Latest ArticlesCO2 electrolysis into formate is a promising technology with the potential to simultaneously alleviate energy shortages and global warming. However, the limited stability of the catalysts during long-term electrolysis hinders their widespread implementation. Herein, we show that a core-shell bimetallic BiAg catalyst with a multifaceted Janus structure at its core can achieve a stability of up to 300 h with a formate faradaic efficiency (FEformate) over 90% at −0.75 V vs. RHE (reversible hydrogen electrode) in an H-type cell. Our investigations reveal the important role of the Janus structure on the transfer of electrons, favoring their delocalization across the catalyst and enhancing their mobility. We propose that the compressive strain inclined to grain boundaries within this structure would lower the energy barrier for electrons transfer and promotes the cooperation between Ag and Bi. Indeed, Ag initiates the activation of CO2 through a series of cascade reactions and is subsequently hydrogenated on Bi. Additionally, our study suggests that Ag plays a crucial role in stabilizing the catalyst structure after long-term electrolysis. This work highlights a new strategy for tandem CO2 electrolysis, providing novel insights for the design of formate formation catalysts.
RNA modifications play vital regulatory roles in biological systems. Dysregulated RNA modifications themselves or their regulators are associated with various diseases, including cancers and immune related diseases. However, to the best of our knowledge, RNA modifications in peripheral white blood cells (immune cells) have not been systematically investigated before. Here we utilized hydrophilic interaction liquid chromatography-tandem mass spectrometry (HILIC-MS/MS) for the quantification of 19 chemical modifications in total RNA and 17 chemical modifications in small RNA in peripheral white blood cells from breast cancer patients and healthy controls. We found out 13 RNA modifications were up-regulated in total RNA samples of breast cancer patients. For small RNA samples, only N6-methyladenosine (m6A) was down-regulated in breast cancer patients (P < 0.0001). Receiver operating characteristic (ROC) curves analysis showed that N4-acetylcytidine (ac4C) in total RNA had an area under curve (AUC) value of 0.833, and m6A in small RNA had an AUC value of 0.994. Our results further illustrated that RNA modifications may play vital roles in immune cell biology of breast cancer, and may act as novel biomarkers for the diagnosis of breast cancer.
Colon-targeted oral drug delivery systems are one of the most promising therapeutic strategies for alleviating and curing inflammatory bowel disease (IBD), but they still face challenges in successfully passing through the harsh gastrointestinal environment and intestinal mucus barrier. To overcome the gastrointestinal barriers for oral drug delivery mentioned above, a "spore-like" oral nanodrug delivery platform (Cur/COS/SC NPs) has been developed. Firstly, chitooligosaccharides (COS) are encapsulated on the surface of Curcumin nanoparticles (Cur NPs) to form carrier-free nanoparticles (Cur/COS NPs). Subsequently, inspired by the natural high resistance of spore coat (SC), SC is chosen as the "protective umbrella" to encapsulate Cur/COS NPs for precision targeted therapy of IBD. After oral administration, SC can effectively protect NPs through the rugged gastrointestinal environment and exhibit excellent intestinal mucus penetration characteristics. Moreover, the negatively-charged Cur/COS/SC NPs specifically target positively-charged inflamed colon via electrostatic interactions. It is demonstrated that Cur/COS/SC NPs can promote the expression of tight junction proteins, inhibit aberrant activation of the Toll-like receptor 4/myeloid differentiation primary response gene 88/nuclear factor-κB (TLR4/MyD88/NF-κB) signaling pathway, and downregulate the levels of pro-inflammatory factors, exhibiting excellent anti-inflammatory effects. Notably, it is found that Cur/COS/SC NPs can significantly increase the richness and diversity of gut microbiota, and restore the homeostasis of gut microbiota by inhibiting pathogenic bacteria and promoting probiotics. Hence, Cur/COS/SC NPs provide a safe, efficient, and feasible new strategy for IBD treatment.
Aqueous zinc-based energy storage devices (ZESDs) have garnered considerable interest because of their high specific capacity, abundant zinc reserves, excellent safety, and environmental friendliness. In recent years, various types of boron, nitrogen co-doped carbon (BNC) materials have been developed to improve electrochemical performance of ZESDs. To promote the advancement of these technologies, we herein give a comprehensive review of the progress in BNC materials for ZESDs. The different synthetic methods employed in the preparation of BNC materials, including direct carbonization, template method, chemical vapor deposition, hydrothermal method, etc., are summarized. These methods play a vital role in tailoring the structure, composition, and properties of BNC materials to optimize their performance in energy storage applications. Furthermore, some key achievements of BNC materials in zinc-air batteries and zinc-ion hybrid supercapacitors are elaborated. Lastly, future challenges and development directions of BNC materials in ZESDs are prospected. This comprehensive review could serve as a valuable resource in the energy storage field, providing insights into the potential of BNC materials in zinc-based energy storage technologies.
The synergistic effect of Se with Fe can enhance the catalytic activities of the system for oxidation reactions. Based on this principle, a series of Se/Fe materials have been invented to develop the heterogeneous catalysts with industrial application potential. However, the present methods suffer from the tedious procedures, the high reaction temperature, and the low synthetic efficiency. In this paper, we report the synthesis of Se/Fe materials just by precipitating Fe(NO3)3 with the in situ prepared aqueous NaSe/NaSeO3 under mild conditions. The concise method may resolve the issues hindering the large-scale applications of Se/Fe materials.
In order to protect the environment and economize energy, a nitrogen-fixing photocatalyst, VMCeact, is investigated in this work. This catalyst is prepared from a natural mineral, vermiculite, and modified by Ce-based metal-organic framework, Ce-UiO-66. Vermiculite was treated with formic acid; thus, Ce-UiO-66 particles grew in-situ on vermiculite; then, Ce-UiO-66 particles were activated by ultraviolet irradiation. The vermiculite absorbed visible light with a narrow band gap, and transferred photogenerated electrons to the active sites on Ce-UiO-66. Moreover, the lamella structure of vermiculite protected Ce-UiO-66 during photocatalytic process. Therefore, with only 45.92 wt% of Ce-UiO-66, the nitrogen fixation performance of VMCeact was 2.29 times that of pure activated Ce-UiO-66 particles under 455 nm light irradiation (apparent quantum efficiency of 4.49%), and retained at least 96.05% performance after 7 × 24 h of photocatalytic reaction. This cost-reduced, efficient and stable photocatalyst has the opportunity to facilitate environmentally friendly ammonia production.
Although lots of efforts have been devoted on new less hygroscopic dopants to address problems in hole transport materials (HTM), the long-time post-oxidation and the volatilization of 4-tert-butylpyridine (tBP) are still issues. A new doping mechanism for spiro-OMeTAD by disulfiram (TETD) is revealed in this work. Owing to its disulfide bond, TETD can be activated easily to produce reactive sulfur for the rapid oxidation of spiro-OMeTAD in the absence of oxygen with formation of [spiro-OMeTAD•]+[SC(S)N(C2H5)2]-. Thus, in this situation, the Li+ ion has the opportunity to coordinate tBP and fix each other in HTM film. DFT calculations suggest that the resulting favorable energy (with a ΔE of −1.29 eV) must come from the mutual interactions among Li+, TFSI−, and tBP, which is different from the well-known doping process that tBP would not participate in the doping reaction. As a result, the introduction of a new radical into the HTM greatly reduce device performance fluctuations due to the environmental dependence and inhibit tBP volatilizing for enhanced long-term stability.
The alkaline hydrogen evolution reaction (HER) is a crucial process for sustainable hydrogen production, yet it requires efficient and stable electrocatalysts to overcome the high activation energy barrier. The article discusses a novel strategy for enhancing the performance of Ni-Fe layered double hydroxide (Ni-Fe LDH) in the alkaline HER by modifying it with a frustrated Lewis acid-base pair (FLP) constructed through vacancy engineering. The study found that the modified Ni-Fe LDH exhibited improved alkaline HER performance. Density functional theory (DFT) calculations demonstrate that the introduction of FLP can activate water and protons more efficiently than monometallic sites, thus reducing the alkaline HER energy barrier and overpotential. In HER under alkaline conditions, the Volmer step involves an additional hydrolysis dissociation compared to acidic conditions, which is one of the factors contributing to the slow reaction kinetics. This paper demonstrates that FLPs can alter the rate-determining step in alkaline HER from the Volmer step to a step with a lower energy barrier, more suitable for hydrogen desorption. The work provides new insights into the role of FLPs in regulating the mechanism and kinetics of HER and opens a new direction for the design and optimization of LDH-based and other electrocatalysts.
Fuel cell electric vehicles hold great promise for a diverse range of applications in reducing greenhouse gas emissions. In power fuel cell systems, hydrogen fuel serves as an energy vector. To ensure its suitability, it is necessary for the quality of hydrogen to adhere to the standards set by ISO 14687:2019, which sets maximum limits for 14 impurities in hydrogen, aiming to prevent any degradation of fuel cell performance. Ammonia (NH3) is a prominent pollutant in fuel cells, and accurate measurements of its concentration are crucial for hydrogen fuel cell quantity. In this study, a novel detection platform was developed for determining NH3 in real hydrogen samples. The online analysis platform integrates a self-developed online dilution module with a Fourier transform infrared spectrometer (ODM-FTIR). The ODM-FTIR can be operated fully automatically with remote operation. Under the optimum conditions, this method achieved a wide linear range between (50~1000) nmol/mol. The limit of detection (LOD) was as low as 2 nmol/mol with a relative standard deviation (RSD, n = 7) of 3.6% at a content of 50 nmol/mol. To ensure that the quality of the hydrogen products meets the requirement of proton exchange membrane fuel cell vehicles (PEMFCV), the developed ODM-FTIR system was applied to monitor the NH3 content in Chengdu Hydrogen Energy Co., Ltd. for 21 days during Chengdu 2021 FISU World University Games. The proposed method retains several unique advantages, including a low detection limit, excellent repeatability, high accuracy, high speed, good stability, and calibration flexibility. It is an effective analytical method for accurately quantifying NH3 in hydrogen, especially suitable for online analysis. It also provides a new idea for the analysis of other impurity components in hydrogen.
The cross-photodimerization often comes with the formation of undesired and competitive homo-photodimer as side products. Herein, we report a series of highly selective [4 + 4] cross-photodimerization between anthracene and 4a-azoniaanthracene derivatives within a cucurbit[10]uril (CB[10]) host in water. Heteroternary inclusion complexes were formed through encapsulation of donor (D1-D2, anthracene derivative) and acceptor (A1-A3, 4a-azoniaanthracene derivatives) pairs in CB[10]. In the presence of CB[10] (1.0 equiv.), the [4 + 4] cross-photodimerization between D1 and A1/A2/A3 efficiently gave a single racemic cross-photodimer. Furthermore, the cross-photodimerization between 9-substituted anthracene D2 and A1/A3 was catalyzed by CB[10] (0.1 equiv.) to quantitatively yield a cross-photodimer with high regioselectivity. Efficient formation of selective cross-photodimers could be attributed to the exclusive encapsulation of D-A hetero-guest pairs in CB[10] and the confinement effect of the CB[10] host cavity. Our study further proves host–guest complexation as a powerful strategy for cross-cycloaddition reactions with high efficiency.
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