Compared with the traditional electrolysis of water to produce hydrogen, urea-assisted electrolysis of water to produce hydrogen has significant advantages and has received extensive attention from researchers. Unfortunately, urea oxidation reaction (UOR) involves a complex six-electron transfer process leading to high overpotential, which forces researchers to develop high-performance UOR catalysts to drive the development of urea-assisted water splitting. Based on the UOR mechanism and extensive literature research, this review summarizes the strategies for preparing highly efficient UOR catalysts. First, the UOR mechanism is introduced and the characteristics of excellent UOR catalysts are pointed out. Aiming at this, the following modulation strategies are proposed to improve the catalytic performance based on summarizing various literature: 1) Accelerating the active phase formation to reduce initial potential; 2) Creating double active sites to trigger a new UOR mechanism; 3) Accelerating urea adsorption and promoting C─N bond cleavage to ensure the effective conduct of UOR; 4) Promoting the desorption of CO2 to improve stability and prevent catalyst poisoning; 5) Promoting electron transfer to overcome the inherent slow dynamics of UOR; 6) Increasing active sites or active surface area. Then, the application of UOR in electrochemical devices is summarized. Finally, the current deficiencies and future directions are discussed.

Modulation Strategies for the Preparation of High-Performance Catalysts for Urea Oxidation Reaction and Their Applications.

Among various methods of developing hydrogen energy, electrocatalytic water splitting for hydrogen production is one of the approaches to achieve the goal of zero carbon emissions. It is of great significance to develop highly active and stable catalysts to improve the efficiency of hydrogen production. In recent years, the construction of nanoscale heterostructure electrocatalysts through interface engineering can not only overcome the shortcomings of single-component materials to effectively improve their electrocatalytic efficiency and stability but also adjust the intrinsic activity or design synergistic interfaces to improve catalytic performance. Among them, some researchers proposed to replace the slow oxygen evolution reaction at the anode with the oxidation reaction of renewable resources such as biomass to improve the catalytic efficiency of the overall water splitting. The existing reviews in the field of electrocatalysis mainly focus on the relationship between the interface structure, principle, and principle of catalytic reaction, and some articles summarize the performance and improvement schemes of transition metal electrocatalysts. Among them, few studies are focusing on Fe/Co/Ni-based heterogeneous compounds, and there are fewer summaries on the oxidation reactions of organic compounds at the anode. To this end, this paper comprehensively describes the interface design and synthesis, interface classification, and application in the field of electrocatalysis of Fe/Co/Ni-based electrocatalysts. Based on the development and application of current interface engineering strategies, the experimental results of biomass electrooxidation reaction (BEOR) replacing anode oxygen evolution reaction (OER) are discussed, and it is feasible to improve the overall electrocatalytic reaction efficiency by coupling with hydrogen evolution reaction (HER). In the end, the challenges and prospects for the application of Fe/Co/Ni-based heterogeneous compounds in water splitting are briefly discussed.

Recent advances in interface engineering of Fe/Co/Ni-based heterostructure electrocatalysts for water splitting.

CuS nanoparticles: An Efficient Electrocatalyst for Hydrogen Evolution Reaction in a wide pH range

Urea is a typical contaminant present in wastewater which may cause severe environmental problems. Electrochemical catalytic oxidation of urea has emerged as an efficient approach to solve this problem. Nevertheless, the current nickel-based catalysts (e.g., nickel hydroxide/sulfides) feature a high metal content. It not only lowers the utilization efficiency of nickel but also causes secondary pollution to the environment. Here, nickel-doped carbon dots (Ni-CDs) with an excellent and stable catalytic activity for the electrocatalytic urea oxidation reaction (UOR) are reported. Specifically, carbon dots (CDs) with abundant functional groups are synthesized by a one-pot hydrothermal method and then Ni-CDs with a very low metal content (1.1 at%) are prepared. The Ni2+ sites by coordination with carboxylic groups on the CDs provide excellent electrocatalytic activity and excellent durability for the UOR, as demonstrated by an anodic current density of 100 mA cm-2 at a potential of 1.38 V (vs RHE) and similar experimental results in practical application. To the best of knowledge, this is the first report of CDs-based materials applied for the UOR, which opens an important new area of applicability for CDs as well as broadens the scope of the materials for electrochemical catalysis of urea.

Nickel-Doped Carbon Dots as an Efficient and Stable Electrocatalyst for Urea Oxidation.

A 3-D porous structure of Ni-Fe-S nanosheets was created using a dynamic hydrogen bubble template (DHBT), which promotes active site exposure, on a nickel foam substrate as an efficient electrode...

Modulation of active surface sites on Ni-Fe-S by dynamic hydrogen bubble template method for energy-saving hydrogen production

Most plasmalemmal proteins are organized into clusters to modulate various cellular functions. However, the machineries that regulate protein clustering remain largely unclear. Here, with EGFR as an example, we directly and in detail visualized the entire process of EGFR from synthesis to secretion onto the plasma membrane (PM) using a high-speed, high-resolution spinning-disk confocal microscope. First, colocalization imaging revealed that EGFR secretory vesicles underwent transport from the ER to the Golgi to the PM, eventually forming different distribution forms on the apical and basal membranes; that is, most EGFR formed larger clusters on the apical membrane than the basal membrane. A dynamic tracking image and further siRNA interference experiment confirmed that fusion of secretory vesicles with the plasma membrane led to EGFR clusters, and we showed that EGFR PM clustering may be intimately related to EGFR signaling and cell proliferation. Finally, we found that the size and origin of the secretory vesicles themselves may determine the difference in the distribution patterns of EGFR on the PM. More importantly, we showed that actin influenced the EGFR distribution by controlling the fusion of secretory vesicles with the PM. Collectively, a comprehensive understanding of the EGFR secretion process helps us to unravel the EGFR clustering process and elucidate the key factors determining the differences in the spatial distribution of EGFR PM, highlighting the correlation between EGFR secretion and its PM distribution pattern.

https://downloads.spj.sciencemag.org/research/2022/9835035.pdf

Mechanistic Insights into Membrane Protein Clustering Revealed by Visualizing EGFR Secretion

Insulin receptor (INSR) is a key protein in the INSR signaling pathway and plays a critical role in biological processes, especially in the regulation of glucose homeostasis. Many metabolic diseases are often accompanied by abnormal INSR signaling. However, the specific effector mechanisms regulating insulin resistance and the distribution patterns of INSR during cell membrane activation remain unclear. Here, we investigated the changes in the distribution of INSR during activation using super-resolution imaging. By observing the connection between INSR activation and its distribution, we found that insulin resistance inhibits its receptor clustering. More importantly, we found that INSR has a highly co-localized relationship with the skeletal protein βII-spectrin. Specific knockout of βII-spectrin inhibited the interaction of INSR with GLUT4 and affected the normal metabolism of glucose. Our work elucidates the effects of insulin activation and insulin resistance on INSR distribution and reveals a potential relationship between INSR and cytoskeleton at the single molecule level, which promotes a deeper understanding of the roles associated with insulin signaling and insulin resistance.

Mechanism of INSR clustering with insulin activation and resistance revealed by super-resolution imaging.

Metal-based pH sensor has wide applications in industrial monitoring, soil environment, marine safety, and other fields. In this study, we proposed to renew the antimony-based sensor by physical polishing and electrochemical cathode reduction. Compared with before polishing, the pH response sensitivity after polishing increased from 0.034 V/pH to 0.042 V/pH, electrochemical cathode reduction renewed the pH response sensitivity improved from 0.018 V/pH to 0.032 V/pH (10 min) and 0.043 V/pH (30 min). The reasons for the deterioration of the pH response performance of the antimony-based sensor were analyzed by SEM, EDS, and XRD, and the renewable mechanisms of the sensor were proposed. The renewable effect of electrochemical cathode reduction on the degradation of sensor accuracy was evaluated for long-term monitoring. It is expected to realize remote online renewal of sensors under on-site unattended conditions, to reduce operation and maintenance costs of the sensor. These results provide solutions for the repeated regeneration of metal-based pH sensors which were degraded in performance and have significance for promoting the development and wide applications of renewable pH sensors. 

Renewable antimony-based pH sensor

Potato is an important food crop that occupies lesser area but has greater production than rice and wheat. However, potato production is affected by numerous biotic and abiotic stresses, among which Fusarium dry rot is a disease that has significant effect on potato production, storage, and processing. However, the role of DNA methylation in regulating potato response to Fusarium toxin deoxynivalenol (DON) stress is still not fully understood. In this study, we performed DNA methylome and transcriptome analyses of potato tubers treated with five concentrations of DON. The global DNA methylation levels in potato tubers treated with different concentrations of DON showed significant changes relative to those in the control. In particular, the 20 ng/ml treatment showed the largest decrease in all three contexts of methylation levels, especially CHH contexts in transposon regions. The differentially methylated region (DMR)-associated differentially expressed genes (DEGs) were significantly enriched in resistance-related metabolic pathways, indicating that DNA methylation plays an essential role in potato response to DON stress. Furthermore, we examined lesions on potato tubers infested with Fusarium after treatment. Furthermore, the potato tubers treated with 5 and 35 ng/ml DON had lesions of significantly smaller diameters than those of the control, indicating that DON stress may induce resistance. We speculate that this may be related to epigenetic memory created after DNA methylation changes. The detailed DNA methylome and transcriptome profiles suggest that DNA methylation plays a vital role in potato disease resistance and has great potential for enhancing potato dry rot resistance.

/pdf/genome-wide-profiling-of-dna-methylome-and-transcriptome-1ir21uh9.pdf

Genome-Wide Profiling of DNA Methylome and Transcriptome Reveals Epigenetic Regulation of Potato Response to DON Stress

Impaired insulin release is the key feature of type 2 diabetes. Insulin secretion, mainly mediated by SNARE proteins, is closely related to the blood glucose level. However, the mechanism underlying how glucose controls SNARE proteins to regulate insulin release is largely unexplained. Herein, we investigated the effects of glucose on the subcellular localization and spatial distribution on the plasma membrane (PM) of t-SNAREs (SNAP-25 and STX-1A) using a live-cell confocal microscope and the single-molecule localization imaging technique. Live-cell confocal and dSTORM imaging first revealed that SNAP-25 was mostly localized to the PM as clusters under the basal glucose concentration condition and demonstrated significant colocalization with STX-1A clusters. Furthermore, our data showed that the elevated glucose concentration increased the expression of SNAP-25 and induced more and larger SNAP-25 clusters on the PM, whereas glucotoxicity severely inhibited SNAP-25 transport to the PM and caused fewer and smaller SNAP-25 clusters on the PM. Additionally, we found that glucotoxicity also had an inhibitory effect on the colocalization between SNAP-25 and STX-1A, indicating a decrease of their interactions. Our study sheds light on the regulatory effects of glucose on the functional organization of t-SNAREs at a subcellular and molecular level, thus providing new insights into the mechanisms by which SNAREs regulate insulin release.

Regulatory Mechanisms of SNAP-25-Associated Insulin Release Revealed by Live-Cell Confocal and Single-Molecule Localization Imaging.

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