The rhodium-catalyzed sulfur-directed C–H bond activation and tandem cyclization of enaminothiones with alkynes proceed efficiently. Most products of 1H-isothiochromenes with various substituents are achieved in good yields by regioselective C–C and C–S bonds formation. This protocol has some advantages over the traditional methods in synthesizing 1H-isothiochromenes in terms of stable and easy available coupling substrates, simple and one-pot operation, step and atom economy, and highly unique sulfur-containing heterocyclic products.
{"title":"Synthesis of 1H-Isothiochromenes by Regioselective C–C and C–S Bonds Formation of Enaminothiones with Alkynes under Rhodium Catalysis","authors":"Kelu Yan, Yuhang Sun, Jiangwei Wen, Qiuyun Li, Xinming Yu, Wenxu Shang, Xiu Wang","doi":"10.1039/d5cc01269d","DOIUrl":"https://doi.org/10.1039/d5cc01269d","url":null,"abstract":"The rhodium-catalyzed sulfur-directed C–H bond activation and tandem cyclization of enaminothiones with alkynes proceed efficiently. Most products of 1H-isothiochromenes with various substituents are achieved in good yields by regioselective C–C and C–S bonds formation. This protocol has some advantages over the traditional methods in synthesizing 1H-isothiochromenes in terms of stable and easy available coupling substrates, simple and one-pot operation, step and atom economy, and highly unique sulfur-containing heterocyclic products.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"41 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853831","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}
Sahil Thakur, Ayush Badoni, Samriti Sharma, A. Savoyant, Hendrik Christoffel Swart, Mikhael Bechelany, Andrej Kuznetsov, Jai Prakash
We report on facile hydrothermal synthesis of 2H and 1T/2H mixed-phase MoS2 nanosheets using different organic sulfur precursors with varying sulfur release tendencies. 1T/2H MoS2 demonstrated direct solar light-driven photocatalysis and adsorption recyclability, attributed to phase synergy and improved charge separation.
{"title":"Facile Synthesis of Mixed Phase 1T/2H-MoS2 Heterostructured Nanosheets with Highly Efficient Solar Light-Driven Photocatalyst and Recyclable Adsorbent","authors":"Sahil Thakur, Ayush Badoni, Samriti Sharma, A. Savoyant, Hendrik Christoffel Swart, Mikhael Bechelany, Andrej Kuznetsov, Jai Prakash","doi":"10.1039/d5cc01431j","DOIUrl":"https://doi.org/10.1039/d5cc01431j","url":null,"abstract":"We report on facile hydrothermal synthesis of 2H and 1T/2H mixed-phase MoS2 nanosheets using different organic sulfur precursors with varying sulfur release tendencies. 1T/2H MoS2 demonstrated direct solar light-driven photocatalysis and adsorption recyclability, attributed to phase synergy and improved charge separation.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"6 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853830","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}
Matrix thickness surrounding PbS colloidal quantum dots (CQDs) significantly influences charge transport in photovoltaic devices. Through an anchoring and post-depositional-growth strategy utilizing thiazoline-2-thiol (TT), this study achieves reduced matrix thickness and strengthened inter-dot coupling. These improvements elevate the power conversion efficiency from 12.1% to 13.6%.
{"title":"Anchoring and Post-Depositional Growth Enables Matrix Manipulation of PbS QD Inks and Efficient Solar Cells","authors":"Haotian Gao, Leliang Song, Kunyuan Lu, Qingda Chang, Haoyu Zhao, Xiaobo Ding, Qianqian Lin, Chuang Zhang, Zeke Liu, Wanli Ma","doi":"10.1039/d5cc01816a","DOIUrl":"https://doi.org/10.1039/d5cc01816a","url":null,"abstract":"Matrix thickness surrounding PbS colloidal quantum dots (CQDs) significantly influences charge transport in photovoltaic devices. Through an anchoring and post-depositional-growth strategy utilizing thiazoline-2-thiol (TT), this study achieves reduced matrix thickness and strengthened inter-dot coupling. These improvements elevate the power conversion efficiency from 12.1% to 13.6%.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"17 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853835","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}
Mitochondrial autophagy is closely related to abnormal NAD(P)H and pH. Here, we synthesized a dual-response fluorescent probe with high selectivity for NAD(P)H and sensitivity for physiological pH range, for simultaneous imaging analysis of mitochondrial NAD(P)H and pH, holding potential as a novel tool for understanding mitochondria-associated diseases.
{"title":"A dual-response fluorescent probe Rh-O-QL for simultaneous monitoring NAD(P)H and pH during mitochondrial autophagy","authors":"Liandi Guan, Wanting Hu, Shiyu Zhang, Yongjian Ai, Qionglin Liang","doi":"10.1039/d5cc00961h","DOIUrl":"https://doi.org/10.1039/d5cc00961h","url":null,"abstract":"Mitochondrial autophagy is closely related to abnormal NAD(P)H and pH. Here, we synthesized a dual-response fluorescent probe with high selectivity for NAD(P)H and sensitivity for physiological pH range, for simultaneous imaging analysis of mitochondrial NAD(P)H and pH, holding potential as a novel tool for understanding mitochondria-associated diseases.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"30 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143846989","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}
The electrocatalytic conversion of wastewater nitrate (NO3-) to ammonia (NH3) under industrial-grade current densities at ambient conditions presents a sustainable alternative to the energy-intensive Haber-Bosch process, yet remains fundamentally challenging. Here, a highly efficient NO3- to NH3 electrocatalyst with single Fe atoms dispersing on graphdiyne (GDY) is constructed through an in-situ growth method. Experimental analysis demonstrates the formation of high-density atomic active sites on GDY, ensuring the high intrinsic activity of the electrocatalyst. Besides, the newly formed sp-C~Fe chemical bonds bridged GDY and Fe atoms provides a well-defined channel for selectively and efficiently transferring electrons from the active sites to the reactants/key intermediates, allowing for the selective NO3- activation and efficient protonation. This atomic-scale electronic modulation enables exceptional nitrate reduction performance, achieving record-high Faradaic efficiency (40.17%) and ammonia yield (106.65 μmol h⁻¹ cm⁻²) while maintaining operational stability.
在工业级电流密度的环境条件下，通过电催化将废水中的硝酸盐（NO3-）转化为氨气（NH3），是高能耗的哈伯-博什工艺的一种可持续替代方法，但从根本上讲仍具有挑战性。本文通过一种原位生长方法，构建了一种在石墨二乙烯（GDY）上分散有单个铁原子的高效 NO3- to NH3 电催化剂。实验分析表明，GDY 上形成了高密度的原子活性位点，确保了电催化剂的高内在活性。此外，新形成的 sp-C~Fe 化学键将 GDY 和铁原子桥接在一起，为电子从活性位点选择性地高效转移到反应物/关键中间产物提供了明确的通道，从而实现了选择性 NO3- 活化和高效质子化。这种原子尺度的电子调制实现了卓越的硝酸盐还原性能，达到了创纪录的高法拉第效率（40.17%）和氨产量（106.65 μmol h-¹ cm-²），同时保持了运行稳定性。
{"title":"Single-Atom Fe Anchored Graphdiyne for High-Efficiency Nitrate-to-Ammonia Conversion at Ambient Conditions","authors":"Jiayu Yan, Lu Qi, Zhiqiang Zheng, Zhaoyang Chen, Qi Wang, Yurui Xue","doi":"10.1039/d5cc01394a","DOIUrl":"https://doi.org/10.1039/d5cc01394a","url":null,"abstract":"The electrocatalytic conversion of wastewater nitrate (NO3-) to ammonia (NH3) under industrial-grade current densities at ambient conditions presents a sustainable alternative to the energy-intensive Haber-Bosch process, yet remains fundamentally challenging. Here, a highly efficient NO3- to NH3 electrocatalyst with single Fe atoms dispersing on graphdiyne (GDY) is constructed through an in-situ growth method. Experimental analysis demonstrates the formation of high-density atomic active sites on GDY, ensuring the high intrinsic activity of the electrocatalyst. Besides, the newly formed sp-C~Fe chemical bonds bridged GDY and Fe atoms provides a well-defined channel for selectively and efficiently transferring electrons from the active sites to the reactants/key intermediates, allowing for the selective NO3- activation and efficient protonation. This atomic-scale electronic modulation enables exceptional nitrate reduction performance, achieving record-high Faradaic efficiency (40.17%) and ammonia yield (106.65 μmol h⁻¹ cm⁻²) while maintaining operational stability.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"9 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143846911","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}
Shintaro Yoshida, William James Movick, Keisuke Obata, Kazuhiro Takanabe
The oxidative coupling of methane (OCM) was investigated using various alkali metal salts supported on SiO2. The addition of H₂O enhances both the methane conversion rate and selectivity across all alkali metal salts, which suggests there is an OH-radical-mediated pathway that is facilitated by the surface formation of alkali peroxide. To explain the observed experimental differences, we explored the interactive energetics of alkali–anion pairs with a particular focus on the stabilization of alkali peroxide intermediates by anion species. Anion polarizability is indicative of the alkali ion's degree of freedom and positively correlated with the catalytic performance due to formation capability of catalytic alkali peroxide species. This insight highlights the critical role of the reaction of surface alkali peroxide with H₂O as a key elementary step in OCM.
{"title":"Systematic exploration of alkali–anion pairs for descriptor identification in OH-mediated methane coupling","authors":"Shintaro Yoshida, William James Movick, Keisuke Obata, Kazuhiro Takanabe","doi":"10.1039/d5cc01090j","DOIUrl":"https://doi.org/10.1039/d5cc01090j","url":null,"abstract":"The oxidative coupling of methane (OCM) was investigated using various alkali metal salts supported on SiO2. The addition of H₂O enhances both the methane conversion rate and selectivity across all alkali metal salts, which suggests there is an OH-radical-mediated pathway that is facilitated by the surface formation of alkali peroxide. To explain the observed experimental differences, we explored the interactive energetics of alkali–anion pairs with a particular focus on the stabilization of alkali peroxide intermediates by anion species. Anion polarizability is indicative of the alkali ion's degree of freedom and positively correlated with the catalytic performance due to formation capability of catalytic alkali peroxide species. This insight highlights the critical role of the reaction of surface alkali peroxide with H₂O as a key elementary step in OCM.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"24 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832324","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}
We present a simple mixed-linker strategy to enhance the photocatalytic oxidation activity and stability of covalent organic frameworks semiconductors. The TpTfbPa-COF, featuring an unconventional reversed AA-stacking structure with both imine and ketoamine linkages, exhibits excellent structural stability and superior photocatalytic performance compared to the fully imine-linked TfbPa-COF and the fully ketoamine-linked TpPa-COF.
{"title":"Mixed-Linker Strategy in Covalent Organic Frameworks for Enhanced Sunlight-Driven Photocatalytic Oxidation Activity and Stability","authors":"Jikuan Qiu, Xinchun Xue, Kangna Zhang, Xiaoxin Tian, Wenrui Wan, Tingting Fan, Zhiyong Li, Huiyong Wang, Yuling Zhao","doi":"10.1039/d5cc01192b","DOIUrl":"https://doi.org/10.1039/d5cc01192b","url":null,"abstract":"We present a simple mixed-linker strategy to enhance the photocatalytic oxidation activity and stability of covalent organic frameworks semiconductors. The TpTfbPa-COF, featuring an unconventional reversed AA-stacking structure with both imine and ketoamine linkages, exhibits excellent structural stability and superior photocatalytic performance compared to the fully imine-linked TfbPa-COF and the fully ketoamine-linked TpPa-COF.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"27 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832203","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}
Alexander Mondragón-Díaz, Steven P. Kelley, Nilay Hazari, Wesley H. Bernskoetter
The synthesis of a new air-stable SPS pincer ligand that supports a Ru catalyst for CO2 hydrogenation to formate is described. This rare S-donor based pincer system gives higher activity compared to related PNP supported Ru catalysts and is less dependent on Lewis acidic Li co-catalysts for achieving high turnover numbers. The SPS ligated Ru catalyst is also active for N-formylation of amines with CO2.
{"title":"A highly active sulfur based pincer ruthenium catalyst for CO2 hydrogenation","authors":"Alexander Mondragón-Díaz, Steven P. Kelley, Nilay Hazari, Wesley H. Bernskoetter","doi":"10.1039/d5cc01194a","DOIUrl":"https://doi.org/10.1039/d5cc01194a","url":null,"abstract":"The synthesis of a new air-stable SPS pincer ligand that supports a Ru catalyst for CO<small><sub>2</sub></small> hydrogenation to formate is described. This rare S-donor based pincer system gives higher activity compared to related PNP supported Ru catalysts and is less dependent on Lewis acidic Li co-catalysts for achieving high turnover numbers. The SPS ligated Ru catalyst is also active for <em>N</em>-formylation of amines with CO<small><sub>2</sub></small>.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"3 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832325","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}
The incorporation of bromide ions (Br–) as electrolyte additives fundamentally alters the reaction mechanism of alkaline Ag-Zn batteries, effectively suppressing the shuttle effect and mitigating cathode dissolution. Furthermore, a self-supporting polymer-based silver cathode has been engineered to accommodate volume changes during cycling, thereby minimizing capacity degradation. As a result, the halide-mediated Ag-Zn battery demonstrates exceptional cycling stability over 330 cycles, delivering a high Coulombic efficiency exceeding 99.3% with excellent capacity retention. Notably, the system achieves a high areal capacity of 2.3 mAh cm–², highlighting its potential for practical applications in high-performance rechargeable batteries.
{"title":"Halide-mediated Ag-Zn batteries in alkaline electrolytes","authors":"Jiajie Shen, Wenjiao Ma, Jianhui Jin, Huijian Wang, Xiao Liang","doi":"10.1039/d5cc01489a","DOIUrl":"https://doi.org/10.1039/d5cc01489a","url":null,"abstract":"The incorporation of bromide ions (Br–) as electrolyte additives fundamentally alters the reaction mechanism of alkaline Ag-Zn batteries, effectively suppressing the shuttle effect and mitigating cathode dissolution. Furthermore, a self-supporting polymer-based silver cathode has been engineered to accommodate volume changes during cycling, thereby minimizing capacity degradation. As a result, the halide-mediated Ag-Zn battery demonstrates exceptional cycling stability over 330 cycles, delivering a high Coulombic efficiency exceeding 99.3% with excellent capacity retention. Notably, the system achieves a high areal capacity of 2.3 mAh cm–², highlighting its potential for practical applications in high-performance rechargeable batteries.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"23 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143831988","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}
Monika Halat, Magdalena Klimek-Chodacka, Agnieszka Domagała, Grzegorz Zając, Tomasz Oleszkiewicz, Josef Kapitán, Rafal Baranski
Chiroptical studies of the SpyCas9 protein are extremely rare. Nondestructive methods are needed to characterize its active ribonucleoprotein form. Using Raman optical activity (ROA) and circularly polarized luminescence (CPL), we present a new approach to detect key biomolecules involved in CRISPR-Cas technology while preserving their original nucleolytic activity.
{"title":"Chiral sensing combined with nuclease activity assay to track Cas9 dynamics in solution: ROA and CPL study","authors":"Monika Halat, Magdalena Klimek-Chodacka, Agnieszka Domagała, Grzegorz Zając, Tomasz Oleszkiewicz, Josef Kapitán, Rafal Baranski","doi":"10.1039/d5cc00971e","DOIUrl":"https://doi.org/10.1039/d5cc00971e","url":null,"abstract":"Chiroptical studies of the SpyCas9 protein are extremely rare. Nondestructive methods are needed to characterize its active ribonucleoprotein form. Using Raman optical activity (ROA) and circularly polarized luminescence (CPL), we present a new approach to detect key biomolecules involved in CRISPR-Cas technology while preserving their original nucleolytic activity.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"67 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832067","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}
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