG Technical University of Munich Munich Germany Department of Clinical Psychology and Psychotherapy Institute of Psychology and Education Ulm University Ulm Germany Contribution: Data curation (lead) Formal analysis (lead) Investigation (equal) Visualization (lead) Writing - original draft (lead) Writing - review & editing (equal) Institute of Clinical Psychology and Psychotherapy Technische Universität Dresden Dresden Germany Contribution: Conceptualization (equal) Investigation (equal) Project administration (lead) Supervision (lead) Writing - original draft (supporting) Writing - review & editing (equal) Contribution: Conceptualization (lead) Funding acquisition (lead) Methodology (equal) Resources (lead) Supervision (lead) Writing - review & editing (equal)

During the coronavirus disease 2019 (COVID-19) pandemic, mental health burden of university members sharply increased. Specific interventions to address pandemic-related psychological distress did not yet exist. Current studies show that digital interventions reduce this burden, the investigation of changes in resilience as an outcome is lacking in these studies though. We therefore developed and evaluated the internet- and mobile-based intervention “bounce” to foster resilience, reduce perceived stress, and psychological symptom burden among university members during the pandemic. The 8-week, unguided internet- and mobile-based intervention consists of one mandatory module promoting resilience and six optional modules on pandemic-related topics. The study was designed as a one-arm, longitudinal pilot study with a baseline and postintervention assessment and self-reported resilience, perceived stress, and psychological symptom burden as outcome measures. The use and acceptance of the intervention modules were recorded and analyzed. A total of 798 individuals were given access to the intervention ( n = 70 employees, n = 728 students, M = 26.05 years, 71.8% women). Of these, 273 participants (34%) completed the postassessment. On average, participants logged on to the intervention platform four times and completed an average of 1.90 (SD = 1.64) modules. The intervention as a whole and all modules were well accepted by participants. Intention-to-treat analyses showed a significant increase in resilience ( t = −4.69, p < 0.001, d = 0.23) and a significant reduction in perceived stress ( t = 6.50, p < 0.001, d = 0.32), and psychological symptom burden ( t = 3.59, p < 0.001, d = 0.18) from baseline to postintervention. This study demonstrates that digital interventions can be easily developed and used as means to reduce mental health burden in large populations during a pandemic. The need for randomized controlled trials with follow-up assessments to examine longer-term e

关键词： COVID-19 pandemic digital mental health intervention faculty prevention psychological resilience psychological stress students

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The equity group: Supporting Cochrane's social responsibility of improving health equity

Cochrane Evidence Synthesis and Methods

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Cochrane Evidence Synthesis and Methods 2023年第3期1卷

作者： Roses Parker Jennifer Petkovic Jordi Pardo Pardo Andrea Darzi Omar Dewidar Joanne Khabsa Elizabeth Kristjansson Tamara Lotfi Olivia Magwood Lawrence Mbuagbaw Kevin Pottie Alison Riddle Ammar Saad Eve Tomlinson Peter Tugwell Vivian Welch The Cochrane Collaboration London UK Contribution: Conceptualization Data curation Formal analysis Methodology Project administration Resources Validation Visualization Writing - original draft Writing - review & editing Bruyère Research Institute and University of Ottawa Ottawa Ontario Canada Contribution: Conceptualization Data curation Formal analysis Methodology Supervision Writing - original draft Writing - review & editing Department of Medicine Faculty of Medicine University of Ottawa Ottawa Ontario Canada Ottawa Hospital Research Institute Ottawa Methods Centre Ottawa Ontario Canada Department of Health Research Methods Evidence and Impact McMaster University Hamilton Ontario Canada Department of Anesthesia Faculty of Health Sciences McMaster University Hamilton Ontario Canada Michael G. DeGroote National Pain Center McMaster University Hamilton Ontario Canada Contribution: Data curation Validation Visualization Writing - review & editing Contribution: Conceptualization Validation Writing - original draft Writing - review & editing Clinical Research Institute American University of Beirut Medical Center Beirut Lebanon Contribution: Conceptualization Validation Writing - review & editing School of Psychology Faculty of Social Sciences University of Ottawa Ottawa Ontario Canada Bruyère Research Institute Ottawa Ontario Canada The Interdisciplinary School of Health Sciences University of Ottawa Ottawa Ontario Canada Department of Pediatrics McMaster University Hamilton Ontario Canada Biostatistics Unit Father Sean O'Sullivan Research Centre St Joseph's Healthcare Hamilton Ontario Canada Centre for Development of Best Practices in Health (CDBPH) Yaoundé Central Hospital Yaoundé Cameroon Department of Global Health Division of Epidemiology and Biostatistics Stellenbosch University Cape Town South Africa Departments of Family Medicine Epidemiology and Biostatistics Western University London Ontario Canada School of Epidemiol

Introduction Health equity is a moral and ethical imperative for clinicians, researchers, policymakers, and all who use health research. Both Cochrane and the Campbell Collaboration have focused on health equity for many years. Methods The new Equity Group will continue and expand this work by designing a program of projects aiming to (1) promote equity in the evidence base, (2) ensure equitable processes for stakeholder engagement, (3) produce high-priority, equity-focused evidence syntheses, (4) build capacity for equity design, analysis, and reporting, and (5) promote equity in implementation tools. Results We will build on our current network of collaborators and create a group structure striving to recruit across the PROGRESS-Plus characteristics. Conclusion We invite readers to join our cause and contribute wherever they are able. Together, we can help Cochrane achieve its social responsibility of improving health equity at a planetary level.

关键词： diversity and inclusion evidence synthesis health equity PROGRESS-Plus social determinants of health stakeholder engagement systematic reviews

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Functional organization of extracellular hyaluronan, CD44, and RHAMM

Proteoglycan Research

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Proteoglycan Research 2023年第2期1卷

作者： Mary K. Cowman Eva A. Turley Department of Biomedical Engineering Tandon School of Engineering New York University New York New York USA Department of Orthopedic Surgery Grossman School of Medicine New York University New York New York USA Eva A. Turley London Regional Cancer Program London Health Sciences Centre Lawson Health Research Institute Room A4-931A 790 Commissioners Rd East London ON N6A 4L6 Canada. Contribution: Conceptualization Formal analysis Methodology Project administration Visualization Writing - original draft Writing - review & editing London Regional Cancer Program London Health Sciences Centre Lawson Health Research Institute London Ontario Canada Department of Oncology Schulich School of Medicine and Dentistry Western University London Ontario Canada Department of Biochemistry Schulich School of Medicine and Dentistry Western University London Ontario Canada Department of Surgery Schulich School of Medicine and Dentistry Western University London Ontario Canada Contribution: Conceptualization Data curation Formal analysis Funding acquisition Investigation Methodology Project administration Resources Visualization Writing - original draft Writing - review & editing

The integral membrane protein CD44 is constitutively expressed in most tissues, and is the primary cell surface receptor for hyaluronan (HA). HA is the key scaffolding organizer of proteoglycans and receptors in the extracellular matrix. CD44 is expressed as cell type-specific and context-specific alternatively spliced isoforms with variable glycosylation and interreceptor interactions. CD44 plays a critical role in the organization and patterning of domains in the cell membrane, achieved through linking the cortical actin cytoskeleton with the pericellular HA matrix. This functional and spatial organization of CD44 and HA maintains a protective and homeostatic cellular microenvironment. Tissue injury and cellular stress result in HA fragmentation and unconventional export of the CD44 coreceptor, RHAMM, which collectively alter the homeostatic organization of CD44/HA. The resulting interplay among HA, HA fragments, CD44 and RHAMM triggers cellular responses such as cell motility that contribute to tissue repair, and disease processes. Here we review current understanding of the structural biology of HA, CD44, and RHAMM, and provide an overview of their known functional organization and patterning at the cell surface. Changes in their surface organization act as sensors for detecting danger, and are critical to the understanding of consequent intracellular signaling and response mechanisms to cellular stress.

关键词： CD44 extracellular matrix hyaluronan pericellular matrix RHAMM

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Living cell-laden hydrogels: Unleashing the future of responsive biohybrid systems

Responsive Materials

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Responsive Materials 2023年第1期1卷

作者： Xuejia Hu Bing Lei Sen-Sen Li Lu-Jian Chen Quan Li Department of Electronic Engineering School of Electronic Science and Engineering Fujian Key Laboratory of Ultrafast Laser Technology and Applications Xiamen University Xiamen China Contribution: Conceptualization (equal) Data curation (equal) Funding acquisition (supporting) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Formal analysis (supporting) Visualization (equal) Writing - original draft (equal) Writing - review & editing (equal) Contribution: Funding acquisition (supporting) Visualization (supporting) Writing - original draft (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (equal) Funding acquisition (lead) Project administration (equal) Resources (lead) Writing - original draft (equal) Writing - review & editing (equal) Institute of Advanced Materials and School of Chemistry and Chemical Engineering Southeast University Nanjing China Lu-Jian Chen and Quan Li. Contribution: Conceptualization (equal) Validation (supporting) Writing - original draft (supporting) Writing - review & editing (supporting)

Responsive biohybrid systems have the potential to overcome limitations of both natural and artificial machines in terms of efficiency, accuracy, and functionality. As functional units, living cells act as bricks for building biohybrid machines, where the extracellular matrix mimics hydrogels to act as ideal biological concrete. Combining living cells with hydrogels offers unique advantages in simulating human tissues or organs, which unleashes the future of biohybrid systems, and thus has attracted extensive attention. Herein, recent progress in cell-laden hydrogel-based responsive biohybrid systems is summarized to provide a basic understanding of how these systems are built from the bottom up and how to achieve the complex functions. This review focuses on advanced manufacturing technologies for responsive biohybrid systems, including laden cells in hydrogel matrices, three-dimensional bioprinting, and microfluidic manufacturing. Subsequently, the innovative applications of these works, including actuators, sensors, and engineered functional materials, are presented, along with different triggering mechanisms that are highlighted. Finally, the current challenges and future opportunities in the field are addressed. This review provides a unique perspective and is hoped to inspire fields such as biohybrid technologies, soft robots, and tissue engineering.

关键词： hydrogel living cell responsive biohybrid system soft robot

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Implications of Sea Breezes on Air Quality Monitoring in a Coastal Urban Environment: Evidence From High Resolution Modeling of NO2and O3

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Journal of Geophysical Research: Atmospheres 2023年第11期128卷 e2022JD037860-e2022JD037860页

作者： Bo Wang Jeffrey A. Geddes Taylor J. Adams Elena S. Lind Brian C. McDonald Jian He Colin Harkins Dan Li Gabriele G. Pfister Department of Earth and Environment Boston University MA Boston USA B. Wang Contribution: Conceptualization Methodology Formal analysis Investigation Resources Writing - original draft Writing - review & editing Visualization Contribution: Conceptualization Methodology Formal analysis Investigation Resources Data curation Writing - review & editing Supervision Project administration Funding acquisition Contribution: Resources Writing - review & editing Department of Electrical and Computer Engineering Virginia Tech VA Blacksburg USA Now at NASA Goddard Space Flight Center Greenbelt MD USA Chemical Sciences Laboratory NOAA Earth System Research Laboratories CO Boulder USA Cooperative Institute for Research in Environmental Sciences University of Colorado CO Boulder USA Contribution: Methodology Resources Writing - review & editing Atmospheric Chemistry Observations and Modeling Laboratory NCAR CO Boulder USA Contribution: Conceptualization Resources Writing - review & editing

Coastal urban environments face unique challenges associated with air quality-meteorology interactions. In this study, high resolution chemical transport modeling over the Greater Boston area was performed to improve our understanding of sea breezes impacts on the spatiotemporal variability of primary and secondary pollutants. We perform WRF-Chem simulations at 3 km resolution over June 22 to 10 July 2019 (a period that included 10 sea breeze occurrences), and use Pandora tropospheric NO 2 column, surface air quality monitoring, and vertical meteorological aircraft profiles for evaluation. The model generally reproduces observed spatiotemporal variability of air pollution during sea breezes well. Tropospheric columns of NO 2 predicted by the model and observed by the Pandora instrument show that sea breezes are associated with rapid increases and steep gradients in tropospheric NO 2 and confirm accumulation of local primary emissions. Spatial heterogeneity in tropospheric NO 2 is strongly governed by inland penetration lengths of the sea breeze front. Process diagnostics show that three sea-breeze days where O 3 observations recorded hourly concentrations >70 ppb have both efficient net chemical O 3 production in the boundary layer (>10 ppb/hr) and rapid O 3 convergence in the near-surface convergence zone (>20 ppb/hr). During sea breezes, interactions between photochemistry, the convergence zone inland penetration, and urban NO x titration effects, contribute to strong heterogeneity and high O 3 inland that is not captured by the current monitoring network. We discuss monitoring needs and model applications for the sea breeze scenarios, with broad implications for air quality monitoring in coastal urban environments. High resolution WRF-Chem modeling reproduces observed spatiotemporal variability of NO 2 and O 3 during sea breezes in the Greater Boston area Model results suggest high O 3 pollution and NO 2 column spatial variability associated with sea breezes is n

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Dominant immune cells in pregnancy and pregnancy complications: T helper cells (TH1/TH2, TH17/Treg cells), NK cells, MDSCs, and the immune checkpoints

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Cell Biology International 2022年第3期47卷

作者： Mojgan Esparvarinha Sahar Madadi Lida Aslanian-Kalkhoran Hamid Nickho Sanam Dolati Helen Pia Shahla Danaii Department of Immunology Faculty of Medicine Tabriz University of Medical Sciences Tabriz Iran Immunology Research Center Tabriz University of Medical Sciences Tabriz Iran Contribution: Formal analysis Funding acquisition Investigation Methodology Writing - original draft Writing - review & editing Women's Reproductive Health Research Center Tabriz University of Medical Sciences Tabriz Iran Contribution: Formal analysis Resources Contribution: Formal analysis Writing - original draft Writing - review & editing Department of Immunology School of Medicine Iran University of Medical Sciences Tehran Iran Immunology Research Center Institute of Immunology and Infectious Diseases Iran University of Medical Sciences Tehran Iran Contribution: Methodology Visualization Writing - original draft Writing - review & editing Physical Medicine and Rehabilitation Research Center Aging Research Institute Tabriz University of Medical Sciences Tabriz Iran Contribution: Investigation Validation Stem Cell Research Center Tabriz University of Medical Sciences Tabriz Iran Contribution: Funding acquisition Software Validation Gynecology Department Eastern Azerbaijan ACECR ART Centre Eastern Azerbaijan branch of ACECR Tabriz Iran Contribution: Data curation Methodology

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Upgrading Kolbe Electrolysis—Highly Efficient Production of Green Fuels and Solvents by Coupling Biosynthesis and Electrosynthesis

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Angewandte Chemie 2022年第50期134卷

作者： Niklas Teetz Prof. Dr. Dirk Holtmann Prof. Dr. Falk Harnisch Dr. Markus Stöckl Institute of Bioprocess Engineering and Pharmaceutical Technology University of Applied Sciences Mittelhessen Wiesenstrasse 14 35390 Giessen Germany Sustainable Electrochemistry Department of Chemical Technology DECHEMA Research Institute Theodor-Heuss-Allee 25 60486 Frankfurt am Main Germany Contribution: Data curation (equal) Investigation (lead) Writing - original draft (lead) Writing - review & editing (equal) Contribution: Conceptualization (equal) Funding acquisition (lead) Methodology (supporting) Project administration (lead) Supervision (supporting) Writing - review & editing (equal) Department of Environmental Microbiology UFZ – Helmholtz-Centre for Environmental Research GmbH Permoserstraße 15 04318 Leipzig Germany Contribution: Data curation (equal) Formal analysis (equal) Supervision (supporting) Validation (lead) Writing - review & editing (equal) Contribution: Conceptualization (equal) Funding acquisition (supporting) Methodology (lead) Project administration (supporting) Resources (lead) Supervision (lead) Visualization (lead) Writing - original draft (supporting) Writing - review & editing (equal)

The chemical industry is transitioning to more sustainable and biobased processes. One key element of this transition is coupling energy fluxes and feedstock utilization for optimizing processes, routes and efficiencies. Here, we show for the first time the coupling of the Kolbe electrolysis at the anode with a subsequent microbial conversion of the cathodically produced co-product hydrogen. Kolbe electrolysis of valeric acid yields the liquid drop-in fuel additive n -octane. Subsequently, the solvent isopropanol is produced by resting Cupriavidus necator cells using gaseous electrolysis products (esp. CO 2 and H 2 ). The resting microbial cells show carbon efficiencies of up to 41 % and Coulombic/Faradaic efficiencies of 60 % and 80 % for anodic and cathodic reactions, respectively. The implementation of a paired electrolyser resulted in superior process performances with overall efficiencies of up to 64.4 %.

关键词： Biosynthesis Cupriavidus necator Electrobiorefinery Kolbe Electrolysis Process Coupling

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Metformin use is associated with decreased asthma exacerbations in adolescents and young adults

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Pediatric Pulmonology 2023年第1期59卷

作者： Erhan Ararat MD Reid D. Landes PhD Erick Forno MD, MPH Emir Tas MD Tamara T. Perry MD Department of Biostatistics College of Medicine University of Arkansas for Medical Sciences Little Rock Arkansas USA Contribution: Methodology Software Formal analysis Writing - review & editing Writing - original draft Visualization Data curation Validation Supervision Division of Pediatric Pulmonary Allergy and Sleep Medicine Indiana University School of Medicine Indianapolis Indiana USA Contribution: Writing - review & editing Conceptualization Supervision Division of Pediatric Endocrinology UPMC Children's Hospital of Pittsburgh Pittsburgh Pennsylvania USA Contribution: Conceptualization Writing - review & editing Department of Pediatrics Allergy and Immunology University of Arkansas for Medical Sciences and Arkansas Children's Research Institute Little Rock Arkansas USA Contribution: Conceptualization Writing - review & editing Supervision

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