As hydrogen has been increasingly considered as promising sustainable energy supply, electrochemical overall water splitting driven by highly efficient non‐noble metal electrocatalysts has aroused ...extensive attention. Transition metal phosphides (TMPs) have demonstrated remarkable electrocatalytic performance, including high activity and robust durability towards hydrogen evolution reaction (HER) in acidic and alkaline as well as neutral electrolytes. In this Review, up‐to‐date progress of TMP‐based HER electrocatalysts is summarized. Various synthesis strategies of TMPs based on selected phosphorus sources are presented, and the reaction mechanisms of HER as well as the contribution of phosphorus in the TMPs to HER activity are briefly discussed. The multiscale approaches for promoting the activity and stability of TMP‐based catalysts are discussed with respect to intrinsic electronic structure, hybrids, microstructure, and working electrode interface. Some crucial issues and future perspectives of TMPs are pointed out. These modulated approaches and challenges are also instructive for constructing other high‐activity energy‐related electrocatalysts.
Transitioning to hydrogen: In this Review, up‐to‐date progress of transition metal phosphide (TMP)‐based hydrogen evolution reaction (HER) electrocatalysts is summarized. Various synthesis strategies and the HER reaction mechanisms of TMP‐based catalysts are briefly discussed. In addition, multiscale approaches with respect to electronic structure, hybrids, microstructure, and working electrode interface are discussed for promoting HER performances.
Recent years have witnessed an upsurge of interest in exploiting advanced photo‐/electrocatalysts for efficient energy conversion and environmental remediation. Constructing internal electric fields ...has been highlighted as a rising star to help facilitate various catalytic processes, with the merits of promoting charge transfer/separation, optimizing redox potential and creating effective active/adsorption sites. Internal electric fields are usually formed by the polarization of uneven charge distributions between different constituent layers, which widely exist in piezoelectrics, polar surface terminations, and heterostructure materials. Herein, a groundbreaking and interdisciplinary overview of the latest advances in the construction of internal electric fields to improve photo(electro)catalytic and electrocatalytic activity is provided. This critical review begins with an encyclopedic summary of the classification, advantages, and synthesis strategies of internal electric fields. Subsequently, the identification methods are thoroughly discussed based on the characterization techniques, experiments, and theoretical calculations, which can provide profound guidance for the in‐depth study of internal electric fields. To elaborate the theory–structure–activity relationships for internal electric fields, the corresponding reaction mechanisms, modification strategies, and catalytic performance are jointly discussed, along with a discussion of their practical energy and environmental applications. Finally, an insightful analysis of the challenges and future prospects for internal electric field‐based catalysts are discussed.
This review provides a clear understanding of the classification, advantages, creation, and identification of internal electric fields and the dramatic improvements in energy and environmental catalysis that result.
Septic arthritis, characterized as one of the most aggressive joint diseases, is primarily attributed to
(
) and often results from hematogenous dissemination. Even with prompt treatment, septic ...arthritis frequently inflicts irreversible joint damage, leading to sustained joint dysfunction in a significant proportion of patients. Despite the unsatisfactory outcomes, current therapeutic approaches for septic arthritis have remained stagnant for decades. In the clinical context, devising innovative strategies to mitigate joint damage necessitates a profound comprehension of the pivotal disease mechanisms. This entails unraveling how bacterial virulence factors interact with host elements to facilitate bacterial invasion into the joint and identifying the principal drivers of joint damage. Leveraging animal models of septic arthritis emerges as a potent tool to achieve these objectives. This review provides a comprehensive overview of the historical evolution and recent advancements in septic arthritis models. Additionally, we address practical considerations regarding experimental protocols. Furthermore, we delve into the utility of these animal models, such as their contribution to the discovery of novel bacterial virulence factors and host elements that play pivotal roles in the initiation and progression of septic arthritis. Finally, we summarize the latest developments in novel therapeutic strategies against septic arthritis, leveraging insights gained from these unique animal models.
A radical di‐ and trichloromethylation/cyclization of unactivated alkenes was developed with commercially available dichloromethane and chloroform as di‐and trichloromethyl radical sources under ...metal‐free conditions. Variously substituted di‐ and trichloromethylated pyrrolo‐ and piperidino‐quinazolinones were obtained in 47–94% yields. Additionally, dibromomethylation/cyclization was also achieved under standard conditions when CH2Br2 was utilized. Moreover, the obtained dichloromethylated product can be transformed into 1′H‐spirocyclopropane‐1,3′‐pyrrolo2,1‐bquinazolin‐9′(2′H)‐one after treating by KOH.
Diacyl peroxides, which can be easily synthesized from corresponding carboxylic acids, are commonly utilized as radical initiators and one electron oxidants. Under thermal, transition-metal catalysis ...or irradiation conditions the cleavage of relatively weak O-O bonds would occur followed by CO
2
extrusion to generate the corresponding aryl or alkyl radicals. Thus, diacyl peroxides can be employed as ideal arylating and alkylating reagents in organic synthesis, including C-H/N-H arylation/alkylation, aryl/alkyl radical addition to unsaturated bonds, hetero arylation/alkylation, eliminative arylation/alkylation, perfluoroalkylation
etc.
Moreover, these arylation/alkylation protocols have been successfully utilized in the synthesis and late-stage functionalization of natural products as well as bioactive molecules. In this review, recent advances on arylation and alkylation using diacyl peroxides as aryl and alkyl radical sources are summarized and discussed.
This feature article describes the recent achievements in utilizing diacyl peroxides as arylating and alkylating reagents in organic synthesis
via
the formation of aryl and alkyl radicals.
A visible‐light induced radical 1,2‐aryl migration of α,α‐diarylallyl alcohols was developed under mild and metal‐free conditions. Commercially available CHCl3 and CH2Cl2 were used as tri‐ and ...dichloromethyl radical precursors. Structurally diverse β‐polochloromethylated ketones were obtained in good to moderate yields via neophyl‐type rearrangement. Besides, the polychloromethyl group can be easily transformed into other useful functional groups.
A visible‐light induced radical 1,2‐aryl migration of α,α‐diarylallyl alcohols was developed toward β‐polochloromethylated ketones with commercially available CHCl3 and CH2Cl2 as tri‐ and dichloromethyl radical precursors.
As an abundant and attractive element, the emergence of new carbon-based materials brings revolutionary development in material science and technology. Carbon-based materials have spawned ...considerable interest for fabricating polymer composites/nanocomposites with greatly improved mechanical, thermal, gas barrier, conductivity, and flame retardant performance. In this review, the importance of carbon-based materials and the necessity of fire resistance for polymeric materials are initially introduced. Then, the fundamental flame retardant mechanisms and experimental analytical techniques are described to understand the relationship between structures and flame retardant properties. The main section is dedicated to the preparation and properties of multifunctional polymer composites/nanocomposites with carbon-based materials, with special emphasis on the flame retardant properties of these materials. A wide variety of carbon-based materials are discussed for use in flame retardant polymer nanocomposite, including graphite, graphene, carbon nanotubes, fullerenes as well as some new emerging carbon forms (carbon nitride, carbon aerogels, etc). Finally, a brief outlook at the developments in carbon-based materials for flame retardant polymeric composites is given by discussing the major progress, opportunities, and challenges.
Molecules with di‐ or trichloromethyl group are widely existed in natural products and man‐made structures that represent special activities in pharmaceuticals and agrochemicals. Besides, ...polychloromethyl‐containing compounds are also high valuable intermediates in organic synthesis and also can be used as functional materials. Therefore, significant efforts have been made toward the incorporation of polychloromethyl groups into certain structures. In this field, a variety of polychloromethyl reagents, such as CH2Cl2, HCCl3, CCl4, TMSCCl3, TMSCCl2H, etc. have been utilized as the di‐ or trichloromethyl sources toward polychloromethylated structures through radical, nucleophilic, and other reaction patterns. In this review, we summarized and discussed the recent achievements in the synthesis of polychloromethylated compounds, mainly focused on the employment of different polychloromethyl reagents. Most of the works we investigated were reported after 2010. Mechanism discussions and outlooks were also given.
A radical alkylarylation of 2‐aryl‐N‐methacryloyl indoles via autoxidation of alkylboronic acids was developed under metal‐free conditions for the construction of indolo2,1‐aisoquinolinone ...derivatives. Primary and secondary alkyl boronic acids were utilized as suitable alkyl sources with O2 as the clean and green oxidant in a simple operate mode. Moreover, this protocol can also be applied to the construction of benzimidazo‐2,1‐aisoquinolinone derivatives.
An iron(II)‐catalyzed three‐component reaction was developed for the construction of trichloromethylated 3‐benzylquinoxalin‐2(1H)‐ones. This reaction was conducted through the trichloromethylation of ...alkenes with quinoxalin‐2(1H)‐ones using commercially available chloroform as trichloromethyl radical source, which provided a convenient approach toward trichloromethylated 3‐benzylquinoxalin‐2(1H)‐ones.
