The optoelectronic properties of lead halide perovskite nanocrystals (NCs) have garnered significant research interest over the past few years. Herein, we investigated an efficient charge transfer process associated with exciton dynamics between the lead halide perovskite NCs and 5,10,15-tris(4-cyanophenyl)corrole (TCPC). TCPC extracts the holes from the CsPbBr3 NCs, resulting in photoluminescence (PL) quenching of CsPbBr3 NCs. The change in PL intensity and lifetime due to charge transfer was investigated using PL and UTAS analysis. Our study suggested that the quenching of PL intensity is due to the combination of static and dynamic quenching mechanisms. The optical and structural analyses confirm that the charge transfer process occurred without degradation of the perovskite NCs. Along with UTAS, the PL quenching is further investigated using the XPS, UPS, and absolute photoluminescence quantum yield (PLQY), which confirms the charge transfer dynamics between CsPbBr3 and TCPC.
{"title":"Efficient Charge Transfer From CsPbBr<sub>3</sub> Nanocrystals to Free Base Tricyanophenyl Corroles.","authors":"Ravi, Divyansh Dhiman, Sanyam Jain, Muniappan Sankar, Rajiv Kumar Singh, Prasenjit Kar","doi":"10.1002/asia.70434","DOIUrl":"https://doi.org/10.1002/asia.70434","url":null,"abstract":"<p><p>The optoelectronic properties of lead halide perovskite nanocrystals (NCs) have garnered significant research interest over the past few years. Herein, we investigated an efficient charge transfer process associated with exciton dynamics between the lead halide perovskite NCs and 5,10,15-tris(4-cyanophenyl)corrole (TCPC). TCPC extracts the holes from the CsPbBr<sub>3</sub> NCs, resulting in photoluminescence (PL) quenching of CsPbBr<sub>3</sub> NCs. The change in PL intensity and lifetime due to charge transfer was investigated using PL and UTAS analysis. Our study suggested that the quenching of PL intensity is due to the combination of static and dynamic quenching mechanisms. The optical and structural analyses confirm that the charge transfer process occurred without degradation of the perovskite NCs. Along with UTAS, the PL quenching is further investigated using the XPS, UPS, and absolute photoluminescence quantum yield (PLQY), which confirms the charge transfer dynamics between CsPbBr<sub>3</sub> and TCPC.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":" ","pages":"e70434"},"PeriodicalIF":3.3,"publicationDate":"2025-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145555910","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Anjana Singha, Peeyush Pandey, Rolly Yadav, Nitul Kalita, Chivukula V Sastri, Mohammad Qureshi
High electronic conductivity and specific capacitance are critical challenges for free-standing electrodes in neutral electrolyte-based supercapacitors (SCs). This study introduces a 1D/2D heterostructure electrode composed of reduced graphene oxide/polyaniline/cerium-metal-organic framework (rGO/PANI/Ce-MOF), demonstrating enhanced mechanical strength, flexibility, and electrical conductivity. The integration of rGO into the in situ polymerized PANI and Ce-MOF facilitates improved charge transport under neutral electrolytic conditions. Additionally, hydrogen bond interactions were engineered using electrolyte additives, propanol, 1,2-propanediol, and glycerol (Gly) with water molecules to boost ion mobility. The rGO/PANI/Ce-MOF electrode achieved a specific capacitance of 1180 ± 5% F g-1 at 2 A g-1in 1 M Na2SO4, which further increased to 1346 ± 5% F g-1 in a Gly-modified electrolyte under the same conditions. Density functional theory (DFT) calculations using Na+(H2O)4 clusters provided molecular insights into ion interactions, while distribution of relaxation time (DRT) analysis of electrochemical impedance data revealed improved electrode kinetics. An assembled asymmetric SC delivered 205 F g-1, an energy density of 113 ± 5% W h kg-1 at a power density of 1.1 ± 5% kW kg-1, and excellent cycling stability 98% retention. These results underscore the promise of 1D/2D rGO/PANI/Ce-MOF heterostructures and tailored electrolytes for high-performance, flexible energy storage in neutral conditions.
高电导率和比电容是中性电解质基超级电容器(SCs)中独立电极的关键挑战。本研究介绍了一种由还原氧化石墨烯/聚苯胺/铈金属有机骨架(rGO/PANI/Ce-MOF)组成的1D/2D异质结构电极,具有增强的机械强度、柔韧性和导电性。将氧化石墨烯整合到原位聚合聚苯胺和Ce-MOF中,有助于改善中性电解条件下的电荷输运。此外,使用电解质添加剂丙醇、1,2-丙二醇和甘油(Gly)与水分子进行氢键相互作用,以提高离子的迁移率。rGO/PANI/Ce-MOF电极在2 a g- 1in 1 M Na2SO4条件下的比电容为1180±5% F g- 1,在相同条件下,在gly修饰的电解液中进一步提高到1346±5% F g- 1。使用Na+(H2O)4簇的密度泛函理论(DFT)计算提供了离子相互作用的分子见解,而电化学阻抗数据的弛豫时间分布(DRT)分析揭示了电极动力学的改进。组装的非对称SC在1.1±5% kW kg- 1的功率密度下提供205 F g- 1,能量密度为113±5% W h kg- 1,并且具有优异的循环稳定性98%的保留率。这些结果强调了1D/2D rGO/PANI/Ce-MOF异质结构和定制电解质在中性条件下高性能、柔性储能的前景。
{"title":"Controlling Diffusion Dynamics Through Additive Electrolyte Chemistry in Flexible Free-Standing Electrode With Unified 1D-2D Morphologies.","authors":"Anjana Singha, Peeyush Pandey, Rolly Yadav, Nitul Kalita, Chivukula V Sastri, Mohammad Qureshi","doi":"10.1002/asia.70453","DOIUrl":"https://doi.org/10.1002/asia.70453","url":null,"abstract":"<p><p>High electronic conductivity and specific capacitance are critical challenges for free-standing electrodes in neutral electrolyte-based supercapacitors (SCs). This study introduces a 1D/2D heterostructure electrode composed of reduced graphene oxide/polyaniline/cerium-metal-organic framework (rGO/PANI/Ce-MOF), demonstrating enhanced mechanical strength, flexibility, and electrical conductivity. The integration of rGO into the in situ polymerized PANI and Ce-MOF facilitates improved charge transport under neutral electrolytic conditions. Additionally, hydrogen bond interactions were engineered using electrolyte additives, propanol, 1,2-propanediol, and glycerol (Gly) with water molecules to boost ion mobility. The rGO/PANI/Ce-MOF electrode achieved a specific capacitance of 1180 ± 5% F g<sup>-</sup> <sup>1</sup> at 2 A g<sup>-</sup> <sup>1</sup>in 1 M Na<sub>2</sub>SO<sub>4</sub>, which further increased to 1346 ± 5% F g<sup>-</sup> <sup>1</sup> in a Gly-modified electrolyte under the same conditions. Density functional theory (DFT) calculations using Na<sup>+</sup>(H<sub>2</sub>O)<sub>4</sub> clusters provided molecular insights into ion interactions, while distribution of relaxation time (DRT) analysis of electrochemical impedance data revealed improved electrode kinetics. An assembled asymmetric SC delivered 205 F g<sup>-</sup> <sup>1</sup>, an energy density of 113 ± 5% W h kg<sup>-</sup> <sup>1</sup> at a power density of 1.1 ± 5% kW kg<sup>-</sup> <sup>1</sup>, and excellent cycling stability 98% retention. These results underscore the promise of 1D/2D rGO/PANI/Ce-MOF heterostructures and tailored electrolytes for high-performance, flexible energy storage in neutral conditions.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":" ","pages":"e70453"},"PeriodicalIF":3.3,"publicationDate":"2025-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145555933","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Supercritical carbon dioxide (scCO2) is well-known for its low viscosity and high diffusivity, which are widely utilized in CO2 transportation and storage processes within the carbon capture, utilization, and storage (CCUS) strategy. Additionally, its strong solvation capacity, environmental benignity, and facile separation make it an attractive solvent for organic synthesis. In this study, we successfully apply scCO2 in CO2 cycloaddition with epoxides for continuous cyclic carbonate synthesis using our developed imidazolium-based polymer-supported ionic liquid (Im-PSIL) catalysts. The application of this scCO2-assisted catalytic system to five different epoxide substrates, including essential industrial chemicals such as epichlorohydrin and glycidol, delivered moderate to excellent yields, highlighting its high value for the chemical industry.
{"title":"Continuous-Flow Synthesis of Cyclic Carbonate With Supercritical CO2 Using Polystyrene-Supported Imidazolium Catalysts","authors":"Zhibo Yu, Haruro Ishitani, Shu Kobayashi","doi":"10.1002/asia.202500980","DOIUrl":"10.1002/asia.202500980","url":null,"abstract":"<p>Supercritical carbon dioxide (scCO<sub>2</sub>) is well-known for its low viscosity and high diffusivity, which are widely utilized in CO<sub>2</sub> transportation and storage processes within the carbon capture, utilization, and storage (CCUS) strategy. Additionally, its strong solvation capacity, environmental benignity, and facile separation make it an attractive solvent for organic synthesis. In this study, we successfully apply scCO<sub>2</sub> in CO<sub>2</sub> cycloaddition with epoxides for continuous cyclic carbonate synthesis using our developed imidazolium-based polymer-supported ionic liquid (Im-PSIL) catalysts. The application of this scCO<sub>2</sub>-assisted catalytic system to five different epoxide substrates, including essential industrial chemicals such as epichlorohydrin and glycidol, delivered moderate to excellent yields, highlighting its high value for the chemical industry.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":"20 24","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://aces.onlinelibrary.wiley.com/doi/epdf/10.1002/asia.202500980","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145555927","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}