Achieving white‐light emission, especially white circularly polarized luminescence (CPL) from a single‐phase material is challenging. Herein, a pair of chiral CuI coordination polymers (1‐M and 1‐P) ...have been prepared by the asymmetrical assembly of achiral ligands and Cu2I2 clusters. The compounds display dual emission bands and can be used as single‐phase white‐light phosphors, achieving a “warm”‐white‐light‐emitting diode with an ultra‐high color rendering index (CRI) of 93.4 and an appropriate correlated color temperature (CCT) of 3632 K. Meanwhile, corresponding CPL signals with maximum dissymmetry factor |glum|=8×10−3 have been observed. Hence, intrinsic white‐light emission and CPL have been realized simultaneously in coordination polymers for the first time. This work gains insight into the nature of chiral assembly from achiral units and offers a prospect for the development of single‐phase white‐CPL materials.
A pair of chiral CuI coordination polymers (1‐P/M) were produced from achiral precursors by crystallization‐driven symmetry‐breaking assembly. The enantiomers feature unique helical layered structures and tunable dual‐emission photoluminescence, achieving intrinsic “warm”‐white emitting with an ultra‐high color rendering index (93.4) and circularly polarized luminescence with a remarkable dissymmetry factor (8×10−3) simultaneously.
Scope
Gallic acid (GA) is a dietary phenolic acid found in tea, red wine, and some plants. It exhibits anti‐oxidative and anti‐inflammatory activities. Recent studies have revealed that GA has ...beneficial effects against several cardiovascular diseases; however, whether GA attenuates pressure‐overload‐induced cardiac hypertrophy and the underlying mechanism remains unclear.
Methods and results
Primary cardiomyocyte hypertrophy is stimulated with angiotensin II (Ang II). Cardiac hypertrophic remodeling is induced in mice by transverse aortic constriction (TAC). Myocardial function is evaluated by echocardiographic and hemodynamic analyses, while cardiac tissues are analyzed by histological staining. It is observed that GA significantly decreases Ang II‐induced increases in cardiomyocyte size in vitro. Administration of GA in mice markedly improves TAC‐induced cardiac dysfunction and attenuates pathological changes, including cardiac myocyte hypertrophy, fibrosis, inflammation, and oxidative stress. Mechanistically, GA inhibits ULK1 and activates autophagy, which induces the degradation of EGFR, gp130, and calcineurin A, thereby inhibiting the downstream signaling cascades (AKT, ERK1/2, JAK2/STAT3, and NFATc1).
Conclusions
The results demonstrate for the first time that GA prevents myocardial hypertrophy and dysfunction via an autophagy‐dependent mechanism. Thus, GA represents a promising therapeutic candidate for treating cardiac hypertrophy and heart failure.
Gallic acid (GA), a type of dietary phenolic acid found in tea and other plants, prevents angiotensin II‐induced cardiomyocyte hypertrophy and pressure overload‐induced myocardial dysfunction. Mechanistically, GA enhances autophagy activation which promotes degradation of epidermal growth factor receptor, glycoprotein 130 and calcineurin A resulting in inhibition of downstream signaling cascades.
For effective application of electrospinning and electrospun fibrous meshes in wound dressing, we have in situ electrospun poly(vinyl pyrrolidone)/iodine (PVP/I), PVP/poly(vinyl pyrrolidone)-iodine ...(PVPI) complex, and poly(vinyl butyral) (PVB)/PVPI solutions into fibrous membranes by a handheld electrospinning apparatus. The morphologies of the electrospun fibers were examined by SEM, and the hydrophobicity, gas permeability, and antibacterial properties of the as-spun meshes were also investigated. The flexibility and feasibility of in situ electrospinning PVP/I, PVP/PVPI, and PVB/PVPI membranes, as well as the excellent gas permeabilities and antibacterial properties of the as-spun meshes, promised their potential applications in wound healing.
Cobalt–nitrogen–carbon is hitherto considered as one of the most satisfactory alternatives to precious metal catalysts for oxygen electrocatalysts. However, precisely tuning the local coordination of ...Co sites and thus engineering d‐orbital electron configuration to optimize the binding energy of the intermediates remains a huge challenge. Herein, a robust electrostatic self‐assembly strategy is developed to engineer penta‐coordinated Co sites by introducing axial O ligands with atomic‐level precision to form CoN4O1 configurations on MXene nanosheets (CoN4‐O/MX). The optimized CoN4‐O/MX demonstrates outstanding bifunctional electrocatalytic performance with a small potential gap of 0.72 V, significantly outperforming the cobalt–nitrogen–carbon catalyst with plane‐symmetric CoN4 sites and precious metal counterparts. The Zn–air batteries integrated with CoN4‐O/MX provide an outstanding peak power density of 182.8 mW cm−2 and a long‐term cyclability for 250 h. Density functional theory calculations reveal that CoO coordination induces electronic delocalization to draw off partial electrons from the dz2 orbital, which forms unsaturated orbital filling and lifts the energy level, resulting in a stronger Lewis basicity to facilitate electron injection into the intermediate. The study presented here provides not only a novel methodology to achieve precise control of heteroatom coordination, but also a fundamental understanding about the structure–activity relationships of dz2 orbitals.
A robust electrostatic self‐assembly strategy is developed to engineer penta‐coordinated Co sites by introducing axial O ligands with atomic‐level precision to form CoN4O1 configurations. CoO coordination induces electronic delocalization to regulate Co 3d orbitals energy level and dz2 orbital occupancy, resulting in improved OH* intermediate activation abilities and outstanding ORR performance compared to cobalt–nitrogen–carbon with symmetric Co‐N4 sites.
The emergence of drug-resistant microbes has become a threat to global health, and microbial infections severely limit the use of healthcare materials. To achieve efficient antimicrobial therapy, ...supramolecular hydrogels demonstrate unprecedented advantages in medical applications due to the tunable and reversible nature of their supramolecular interactions and the capability of hydrogels to incorporate various therapeutic agents. Herein, antimicrobial hydrogels are categorized according to their inherent antimicrobial properties or based on their roles in encapsulating antimicrobial materials. Moreover, strategies to further enhance the antimicrobial efficacy of hydrogels are highlighted, such as the incorporation of antifouling agents or the enabling of response towards physiological cues. We envision that supramolecular hydrogels, in combination with modern medical technology and devices, will contribute to the development of efficient and safe systems for antimicrobial therapy.
The programmable nature of supramolecular interactions enables various supramolecular hydrogels to perform antimicrobial therapy.
Abstract
Aims
Chemokine-mediated monocyte infiltration into the damaged heart represents an initial step in inflammation during cardiac remodelling. Our recent study demonstrates a central role for ...chemokine receptor CXCR2 in monocyte recruitment and hypertension; however, the role of chemokine CXCL1 and its receptor CXCR2 in angiotensin II (Ang II)-induced cardiac remodelling remain unknown.
Methods and results
Angiotensin II (1000 ng kg−1 min−1) was administrated to wild-type (WT) mice treated with CXCL1 neutralizing antibody or CXCR2 inhibitor SB265610, knockout (CXCR2 KO) or bone marrow (BM) reconstituted chimeric mice for 14 days. Microarray revealed that CXCL1 was the most highly upregulated chemokine in the WT heart at Day 1 after Ang II infusion. The CXCR2 expression and the CXCR2+ immune cells were time-dependently increased in Ang II-infused hearts. Moreover, administration of CXCL1 neutralizing antibody markedly prevented Ang II-induced hypertension, cardiac dysfunction, hypertrophy, fibrosis, and macrophage accumulation compared with Immunoglobulin G (IgG) control. Furthermore, Ang II-induced cardiac remodelling and inflammatory response were also significantly attenuated in CXCR2 KO mice and in WT mice treated with SB265610 or transplanted with CXCR2-deficienct BM cells. Co-culture experiments in vitro further confirmed that CXCR2 deficiency inhibited macrophage migration and activation, and attenuated Ang II-induced cardiomyocyte hypertrophy and fibroblast differentiation through multiple signalling pathways. Notably, circulating CXCL1 level and CXCR2+ monocytes were higher in patients with heart failure compared with normotensive individuals.
Conclusions
Angiotensin II-induced infiltration of monocytes in the heart is largely mediated by CXCL1–CXCR2 signalling which initiates and aggravates cardiac remodelling. Inhibition of CXCL1 and/or CXCR2 may represent new therapeutic targets for treating hypertensive heart diseases.
Aberrant glucose metabolism and immune evasion are recognized as two hallmarks of cancer, which contribute to poor treatment efficiency and tumor progression. Herein, a novel material system ...consisting of a glucose and TEMPO (2,2,6,6‐tetramethylpiperidin‐1‐yl)oxyl) at the distal ends of PEO‐b‐PLLA block copolymer (glucose‐PEO‐b‐PLLA‐TEMPO), is designed to encapsulate clinical therapeutics CUDC101 and photosensitizer IR780. The specific core–shell rod structure formed by the designed copolymer renders TEMPO radicals excellent stability against reduction‐induced magnetic resonance imaging (MRI) silence. Tumor‐targeting moiety endowed by glucose provides the radical copolymer outstanding multimodal imaging capabilities, including MRI, photoacoustic imaging, and fluorescence imaging. Efficient delivery of CUDC101 and IR780 is achieved to synergize the antitumor immune activation through IR780‐mediated photodynamic therapy (PDT) and CUDC101‐triggered CD47 inhibition, showing M1 phenotype polarization of tumor‐associated macrophages (TAMs). More intriguingly, this study demonstrates PDT‐stimulated p53 can also re‐educate TAMs, providing a combined strategy of using dual tumor microenvironment remodeling to achieve the synergistic effect in the transition from cold immunosuppressive to hot immunoresponsive tumor microenvironment.
This study presents new insights on CUDC101 in the reprogramming of tumor‐associated macrophages toward antitumor M1 phenotype by CD47 inhibition with a glucose‐contained magnetic resonance imaging‐capable supramolecular rod‐like micelle, and phototriggered p53 by codelivery of IR780 can achieve the synergistic effect in the transition from cold immunosuppressive to hot immunoresponsive tumor microenvironment.
Background/Aims: Cardiac remodeling is a critical pathogenetic process leading to heart failure. Suppressor of cytokine signaling-3 (SOCS3) is demonstrated as a key negative regulator of the gp130 ...receptor to inhibit cardiac hypertrophy. However, the role of SOCS3 in deoxycorticosterone-acetate (DOCA)-salt-induced cardiac remodeling remains unclear. Methods: Cardiac-specific SOCS3 knockout (SOCS3cKO) and wild-type (WT) C57BL/6J mice were subjected to uninephrectomy and DOCA-salt for 3 weeks. The effect of SOCS3 on cardiac remodeling and inflammation was evaluated by histological analysis. Gene and protein levels were measured by real-time PCR and immunoblotting analysis. Results: After DOCA-salt treatment, the expression of SOCS3, activation of gp130/JAK/STAT3, cardiac dysfunction and fibrosis in DOCA-salt mice were significantly elevated, which were markedly attenuated by eplerenone, a specific mineralocorticoid receptor (MR) blocker. Moreover, DOCA-salt-induced cardiac dysfunction, hypertrophy, fibrosis and inflammation were aggravated in SOCS3cKO mice, but were significantly reduced in AAV9-SOCS3-injected mice. These effects were mostly associated with activation of gp130/STAT3/AKT/ERK1/2, TGF-β/Smad2/3 and NF-κB signaling pathways. Conclusions: Our data demonstrate that loss of SOCS3 in cardiomyocytes promotes DOCA-salt-induced cardiac remodeling and inflammation, and it may be a novel potential therapeutic target for hypertensive heart disease.
Atomically dispersed metal‐nitrogen‐carbon (M‐N‐C) catalysts have exhibited encouraging oxygen reduction reaction (ORR) activity. Nevertheless, the insufficient long‐term stability remains a ...widespread concern owing to the inevitable 2‐electron byproducts, H2O2. Here, we construct Co‐N‐Cr cross‐interfacial electron bridges (CIEBs) via the interfacial electronic coupling between Cr2O3 and Co‐N‐C, breaking the activity‐stability trade‐off. The partially occupied Cr 3d‐orbitals of Co‐N‐Cr CIEBs induce the electron rearrangement of CoN4 sites, lowering the Co‐OOH* antibonding orbital occupancy and accelerating the adsorption of intermediates. Consequently, the Co‐N‐Cr CIEBs suppress the two‐electron ORR process and approach the apex of Sabatier volcano plot for four‐electron pathway simultaneously. As a proof‐of‐concept, the Co‐N‐Cr CIEBs is synthesized by the molten salt template method, exhibiting dominant 4‐electron selectively and extremely low H2O2 yield confirmed by Damjanovic kinetic analysis. The Co‐N‐Cr CIEBs demonstrates impressive bifunctional oxygen catalytic activity (▵E=0.70 V) and breakthrough durability including 100 % current retention after 10 h continuous operation and cycling performance over 1500 h for Zn‐air battery. The hybrid interfacial configuration and the understanding of the electronic coupling mechanism reported here could shed new light on the design of superdurable M‐N‐C catalysts.
A cross‐interfacial electronic bridges (CIEBs) is constructed via interfacial electronic coupling between Cr2O3 and Co‐N‐C, breaking the trade‐off between activity and stability. The partially occupied Cr 3d‐orbitals of Co‐N‐Cr CIEBs induce the electron rearrangement of CoN4 sites, lowering the Co‐OOH* antibonding orbital occupancy and accelerating the adsorption of intermediates. Consequently, the Co‐N‐Cr CIEBs suppress the two‐electron ORR process and approach the apex of Sabatier volcano plot for four‐electron pathway simultaneously.
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