Pub Date : 2024-10-18DOI: 10.1016/j.cclet.2024.110566
Yu Zhang , Weifeng Lin
Using different external stimuli to control interfacial friction, rather than just pursuing low friction, is a highly attractive research regime due to its economic and scientific importance. One option to achieve such a goal is to use external stimuli that modulate the energy dissipation pathways. In particular, electric stimuli such as surface potential has gained remarkable interest for two reasons: Electrotunable friction has the potential for real-time, in situ manipulation of friction, and external electric stimuli is relatively easy to apply and to remove for reversible change. In this review, we explore the emerging research area of electrotunable friction mainly under the boundary lubrication situation, when the contacting surfaces are separated by a molecularly thin layer, reviewing typical achievements from experiments using electrochemical atomic force microscopy and modified surface force balances, as well as molecular dynamics simulations. Additionally, we explore the theoretical and practical challenges that may need to be tackled in the future.
{"title":"Electrotunable interfacial friction: A brief review","authors":"Yu Zhang , Weifeng Lin","doi":"10.1016/j.cclet.2024.110566","DOIUrl":"10.1016/j.cclet.2024.110566","url":null,"abstract":"<div><div>Using different external stimuli to control interfacial friction, rather than just pursuing low friction, is a highly attractive research regime due to its economic and scientific importance. One option to achieve such a goal is to use external stimuli that modulate the energy dissipation pathways. In particular, electric stimuli such as surface potential has gained remarkable interest for two reasons: Electrotunable friction has the potential for real-time, <em>in situ</em> manipulation of friction, and external electric stimuli is relatively easy to apply and to remove for reversible change. In this review, we explore the emerging research area of electrotunable friction mainly under the boundary lubrication situation, when the contacting surfaces are separated by a molecularly thin layer, reviewing typical achievements from experiments using electrochemical atomic force microscopy and modified surface force balances, as well as molecular dynamics simulations. Additionally, we explore the theoretical and practical challenges that may need to be tackled in the future.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 4","pages":"Article 110566"},"PeriodicalIF":9.4,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143149442","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-17DOI: 10.1016/j.cclet.2024.110496
Jiliang Deng , Guoliang Shi , Zhihang Ye , Quan Xiao , Xiaoting Zhang , Lei Ren , Fangyu Yang , Miao Wang
Histopathological analysis of chronic wounds is crucial for clinicians to accurately assess wound healing progress and detect potential malignancy. However, traditional pathological tissue sections require specific staining procedures involving carcinogenic chemicals. This study proposes an interdisciplinary approach merging materials science, medicine, and artificial intelligence (AI) to develop a virtual staining technique and intelligent evaluation model based on deep learning for chronic wound tissue pathology. This innovation aims to enhance clinical diagnosis and treatment by offering personalized AI-driven therapeutic strategies. By establishing a mouse model of chronic wounds and using a series of hydrogel wound dressings, tissue pathology sections were periodically collected for manual staining and healing assessment. We focused on leveraging the pix2pix image translation framework within deep learning networks. Through CNN models implemented in Python using PyTorch, our study involves learning and feature extraction for region segmentation of pathological slides. Comparative analysis between virtual staining and manual staining results, along with healing diagnosis conclusions, aims to optimize AI models. Ultimately, this approach integrates new metrics such as image recognition, quantitative analysis, and digital diagnostics to formulate an intelligent wound assessment model, facilitating smart monitoring and personalized treatment of wounds. In blind evaluation by pathologists, minimal disparities were found between virtual and conventional histologically stained images of murine wound tissue. The evaluation used pathologists' average scores on real stained images as a benchmark. The scores for virtual stained images were 71.1 % for cellular features, 75.4 % for tissue structures, and 77.8 % for overall assessment. Metrics such as PSNR (20.265) and SSIM (0.634) demonstrated our algorithms' superior performance over existing networks. Eight pathological features such as epidermis, hair follicles, and granulation tissue can be accurately identified, and the images were found to be more faithful to the actual tissue feature distribution when compared to manually annotated data.
{"title":"Unveiling and swift diagnosing chronic wound healing with artificial intelligence assistance","authors":"Jiliang Deng , Guoliang Shi , Zhihang Ye , Quan Xiao , Xiaoting Zhang , Lei Ren , Fangyu Yang , Miao Wang","doi":"10.1016/j.cclet.2024.110496","DOIUrl":"10.1016/j.cclet.2024.110496","url":null,"abstract":"<div><div>Histopathological analysis of chronic wounds is crucial for clinicians to accurately assess wound healing progress and detect potential malignancy. However, traditional pathological tissue sections require specific staining procedures involving carcinogenic chemicals. This study proposes an interdisciplinary approach merging materials science, medicine, and artificial intelligence (AI) to develop a virtual staining technique and intelligent evaluation model based on deep learning for chronic wound tissue pathology. This innovation aims to enhance clinical diagnosis and treatment by offering personalized AI-driven therapeutic strategies. By establishing a mouse model of chronic wounds and using a series of hydrogel wound dressings, tissue pathology sections were periodically collected for manual staining and healing assessment. We focused on leveraging the pix2pix image translation framework within deep learning networks. Through CNN models implemented in Python using PyTorch, our study involves learning and feature extraction for region segmentation of pathological slides. Comparative analysis between virtual staining and manual staining results, along with healing diagnosis conclusions, aims to optimize AI models. Ultimately, this approach integrates new metrics such as image recognition, quantitative analysis, and digital diagnostics to formulate an intelligent wound assessment model, facilitating smart monitoring and personalized treatment of wounds. In blind evaluation by pathologists, minimal disparities were found between virtual and conventional histologically stained images of murine wound tissue. The evaluation used pathologists' average scores on real stained images as a benchmark. The scores for virtual stained images were 71.1 % for cellular features, 75.4 % for tissue structures, and 77.8 % for overall assessment. Metrics such as PSNR (20.265) and SSIM (0.634) demonstrated our algorithms' superior performance over existing networks. Eight pathological features such as epidermis, hair follicles, and granulation tissue can be accurately identified, and the images were found to be more faithful to the actual tissue feature distribution when compared to manually annotated data.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 3","pages":"Article 110496"},"PeriodicalIF":9.4,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143318382","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-16DOI: 10.1016/j.cclet.2024.110554
Yubin Feng , Weihang Zhu , Xinting Yang , Zhe Yang , Chenke Wei , Yukai Guo , Andrew K. Whittaker , Chun Shen , Yue Zhao , Wenrui Qu , Bai Yang , Quan Lin
Gel-based sensors have provided unprecedented opportunities for bioelectric monitoring. Until now, sensors for underwater applicants have remained a notable challenge, as most sensors work effectively in air but swell underwater leading to functional failure. Herein, we introduce an innovative amphibian-inspired high-performance ionogel, where multiple supramolecular interactions in the ionogel's network confer good stretchability, elasticity, conductivity, and the hydrophobic C-F bonds play a key role in diminishing water molecule hydration and provide outstanding environmental stability. These unique properties of ionogels make them suitable as wearable amphibious flexible sensors, and the sensors are capable of highly sensitive and stable human motion monitoring in air and underwater. Integration of the designed sensor into an artificial intelligence drowning alarm system, which recognizes the swimmer's movement status by monitoring the amplitude and frequency, especially in the drowning status for real-time alarms. This work provides novel strategies for motion recognition and hazard monitoring in amphibious environments, meeting the new generation of wearable sensors.
{"title":"Amphibian-inspired conductive ionogel stabilizing in air/water as a wearable amphibious flexible sensor for drowning alarms","authors":"Yubin Feng , Weihang Zhu , Xinting Yang , Zhe Yang , Chenke Wei , Yukai Guo , Andrew K. Whittaker , Chun Shen , Yue Zhao , Wenrui Qu , Bai Yang , Quan Lin","doi":"10.1016/j.cclet.2024.110554","DOIUrl":"10.1016/j.cclet.2024.110554","url":null,"abstract":"<div><div>Gel-based sensors have provided unprecedented opportunities for bioelectric monitoring. Until now, sensors for underwater applicants have remained a notable challenge, as most sensors work effectively in air but swell underwater leading to functional failure. Herein, we introduce an innovative amphibian-inspired high-performance ionogel, where multiple supramolecular interactions in the ionogel's network confer good stretchability, elasticity, conductivity, and the hydrophobic C-F bonds play a key role in diminishing water molecule hydration and provide outstanding environmental stability. These unique properties of ionogels make them suitable as wearable amphibious flexible sensors, and the sensors are capable of highly sensitive and stable human motion monitoring in air and underwater. Integration of the designed sensor into an artificial intelligence drowning alarm system, which recognizes the swimmer's movement status by monitoring the amplitude and frequency, especially in the drowning status for real-time alarms. This work provides novel strategies for motion recognition and hazard monitoring in amphibious environments, meeting the new generation of wearable sensors.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 4","pages":"Article 110554"},"PeriodicalIF":9.4,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143099323","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-16DOI: 10.1016/j.cclet.2024.110555
Shunyu Wang , Yanan Zhu , Yang Zhao , Wanli Nie , Hong Meng
Multiple donor-acceptor (D-A) combinations represent a promising category of thermally activated delayed fluorescence (TADF) materials, offering potential for superior efficiency and stability. However, current systems are predominantly composed of limited donor groups, primarily carbazole-based derivatives. In this work, we developed a series of D-A type materials incorporating helical π-expanded carbazole (CzNaph) and 7H-dinaphtho[1,8-bc:1′,8′-ef]azepine (AzNaph), alongside traditional carbazole, ranging from mono- to tetra-substituted configurations (Dn-A). Through systematic investigation of geometric and electronic structures, the number and positioning of multiple donors are confirmed with significant manipulations on charge transfer characteristics and the S1 state via steric effects. Density functional theory (DFT) calculations reveal that varying the number of π-extended donors within the acceptor framework produces emission colors from ultraviolet to red, providing a diverse range of emitters. Furthermore, the reduced reorganization energy of S1 observed in tetra-substituted Cz and CzNaph, as well as MonoAzN, indicates lower structural relaxation, highlighting these materials' potential as stable luminescent candidates. This study underscores the importance of diverse composing units in achieving efficient and stable TADF emitters with multiple and hetero-donor configurations.
{"title":"Steric effects and electronic manipulation of multiple donors on S0/S1 transition of Dn-A emitters","authors":"Shunyu Wang , Yanan Zhu , Yang Zhao , Wanli Nie , Hong Meng","doi":"10.1016/j.cclet.2024.110555","DOIUrl":"10.1016/j.cclet.2024.110555","url":null,"abstract":"<div><div>Multiple donor-acceptor (D-A) combinations represent a promising category of thermally activated delayed fluorescence (TADF) materials, offering potential for superior efficiency and stability. However, current systems are predominantly composed of limited donor groups, primarily carbazole-based derivatives. In this work, we developed a series of D-A type materials incorporating helical <em>π</em>-expanded carbazole (CzNaph) and 7<em>H</em>-dinaphtho[1,8-<em>bc</em>:1′,8′-<em>ef</em>]azepine (AzNaph), alongside traditional carbazole, ranging from mono- to tetra-substituted configurations (D<sub>n</sub>-A). Through systematic investigation of geometric and electronic structures, the number and positioning of multiple donors are confirmed with significant manipulations on charge transfer characteristics and the S<sub>1</sub> state <em>via</em> steric effects. Density functional theory (DFT) calculations reveal that varying the number of <em>π</em>-extended donors within the acceptor framework produces emission colors from ultraviolet to red, providing a diverse range of emitters. Furthermore, the reduced reorganization energy of S<sub>1</sub> observed in tetra-substituted Cz and CzNaph, as well as MonoAzN, indicates lower structural relaxation, highlighting these materials' potential as stable luminescent candidates. This study underscores the importance of diverse composing units in achieving efficient and stable TADF emitters with multiple and hetero-donor configurations.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 4","pages":"Article 110555"},"PeriodicalIF":9.4,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143149444","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-15DOI: 10.1016/j.cclet.2024.110425
Huaixiang Yang , Miao-Miao Li , Aijun Zhang , Jiefei Guo , Yongqi Yu , Wei Ding
The tert-butyl nitrite as a bifunctional reagent mediated radical alkene difunctionalization has emerged as a powerful strategy for synthesis of structurally diverse oxime-containing compounds. However, the phosphorus-centered radical initiated transformations remain largely elusive. Herein, a visible-light-induced radical phosphinoyloximation of alkenes with secondary phosphine oxides and tert-butyl nitrite has been developed under photocatalyst- and metal-free conditions. This protocol features mild conditions, broad substrate scope, good functional tolerance, and operational simplicity, yielding a diverse array of α-phosphinoyl oximes in moderate to good yields with high stereoselectivities. The photomediated homolytic cleavage of ONO bond of tert-butyl nitrite generates the reactive tert-butoxyl radical and persistent NO radical to act as both HAT reagent and the source of oximes.
{"title":"Visible-light-induced photocatalyst- and metal-free radical phosphinoyloximation of alkenes with tert-butyl nitrite as bifunctional reagent","authors":"Huaixiang Yang , Miao-Miao Li , Aijun Zhang , Jiefei Guo , Yongqi Yu , Wei Ding","doi":"10.1016/j.cclet.2024.110425","DOIUrl":"10.1016/j.cclet.2024.110425","url":null,"abstract":"<div><div>The <em>tert</em>-butyl nitrite as a bifunctional reagent mediated radical alkene difunctionalization has emerged as a powerful strategy for synthesis of structurally diverse oxime-containing compounds. However, the phosphorus-centered radical initiated transformations remain largely elusive. Herein, a visible-light-induced radical phosphinoyloximation of alkenes with secondary phosphine oxides and <em>tert</em>-butyl nitrite has been developed under photocatalyst- and metal-free conditions. This protocol features mild conditions, broad substrate scope, good functional tolerance, and operational simplicity, yielding a diverse array of α-phosphinoyl oximes in moderate to good yields with high stereoselectivities. The photomediated homolytic cleavage of O<img>NO bond of <em>tert</em>-butyl nitrite generates the reactive <em>tert</em>-butoxyl radical and persistent NO radical to act as both HAT reagent and the source of oximes.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 3","pages":"Article 110425"},"PeriodicalIF":9.4,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143318525","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Herein, the Cu(III) synthesized from copper plating effluent was developed for the first time to evaluate the onsite degradation performance of heavy metal complexes in the wastewater, thus achieving the purpose of “treating waste with waste”. The results indicated that synthetic Cu(III) presented the excellent decomplexation performance for Cu(II)/Ni(II)-organic complexes. The removal efficiency of Cu(II)/Ni(II)-EDTA significantly increased with increasing Cu(III) dosage, and the degradation of Cu(II)/Ni(II)-EDTA by synthetic Cu(III) system displayed highly pH-dependent reactivity. The radical quencher experiments confirmed that Cu(III) direct oxidation were mainly involved in the degradation of Cu(II)-EDTA. Additionally, the continuous decarboxylation process was proven to be the main degradation pathway of Cu(II)-EDTA in Cu(III) system. The coexisting substances (SO42−, Cl− and fulvic acids) showed little impacts at low level for the removal of Cu(II)/Ni(II)-EDTA, while retarded the degradation of Cu(II)-EDTA slightly at high level, which features high selective oxidation. Encouragingly, it was also effective to remove Cu(II)/Ni(II)-EDTA from in treating actual Cu/Ni-containing wastewater through synthetic Cu(III) treatment.
{"title":"Synthetic Cu(III) from copper plating wastewater for onsite decomplexation of Cu(II)- and Ni(II)-organic complexes","authors":"Junyi Yu , Yin Cheng , Anhong Cai , Xianfeng Huang , Qingrui Zhang","doi":"10.1016/j.cclet.2024.110549","DOIUrl":"10.1016/j.cclet.2024.110549","url":null,"abstract":"<div><div>Herein, the Cu(III) synthesized from copper plating effluent was developed for the first time to evaluate the onsite degradation performance of heavy metal complexes in the wastewater, thus achieving the purpose of “treating waste with waste”. The results indicated that synthetic Cu(III) presented the excellent decomplexation performance for Cu(II)/Ni(II)-organic complexes. The removal efficiency of Cu(II)/Ni(II)-EDTA significantly increased with increasing Cu(III) dosage, and the degradation of Cu(II)/Ni(II)-EDTA by synthetic Cu(III) system displayed highly pH-dependent reactivity. The radical quencher experiments confirmed that Cu(III) direct oxidation were mainly involved in the degradation of Cu(II)-EDTA. Additionally, the continuous decarboxylation process was proven to be the main degradation pathway of Cu(II)-EDTA in Cu(III) system. The coexisting substances (SO<sub>4</sub><sup>2−</sup>, Cl<sup>−</sup> and fulvic acids) showed little impacts at low level for the removal of Cu(II)/Ni(II)-EDTA, while retarded the degradation of Cu(II)-EDTA slightly at high level, which features high selective oxidation. Encouragingly, it was also effective to remove Cu(II)/Ni(II)-EDTA from in treating actual Cu/Ni-containing wastewater through synthetic Cu(III) treatment.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 2","pages":"Article 110549"},"PeriodicalIF":9.4,"publicationDate":"2024-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142699589","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-10DOI: 10.1016/j.cclet.2024.110533
Xinlong Zheng , Zhongyun Shao , Jiaxin Lin , Qizhi Gao , Zongxian Ma , Yiming Song , Zhen Chen , Xiaodong Shi , Jing Li , Weifeng Liu , Xinlong Tian , Yuhao Liu
The realization of high-efficiency photocatalysis is greatly meaningful to overcome the issues of current energy and environment, in which the core factor is the exploration of photocatalysts with promising semiconductor properties. The Cu-based metal sulfide photocatalysts of CuSbS2 and its derivative of bournonite CuPbSbS3 possess the features of earth-abundant elements, strong photostability, visible-light range bandgap, and high absorption coefficient, possessing great potential for the realization of efficient photocatalytic applications. Although the photocatalysts of CuSbS2 and CuPbSbS3 have been investigated in photocatalysis application of hydrogen production and degradation, the exploration process is still in the early-development stage. In this review, the design concept and semiconductor properties of CuSbS2 and CuPbSbS3 are firstly introduced. Subsequently, the photocatalytic applications of CuSbS2 and CuPbSbS3 photocatalysts, mainly including hydrogen production and degradation, are systematically reviewed. Finally, the challenges and prospects for the further exploration of CuSbS2 and CuPbSbS3 photocatalysts are provided.
{"title":"Recent advances of CuSbS2 and CuPbSbS3 as photocatalyst in the application of photocatalytic hydrogen evolution and degradation","authors":"Xinlong Zheng , Zhongyun Shao , Jiaxin Lin , Qizhi Gao , Zongxian Ma , Yiming Song , Zhen Chen , Xiaodong Shi , Jing Li , Weifeng Liu , Xinlong Tian , Yuhao Liu","doi":"10.1016/j.cclet.2024.110533","DOIUrl":"10.1016/j.cclet.2024.110533","url":null,"abstract":"<div><div>The realization of high-efficiency photocatalysis is greatly meaningful to overcome the issues of current energy and environment, in which the core factor is the exploration of photocatalysts with promising semiconductor properties. The Cu-based metal sulfide photocatalysts of CuSbS<sub>2</sub> and its derivative of bournonite CuPbSbS<sub>3</sub> possess the features of earth-abundant elements, strong photostability, visible-light range bandgap, and high absorption coefficient, possessing great potential for the realization of efficient photocatalytic applications. Although the photocatalysts of CuSbS<sub>2</sub> and CuPbSbS<sub>3</sub> have been investigated in photocatalysis application of hydrogen production and degradation, the exploration process is still in the early-development stage. In this review, the design concept and semiconductor properties of CuSbS<sub>2</sub> and CuPbSbS<sub>3</sub> are firstly introduced. Subsequently, the photocatalytic applications of CuSbS<sub>2</sub> and CuPbSbS<sub>3</sub> photocatalysts, mainly including hydrogen production and degradation, are systematically reviewed. Finally, the challenges and prospects for the further exploration of CuSbS<sub>2</sub> and CuPbSbS<sub>3</sub> photocatalysts are provided.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 3","pages":"Article 110533"},"PeriodicalIF":9.4,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143318379","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-10DOI: 10.1016/j.cclet.2024.110528
Hui Zhang , Rong Feng , Wanyi Yu , Hongbei Wei , Tianhong Wu , Peng Zhang , Wenhai Bian , Xin Li , Di Gao , Guojun Weng , Zhe Yang , Tony D. James , Xiaolong Sun
Redox dyshomeostasis is a critical factor in the initiation of numerous diseases, making the accurate evaluation of the redox status of the cellular environment an important aspect of physiological research. However, maintaining redox homeostasis relies on a complex and dynamic physiological system involving multiple substrate-enzyme interactions, so its accurately detection remains a challenge. With this research, we developed an activable fluorescence switching platform by incorporating different conjugate acceptors to a fluorophore using ester bonds and resulting in fluorescence quenching due to donor-excited photo-induced electron transfer (d-PeT), which was confirmed through density functional theory calculations. The reaction-based probe was deployed for recognizing all major intracellular reducing sulfur species (RSS), including H2S, cysteine (Cys), homocysteine (Hcy), glutathione (GSH), and protein free thiols. The quenched fluorescence was significantly recovered by RSS, through releasing the fluorophore and diminishing the d-PeT effect. Furthermore, the fluorescent probe was used for the sensing and imaging RSS in living cells, demonstrating good cell-permeability, low cytotoxicity, and negative correlation with reactive oxygen species content, enabling the evaluating of global thiols redox state in HepG2 cellular lines during ferroptosis processes.
{"title":"Evaluating the global thiols redox state in living cells using a reducing sulfur species responsive fluorescence switching platform","authors":"Hui Zhang , Rong Feng , Wanyi Yu , Hongbei Wei , Tianhong Wu , Peng Zhang , Wenhai Bian , Xin Li , Di Gao , Guojun Weng , Zhe Yang , Tony D. James , Xiaolong Sun","doi":"10.1016/j.cclet.2024.110528","DOIUrl":"10.1016/j.cclet.2024.110528","url":null,"abstract":"<div><div>Redox dyshomeostasis is a critical factor in the initiation of numerous diseases, making the accurate evaluation of the redox status of the cellular environment an important aspect of physiological research. However, maintaining redox homeostasis relies on a complex and dynamic physiological system involving multiple substrate-enzyme interactions, so its accurately detection remains a challenge. With this research, we developed an activable fluorescence switching platform by incorporating different conjugate acceptors to a fluorophore using ester bonds and resulting in fluorescence quenching due to donor-excited photo-induced electron transfer (<em>d</em>-PeT), which was confirmed through density functional theory calculations. The reaction-based probe was deployed for recognizing all major intracellular reducing sulfur species (RSS), including H<sub>2</sub>S, cysteine (Cys), homocysteine (Hcy), glutathione (GSH), and protein free thiols. The quenched fluorescence was significantly recovered by RSS, through releasing the fluorophore and diminishing the <em>d</em>-PeT effect. Furthermore, the fluorescent probe was used for the sensing and imaging RSS in living cells, demonstrating good cell-permeability, low cytotoxicity, and negative correlation with reactive oxygen species content, enabling the evaluating of global thiols redox state in HepG2 cellular lines during ferroptosis processes.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 4","pages":"Article 110528"},"PeriodicalIF":9.4,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143149449","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-10DOI: 10.1016/j.cclet.2024.110532
Kaili Wang , Pengcheng Liu , Mingzhe Wang , Tianran Wei , Jitao Lu , Xingling Zhao , Zaiyong Jiang , Zhimin Yuan , Xijun Liu , Jia He
Unraveling the essence of electronic structure effected by d-d orbital coupling of transition metal and methanol oxidation reaction (MOR) performance can fundamentally guide high efficient catalyst design. Herein, density functional theory (DFT) calculations were performed at first to study the d–d orbital interaction of metallic PtPdCu, revealing that the incorporation of Pd and Cu atoms into Pt system can enhance d-d electron interaction via capturing antibonding orbital electrons of Pt to fill the surrounding Pd and Cu atoms. Under the theoretical guidance, PtPdCu medium entropy alloy aerogels (PtPdCu MEAAs) catalysts have been designed and systematically screened for MOR under acid, alkaline and neutral electrolyte. Furthermore, DFT calculation and in-situ fourier transform infrared spectroscopy analysis indicate that PtPdCu MEAAs follow the direct pathway via formate as the reactive intermediate to be directly oxidized to CO2. For practical direct methanol fuel cells (DMFCs), the PtPdCu MEAAs-integrated ultra-thin catalyst layer (4∼5 μm thickness) as anode exhibits higher peak power density of 35 mW/cm2 than commercial Pt/C of 20 mW/cm2 (∼40 μm thickness) under the similar noble metal loading and an impressive stability retention at a 50-mA/cm2 constant current for 10 h. This work clearly proves that optimizing the intermediate adsorption capacity via d-d orbital coupling is an effective strategy to design highly efficient catalysts for DMFCs.
{"title":"Modulating d-d orbitals coupling in PtPdCu medium-entropy alloy aerogels to boost pH-general methanol electrooxidation performance","authors":"Kaili Wang , Pengcheng Liu , Mingzhe Wang , Tianran Wei , Jitao Lu , Xingling Zhao , Zaiyong Jiang , Zhimin Yuan , Xijun Liu , Jia He","doi":"10.1016/j.cclet.2024.110532","DOIUrl":"10.1016/j.cclet.2024.110532","url":null,"abstract":"<div><div>Unraveling the essence of electronic structure effected by d-d orbital coupling of transition metal and methanol oxidation reaction (MOR) performance can fundamentally guide high efficient catalyst design. Herein, density functional theory (DFT) calculations were performed at first to study the d–d orbital interaction of metallic PtPdCu, revealing that the incorporation of Pd and Cu atoms into Pt system can enhance d-d electron interaction <em>via</em> capturing antibonding orbital electrons of Pt to fill the surrounding Pd and Cu atoms. Under the theoretical guidance, PtPdCu medium entropy alloy aerogels (PtPdCu MEAAs) catalysts have been designed and systematically screened for MOR under acid, alkaline and neutral electrolyte. Furthermore, DFT calculation and <em>in-situ</em> fourier transform infrared spectroscopy analysis indicate that PtPdCu MEAAs follow the direct pathway <em>via</em> formate as the reactive intermediate to be directly oxidized to CO<sub>2</sub>. For practical direct methanol fuel cells (DMFCs), the PtPdCu MEAAs-integrated ultra-thin catalyst layer (4∼5 μm thickness) as anode exhibits higher peak power density of 35 mW/cm<sup>2</sup> than commercial Pt/C of 20 mW/cm<sup>2</sup> (∼40 μm thickness) under the similar noble metal loading and an impressive stability retention at a 50-mA/cm<sup>2</sup> constant current for 10 h. This work clearly proves that optimizing the intermediate adsorption capacity <em>via</em> d-d orbital coupling is an effective strategy to design highly efficient catalysts for DMFCs.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 4","pages":"Article 110532"},"PeriodicalIF":9.4,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143098703","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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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