Wiley最新文献

Cross-linking mass spectrometry (XL-MS) has seen significant improvements which have enhanced its utility for studying protein-protein interactions (PPIs), primarily due to the emergence of novel crosslinkers and the development of streamlined analysis workflows. Nevertheless, poor membrane permeability and side reactions with water limit the extent of productive intracellular crosslinking events that can be achieved with current crosslinkers. To address these problems, we have synthesized a novel crosslinker with o-nitrobenzyl-based photoresponsive groups. These o-nitrobenzyl ester (o-NBE) groups enhance the stability and hydrophobic properties of the crosslinker and add the potential for temporal resolution, i.e. the ability to control the initiation of the crosslinking reaction. Upon exposure to UV light the resulting aldehyde product reacts with adjacent amino groups and subsequent reductive amination of the formed Schiff-bases yields stable secondary amine linkages. This controlled activation mechanism enables precise UV-triggered protein crosslinking. We demonstrate proof-of principle of our o-NBE cross-linker to reliably detect PPIs by XL-MS using a recombinant model protein. We also demonstrate its ability to enter intact Hela cells, thereby indicating its future potential as a useful tool to study PPIs within the cellular environment.

Nitric oxide (NO) is one of the byproducts of nitrogen metabolism. Excess amount of NO is scavenged by phytoglobins. The role of phytoglobin mediated NO homoeostasis in modulation of nitrate transporters was investigated using NO scavenger cPTIO, phytoglobin overexpressing rice and Arabidopsis. Growing plants under low nitrate leads to generation of reduced levels of NO accompanied by elevated expression of high affinity transporters (HATs) such as NRT2.1, NRT2.3 and NRT2.4. Scavenging of NO by cPTIO under optimal nitrate caused enhanced HATs expression. Phytoglobin overexpressing Arabidopsis showed improved growth and enhanced expression of HATs under low nitrogen in comparison to WT. Pretreatment of optimal nitrate grown plants with NO scavenger cPTIO enhanced HATs expression and shifting of these primed plants from optimal to low nitrate leads to further elevation of HATs expression accompanied by enhanced nitrogen uptake and its accumulation with positive effect on growth. Phytoglobin overexpression in rice leads to enhanced HATs expression, improved growth, nitrogen accumulation under low nitrate. Pgb OE lines showed enhanced accumulation of amino acids. Taken together our results suggest an important role of phytoglobins in nitrogen uptake and assimilation.

In grass cell walls, ferulic acid (FA) serves as an important cross-linker between cell wall polymers, such as arabinoxylan (AX) and lignin, affecting the physicochemical properties of the cell walls as well as the utilization properties of grass lignocellulose for biorefinering. Here, we demonstrate that hydroxycinnamaldehyde dehydrogenase (HCALDH) plays a crucial role in the biosynthesis of the FA used for cell wall feruloylation in rice (Oryza sativa). Bioinformatic and gene expression analyses of aldehyde dehydrogenases (ALDHs) identified two rice ALDH subfamily 2C members, OsHCALDH2 (OsALDH2C2) and OsHCALDH3 (OsALDH2C3), potentially involved in cell wall feruloylation in major vegetative tissues of rice. CRISPR-Cas9 genome editing of OsHCALDH2 and OsHCALDH3 revealed that the contents of AX-bound ferulate were reduced by up to ~45% in the cell walls of the HCALDH-edited mutants, demonstrating their roles in cell wall feruloylation. The abundance of hemicellulosic sugars including arabinosyl units on AX was notably reduced in the cell walls of the HCALDH-edited mutants, whereas cellulose and lignin contents remained unaffected. In addition to reducing cell wall-bound ferulate, the loss of OsHCALDH2 and/or OsHCALDH3 also partially reduced cell wall-bound p-coumarate and sinapate in the vegetative tissues of rice, whereas it did not cause detectable changes in the amount of γ-oryzanol (feruloyl sterols) in rice seeds. Furthermore, the HCALDH-edited mutants exhibited improved cell wall saccharification efficiency, both with and without alkaline pretreatment, plausibly due to the reduction in cell wall cross-linking FA. Overall, HCALDH appears to present a potent bioengineering target for enhancing utilization properties of grass lignocellulose.

We describe novel amine-mediated transformation of alkynyl ketones and amides to generate 2-methylene-2H-pyrans, substituted 3-hydroxy-9H-fluoren-9-ones, and amine-incorporated arenes. These cascade processes are initiated by conjugate addition of secondary amine followed by hydrolysis of the enamine/vinylogous amide intermediates. The product distribution is highly sensitive to the steric and electronic effects of the substituents on both the alkyne moieties, the tether structure connecting them, and the nature of the amine. Alkynyl amide participates in the Alder-ene reaction favorably to generate more reactive allene amide that reacts with amine to generate amine-incorporated arene products. These metal-free cascade reactions are a useful synthetic method that can be exploited for the construction of various hetero- and carbocyclic systems.

The rapid transfer and separation of photogenerated electrons is very important for the improvement of photocatalytic efficiency. Here, chiral induced spin selectivity effect (CISS effect) was developed to accelerate electron transfer for efficient photocatalytic hydrogen production. A chiral and achiral racemic supramolecular Pd(II) complex nanofiber was fabricated via supramolecular self-assembly of chiral L-Py or its racemes with Pd(II) and used to modify carbon nitride (g-C₃N₄). The obtained chiral photocatalyst L-Py-Pd/g-C₃N₄-4 and achiral photocatalyst Rac-Pd/g-C₃N₄-4, show enhanced photocatalytic activities with hydrogen evolution rates of 2476 and 1339 μmol g^-1 h^-1, respectively, while that of pure g-C₃N₄ is 30.5 μmol g^-1 h^-1. Chiral photocatalyst has 85 % higher activity than achiral one and is 82.5-fold of pure g-C₃N₄, due to better suppression of the recombination of photogenerated electron-hole pairs in the interface of g-C₃N₄ contact with chiral molecule. Spectral tests and photoelectrochemical tests proved that the chiral supramolecular Pd(II) complex can act both as an electron spin filter and hydrogen reduction catalytic center to enhance photocatalytic efficiency. This work offers a new route to facilitate electron transfer by the CISS effect for photocatalytic hydrogen evolution.

The large anomalous Nernst effect in magnetic Weyl semimetals is one of the most intriguing transport phenomena, which draws significant attention for its potential applications in topological thermoelectrics. Despite frequent reports of substantial anomalous Nernst conductivity (ANC), methods to optimize Nernst thermoelectrics remain limited. The research reveals that the magnitude of the ANC is directly related to the sum of the anomalous Nernst and Hall angles. While the sign of the anomalous Hall angle is relatively stable in a certain material, the sign of the anomalous Nernst angle can be intrinsically tuned. Therefore, the ANC can be effectively optimized by regulating these angles to work in concert. This finding is verified by experimental modulation from iron-doped magnetic topological material Co₃Sn₂S₂. Additionally, a robust TlnT scaling law of the ANC over the temperature range of 40 to 140 K is observed in all studied samples, suggesting an intrinsic origin of the ANC. Considering the common opposite sign of the anomalous Nernst and Hall angles in many magnetic topological materials, the research offers an applicable scheme for optimizing the Nernst thermoelectrics.

Non-invasive biosensors have attracted attention for their potential to obtain continuous, real-time physiological information through measurements of biochemical markers, such as one of the most important-glucose, in biological fluids. Although some optical sensing materials are used in non-invasive devices for continuous glucose monitoring (CGM), surface or localized plasmon sensing material are seldom applied in CGM owing to modest sensitivity and bulk sensing apparatus. Herein, a metasurface (MGMSPR) biosensor based on the metasurface plasmon resonance chip modified with heterostructured Ti₃C₂ MXene-Graphene oxide (MG) is reported, which potentially enables ultra-sensitive glucose detection. The sensor consists of a dual-channel microfluidic device integrated with silver mirror enhanced MGMSPR chips. Not only does it promote the entry of glucose oxidase (GOD) into the internal pores and enhance the stable fixation of GOD in the membrane, but also the integration of MG material provides a high specific surface area and unique electronic properties, thereby significantly enhancing the sensitivity of the MGMSPR sensor. The detection limit of MGMSPR biosensor is 106.8 µM. This pioneering approach opens new avenues for monitoring physiological parameters and process analytical technology on an optical platform, providing continuous health monitoring and production process control through optical sensors.

Minimally invasive surgical techniques, including endoscopic and robotic procedures, continue to revolutionize patient care, for their ability to minimize surgical trauma, thus promoting faster recovery and reduced hospital stays. Yet, the suturing of soft tissues ensuring damage-free tissue bonding during these procedures remains challenging due to missing haptics and the fulcrum effect. Laser tissue soldering has potential in overcoming these issues, offering atraumatic seamless tissue fusion. To ensure the precision and safety of laser tissue soldering, the study introduces feedback-controlled fluorescent nanothermometry-guided laser tissue soldering using nanoparticle-protein solders within endoscopic and robotic contexts. Temperature-sensitive fluorescent nanoparticles embedded in the solder provide surgeons with immediate feedback on tissue temperatures during laser application, all while within the confines of minimally invasive (robotic) surgical setups. By integrating fluorescent nanothermometry-guided laser tissue surgery into endoscopic and robotic surgery, the study paves the way for a new approach for safe and atraumatic soft tissue joining, especially in regions where traditional suturing is unfeasible.

Nuclear energy makes large contributions toward meeting global energy needs, but societal concerns remain high given the impacts of the intended release of radioactive materials including ¹²⁹I and ¹³¹I. In this paper we explore the use of a homologous series of acyclic CB[n] type hosts (H1-H4) as adsorbents of iodine from the vapor phase. We find that H2-H4, but not H1 - perform well in this application with uptake capacities of 2.2 g g^-1, 1.5 g g^-1, and 1.9 g g^-1, respectively. The chemisorptive uptake process involves partial oxidation of catechol walled H2 to quinone walled host and capture of I₃ ^- and I₅ ^-. Solid H2 can be regenerated by treatment with Na₂S₂O₄ and reused at least five times. The x-ray crystal structure of H2 is also reported.