The development of photocatalytic systems that enable the simultaneous production of H2O2 and value-added organic chemicals presents a dual advantage: generating valuable products while maximizing the utilization of solar energy. Despite the potential, there are relatively few reports on photocatalysts capable of such dual functions. In this study, we synthesized a series of donor-acceptor covalent organic frameworks (COFs), designated as JUC-675 to JUC-677, to explore their photocatalytic efficiency in the co-production of H2O2 and N-benzylbenzaldimine (BBAD).
View Article and Find Full Text PDFPhoto-driven cross-coupling of o-arylenediamines and alcohols has emerged as an alternative for the synthesis of bio-active benzimidazoles. However, tackling the key problem related to efficient adsorption and activation of both coupling partners over photocatalysts towards activity enhancement remains a challenge. Here, we demonstrate an efficient interface synergy strategy by coupling exposed oxygen vacancies (V) and Pd Lewis acid sites for benzimidazole and hydrogen (H) coproduction over Pd-loaded TiO nanospheres with the highest photoredox activity compared to previous works so far.
View Article and Find Full Text PDFLight-driven photoredox catalysis presents a promising approach for the activation and conversion of methane (CH) into high value-added chemicals under ambient conditions. However, the high C-H bond dissociation energy of CH and the absence of well-defined C-H activation sites on catalysts significantly limit the highly efficient conversion of CH toward multicarbon (C) hydrocarbons, particularly ethylene (CH). Herein, we demonstrate a bimetallic design of Ag nanoparticles (NPs) and Pd single atoms (SAs) on ZnO for the cascade conversion of CH into CH with the highest production rate compared with previous works.
View Article and Find Full Text PDFVascular restenosis following angioplasty continues to pose a significant challenge. The heterocyclic trioxirane compound [1, 3, 5-tris((oxiran-2-yl)methyl)-1, 3, 5-triazinane-2, 4, 6-trione (TGIC)], known for its anticancer activity, was utilized as the parent ring to conjugate with a non-steroidal anti-inflammatory drug, resulting in the creation of the spliced conjugated compound BY1. We found that BY1 induced ferroptosis in VSMCs as well as in neointima hyperplasia.
View Article and Find Full Text PDFPyroptosis plays a critical role in the pathogenesis of mental disorders. However, its specific role and mechanism in arsenic (As)-induced generalized anxiety disorder (GAD) remain elusive. We utilized the data from CtdBbase, Phenopedia and DisGeNet to analyze genes that interact with arsenic poisoning and GAD.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2023
Solar-driven CO reduction integrated with C-C/C-X bond-forming organic synthesis represents a substantially untapped opportunity to simultaneously tackle carbon neutrality and create an atom-/redox-economical chemical synthesis. Herein, we demonstrate the first cooperative photoredox catalysis of efficient and tunable CO reduction to syngas, paired with direct alkylation/arylation of unactivated allylic sp C-H bonds for accessing allylic C-C products, over SiO -supported single Ni atoms-decorated CdS quantum dots (QDs). Our protocol not only bypasses additional oxidant/reductant and pre-functionalization of organic substrates, affording a broad of allylic C-C products with moderate to excellent yields, but also produces syngas with tunable CO/H ratios (1 : 2-5 : 1).
View Article and Find Full Text PDFThe ubiquity of solid-liquid interfaces in nature and the significant role of their atomic-scale structure in determining interfacial properties have led to intensive research. Particularly in electrocatalysis, however, a molecular-level picture that clearly describes the dynamic interfacial structures and organizations with their correlation to preferred reaction pathways in electrochemical reactions remains poorly understood. In this review, CO electroreduction reaction (CORR) is spatially and temporally understood as a result of intricate interactions at the interface, in which the interfacial features are highly relevant.
View Article and Find Full Text PDFBenzimidazoles are a versatile class of scaffolds with important biological activities, whereas their synthesis in a lower-cost and more efficient manner remains a challenge. Here, we demonstrate a conceptually new radical route for the high-performance photoredox coupling of alcohols and diamines to synthesize benzimidazoles along with stoichiometric hydrogen (H ) over Pd-decorated ultrathin ZnO nanosheets (Pd/ZnO NSs). The mechanistic study reveals the unique advantage of ZnO NSs over other supports and particularly that the features of Pd nanoparticles in facilitating the cleavage of the α-C-H bond of alcohols and adsorbing subsequently-generated C-centered radicals hold the key to turning on the reaction.
View Article and Find Full Text PDFPhotocatalytic epoxide alcoholysis through C-O bond cleavage and formation has emerged as an alternative to synthesizing anti-tumoral pharmaceuticals and fine chemicals. However, the lack of crucial evidence to interpret the interaction between reactants and photocatalyst surface makes it challenging for photocatalytic epoxide alcoholysis with both high activity and regioselectivity. In this work, we report the hierarchical ZnIn S @CdS photocatalyst for epoxide alcoholysis with high regioselectivity nearly 100 %.
View Article and Find Full Text PDFSemiconductor quantum dots have been emerging as one of the most ideal materials for artificial photosynthesis. Here, we report the assembled ZnS-CdS hybrid heterostructure for efficient coupling cooperative redox catalysis toward the oxidation of 1-phenylethanol to acetophenone/2,3-diphenyl-2,3-butanediol (pinacol) integrated with the reduction of protons to H. The strong interaction and typical type-I band-position alignment between CdS quantum dots and ZnS quantum dots result in efficient separation and transfer of electron-hole pairs, thus distinctly enhancing the coupled photocatalyzed-redox activity and stability.
View Article and Find Full Text PDFSimultaneously utilizing photogenerated electrons and holes in one photocatalytic system to synthesize value-added chemicals and clean hydrogen (H) energy meets the development requirements of green chemistry. Herein, we report a binary material of CdS/BiVO combining one-dimensional (1D) CdS nanorods (NRs) with two-dimensional (2D) BiVO nanosheets (NSs) constructed through a facile electrostatic self-assembly procedure for the selectively photocatalytic oxidation of aromatic alcohols integrated with H production, which exhibits significantly enhanced photocatalytic performance. Within 2 h, the conversion of aromatic alcohols over CdS/BiVO-25 was approximately 9-fold and 40-fold higher than that over pure CdS and BiVO, respectively.
View Article and Find Full Text PDFBackground: Primary gastric linitis plastica (GLP) is a distinct phenotype of gastric cancer with poor survival. Comprehensive molecular profiles and putative therapeutic targets of GLP remain undetermined.
Methods: We subjected 10 tumor-normal tissue pairs to whole exome sequencing (WES) and whole transcriptome sequencing (WTS).
S-adenosyl-L-homocysteine hydrolase (SAHase) is an important regulator in the methylation reactions in many organisms and thus is crucial for numerous cellular functions. In recent years, SAHase has become one of the popular targets for drug design, and SAHase inhibitors have exhibited potent antiviral activity. In this study, we established the complex-based pharmacophore models based on the known crystal complex of SAHase (PDB ID: 1A7A) to screen the drug-likeness compounds of ChEMBL database.
View Article and Find Full Text PDFSemiconductor-based photoredox catalysis brings an innovative strategy for sustainable organic transformation (e.g., C-C/C-X bond formation), via radical coupling under mild conditions.
View Article and Find Full Text PDFA series of novel pentanediamide derivatives were designed, synthesized and evaluated as S-adenosyl-l-homocysteine hydrolase (SAHase) inhibitors in this study. Some compounds showed good inhibitory activity against SAHase. The optimal compound 7i showed good inhibitory activity against SAHase with IC value of 3.
View Article and Find Full Text PDFObjectives: Thrombospondin 1 (THBS1) is known to play a key role in tumor metastasis, and aberrant DNA methylation is one of the mechanisms regulating THBS1. The present study investigated whether methylated THBS1 in circulating cell-free DNA from preoperative peritoneal lavage fluid (PPLF) and peripheral blood could be used as a potential biomarker for predicting peritoneal dissemination in gastric cancer (GC) patients.
Methods: The status of THBS1 methylation was detected by quantitative methylation-specific PCR (MSP) in tumor tissues, paired PPLF, and serum from 92 GC patients.
Merging hydrogen (H) evolution with oxidative organic synthesis in a semiconductor-mediated photoredox reaction is extremely attractive because the clean H fuel and high-value chemicals can be coproduced under mild conditions using light as the sole energy input. Following this dual-functional photocatalytic strategy, a dreamlike reaction pathway for constructing C-C/C-X (X = C, N, O, S) bonds from abundant and readily available X-H bond-containing compounds with concomitant release of H can be readily fulfilled without the need of external chemical reagents, thus offering a green and fascinating organic synthetic strategy. In this review, we begin by presenting a concise overview on the general background of traditional photocatalytic H production and then focus on the fundamental principles of cooperative photoredox coupling of selective organic synthesis and H production by simultaneous utilization of photoexcited electrons and holes over semiconductor-based catalysts to meet the economic and sustainability goal.
View Article and Find Full Text PDFMetal phosphides (MPs) with unique and desirable physicochemical properties provide promising potential in practical applications, such as the catalysis, gas/humidity sensor, environmental remediation, and energy storage fields, especially for transition metal phosphides (TMPs) and MPs consisting of group IIIA and IVA metal elements. Most studies, however, on the synthesis of MP nanomaterials still face intractable challenges, encompassing the need for a more thorough understanding of the growth mechanism, strategies for large-scale synthesis of targeted high-quality MPs, and practical achievement of functional applications. This review aims at providing a comprehensive update on the controllable synthetic strategies for MPs from various metal sources.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2021
Photocatalytic reduction of CO to solar fuels and/or fine chemicals is a promising way to increase the energy supply and reduce greenhouse gas emissions. However, the conventional reaction system for CO photoreduction with pure H O or sacrificial agents usually suffers from low catalytic efficiency, poor stability, or cost-ineffective atom economy. A recent surge of developments, in which photocatalytic CO valorization is integrated with selective organic synthesis into one reaction system, indicates an efficient modus operandi that enables sufficient utilization of photogenerated electrons and holes to achieve the goals for sustainable economic and social development.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
March 2021
Solar-driven syngas production by CO reduction provides a sustainable strategy to produce renewable feedstocks. However, this promising reaction often suffers from tough CO activation, sluggish oxidative half-reaction kinetics and undesired by-products. Herein, we report a function-oriented strategy of deliberately constructing black phosphorus quantum dots-ZnIn S (BP/ZIS) heterostructures for solar-driven CO reduction to syngas, paired with selectively oxidative C-N bond formation, in one redox cycle.
View Article and Find Full Text PDFThe strain which degraded steviol glycosides to steviol (STE) was screened and isolated from soil samples. A phylogenetic tree was constructed and used to determine the taxonomic status of the strain. 16S rDNA sequence was ultimately used to identify the strain as XJ.
View Article and Find Full Text PDFThe performance of transition metal hydroxides, as cocatalysts for CO photoreduction, is significantly limited by their inherent weaknesses of poor conductivity and stacked structure. Herein, we report the rational assembly of a series of transition metal hydroxides on graphene to act as a cocatalyst ensemble for efficient CO photoreduction. In particular, with the Ru-dye as visible light photosensitizer, hierarchical Ni(OH) nanosheet arrays-graphene (Ni(OH)-GR) composites exhibit superior photoactivity and selectivity, which remarkably surpass other counterparts and most of analogous hybrid photocatalyst system.
View Article and Find Full Text PDFEvid Based Complement Alternat Med
June 2020
The purpose of this study is to investigate the effect of Ledeb. extract (APLE) on lipopolysaccharide- (LPS-) induced cell damage in hepatocytes with a focus on antioxidant and anti-inflammatory activities. Total antioxidant and anti-inflammatory activities of APLE itself were analyzed and phytochemical analysis was performed.
View Article and Find Full Text PDFIncorporating different materials, such as metal sulfides, with metal-organic frameworks (MOFs) to develop MOF-based multifunctional composites with enhanced performance is an important area of research. However, the intrinsically high interfacial energy barrier significantly restricts the heterogeneous nucleation and nanoassembly of metal sulfides onto MOFs during the wet chemistry synthesis process. Herein, taking advantage of the natural tailorability of MOFs, the precise and controllable growth of metal sulfide nanoparticles (NPs) (CdS, ZnS, CuS and Ag2S) at the coordinatively unsaturated metal sites (CUSs) of MOFs to form MOF@metal sulfide composites under mild conditions is achieved via a cysteamine-assisted coordination-driven route.
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