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Nature Materials Jul 2024The voltage penalty driving water dissociation (WD) at high current density is a major obstacle in the commercialization of bipolar membrane (BPM) technology for energy...
The voltage penalty driving water dissociation (WD) at high current density is a major obstacle in the commercialization of bipolar membrane (BPM) technology for energy devices. Here we show that three materials descriptors, that is, electrical conductivity, microscopic surface area and (nominal) surface-hydroxyl coverage, effectively control the kinetics of WD in BPMs. Using these descriptors and optimizing mass loading, we design new earth-abundant WD catalysts based on nanoparticle SnO synthesized at low temperature with high conductivity and hydroxyl coverage. These catalysts exhibit exceptional performance in a BPM electrolyser with low WD overvoltage (η) of 100 ± 20 mV at 1.0 A cm. The new catalyst works equivalently well with hydrocarbon proton-exchange layers as it does with fluorocarbon-based Nafion, thus providing pathways to commercializing advanced BPMs for a broad array of electrolysis, fuel-cell and electrodialysis applications.
PubMed: 38951650
DOI: 10.1038/s41563-024-01943-8 -
Communications Biology Jun 2024Light is a significant factor for living organisms with photosystems, like microbial rhodopsin-a retinal protein that functions as an ion pump, channel, and sensory...
Light is a significant factor for living organisms with photosystems, like microbial rhodopsin-a retinal protein that functions as an ion pump, channel, and sensory transduction. Gloeobacter violaceus PCC7421, has a proton-pumping rhodopsin gene, the Gloeobacter rhodopsin (GR). The helix-turn-helix family of transcriptional regulators has various motifs, and they regulate gene expression in the presence of various metal ions. Here, we report that active proton outward pumping rhodopsin interacted with the helix-turn-helix transcription regulator and regulated gene expression. This interaction is confirmed using ITC analysis (K of 8 μM) and determined the charged residues required. During in vitro experiments using fluorescent and luciferase reporter systems, ATP-binding cassette (ABC) transporters and the self-regulation of G. violaceus transcriptional regulator (GvTcR) are regulated by light, and gene regulation is observed in G. violaceus using the real-time polymerase chain reaction. These results expand our understanding of the natural potential and limitations of microbial rhodopsin function.
Topics: ATP-Binding Cassette Transporters; Light; Gene Expression Regulation, Bacterial; Transcription Factors; Cyanobacteria; Proton Pumps; Bacterial Proteins; Rhodopsins, Microbial; Rhodopsin
PubMed: 38951607
DOI: 10.1038/s42003-024-06471-4 -
Nature Nanotechnology Jul 2024
PubMed: 38951596
DOI: 10.1038/s41565-024-01699-x -
The Journal of Physical Chemistry. A Jul 2024We provide an approach to sample rare events during classical ab initio molecular dynamics and quantum wavepacket dynamics. For classical AIMD, a set of fictitious...
We provide an approach to sample rare events during classical ab initio molecular dynamics and quantum wavepacket dynamics. For classical AIMD, a set of fictitious degrees of freedom are introduced that may harmonically interact with the electronic and nuclear degrees of freedom to steer the dynamics in a conservative fashion toward energetically forbidden regions. A similar approach when introduced for quantum wavepacket dynamics has the effect of biasing the trajectory of the wavepacket centroid toward the regions of the potential surface that are difficult to sample. The approach is demonstrated for a phenol-amine system, which is a prototypical problem for condensed phase-proton transfer, and for model potentials undergoing wavepacket dynamics. In all cases, the approach yields trajectories that conserve energy while sampling rare events.
PubMed: 38951489
DOI: 10.1021/acs.jpca.3c07385 -
Biomolecular NMR Assignments Jun 2024The α-synuclein (α-syn) amyloid fibrils are involved in various neurogenerative diseases. Solid-state NMR (ssNMR) has been showed as a powerful tool to study α-syn...
The α-synuclein (α-syn) amyloid fibrils are involved in various neurogenerative diseases. Solid-state NMR (ssNMR) has been showed as a powerful tool to study α-syn aggregates. Here, we report the H, C and N back-bone chemical shifts of a new α-syn polymorph obtained using proton-detected ssNMR spectroscopy under fast (95 kHz) magic-angle spinning conditions. The manual chemical shift assignments were cross-validated using FLYA algorithm. The secondary structural elements of α-syn fibrils were calculated using C chemical shift differences and TALOS software.
PubMed: 38951472
DOI: 10.1007/s12104-024-10186-2 -
Journal of Fluorescence Jul 2024Designed and synthesized linear pyrazine-based D-π-A-π-A probe is investigated to study the colorimetric and emission properties with different polarity index...
Designed and synthesized linear pyrazine-based D-π-A-π-A probe is investigated to study the colorimetric and emission properties with different polarity index solvents. Their molar extinction coefficients were estimated for each solvent. This TLP probe was investigated in THF/water binary solution aggregates, and a redshifted AIE was observed reaching a water fraction of 70%. Also, this TLP probe was applied to the multifunctional, rapid, sensitive and selective detection of acid-base (TFA/TEA) and hydrazine (NH) in colorimetric and fluorimetric sensors. The pyrazine unit probe demonstrated an acidochromic effect and explored the acid-sensing behavior. The TLP probe containing malononitrile functional groups has extensively detected hazardous hydrazine species due to nucleophilic attack of hydrazine at the α-position of dicyano. This TLP probe allowed the quick and fast-sensitive detection of hydrazine hydride with a low detection limit of 1.08 nM. According to the results, the mechanism was confirmed by UV-Vis, PL, NMR and MS spectra for the detection of hydrazine, and further evidence of the protonation-deprotonation process in added TFA/TEA was made by titration studies by H NMR. Therefore, this work can be used for test strip kits for multifunction applications.
PubMed: 38951307
DOI: 10.1007/s10895-024-03825-3 -
Supportive Care in Cancer : Official... Jun 2024This study aimed to compare the effects of a mobile health intervention based on social cognitive theory with standard care on maximal mouth opening, exercise... (Randomized Controlled Trial)
Randomized Controlled Trial
PURPOSE
This study aimed to compare the effects of a mobile health intervention based on social cognitive theory with standard care on maximal mouth opening, exercise compliance, and self-efficacy in patients receiving proton and heavy ion therapy for head and neck cancer.
METHODS
This open-label, parallel-group, randomized, superiority trial involved a self-developed "Health Enjoy System" intervention. We assessed maximal mouth opening, exercise compliance, and self-efficacy at baseline (T), post-treatment (T), and at 1 month (T) and 3 months (T) after radiotherapy. Generalized estimating equations were used to analyze differences between the groups over time, with results reported as P values and 95% confidence intervals (CIs).
RESULTS
The study included 44 participants. At T, the intervention group showed a 6 mm greater increase in maximal interincisal opening than the control group (mean difference = 6.0, 95% CI = 2.4 to 9.5, P = 0.001). There was also a significant difference in exercise compliance between the groups (mean difference = 31.7, 95% CI = 4.6 to 58.8, P = 0.022). However, no significant difference in self-efficacy was found between the groups.
CONCLUSION
This study demonstrated that an mHealth intervention incorporating behavior change theory could effectively enhance or maintain maximal mouth opening in patients undergoing proton and heavy ion therapy for head and neck cancer in China. This approach provides valuable support during and after treatment.
TRIAL REGISTRATION
ChiCTR: ChiCTR2300067550. Registered 11 Jan 2023.
Topics: Humans; Head and Neck Neoplasms; Male; Middle Aged; Female; Proton Therapy; Self Efficacy; Telemedicine; Trismus; Heavy Ion Radiotherapy; Exercise Therapy; Aged; Patient Compliance; Adult
PubMed: 38951291
DOI: 10.1007/s00520-024-08679-w -
Cellular Signalling Jun 2024Diabetes-associated periodontitis (DP) presents severe inflammation and resistance to periodontal conventional treatment, presenting a significant challenge in clinical...
Diabetes-associated periodontitis (DP) presents severe inflammation and resistance to periodontal conventional treatment, presenting a significant challenge in clinical management. In this study, we investigated the underlying mechanism driving the hyperinflammatory response in gingival epithelial cells (GECs) of DP patients. Our findings indicate that lysosomal dysfunction under high glucose conditions leads to the blockage of autophagy flux, exacerbating inflammatory response in GECs. Single-cell RNA sequencing and immunohistochemistry analyses of clinical gingival epithelia revealed dysregulation in the lysosome pathway characterized by reduced levels of lysosome-associated membrane glycoprotein 2 (LAMP2) and V-type proton ATPase 16 kDa proteolipid subunit c (ATP6V0C) in subjects with DP. In vitro stimulation of human gingival epithelial cells (HGECs) with a hyperglycemic microenvironment showed elevated release of proinflammatory cytokines, compromised lysosomal acidity and blocked autophagy. Moreover, HGECs with deficiency in ATP6V0C demonstrated impaired autophagy and heightened inflammatory response, mirroring the effects of high glucose stimulation. Proteomic analysis of acetylation modifications identified altered acetylation levels in 28 autophagy-lysosome pathway-related proteins and 37 sites in HGECs subjected to high glucose stimulation or siATP6V0C. Overall, our finding highlights the pivotal role of lysosome impairment in autophagy obstruction in DP and suggests a potential impact of altered acetylation of relevant proteins on the interplay between lysosome dysfunction and autophagy blockage. These insights may pave the way for the development of effective therapeutic strategies against DP.
PubMed: 38950874
DOI: 10.1016/j.cellsig.2024.111273 -
Environmental Research Jun 2024Proteorhodopsins have been suggested as an important strategy among phototrophs to capture solar energy in marine environments. The goals of this study was to...
Proteorhodopsins have been suggested as an important strategy among phototrophs to capture solar energy in marine environments. The goals of this study was to investigate the diversity of proteorhodopsin genes and to explore their abundance, distribution, and expression in the coastal surface waters of the northern South China Sea, one of the largest marginal seas of the western North Pacific Ocean. Using 21 metagenomes, we recovered proteorhodopsin genes from a wide range of prokaryotic taxa, and chlorophyll a contributed significantly to the community composition of proteorhodopsin-containing microbes. Most proteorhodopsin sequences were predicted to encode green light-absorbing proton pumps and green light-absorbing proteorhodopsin genes were more abundant than blue-absorbing ones. The variations in the conserved residues involved in ion pumping and several uncharacterized proteorhodopsins were observed. The gene abundance pattern of proteorhodopsin types were significantly influenced by the levels of total organic carbon and soluble reactive phosphorus. Gene expression analysis confirmed the importance of proteorhodopsin-based phototrophy and revealed different expressional patterns among major phyla. In tandem, we screened 2,295 metagenome-assembled genomes to describe the taxonomic distribution of proteorhodopsins. Bacteroidota are the key lineages encoding proteorhodopsins, but proteorhodopsins were predicated from members of Proteobacteria, Marinisomatota, Myxococcota, Verrucomicrobiota and Thermoplasmatota. Our study expanded the diversity of proteorhodopsins and improve our understanding on the significance of proteorhodopsin-mediated phototrophy in the marine ecosystem.
PubMed: 38950812
DOI: 10.1016/j.envres.2024.119514 -
Journal of Colloid and Interface Science Jun 2024Amino acids are among the most commercially promising additive solutions for achieving stable zinc anodes. However, greater attention should be given to the limitation...
Overcoming challenges of protonation effects induced by high isoelectric point amino acids through a synergistic strategy towards highly stable and reversible zinc electrode-electrolyte interface.
Amino acids are among the most commercially promising additive solutions for achieving stable zinc anodes. However, greater attention should be given to the limitation arising from the protonation effects induced by high isoelectric point amino acids in the weakly acidic electrolytes of aqueous zinc-ion batteries (AZIBs). In this study, we introduce histidine (HIS) and ethylenediaminetetraacetic acid (EDTA) as hybrid additives into the aqueous electrolyte. Protonated HIS is adsorbed onto the anode interface, inducing uniform deposition and excluding HO from the inner Helmholtz plane (IHP). Furthermore, the addition of EDTA compensates for the limitation of protonated HIS in excluding solvated HO. EDTA reconstructs the solvation structure of Zn, resulting in a denser zinc deposition morphology. The results demonstrate that the Zn||Zn battery achieved a cycling lifespan exceeding 1480 h at 5 mA cm and 5 mAh cm. It also reached over 900 h of cycling at a zinc utilization rate of 70 %. This study provides an innovative perspective for advancing the further development of AZIBs.
PubMed: 38950470
DOI: 10.1016/j.jcis.2024.06.166