Xiang Hu, Jinghui Wang, Hao Zhu, Heng Zhang, Lin Zhu, Qifeng Liang, Fan Zhang
{"title":"Vinylene-Linked Covalent Organic Frameworks with Ammonium-Promoted-Proton Transfer for Photocatalysis of H2O2 Evolution.","authors":"Xiang Hu, Jinghui Wang, Hao Zhu, Heng Zhang, Lin Zhu, Qifeng Liang, Fan Zhang","doi":"10.1002/chem.202501074","DOIUrl":"https://doi.org/10.1002/chem.202501074","url":null,"abstract":"<p><p>Covalent organic frameworks (COFs) have emerged as effective photocatalysts for the environmentally friendly synthesis of hydrogen peroxide (H2O2) through the oxygen reduction reaction (ORR) under solar sunlight. Besides electron transfer in an ORR process, proton transport also serves as an important role in promoting kinetic rate, which was majorly improved via modifying the chemical structures of COFs, but seldom to be explored through a simple additive composition. In work, we report the preparation of two new vinylene-linked COFs termed g-TDM-COF and g-TBD-COF, respectively. The methoxyl substituents pended on the backbones of these COFs rendered them with hydrogen bond donating capabilities. Combined with their substantial semiconducting properties, the COFs enable photocatalysis of hydroperoxide (H2O2) production. Simply compositing these COFs with ammonium ions markedly improved the photoelectric properties, leading to an over 8-fold enhancement of photocatalytic H2O2 production relative to the neat COFs, and an increase in apparent quantum yields (AQYs) from 0.70% to 4.22% at 500 nm. Such phenomenon could be attributed to the efficient interaction ammonium ions with the COFs via hydrogen-bond interaction, thus favorable for broading light-harvesting, narrowing band gaps, and strengthening proton conductivity, As a consequence, their photocatalytic performance could be distinctly enhanced.</p>","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202501074"},"PeriodicalIF":3.9,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144136064","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Cyanomethylation of Aldehydes on an Electrochemical Microflow System and Utility of Machine Learning-Assisted Examination of the Reaction Conditions.","authors":"Eisuke Sato, Akine Tani, Tomoyuki Miyao, Shumpei Kunimoto, Shinobu Takizawa, Koichi Mitsudo, Seiji Suga","doi":"10.1002/chem.202501257","DOIUrl":"https://doi.org/10.1002/chem.202501257","url":null,"abstract":"<p><p>Cyanomethylation of carbonyl compounds affords a β-hydroxy nitrile, which is very useful in the field of synthetic organic chemistry. Although several electrochemical methods have also been reported to achieve cyanomethylation of carbonyl compounds, dehydration as a major side reaction is a significant issue that needs to be prevented. An electrochemical flow reactor, free from side reactions through rapid removal of the reaction solution from the electrode surface, enables the electrochemical cyanomethylation of aldehydes in acetonitrile without any dehydrated side products. To find the \"best\" reaction conditions for each starting material, we used machine learning models. In addition, comparing the machine learning models constructed using various molecular descriptors contributed to understanding the critical molecular properties to proceed the electrochemical cyanomethylation. Our cyanomethylation using a flow system went to completion with a semi-catalytic amount of electrical input, which is not consistent with the conventional basic mechanism, and DFT calculations suggest a radical mechanism.</p>","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202501257"},"PeriodicalIF":3.9,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144136063","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"DNA Tetrahedron-Enhanced Catalytic Hairpin Assembly for In Situ Monitoring of Viral RNA in Host Cells.","authors":"Sha Lu, Ai-Xin Ma, Xiao-Lin Gao, Zhi-Qi Dai, Qing-Nan Li, Yang-Yang Liu, Yi Zhang, Qi Meng, Dai-Wen Pang, Yun-Xi Cui, Deming Kong","doi":"10.1002/chem.202501329","DOIUrl":"https://doi.org/10.1002/chem.202501329","url":null,"abstract":"<p><p>Viruses pose significant threats to global public health and have substantial socio-economic impacts. Developing rapid, sensitive and specific in situ virus detection technologies is crucial for tracking viral genome release, replication in host cells, and intercellular transmission, thus holding great promise in understanding viral infection mechanisms, enabling early diagnosis, screening antiviral drugs, and formulating prevention and treatment strategies. In this study, we present a multifunctional tetrahedral DNA nanostructure (TDN)-based system designed to monitor viral RNA levels in host cells in situ. The system employs a TDN-based hyperbranched catalytic hairpin assembly (CHA) reaction to achieve rapid and powerful signal amplification, generating specific fluorescence resonance energy transfer (FRET) signals in response to target viral RNA. Using Japanese encephalitis virus (JEV) as a model, we developed the THA@JEV system responding to JEV-RNA. This system demonstrated rapid and sensitive detection of JEV-RNA within 12 min in a cell-free environment, enabling real-time imaging of JEV-RNA in situ within host cells. The integrated TDN structure enhanced the biological stability of the probes and ensured their reliability under various stress conditions and microenvironments. This TDN-based sensor system shows significant potential for elucidating viral infection pathways and advancing related virology research, as well as for screening antiviral drugs.</p>","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202501329"},"PeriodicalIF":3.9,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144126342","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Unleashing the Biosensing Potential of 2D Inorganic Nanomaterials: The Journey of a Decade.","authors":"Ikshika Sharely, Shubhi Joshi, Panchali Barman, Mayank Maan, Naveen Kaushal, Avneet Saini","doi":"10.1002/chem.202501080","DOIUrl":"https://doi.org/10.1002/chem.202501080","url":null,"abstract":"<p><p>With the growing need for rapid, sensitive and accurate point-of-care biosensors, two-dimensional (2D) nanomaterials have gained significant attention, establishing them as versatile candidates for advanced biomedical applications. Biosensors utilizing 2D nanomaterials enable real-time disease monitoring, allowing for prompt intervention and therapy, tracking of physiological activities, enhancing the understanding of human biosystem. Since they are cost-effective and user-friendly, 2D nanomaterials have been utilized in commercial biosensors. Over the past decade, graphene and its derivatives have been the most studied 2D nanomaterials, due to their large surface area, tuneable electronic and optical properties, which significantly enhances their sensitivity and specificity. Nevertheless, recently discovered 2D nanomaterials, including MXenes, black phosphorus and hexagonal boron nitride, remain largely unexplored. Despite their numerous applications, the broader potential of these materials in biosensing remains insufficiently explored in current literature. This review offers a comprehensive perspective by specifically focussing on inorganic 2D nanomaterials, an area that remains underrepresented in the literature. It provides an in-depth overview of their unique physicochemical properties and how these features contribute towards enhancing the performance of biosensors, thereby offering new and valuable insights into their emerging role in advanced biomedical diagnostics.</p>","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202501080"},"PeriodicalIF":3.9,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144126354","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Michael J Holzmann, Eric R Westphal, Kenneth M Plackowski, Melissa L Meyerson, John K Grey, Koushik Ghosh
{"title":"Divergent Responses of Carbon Nitride Dot-Based Amorphous Species and Small Molecule Hybrids to Trace Level Analytes.","authors":"Michael J Holzmann, Eric R Westphal, Kenneth M Plackowski, Melissa L Meyerson, John K Grey, Koushik Ghosh","doi":"10.1002/chem.202501495","DOIUrl":"https://doi.org/10.1002/chem.202501495","url":null,"abstract":"<p><p>Bottom-up synthesis of carbon nitride dots (CNDs) offers a versatile platform for the creation of diverse nanomaterials with tunable properties. Here, we report a facile hydrothermal approach using citric acid and urea as precursors to synthesize CNDs with varying degrees of condensation and crystallinity. By carefully controlling reaction conditions and post-synthetic treatments, we obtained two distinct fractions: a polycrystalline fraction composed of small-molecule hybrids and an amorphous fraction containing CNDs. We then sought to understand how the dominant species in these fractions impact sensing abilities using trace-level explosive exemplars. The results have important implications for sensing and related applications where understanding the complex interplay between synthetic conditions and post-synthetic processing play vital roles in determining the final properties of CND materials.</p>","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202501495"},"PeriodicalIF":3.9,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144131767","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Claudia Honisch, Martina Rotondo, Mario Monaco, Stefano Tartaggia, Rohanah Hussain, Giuliano Siligardi, Paolo Ruzza
{"title":"Enhanced Protein Photo-Stability Analysis Using SRCD in the Presence of Phospholipid SUVs.","authors":"Claudia Honisch, Martina Rotondo, Mario Monaco, Stefano Tartaggia, Rohanah Hussain, Giuliano Siligardi, Paolo Ruzza","doi":"10.1002/chem.202500792","DOIUrl":"https://doi.org/10.1002/chem.202500792","url":null,"abstract":"<p><p>The interaction between lipids and proteins impacts on a multitude of cellular processes and may contribute to the onset of several pathologies and ageing. Such processes are frequently linked to oxidative stress, whereby polyunsaturated fatty acids act as substrates for in vivo lipoxidation. The subsequent lipid peroxidation and/or isomerisation is known to affect membrane organization, as well as to modify proteins and DNA, leading to functional alterations. Aim of this study was to evaluate the capacity of UV denaturation experiments to induce lipid modification and to investigate the influence of lipid presence on the conformational stability of selected soluble model proteins. To this end, the UV-denaturation experiment developed at the B23 beamline of the Diamond Light Source (UK) is employed, which high photon flux and brilliance of the incident beamlight induce protein denaturation when repeated consecutive synchrotron radiation circular dichroism spectra are acquired in the far-UV region, diagnostic of protein folding. This allows the estimation of protein photostability. Our findings show that the presence of lipid vesicles (SUVs) significantly impacts the UV-denaturation of proteins, preserving the native structure in proteins with a high helical content. This suggests that lipids may play a protective role against light-induced damage to proteins.</p>","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202500792"},"PeriodicalIF":3.9,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144131896","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yue-Qi Liu, Wen-Hao Pan, Lin-Xia He, Chenglong Han, Tong Lu, Ning-Ning Zhang, Kun Liu
{"title":"Coordination-Controlled Synthesis of Aluminum Nanoparticles: Insights from AlH3·(NMP) x Complexes.","authors":"Yue-Qi Liu, Wen-Hao Pan, Lin-Xia He, Chenglong Han, Tong Lu, Ning-Ning Zhang, Kun Liu","doi":"10.1002/chem.202500415","DOIUrl":"https://doi.org/10.1002/chem.202500415","url":null,"abstract":"<p><p>The controlled chemical synthesis of Aluminum nanocrystals (Al NCs) is crucial for their applications in plasmonics, photocatalysis, and optoelectronics. However, there is still a lack of correlation between the precursor of Al hydride N-methylpyrrolidine (AlH3·(NMP)x) and the Al NC synthesis outcomes . Here, we report the synthesis of AlH3·(NMP)x complexes with different coordination numbers (x from 1.0 to 2.0) and their characterization as precursors regulating the morphology of Al NCs. We isolated AlH3·(NMP)1.0 single crystals from AlH3·(NMP)x mixtures and successfully elucidated the structure of H3Al·(NMP)1.0 through single-crystal X-ray diffraction. Importantly, H3Al·(NMP)1.0 exhibited the fastest decomposition rate, yielding highly monodisperse Al NCs with well-defined shapes and the narrowest size distribution, while higher coordination numbers led to increased polydispersity and irregular morphologies. Additionally, we observed distinct multipole plasmonic resonances in Al NCs synthesized from lower coordination number precursors, highlighting their superior optical properties. This work establishes a direct correlation between precursor coordination chemistry and Al NC synthesis outcomes, providing a foundation for optimizing nanoparticle production for advanced material applications.</p>","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202500415"},"PeriodicalIF":3.9,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144131764","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lisa M S Stiegler, Vincent Wedler, İdil Büküşoğlu, Andreas Hirsch, Wolfgang Peukert, Johannes Walter
{"title":"Investigation of the Degree of Functionalization and Colloidal Stability of Shell-by-Shell Functionalized TiO2 Nanoparticles as a Function of Different Phosphonic Acid Chain Lengths.","authors":"Lisa M S Stiegler, Vincent Wedler, İdil Büküşoğlu, Andreas Hirsch, Wolfgang Peukert, Johannes Walter","doi":"10.1002/chem.202501008","DOIUrl":"https://doi.org/10.1002/chem.202501008","url":null,"abstract":"<p><p>In this work, a series of Shell-by-Shell (SbS)-functionalized colloidal systems consisting of 6 nm TiO2 anatase nanoparticles (NPs), one of the phosphonic acids (PAs) propylphosphonic acid (PAC3), hexylphosphonic acid (PAC6), dodecylphosphonic acid (PAC12), tetradecylphosphonic acid (PAC14), hexadecylphosphonic acid (PAC16), octadecylphosphonic acid (PAC18) and the amphiphile sodium dodecylbenzenesulfonate (SDBS) were prepared, resulting in TiO2-PACX@SDBS (X = 3, 6, 12, 14, 16, or 18) NPs dispersed in deionized water (DIW). During the whole functionalization process, the NPs were subjected to thermogravimetric analysis (TGA) to gain insights into their degree of functionalization and respective thermal stability. In addition, the colloidal stability of the NPs as a function of PA chain length was analyzed by analytical ultracentrifugation (AUC). By combining both TGA and AUC, it was found that the resulting hierarchical NP architectures form agglomerates, with the degree of agglomeration depending on the length of the PA used for the first-shell functionalization. This allows conclusions to be drawn about the efficiency of the overlap between the PA and the SDBS carbon chain.</p>","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202501008"},"PeriodicalIF":3.9,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144126345","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Conformational switch in the alpha-synuclein C-terminus domain directs its fibril polymorphs.","authors":"Kensuke Ikenaka, Cesar Aguirre, Yohei Miyanoiri, Masatomo So, Hajime Tamaki, Takahiro Maruno, Junko Doi, Nan Wang, Keiichi Yamaguchi, Kichitaro Nakajima, Yu Yamamori, Hiroko Inoura, Chi-Jing Choong, Keita Kakuda, Takahiro Ajiki, Yasuyoshi Kimura, Tatsuhiko Ozono, Kousuke Baba, Seiichi Nagano, Yoshitaka Nagai, Hirotsugu Ogi, Susumu Uchiyama, Yoh Matsuki, Kentaro Tomii, Yuji Goto, Hideki Mochizuki","doi":"10.1002/chem.202500650","DOIUrl":"https://doi.org/10.1002/chem.202500650","url":null,"abstract":"<p><p>α-Synuclein (αSyn) inclusions are a pathological hallmark of several neurodegenerative diseases disorders. While cryo-electron microscopy studies have revealed distinct fibril polymorphs across different synucleinopathies, the molecular switches controlling polymorphism remain unveiled. In this study, we found that fibril morphology is associated with the conformational state of monomeric αSyn. Through systematic evaluation of the ionic strength and temperature, we generated two distinct polymorphs: a twisted morphology at low ionic strength and temperature, and a rod-like morphology at higher ionic strength and temperature. Using solid-state NMR, we revealed that both polymorphs share a highly conserved core structure, with morphological differences arising probably from distinct structural arrangements at the protofilament interfaces. Furthermore, we found that a specific conformational change in the C-terminal domain of the monomeric αSyn serves as a molecular switch for the formation of polymorphs. Interestingly, this conformational change can also be triggered by calcium binding to the C-terminus, connecting environmental factors to specific fibril architectures. Our results reveal a conformational role for the C-terminal domain that influences aSyn fibril morphology, providing significant insights into the fibrogenesis of αSyn.</p>","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202500650"},"PeriodicalIF":3.9,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144131854","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Aashish Joshi, Sachidananda Mohapatra, Amit Gupta, Bhanu Nandan
{"title":"Review of Metal Nitrides for Lithium-Sulfur Batteries: Design, Mechanisms and Prospects.","authors":"Aashish Joshi, Sachidananda Mohapatra, Amit Gupta, Bhanu Nandan","doi":"10.1002/chem.202500971","DOIUrl":"https://doi.org/10.1002/chem.202500971","url":null,"abstract":"<p><p>Lithium-sulfur batteries emerge as the next generation battery technology owing to its high theoretical capacity and energy density. However, sluggish redox reactions coupled with severe volume alterations result in under achievement of the merits. Additionally, the atrocious shuttle effect prompts premature failure thereby limiting life cycle count. Transition metal nitrides with excellent properties including good electrical conductivity and catalytic effects have been investigated as functional materials to address the challenges of LSB. Mainly, transition metal nitrides as well as their composites have been employed as hosts and interlayers to boost reaction kinetics and enhance the cycle life. This review focusses on the fundamental mechanisms of metal nitrides towards capture and catalysis of polysulfides. The article highlights battery performance attained with key metal nitrides with inclusion of the synthesis procedures, morphology and size effects. Further, the possible principles for the design of metal nitrides along with future directions are discussed.</p>","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202500971"},"PeriodicalIF":3.9,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144126349","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}