Indirect H2O2 synthesis without H2 Fink, Arthur G; Delima, Roxanna S; Rousseau, Alexandra R ...
Nature communications,
01/2024, Letnik:
15, Številka:
1
Journal Article
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Abstract
Industrial hydrogen peroxide (H
2
O
2
) is synthesized using carbon-intensive H
2
gas production and purification, anthraquinone hydrogenation, and anthrahydroquinone oxidation. ...Electrochemical hydrogenation (ECH) of anthraquinones offers a carbon-neutral alternative for generating H
2
O
2
using renewable electricity and water instead of H
2
gas. However, the H
2
O
2
formation rates associated with ECH are too low for commercialization. We report here that a membrane reactor enabled us to electrochemically hydrogenate anthraquinone (0.25 molar) with a current efficiency of 70% at current densities of 100 milliamperes per square centimeter. We also demonstrate continuous H
2
O
2
synthesis from the hydrogenated anthraquinones over the course of 48 h. This study presents a fast rate of electrochemically-driven anthraquinone hydrogenation (1.32 ± 0.14 millimoles per hour normalized per centimeter squared of geometric surface of electrode), and provides a pathway toward carbon-neutral H
2
O
2
synthesis.
Different rituximab protocols are used to treat membranous nephropathy. We compared two rituximab protocols in patients with membranous nephropathy.
Twenty-eight participants from the NICE cohort ...received two infusions of 1-g rituximab at 2-week intervals, whereas 27 participants from the Prospective Randomized Multicentric Open Label Study to Evaluate Rituximab Treatment for Membranous Nephropathy (GEMRITUX) cohort received two infusions of 375 mg/m
at 1-week interval. We measured serum rituximab levels and compared remission at month 6 and before any treatment modification and analyzed factors associated with remission and relapses.
Remissions occurred in 18 (64%) versus eight (30%) from the NICE and GEMRITUX cohort (
=0.02) at month 6, respectively, and in 24 (86%) versus 18 (67%) participants (
=0.12) before treatment modification, respectively. Median time to remission was 3 interquartile range (IQR), 3-9 and 9 IQR, 6-12 months for NICE and GEMRITUX cohorts respectively (
=0.01). Participants from the NICE cohort had higher circulating level of rituximab and lower CD19 counts (3.3 µg/L IQR, 0.0-10.8 versus 0.0 IQR, 0.0-0.0
<0.001 and 0.0 IQR, 0.0-2.0 versus 16.5 IQR, 2.5-31.0
<0.001) at month 3, lower level of anti-PLA2R1 antibodies at month 6 (0.0 IQR, 0.0-8.0 versus 8.3 IQR, 0.0-73.5
=0.03). In the combined study population, lower epitope spreading at diagnosis and higher rituximab levels at month 3 were associated with remissions at month 6 (13/26 (50%) versus 22/29 (76%)
=0.05 and 2.2 µg/ml IQR, 0.0-10.9 versus 0.0 µg/ml IQR, 0.0-0.0
<0.001 respectively). All non-spreaders entered into remission whatever the protocol. Eight of the 41 participants who reached remission had relapses. Epitope spreading at diagnosis (8/8 (100%) versus 16/33 (48%)
=0.01) and incomplete depletion of anti-PLA2R1 antibodies at month 6 (4/8 (50%) versus 5/33 (9%)
=0.05) were associated with relapses.
Our work suggests that higher dose rituximab protocol is more effective on depletion of B-cells and lack of epitope spreading is associated with remission of membranous nephropathy.
The role of the gut microbiota in Crohn's disease (CD) is established and fecal microbiota transplantation (FMT) is an attractive therapeutic strategy. No randomized controlled clinical trial results ...are available. We performed a randomized, single-blind, sham-controlled pilot trial of FMT in adults with colonic or ileo-colonic CD.
Patients enrolled while in flare received oral corticosteroid. Once in clinical remission, patients were randomized to receive either FMT or sham transplantation during a colonoscopy. Corticosteroids were tapered and a second colonoscopy was performed at week 6. The primary endpoint was the implantation of the donor microbiota at week 6 (Sorensen index > 0.6).
Eight patients received FMT and nine sham transplantation. None of the patients reached the primary endpoint. The steroid-free clinical remission rate at 10 and 24 weeks was 44.4% (4/9) and 33.3% (3/9) in the sham transplantation group and 87.5% (7/8) and 50.0% (4/8; one patient loss of follow-up while in remission at week 12 and considered in flare at week 24) in the FMT group. Crohn's Disease Endoscopic Index of Severity decreased 6 weeks after FMT (p = 0.03) but not after sham transplantation (p = 0.8). Conversely, the CRP level increased 6 weeks after sham transplantation (p = 0.008) but not after FMT (p = 0.5). Absence of donor microbiota engraftment was associated with flare. No safety signal was identified.
The primary endpoint was not reached for any patient. In this pilot study, higher colonization by donor microbiota was associated with maintenance of remission. These results must be confirmed in larger studies (NCT02097797). Video abstract.
Industrial hydrogenation consumes ~11 Mt of fossil-derived H2 gas yearly. Our group invented a membrane reactor to bypass the need to use H2 gas for hydrogenation chemistry. The membrane reactor ...sources hydrogen from water and drives reactions using renewable electricity. In this reactor, a thin piece of Pd separates an electrochemical hydrogen production compartment from a chemical hydrogenation compartment. The Pd in the membrane reactor acts as (i) a hydrogen-selective membrane, (ii) a cathode, and (iii) a catalyst for hydrogenation. Herein, we report the use of atmospheric mass spectrometry (atm-MS) and gas chromatography mass spectrometry (GC-MS) to demonstrate that an applied electrochemical bias across a Pd membrane enables efficient hydrogenation without direct H2 input in a membrane reactor. With atm-MS, we measured a hydrogen permeation of 73%, which enabled the hydrogenation of propiophenone to propylbenzene with 100% selectivity, as measured by GC-MS. In contrast to conventional electrochemical hydrogenation, which is limited to low concentrations of starting material dissolved in a protic electrolyte, the physical separation of hydrogen production from utilization in the membrane reactor enables hydrogenation in any solvent or at any concentration. The use of high concentrations and a wide range of solvents is particularly important for reactor scalability and future commercialization.
Abstract
Background
To compare the rate of postpartum depression (PPD) during the first COVID-19 lockdown with the rate observed prior to the pandemic, and to examine factors associated with PPD.
...Methods
This was a prospective study. Women who gave birth during the first COVID-19 lockdown (spring 2020) were offered call-interviews at 10 days and 6–8 weeks postpartum to assess PPD using the Edinburgh Postnatal Depression Scale (EPDS). Post-traumatic symptoms (Perinatal Post-traumatic Stress Disorder Questionnaire, PPQ), couple adjustment, and interaction and mother-to-infant bonding were also evaluated. The observed PPD rate was compared to the one reported before the pandemic. Factors associated with an increased risk of PPD were studied. The main outcome measures were comparison of the observed PPD rate (EPDS score > 12) to pre-pandemic rate.
Results
Of the 164 women included, 27 (16.5% 95%CI: 11.14–23.04) presented an EPDS score > 12 either at 10 days or 6–8 weeks postpartum. This rate was similar to the one of 15% reported prior to the pandemic (
p
= 0.6). Combined EPDS> 12 or PPQ > 6 scores were observed in 20.7% of the mothers 95%CI: 14.8–0.28. Maternal hypertension/preeclampsia (
p
= 0.007), emergency cesarean section (
p
= 0.03), and neonatal complications (
p
= 0.008) were significantly associated with an EPDS> 12 both in univariate and multivariate analysis (OR = 10 95%CI: 1.5–68.7, OR = 4.0995%CI: 1.2–14, OR = 4.0295%CI: 1.4–11.6, respectively).
Conclusions
The rate of major PPD in our population did not increase during the first lockdown period. However, 20.7% of the women presented with post-traumatic/depressive symptoms.
Trial registration
NCT04366817.
...the interface may have selected family members who were digitally educated. ...the CCOFS developed for the present study was not validated prior to the study. ...before–after studies are ...associated with major biases stemming from regression to the mean and the Hawthorne effect.
In a large retrospective study, we assessed the putative use of circulating microvesicles (MVs), as innovative biomarkers of radiation toxicity in a cohort of 208 patients with prostate ...adenocarcinoma overexposed to radiation. The level of platelet (P)-, monocyte (M)- and endothelial (E)-derived MVs were assessed by flow cytometry. Rectal bleeding toxicity scores were collected at the time of blood sampling and during the routine follow-up and were tested for association with MVs using a multivariate logistic regression. MVs dosimetric correlation was investigated using dose volume histograms information available for a subset of 36 patients. The number of PMVs was significantly increased in patients with highest toxicity grades compared to lower grades. Risk prediction analysis revealed that increased numbers of PMVs, and an increased amount of MMVs relative to EMVs, were associated with worst rectal bleeding grade compared to the time of blood sampling. Moreover, a significant correlation was found between PMV and MMV numbers, with the range of doses up to the median exposure (40 Gy) of bladder/rectum and anterior rectal wall, respectively. MVs could be considered as new biomarkers to improve the identification of patients with high toxicity grade and may be instrumental for the prognosis of radiation therapy complications.
The optimal treatment duration and the nature of regimen of antibiotics (monotherapy or combination therapy) for Pseudomonas aeruginosa ventilator‑associated pneumonia (PA-VAP) remain debated. The ...aim of this study was to evaluate whether a combination antibiotic therapy is superior to a monotherapy in patients with PA-VAP in terms of reduction in recurrence and death, based on the 186 patients included in the iDIAPASON trial, a multicenter, randomized controlled trial comparing 8 versus 15 days of antibiotic therapy for PA-VAP.
Patients with PA-VAP randomized in the iDIAPASON trial (short-duration-8 days vs. long-duration-15 days) and who received appropriate antibiotic therapy were eligible in the present study. The main objective is to compare mortality at day 90 according to the antibiotic therapy received by the patient: monotherapy versus combination therapy. The primary outcome was the mortality rate at day 90. The primary outcome was compared between groups using a Chi-square test. Time from appropriate antibiotic therapy to death in ICU or to censure at day 90 was represented using Kaplan-Meier survival curves and compared between groups using a Log-rank test.
A total of 169 patients were included in the analysis. The median duration of appropriate antibiotic therapy was 14 days. At day 90, among 37 patients (21.9%) who died, 17 received monotherapy and 20 received a combination therapy (P = 0.180). Monotherapy and combination antibiotic therapy were similar for the recurrence rate of VAP, the number of extra pulmonary infections, or the acquisition of multidrug-resistant (MDR) bacteria during the ICU stay. Patients in combination therapy were exposed to mechanical ventilation for 28 ± 12 days, as compared with 23 ± 11 days for those receiving monotherapy (P = 0.0243). Results remain similar after adjustment for randomization arm of iDIAPASON trial and SOFA score at ICU admission.
Except longer durations of antibiotic therapy and mechanical ventilation, potentially related to increased difficulty in achieving clinical cure, the patients in the combination therapy group had similar outcomes to those in the monotherapy group.
NCT02634411 , Registered 15 December 2015.
The objective of the work was to develop and validate methods for the total Hg and methylmercury (MeHg) in breast milk that could be further used to obtain first data on chemical contamination of ...French breast milk. For total Hg determination, the potential of two techniques, namely Advanced Mercury Analyzer (AMA) and ICP MS, was compared. For MeHg determination, ICP MS detection associated to a quantification by isotopic dilution was used and the potential of a preliminary separation by gas or liquid chromatography was evaluated and discussed. The optimization studies have shown that AMA for total Hg determination and HPLC – ID – ICP MS, after a preconcentration step by freeze-drying, for MeHg quantification were the most relevant methods to use for epidemiologic studies. The figures of merit for both methods were evaluated by means of accuracy profiles in terms of limits of quantification (1.82 and 1.35µg Hg/kg dry weight, corresponding to 0.22 and 0.16µg Hg/kg wet basis for total Hg and MeHg, respectively), repeatability (2–11% and 3–8% for total Hg and MeHg respectively), intermediate precision reproducibility (4–12% and 4–8% for total Hg and MeHg respectively) and trueness bias (−0.1–9% and −4–0% for total Hg and MeHg respectively). The methods were then applied to 180 breast milk samples. Total Hg concentrations ranged from <LD to 16.9µg Hg/kg wet basis (<LD to 142µg Hg/kg dry weight) and the MeHg contents from <LD to 0.43µg Hg/kg wet basis (<LD to 3.67µg Hg/kg dry weight).
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•Ability of AMA and HPLC – ID – ICP MS to perform Hg ang MeHg determination respectively was demonstrated.•Both methods were successfully applied to analyze 180 samples of breast milk.•MeHg was accounting for around 8 -36% of the total mercury.
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