In the electrocatalytic CO reduction reaction (CORR), the strategic design of a catalytic well capable of regulating the overall confinement effects of catalytic sites holds significant promise for enhancing multiple-electron transfer and C─C coupling efficiency, particularly for the generation of C products. Here, a series of Cu-salphen-based covalent organic frameworks (COFs) featuring hydroxyl-induced catalytic well are synthesized, which demonstrate successful application in electrocatalytic CORR to yield multiple-electron transferred products. The meticulously engineered catalytic well, facilitated by multi-hydroxyl groups, manifests robust confinement effects, facilitating selective adsorption, enrichment, and activation of CO, intermediate stabilization, and reduction of energy barriers for electrocatalytic CORR.
View Article and Find Full Text PDFStrategies that can introduce catalytic auxiliary into electrocatalysts to boost the performance of electrocatalytic CO reduction reaction (CORR) are meaningful in exploring hybrid electrocatalytic systems. Here, a series of hybrid electrocatalysts (Cu NCs@MOF-545-M, M=Fe, Co and Ni) have been prepared by assembly Cu NCs with MOF-545-M (M=Fe, Co and Ni) and successfully applied in electrocatalytic CORR. In the obtained MOF-545-M (M=Fe, Co and Ni), the integration of Cu NCs with MOF-545-M (M=Fe, Co and Ni) can create a hybrid electrocatalytic system that enhances the charge transfer efficiency and electrocatalytic CORR activity.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2024
The applications of indirect electrocatalysis toward potential industrial processes are drastically limited by the utilization or processing forms of electrocatalysts. The remaining challenges of electrocatalysts like the recycling in homogeneous systems or pulverization in heterogeneous systems call for advanced processing forms to meet the desired requirements. Here, we report a series of metalloporphyrin-based polymer fibers (M-PF, M=Ni, Cu and Zn) through a rigid-flexible polymerization strategy based on rigid metalloporphyrin and flexible thiourea units that can be applied as heterogeneous redox-mediators in indirect electrocatalysis.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2024
Porous crystalline conjugated macrocyclic materials (CMMs) possess high porosity, tunable structure/function and efficient charge transport ability owing to their planar macrocyclic conjugated π-electron system, which make them promising candidates for applications in energy storage. In this review, we thoroughly summarize the timely development of porous crystalline CMMs in energy storage related fields. Specifically, we summarize and discuss their structures and properties.
View Article and Find Full Text PDFUltra-low temperature resistant adhesive is highly desired yet scarce for material adhesion for the potential usage in Arctic/Antarctic or outer space exploration. Here we develop a solvent-free processed low-temperature tolerant adhesive with excellent adhesion strength and organic solvent stability, wide tolerable temperature range (i.e.
View Article and Find Full Text PDFHydrazone-linked covalent organic frameworks (COFs) with structural flexibility, heteroatomic sites, post-modification ability and high hydrolytic stability have attracted great attention from scientific community. Hydrazone-linked COFs, as a subclass of Schiff-base COFs, was firstly reported in 2011 by Yaghi's group and later witnessed prosperous development in various aspects. Their adjustable structures, precise pore channels and plentiful heteroatomic sites of hydrazone-linked structures possess much potential in diverse applications, for example, adsorption/separation, chemical sensing, catalysis and energy storage, etc.
View Article and Find Full Text PDFHepatobiliary Surg Nutr
April 2024
Background: Adequate evaluation of degrees of liver cirrhosis is essential in surgical treatment of hepatocellular carcinoma (HCC) patients. The impact of the degrees of cirrhosis on prediction of post-hepatectomy liver failure (PHLF) remains poorly defined. This study aimed to construct and validate a combined pre- and intra-operative nomogram based on the degrees of cirrhosis in predicting PHLF in HCC patients using prospective multi-center's data.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
June 2024
Visible-light sensitive and bi-functionally favored CO reduction (CRR)/evolution (CER) photocathode catalysts that can get rid of the utilization of ultraviolet light and improve sluggish kinetics is demanded to conquer the current technique-barrier of traditional Li-CO battery. Here, a kind of redox molecular junction spc metal-covalent organic framework (i.e.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
June 2024
Precise design and tuning of Zn hopping/transfer sites with deeper understanding of the dendrite-formation mechanism is vital in artificial anode protective coating for aqueous Zn-ion batteries (AZIBs). Here, we probe into the role of anode-coating interfaces by designing a series of anhydride-based covalent organic frameworks (i.e.
View Article and Find Full Text PDFEffective personal protection is crucial for controlling infectious disease spread. However, commonly used personal protective materials such as disposable masks lack antibacterial/antiviral function and may lead to cross infection. Herein, a polyethylene glycol-assisted solvent-free strategy is proposed to rapidly synthesize a series of the donor-acceptor metal-covalent organic frameworks (MCOFs) (i.
View Article and Find Full Text PDFThe precise tuning of components, spatial orientations, or connection modes for redox units is vital for gaining deep insight into efficient artificial photosynthetic overall reaction, yet it is still hard achieve for heterojunction photocatalysts. Here, we have developed a series of redox molecular junction covalent organic frameworks (COFs) () for artificial photosynthetic overall reaction. The covalent connection between TAPP-Zn and multidentate TTF endows various connection modes between water photo-oxidation (multidentate TTF) and CO photoreduction (TAPP-Zn) centers that can serve as desired platforms to study the possible interactions between redox centers.
View Article and Find Full Text PDFLenvatinib is a standard therapy option for advanced hepatocellular carcinoma (HCC), but resistance limits clinical benefits. In this study, we identified inhibition of ROS levels and reduced redox status in Lenvatinib-resistant HCC. Integrating RNA-seq with unbiased whole-genome CRISPR-Cas9 screen analysis indicated LINC01607 regulated the P62 to enhance drug resistance by affecting mitophagy and antioxidant pathways.
View Article and Find Full Text PDFThe efficient CO electroreduction into high-value products largely relies on the CO adsorption/activation or electron-transfer of electrocatalysts, thus site-specific functionalization methods that enable boosted related interactions of electrocatalysts are much desired. Here, an oriented coordination strategy is reported to introduce N-rich auxiliary (i.e.
View Article and Find Full Text PDFBackground: Immunotherapy plays an increasingly critical role in the systemic treatment of HCC. This current study aimed to establish a novel prognostic predictor of Programmed death 1 (PD-1) inhibitor therapy in hepatocellular carcinoma (HCC) independent of Child-Pugh grade.
Methods: Our study screened patients with HCC who received PD-1 inhibitors at Tongji Hospital Affiliated to Tongji Medical College of Huazhong University of Science and Technology from January 2018 to December 2020.
The inhomogeneous consumption of anions and direct contact between electrolyte and anode during the Zn-deposition process generate Zn-dendrites and side reactions that can aggravate the space-charge effect to hinder the practical implementation of zinc-metal batteries (ZMBs). Herein, electrospray has been applied for the scalable fabrication (>10 000 cm in a batch-experiment) of hetero-metallic cluster covalent-organic-frameworks (MCOF-Ti Cu ) nanosheet-coating (MNC) with integrated micro space electrostatic field for ZMBs anode protection. The MNC@Zn symmetric cell presents ultralow overpotential (≈72.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2023
The full reaction photosynthesis of H O that can combine water-oxidation and oxygen-reduction without sacrificial agents is highly demanded to maximize the light-utilization and overcome the complex reaction-process of anthraquinone-oxidation. Here, a kind of oxidation-reduction molecular junction covalent-organic-framework (TTF-BT-COF) has been synthesized through the covalent-coupling of tetrathiafulvalene (photo-oxidation site) and benzothiazole (photo-reduction site), which presents visible-light-adsorption region, effective electron-hole separation-efficiency and photo-redox sites that enables full reaction generation of H O . Specifically, a record-high yield (TTF-BT-COF, ≈276 000 μM h g ) for H O photosynthesis without sacrificial agents has been achieved among porous crystalline photocatalysts.
View Article and Find Full Text PDFThe elaborate design of powerful Li-S binders with extended-functions like polysulfides adsorption/catalysis and Li hopping/transferring in addition to robust adhesion-property has remained a challenge. Here, an in situ cathode-interweaving strategy based on metalloporphyrin based covalent-bonding organic polymer (M-COP, M = Mn, Ni, and Zn) binders is reported for the first time. Thus-produced functional binders possess excellent mechanical-strengths, polysulfides adsorption/catalysis, and Li hopping/transferring ability.
View Article and Find Full Text PDFAnisotropically hybridized porous crystalline Li-S battery separators based on porous crystalline materials that can meet the multiple functionalities of both anodic and cathodic sides are much desired for Li-S battery yet still challenging in directional design. Here, an anisotropically hybridized separator (CPM) based on an ionic liquid-modified porphyrin-based covalent-organic framework (COF-366-OH-IL) and catalytically active metal-organic framework (Ni (HITP) ) that can integrate the lithium-polysulfides (LiPSs) adsorption/catalytic conversion and ion-conduction sites together to directionally meet the requirements of electrodes is reported. Remarkably, the-obtained separator exhibits an exceptional high Li transference-number (t = 0.
View Article and Find Full Text PDFBackground: Intrahepatic cholangiocarcinoma (ICC) is the second most common liver malignancy after hepatocellular carcinoma (HCC), with a dismal prognosis and high heterogeneity. The oncological advantages of anatomical resection (AR) and nonanatomical resection (NAR) in HCC have been studied, but surgical strategies for ICC remain controversial with insufficient investigations.
Materials And Methods: From Jan 2013 to Dec 2016, 3880 consecutive patients were retrospectively reviewed from a single center.