Tuning Internal Strain in Metal-Organic Frameworks via Vapor Phase Infiltration for CO2 Reduction.

A gas-phase approach to form Zn coordination sites on metal-organic frameworks (MOFs) by vapor-phase infiltration (VPI) was developed. Compared to Zn sites synthesized by the solution-phase method, VPI samples revealed approximately 2.8 % internal strain. Faradaic efficiency towards conversion of CO2 to CO was enhanced by up to a factor of four, and the initial potential was positively shifted by 200-300 mV. Using element-specific X-ray absorption spectroscopy, the local coordination environment of the Zn center was determined to have square-pyramidal geometry with four Zn-N bonds in the equatorial plane and one Zn-OH2 bond in the axial plane. The fine-tuned internal strain was further supported by monitoring changes in XRD and UV/Visible absorption spectra across a range of infiltration cycles. The ability to use internal strain to increase catalytic activity of MOFs suggests that applying this strategy will enhance intrinsic catalytic capabilities of a variety of porous materials.

Photo/Bio-Electrochemical Systems for Environmental Remediation and Energy Harvesting.

Water and energy systems are interdependent: water is utilized in each stage of energy production, and energy is required to extract, treat, and deliver water for many uses. However, energy and water systems are usually developed and managed independently. In the quest to develop environmentally friendly and energy-efficient solutions for water and energy issues, photoelectrochemical (PEC) energy conversion and microbial electrochemical (MEC) systems show profound potential for addressing environmental remediation problems and harvesting energy simultaneously. Herein, PEC, MEC, and their variant hybrid systems toward energy conversion and environmental remediation are summarized and discussed.

Cleaving DNA-model phosphodiester with Lewis acid-base catalytic sites in bifunctional Zr-MOFs.

Organophosphates exist in many biomolecules. The design of artificial nucleases for efficient P-O bond cleavage is essential for the fields of genetic engineering and molecular biology. Herein, metal-organic frameworks (MOFs) with cooperatively isolated multi-catalytic active sites were utilized as heterogeneous catalysts for the hydrolytic cleavage of bis(p-nitrophenyl) phosphate (BNPP).

The ALERT scale: an observational study of early prediction of adverse hospital outcome for medical patients.

OBJECTIVES: Some medical patients are at greater risk of adverse outcomes than others and may benefit from higher observation hospital units. We constructed and validated a model predicting adverse hospital outcome for patients. Study results may be used to admit patients into planned tiered care units. Adverse outcome comprised death or cardiac arrest during the first 30 days of hospitalisation, or transfer to intensive care within the first 48 h of admission. SETTING: The study took place at two tertiary teaching hospitals and two community hospitals in Winnipeg, Manitoba, Canada. PARTICIPANTS: We analysed data from 4883 consecutive admissions at a tertiary teaching hospital to construct the Early Prediction of Adverse Hospital Outcome for Medical Patients (ALERT) model using logistic regression. Robustness of the model was assessed through validation performed across four hospitals over two time periods, including 65,640 consecutive admissions. OUTCOME: Receiver-operating characteristic curves (ROC) and sensitivity and specificity analyses were used to assess the usefulness of the model. RESULTS: 9.3% of admitted patients experienced adverse outcomes. The final model included gender, age, Charlson Comorbidity Index, Activities of Daily Living Score, Glasgow Coma Score, systolic blood pressure, respiratory rate, heart rate and white cell count. The model was discriminative (ROC=0.83) in predicting adverse outcome. ALERT accurately predicted 75% of the adverse outcomes (sensitivity) and 75% of the non-adverse outcomes (specificity). Applying the same model to each validation hospital and time period produced similar accuracy and discrimination to that in the development hospital. CONCLUSIONS: Used during initial assessment of patients admitted to general medical wards, the ALERT scale may complement other assessment measures to better screen patients. Those considered as higher risk by the ALERT scale may then be provided more effective care from action such as planned tiered care units.