Shuda Liu, Na Dong, Siyuan Wang, Shuyun Meng, Yuqing Li, Dong Liu, Tianyan You
Photoelectrocatalysis plays a vital role in sustainable energy conversion technologies. Yet, the understanding of these reaction mechanisms remains incomplete because of the complexity of photoelectrochemical interfaces and the trace amounts of interfacial substances. Introducing photoexcitation into electrochemical surface-enhanced Raman spectroscopy (EC-SERS) enable monitoring reaction processes of photoelectrocatalysis by the integration of photo/electrochemical characterization and Raman spectroscopy. In this review, we classify this methodology as photo-excited EC-SERS. We first introduce the fundamental aspects of photo-excited EC-SERS, covering principles, substrate materials, and experimental setups. Then, the application of photo-excited EC-SERS in key photoelectrocatalytic reactions, such as water splitting, CO2 reduction, and organic oxidation, is focused. Combined with practical cases, the values of photo-excited EC-SERS in photoelectrocatalytic processes are discussed, including: 1) understand charge transfer interfacial processes; 2) capture transient intermediates in the vibration fingerprints; 3) analyze the mechanism and pathway of photoelectrocatalytic reactions. In addition, we examine the application of photo-excited EC-SERS in biosensors. Finally, we point out the challenges of photo-excited EC-SERS in monitoring photoelectrocatalytic reaction, which we believe will motivate researchers to take advantage of the technology's versatility and applicability to help sustainable energy development.
{"title":"Photo-excited electrochemical surface-enhanced Raman spectroscopy: In situ/Operando insights into photoelectrocatalytic interfaces","authors":"Shuda Liu, Na Dong, Siyuan Wang, Shuyun Meng, Yuqing Li, Dong Liu, Tianyan You","doi":"10.1039/d5cc01605c","DOIUrl":"https://doi.org/10.1039/d5cc01605c","url":null,"abstract":"Photoelectrocatalysis plays a vital role in sustainable energy conversion technologies. Yet, the understanding of these reaction mechanisms remains incomplete because of the complexity of photoelectrochemical interfaces and the trace amounts of interfacial substances. Introducing photoexcitation into electrochemical surface-enhanced Raman spectroscopy (EC-SERS) enable monitoring reaction processes of photoelectrocatalysis by the integration of photo/electrochemical characterization and Raman spectroscopy. In this review, we classify this methodology as photo-excited EC-SERS. We first introduce the fundamental aspects of photo-excited EC-SERS, covering principles, substrate materials, and experimental setups. Then, the application of photo-excited EC-SERS in key photoelectrocatalytic reactions, such as water splitting, CO2 reduction, and organic oxidation, is focused. Combined with practical cases, the values of photo-excited EC-SERS in photoelectrocatalytic processes are discussed, including: 1) understand charge transfer interfacial processes; 2) capture transient intermediates in the vibration fingerprints; 3) analyze the mechanism and pathway of photoelectrocatalytic reactions. In addition, we examine the application of photo-excited EC-SERS in biosensors. Finally, we point out the challenges of photo-excited EC-SERS in monitoring photoelectrocatalytic reaction, which we believe will motivate researchers to take advantage of the technology's versatility and applicability to help sustainable energy development.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"218 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144260578","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 catalytic activity of titanium silicalite-1 (TS-1) in cyclohexanone ammoximation is controlled by the intracrystalline diffusion limitations due to the hydrogen-bonding interactions between the internal Si-OH groups in TS-1 and H2O2, NH3, and NH2OH, while these Si-OH groups can be effectively annealed by an ultraviolet-assisted heat post-treatment, resulting in enhanced activity.
{"title":"Insights into the intracrystalline diffusion limitations of TS-1 in catalytic cyclohexanone ammoximation: effects of the Si-OH groups inside the zeotype micropores.","authors":"Chunhui Xu, Qiang Zhou, Xinqing Lu, Zhonggang Duan, Bitao Xu, Chaoqun Zhang, Weidong Zhu","doi":"10.1039/d5cc02408k","DOIUrl":"https://doi.org/10.1039/d5cc02408k","url":null,"abstract":"<p><p>The catalytic activity of titanium silicalite-1 (TS-1) in cyclohexanone ammoximation is controlled by the intracrystalline diffusion limitations due to the hydrogen-bonding interactions between the internal Si-OH groups in TS-1 and H<sub>2</sub>O<sub>2</sub>, NH<sub>3</sub>, and NH<sub>2</sub>OH, while these Si-OH groups can be effectively annealed by an ultraviolet-assisted heat post-treatment, resulting in enhanced activity.</p>","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":" ","pages":""},"PeriodicalIF":4.3,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144256850","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}
Pulakesh Borah, Diksha J. Baruah, Rituparna Duarah, Manash Ranjan Das
Natural enzymes are the driving force behind essential biochemical reactions in vitro and in vivo, celebrated for their unmatched catalytic efficiency, remarkable bioactivity, and pinpoint accuracy. Yet, their practical application is constrained by prohibitive costs, limited stability, and low reusability. Two-dimensional (2D) nanomaterials have emerged as promising nanozymes, mimicking enzyme functions through their unique properties, including atomic-scale thickness, high surface area, and tunable electronic structures. These features enable superior stability, cost-effectiveness, and adaptability for diverse biomedical and environmental applications. This article examines recent advancements in 2D nanomaterials functionalized with metallic nanoparticles, single atoms, metal oxides, quantum dots, etc. focusing on their catalytic mechanisms, enzyme-mimetic activities, and synthesis methods. It will delve into biomedical applications such as biosensing, bioimaging, therapeutic diagnostics, and oxidative stress management, alongside environmental uses including pollutant sensing and remediation strategies. Future directions for developing robust 2D nanozymes to tackle challenges in healthcare and environmental sustainability will also be highlighted.
{"title":"2D Nanozymes: Bioinspired Innovations for Healthcare and Environmental Applications","authors":"Pulakesh Borah, Diksha J. Baruah, Rituparna Duarah, Manash Ranjan Das","doi":"10.1039/d5cc00180c","DOIUrl":"https://doi.org/10.1039/d5cc00180c","url":null,"abstract":"Natural enzymes are the driving force behind essential biochemical reactions in vitro and in vivo, celebrated for their unmatched catalytic efficiency, remarkable bioactivity, and pinpoint accuracy. Yet, their practical application is constrained by prohibitive costs, limited stability, and low reusability. Two-dimensional (2D) nanomaterials have emerged as promising nanozymes, mimicking enzyme functions through their unique properties, including atomic-scale thickness, high surface area, and tunable electronic structures. These features enable superior stability, cost-effectiveness, and adaptability for diverse biomedical and environmental applications. This article examines recent advancements in 2D nanomaterials functionalized with metallic nanoparticles, single atoms, metal oxides, quantum dots, etc. focusing on their catalytic mechanisms, enzyme-mimetic activities, and synthesis methods. It will delve into biomedical applications such as biosensing, bioimaging, therapeutic diagnostics, and oxidative stress management, alongside environmental uses including pollutant sensing and remediation strategies. Future directions for developing robust 2D nanozymes to tackle challenges in healthcare and environmental sustainability will also be highlighted.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"170 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144252202","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 adsorption of boron on Fe3O4 nanoparticles was studied by metal doping. The changed values in oxygen binding energy of doped Fe3O4 were found to negatively correlate to boron adsorption capacity, where Mg and Zn doped Fe3O4 exhibited an obvious increase by 60% and 15% respectively. The adsorption of boron might preceed by nucleophilic attack of hydoxyl group on magnetite to vacant orbit of boron center.
{"title":"Mechanism of Metal Doping in Regulating Boron Adsorption Performance of Fe3O4 Nanoparticles","authors":"Jiang Yumeng, Yang Annie, Huiqun Ju, Tian yu Li, Jiafei Lyu, Xianghai Guo","doi":"10.1039/d5cc02174j","DOIUrl":"https://doi.org/10.1039/d5cc02174j","url":null,"abstract":"The adsorption of boron on Fe<small><sub>3</sub></small>O<small><sub>4</sub></small> nanoparticles was studied by metal doping. The changed values in oxygen binding energy of doped Fe<small><sub>3</sub></small>O<small><sub>4</sub></small> were found to negatively correlate to boron adsorption capacity, where Mg and Zn doped Fe<small><sub>3</sub></small>O<small><sub>4</sub></small> exhibited an obvious increase by 60% and 15% respectively. The adsorption of boron might preceed by nucleophilic attack of hydoxyl group on magnetite to vacant orbit of boron center.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"44 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144252492","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}
Louxi Chen, Chao-Han Zhang, Junyang Liu, Chuang-Chuang Li
Herein, we report the asymmetric synthesis of venezuelaene's tetracyclic core, featuring a diastereoselective IMDA to construct the [6-5-6-7] skeleton, followed by stereoselective Simmons-Smith reaction, cyclopropane ring-opening, and Wolff rearrangement to install the challenging trans-fused [5-5] ring system.
{"title":"Asymmetric synthesis of venezuelaene’s core with a trans-fused [5-5] ring system","authors":"Louxi Chen, Chao-Han Zhang, Junyang Liu, Chuang-Chuang Li","doi":"10.1039/d5cc02504d","DOIUrl":"https://doi.org/10.1039/d5cc02504d","url":null,"abstract":"Herein, we report the asymmetric synthesis of venezuelaene's tetracyclic core, featuring a diastereoselective IMDA to construct the [6-5-6-7] skeleton, followed by stereoselective Simmons-Smith reaction, cyclopropane ring-opening, and Wolff rearrangement to install the challenging trans-fused [5-5] ring system.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"20 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144252640","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}
Jinsuo Zhang, Chao Wang, Xinlong Chen, Ge Qu, Shiqi Li, Wang Wan, Yunhui Huang
A rapid room-temperature repair method for spent LiFePO4 (LFP) powders and electrodes is presented, achieving restoration within 10 minutes. The process facilitates lithiation kinetics through redox reactions between iodide and triiodide ions and supports reuse. This clean, low-energy method provides promising technology for efficiently recycling LFP cathodes.
{"title":"Rapid Room-Temperature Repair of Spent Lithium Iron Phosphate via Redox Mediators","authors":"Jinsuo Zhang, Chao Wang, Xinlong Chen, Ge Qu, Shiqi Li, Wang Wan, Yunhui Huang","doi":"10.1039/d5cc02549d","DOIUrl":"https://doi.org/10.1039/d5cc02549d","url":null,"abstract":"A rapid room-temperature repair method for spent LiFePO4 (LFP) powders and electrodes is presented, achieving restoration within 10 minutes. The process facilitates lithiation kinetics through redox reactions between iodide and triiodide ions and supports reuse. This clean, low-energy method provides promising technology for efficiently recycling LFP cathodes.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"215 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144252647","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}
Jian-Chen Wu, Heng Yang, Zhi-Wen Luo, Fei-Yang Cao, Yan Pan, Hua Xiao, Jian-Jun Dai
Here we present a new method for synthesizing amide hemiaminal esters through the direct N-methyl C−H esterification of O-tosyl hydroxamates. This approach demonstrates good tolerance for a variety of functional groups and operates under mild, transition-metal-free conditions, thus providing an accessible and effective pathway to hemiaminal esters.
{"title":"Direct N-methyl C−H esterification of O-tosyl hydroxamates to enable facile synthesis of hemiaminal esters†","authors":"Jian-Chen Wu, Heng Yang, Zhi-Wen Luo, Fei-Yang Cao, Yan Pan, Hua Xiao, Jian-Jun Dai","doi":"10.1039/d5cc02570b","DOIUrl":"https://doi.org/10.1039/d5cc02570b","url":null,"abstract":"Here we present a new method for synthesizing amide hemiaminal esters through the direct N-methyl C−H esterification of O-tosyl hydroxamates. This approach demonstrates good tolerance for a variety of functional groups and operates under mild, transition-metal-free conditions, thus providing an accessible and effective pathway to hemiaminal esters.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"559 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144252490","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}
Less stable acceptor-type cyclopropenes are prepared and isolated via blue light promoted photolysis of vinyldiazo compounds. The kinetic measurements indicated that their half-lives were influenced by the concentration, temperature and solvent.
{"title":"Synthesis and Isolation of Less Stable Cyclopropene-1-carboxylates","authors":"Jiahao Ling, Jiabao Tian, Xinhai Zhu, Lei Zhou","doi":"10.1039/d5cc02673c","DOIUrl":"https://doi.org/10.1039/d5cc02673c","url":null,"abstract":"Less stable acceptor-type cyclopropenes are prepared and isolated via blue light promoted photolysis of vinyldiazo compounds. The kinetic measurements indicated that their half-lives were influenced by the concentration, temperature and solvent.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"43 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144252643","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}
Tao Hu, Yuexia Yang, Bijia Zhou, Zhaoming Chen, Fapu Wu, Hu Xiong
β-Galactosidase (GAL) is a lysosomal protease implicated in cellular senescence and various malignant cancers. However, bioluminescent probes for specific GAL detection remain scarce, and their applications are largely limited to transgenic models expressing firefly luciferase (fLuc). Herein, we report a bioluminescent probe, β-Luc, for detecting GAL activity in nontransgenic cells and tumor-bearing mice. β-Luc exhibited high selectivity toward GAL, with a limit of detection of 8.5 mU/mL. Combined with fLuc mRNA-loaded lipid nanoparticles, β-Luc was able to sensitively monitor GAL activity in vitro and in vivo. Based on this strategy, intestinal metastatic tumors were precisely delineated, showing 25.2-fold higher bioluminescence intensity in nontransgenic tumor-bearing mice.
{"title":"β-Galactosidase-activated bioluminescent probe for in vivo tumor imaging","authors":"Tao Hu, Yuexia Yang, Bijia Zhou, Zhaoming Chen, Fapu Wu, Hu Xiong","doi":"10.1039/d5cc02244d","DOIUrl":"https://doi.org/10.1039/d5cc02244d","url":null,"abstract":"β-Galactosidase (GAL) is a lysosomal protease implicated in cellular senescence and various malignant cancers. However, bioluminescent probes for specific GAL detection remain scarce, and their applications are largely limited to transgenic models expressing firefly luciferase (fLuc). Herein, we report a bioluminescent probe, β-Luc, for detecting GAL activity in nontransgenic cells and tumor-bearing mice. β-Luc exhibited high selectivity toward GAL, with a limit of detection of 8.5 mU/mL. Combined with fLuc mRNA-loaded lipid nanoparticles, β-Luc was able to sensitively monitor GAL activity in vitro and in vivo. Based on this strategy, intestinal metastatic tumors were precisely delineated, showing 25.2-fold higher bioluminescence intensity in nontransgenic tumor-bearing mice.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"37 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144252651","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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