Ying Zhang , Chuang Shen , Jiaxu Zhang , Qi Shen , Fei Xu , Shengheng Wang , Jiuyi Hu , Faisal Saleem , Feng Huang , Zhimin Luo
{"title":"Ultrasmall PtCu nanosheets as a broadband phototheranostic agent in near-infrared biowindow","authors":"Ying Zhang , Chuang Shen , Jiaxu Zhang , Qi Shen , Fei Xu , Shengheng Wang , Jiuyi Hu , Faisal Saleem , Feng Huang , Zhimin Luo","doi":"10.1016/j.cclet.2025.111059","DOIUrl":"10.1016/j.cclet.2025.111059","url":null,"abstract":"<div><div>Broadband photothermal and photoacoustic agents in the near-infrared (NIR) biowindow are of significance for cancer phototheranostics. In this work, PtCu nanosheets with an average lateral size of less than 10 nm are synthesized as NIR photothermal and photoacoustic agents <em>in vivo</em>, which show strong light absorption from NIR-I to NIR-II biowindows with the photothermal conversion efficiencies of 20.4% under 808 nm laser and 32.7% under 1064 nm laser. PtCu nanosheets functionalized with folic acid-modified thiol-poly(ethylene glycol) (SH-PEG-FA) present good biocompatibility and 4T1 tumor-targeted effect, which give high-contrast photoacoustic imaging and efficient photothermal ablation of 4T1 tumor in both NIR-I and NIR-II biowindows. Our work significantly broadens applications of noble metal-based nanomaterials in the fields of cancer phototheranostics by rationally designing their structures and modulating their physicochemical properties.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 6","pages":"Article 111059"},"PeriodicalIF":9.4,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143697529","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}
Chaojian Xu , Juxin Yin , Sihong Wang , Yue Pan , Qianhe Zhang , Ningkang Xie , Shuo Yang , Shaowu Lv
{"title":"Aerobic radical polymerization of hydrogels triggered by acetylacetone-transition metal self-initiation","authors":"Chaojian Xu , Juxin Yin , Sihong Wang , Yue Pan , Qianhe Zhang , Ningkang Xie , Shuo Yang , Shaowu Lv","doi":"10.1016/j.cclet.2025.111075","DOIUrl":"10.1016/j.cclet.2025.111075","url":null,"abstract":"<div><div>The performance of hydrogel radical polymerization under ambient conditions is a major challenge because oxygen is an effective radical quencher and the steps to remove or neutralize it are time consuming and laborious. A self-initiating system consisting of transition metals and acetylacetone has been successfully developed. The system is capable of initiating free radical polymerization of hydrogels at room temperature under aerobic conditions, which is attributed to carbon radicals generated by the oxidation of acetylacetone. Some of these carbon radicals reduce oxygen to generate hydroxyl radicals, which together induce self-coagulation of hydrogels. The polymerization system was effective for a variety of monomer and hydrogel swelling and shrinking schemes, and the reaction remained successful when exposed to saturated oxygen. In conclusion, the results demonstrate that the present strategy is an effective approach to addressing the challenge of deoxygenation in polymer synthesis, and provides a convenient method for synthesizing multifunctional hydrogels under ambient conditions.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 7","pages":"Article 111075"},"PeriodicalIF":9.4,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143935031","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}
Jiabin Zhang , Xiaoke Zhang , Lilei Wang , Lingpeng Yan , Xueli Cheng , Tao Li
{"title":"Fluorinated fused azobenzene boron-based polymer acceptors with 1000 nm absorbance edges for all-polymer solar cells","authors":"Jiabin Zhang , Xiaoke Zhang , Lilei Wang , Lingpeng Yan , Xueli Cheng , Tao Li","doi":"10.1016/j.cclet.2025.111064","DOIUrl":"10.1016/j.cclet.2025.111064","url":null,"abstract":"<div><div>Fluorinated fused azobenzene boron (FBAz) is a novel electron-deficient building block for polymer electron acceptors in all-polymer solar cells (all- PSC). The B←N bridging units impart a fixed configuration and low-lying LUMO/HOMO energy. Three polymer acceptor materials (P2f, P3f and P5f) with different fluorine substitution positions by copolymerizing FBAz with indacenodithiophene (IDT), are synthesized and investigated to study the influence of fluorinated forms on the all-polymer solar cell performance. The FBAz units are synthesized in just three steps, facilitating the straightforward production of polymer acceptors P2f, P3f, and P5f. These acceptors exhibit strong light absorption in the visible to near-infrared range of 500–1000 nm and possess suitable LUMO/HOMO energy levels of -3.99/-5.66 eV which are very complementary to that (<em>E</em><sub>LUMO/HOMO</sub> = -3.59/-5.20 eV) of the widely-used polymer donor poly[(ethylhexylthiophenyl)-benzodithiophene-(ethylhexyl)-thienothiophene] (PTB7-Th). All-polymer solar cells (all-PSCs) with PTB7-Th as electron donor and P3f as electron acceptor exhibits highest power conversion efficiencies (PCE) 2.70 %. When PC<sub>61</sub> BM is added as the third component, the device efficiency can reach 5.36%. These preliminary results indicate that FBAz is a promising strong electron acceptor for the development of n-type polymer semiconductors, especially in organic photovoltaics (OPVs). To the best of our knowledge, this is the first example demonstrating the unique photovoltaic properties of the N=N double bond as an acceptor material.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 7","pages":"Article 111064"},"PeriodicalIF":9.4,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143934735","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}
Xinbao Tong , Jiaying Liu , Yanqi Zhao , Jingjun Li , Ye Tian , Qingyi Liu , Shuiying Gao , Rong Cao
{"title":"Metal-organic framework supported carbon quantum dots as white light-emitting phosphor","authors":"Xinbao Tong , Jiaying Liu , Yanqi Zhao , Jingjun Li , Ye Tian , Qingyi Liu , Shuiying Gao , Rong Cao","doi":"10.1016/j.cclet.2025.111058","DOIUrl":"10.1016/j.cclet.2025.111058","url":null,"abstract":"<div><div>The growing environmental concerns regarding rare earth elements in fluorescent powders, along with high production costs, have increased the demand for sustainable alternatives. We propose a promising solution using luminescent metal-organic frameworks (LMOFs) with large surface areas and tunable pore structures, combined with organic carbon quantum dots (CQDs). This study develops a novel white light-emitting diode (WLED) fluorescent powder by incorporating yellow-fluorescent quantum dots (CQDs-Y) into blue-emitting LMOF (ZJU-28), forming the composite material CQDs-Y-n@ZJU-28. The composite exhibits excellent thermal and chemical stability, long-term storage performance, and emits warm white light (CIE: 0.3277, 0.3281) when subjected to excitation at 365 nm, along with an external quantum efficiency (EQE) of 8.85 %. Furthermore, it exhibits tunable emission characteristics and promising LED performance, showcasing a color rendering index (CRI) of 78 and a correlated color temperature of 3384 K. The emitted light undergoes minimal deviation in color towards the white end of the spectrum in the temperature range of 277–437 K, making it an ideal candidate for advanced WLED applications.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 7","pages":"Article 111058"},"PeriodicalIF":9.4,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143934736","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}
Shujun Ning , Zhiyuan Wei , Zhening Chen , Tianmin Wu , Lu Zhang
{"title":"Curvature and defect formation synergistically promote the photocatalysis of ZnO slabs","authors":"Shujun Ning , Zhiyuan Wei , Zhening Chen , Tianmin Wu , Lu Zhang","doi":"10.1016/j.cclet.2025.111057","DOIUrl":"10.1016/j.cclet.2025.111057","url":null,"abstract":"<div><div>Crystal defects and morphological modifications are popular strategies to enhance the catalytic activity of heterogeneous semiconductor photocatalysts. Despite defect engineering and morphology control show their successful applications in ZnO, the effects of curved surface modifications on the photocatalytic performance of ZnO and their interplay with the defect formation remain unclear. To resolve this puzzle, we systemically investigate the joint effects of curvature and defect formation on the electronic structure, optoelectronic properties, and photocatalytic performance of ZnO slabs using first-principles calculations. We find that curvature deformation effectively narrows the electronic bandgap by up to 1.6 eV and shifts the p-/d-band centers, thereby enhancing light absorption in the visible and near-ultraviolet regions. Besides, curvature deformation stimulates self-polarization, facilitating the separation of photo-generated electrons and holes. Also, curvature deformation promotes the formation of defects by reducing defect formation energy (by up to 1.0 eV), thus creating abundant reaction sites for photocatalysis. Intriguingly, the synergistic interaction between curvature and defect deformation further strengthens the self-polarization, narrows the electronic bandgaps, adjusts the p-/d-band centers to improve the optoelectronic properties, and influences the dissociation and free energy barriers of intermediates. Consequently, our findings reveal that this synergy substantially enhances the photocatalytic performance of ZnO slabs, providing deeper insights into the role of defect engineering and morphology control on photocatalysis.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 7","pages":"Article 111057"},"PeriodicalIF":9.4,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143928654","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}
{"title":"Rational catalyst design for N2 electro-reduction: Regulation strategies and quick screen towards enhanced conversion efficiency","authors":"Jinzhou Zheng, Chaozheng He, Chenxu Zhao","doi":"10.1016/j.cclet.2025.111056","DOIUrl":"10.1016/j.cclet.2025.111056","url":null,"abstract":"<div><div>Ammonia is a key industry raw material for fertilizers and the electro-reduction of N<sub>2</sub> (NRR) can be served as a promising method. It is urgently needed to discover advanced catalysts while the lack of design principles still hinders the high-throughput screen of efficient candidates. Herein, we have provided an up-to-date review of NRR catalysts mainly on theoretical works and highlighted the latest achievements on descriptors, which can be served as valid guidance of optimal catalysts. The descriptors are classified with adsorption energy and the corresponding derived ones, which can screen the NRR catalysts from various aspects. Finally, the challenges and opportunities in the descriptor field are presented.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 7","pages":"Article 111056"},"PeriodicalIF":9.4,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143923657","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}
Hui Bian , Xinyi Yuan , Nan Zhang , Zhuo Xu , Juhong Lian , Ruibin Jiang , Junqing Yan , Deng Li , Shengzhong (Frank) Liu
{"title":"Correlating vacancy-defect density with CO2 activation for promoted CO2 methanation over CsPbBr3 photocatalyst","authors":"Hui Bian , Xinyi Yuan , Nan Zhang , Zhuo Xu , Juhong Lian , Ruibin Jiang , Junqing Yan , Deng Li , Shengzhong (Frank) Liu","doi":"10.1016/j.cclet.2025.111034","DOIUrl":"10.1016/j.cclet.2025.111034","url":null,"abstract":"<div><div>Constructing vacancy-decorated metal halide perovskites (MHPs) have emerged as promising pathway to enhance photocatalytic activity and selectivity for solar CO<sub>2</sub> reduction. However, the controllable construction of vacancy defects is still challenging, and our understanding of the roles of these defects, particularly their effects on the adsorption activation of surface reaction molecules, is still insufficient. Herein, we elaborately designed and synthesized adjustable Br vacancies in CsPbBr<sub>3</sub> catalysts by manipulating the dissolution and recrystallization speed of precursors during the ball milling process using solvents with gradient polarities. We found that the Br vacancies could promote the charge separation, while having slight influence on the band structure of CsPbBr<sub>3</sub>. More importantly, temperature-programmed desorption results combined with theoretical calculations revealed that Br vacancies can significantly enhance the adsorption of CO<sub>2</sub> and CO on the surface, specifically increasing the adsorption strength between CO and the active sites. This finding provides a substantial opportunity for achieving high activity and selectivity in photocatalytic CO<sub>2</sub> methanation. Accordingly, a high rate of CO<sub>2</sub> photoreduction to CH<sub>4</sub> up to 17.94 ± 0.81 μmol g<sup>-1</sup> h<sup>-1</sup> along with superior selectivity of 95.8% were acquired for CsPbBr<sub>3<img></sub>HX featuring with the richest Br vacancy defects, which is 18.9-fold compared that of CsPbBr<sub>3<img></sub>CAN with the lowest Br vacancy defects. This investigation deepens insights into action mechanism of defects on halide perovskites catalysts, offering a novel strategy for the high-effective conversion of CO<sub>2</sub> into valuable products.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 7","pages":"Article 111034"},"PeriodicalIF":9.4,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143928655","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}