Xuhui Fan , Fan Wang , Mengjiao Li , Faiza Meharban , Yaying Li , Yuanyuan Cui , Xiaopeng Li , Jingsan Xu , Qi Xiao , Wei Luo
{"title":"Visible light excitation on CuPd/TiN with enhanced chemisorption for catalyzing heck reaction","authors":"Xuhui Fan , Fan Wang , Mengjiao Li , Faiza Meharban , Yaying Li , Yuanyuan Cui , Xiaopeng Li , Jingsan Xu , Qi Xiao , Wei Luo","doi":"10.1016/j.cclet.2024.110299","DOIUrl":"10.1016/j.cclet.2024.110299","url":null,"abstract":"<div><div>In this work, we developed plasmonic photocatalyst composed of CuPd alloy nanoparticles supported on TiN, the optimized Cu<sub>3</sub>Pd<sub>2</sub>/TiN catalyst shows excellent conversion (>96 %) and selectivity (>99 %) for Heck reaction at 50 °C under visible light irradiation. By <em>in-situ</em> spectroscopic investigations, we find that visible light excitation could achieve stable metallic Cu species on the surface of CuPd alloy nanoparticles, thereby eliminating the inevitable surface oxides of Cu based catalyst. The <em>in-situ</em> formed metallic Cu species under irradiation take advantage of the strong interactions of Cu with visible light, and manifest in the localized surface plasmon resonances (LSPR) photoexcitation. Visible light excitation could further promote the charge transfer between catalytic Pd component and the support TiN, resulting in electron-rich Pd sites on CuPd/TiN. Moreover, light excitation on CuPd/TiN generates strong chemisorption of iodobenzene and styrene, favoring the activation of reactants for Heck reaction. DFT calculations suggest that electron-rich CuPd sites ideally lower the activation energy barrier for the coupling reaction. This work provides valuable insights for mechanistic understanding of plasmonic photocatalysis.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 1","pages":"Article 110299"},"PeriodicalIF":9.4,"publicationDate":"2024-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141853367","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}
Gang Hu , Chun Wang , Qinqin Wang , Mingyuan Zhu , Lihua Kang
{"title":"The controlled oxidation states of the H4PMo11VO40 catalyst induced by plasma for the selective oxidation of methacrolein","authors":"Gang Hu , Chun Wang , Qinqin Wang , Mingyuan Zhu , Lihua Kang","doi":"10.1016/j.cclet.2024.110298","DOIUrl":"10.1016/j.cclet.2024.110298","url":null,"abstract":"<div><div>In this paper, low-temperature dielectric-blocked discharge plasma (DBD) was employed for the first time to treat silica-doped H<sub>4</sub>PMo<sub>11</sub>VO<sub>40</sub> (HPAV) catalysts (DBD(Ar/x)-MF-Catal) and apply them in the catalytic methacrolein (MAL) selective oxidation to produce methacrylic acid (MAA). This work investigates in detail the controllable regulation of the concentration of oxidation states on silica-doped HPAV catalysts by adjusting the DBD discharge with controlled changes in voltage, current, treatment time, and treatment medium. It reports the intrinsic correlation between oxidation states and MAL oxidation performance. The research results indicated that the catalytic performance was related to the presence of oxygen vacancies and oxygen species (VO<sup>2+</sup>), and are the main reason for the selective oxidation of MAL to MAA. Besides, the generation of oxygen vacancies and VO<sup>2+</sup> altered localized electrons, which resulted in the easier activation of O<sub>2</sub>. Theoretical calculations of DFT also proved the formation mechanism of oxygen vacancies and VO<sup>2+</sup> and electron properties on high-performance polymers, which elucidated the intrinsic influence of catalyst components. The DBD(Ar/10)-MF-Catal catalysts with suitable VO<sup>2+</sup> and oxygen vacancy concentrations exhibited the highest catalytic performance with 90 % MAL conversion and 70 % MAA selectivity and showed good stability (500 h).</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 2","pages":"Article 110298"},"PeriodicalIF":9.4,"publicationDate":"2024-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141840655","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}
Pengfei Li , Chulin Qu , Fan Wu , Hu Gao , Chengyan Zhao , Yue Zhao , Zhen Shen
{"title":"Robust free-base and metalated corrole radicals with reduction-induced emission","authors":"Pengfei Li , Chulin Qu , Fan Wu , Hu Gao , Chengyan Zhao , Yue Zhao , Zhen Shen","doi":"10.1016/j.cclet.2024.110292","DOIUrl":"10.1016/j.cclet.2024.110292","url":null,"abstract":"<div><div>Preparing free-base porphyrinoid radicals that can function as coordination ligands is a challenging task. Here we report the synthesis of a stable, free-base benzocorrole (<strong>BC</strong>) radical containing only two inner NH protons <em>via</em> a <em>retro</em>-Diels-Alder conversion. The radical character of <strong>BC</strong> was fully supported by crystallographic analysis, spectroscopic evidence, and theoretical calculations. This neutral radical ligand allowed easy insertion of Zn(II), Ga(III), and Pd(II) ions to produce radical complexes. All these radicals exhibited luminescence-on responses under weak reducing atmosphere, corresponding to the conversion to their aromatic anions. The red fluorescence was observed for <strong>BC</strong> and its Zn(II) and Ga(III) complexes, and the near-infrared phosphorescence (>900 nm) was detected for Pd(II) complex at room temperature. Furthermore, Ga(III) corrole exhibited a variation in fluorescence in response to axial coordination. Our findings provide a promising radical platform for coordination and developing novel functional materials with switchable spin and emission.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 2","pages":"Article 110292"},"PeriodicalIF":9.4,"publicationDate":"2024-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141842672","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}
Yanfei Liu , Yaqin Hu , Yifu Tan , Qiwen Chen , Zhenbao Liu
{"title":"Tumor acidic microenvironment activatable DNA nanostructure for precise cancer cell targeting and inhibition","authors":"Yanfei Liu , Yaqin Hu , Yifu Tan , Qiwen Chen , Zhenbao Liu","doi":"10.1016/j.cclet.2024.110289","DOIUrl":"10.1016/j.cclet.2024.110289","url":null,"abstract":"<div><div>Precise tumor targeting and therapy is a major trend in cancer treatment. Herein, we designed a tumor acidic microenvironment activatable drug loaded DNA nanostructure, in which, we made a clever use of the sequences of AS1411 and i-motif, which can partially hybridize, and designed a simple while robust DNA <span>d</span>-strand nanostructure, in which, i-motif sequence was designed to regulate the binding ability of the AS1411 aptamer to target tumor. In the normal physiological environment, i-motif inhibits the targeting ability of AS1411. In the acidic tumor microenvironment, i-motif forms a quadruplex conformation and dissociates from AS1411, restoring the targeting ability of AS1411. Only when acidic condition and tumor cell receptor are present, this nanostructure can be internalized by the tumor cells. Moreover, the structure change of this nanostructure can realize the release of loaded drug. This drug loaded A-I-Duplex DNA structure showed cancer cell and spheroid targeting and inhibition ability, which is promising in the clinical cancer therapy.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 1","pages":"Article 110289"},"PeriodicalIF":9.4,"publicationDate":"2024-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141844767","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}
Entian Cui , Yulian Lu , Zhaoxia Li , Zhilei Chen , Chengyan Ge , Jizhou Jiang
{"title":"Interfacial B-O bonding modulated S-scheme B-doped N-deficient C3N4/O-doped-C3N5 for efficient photocatalytic overall water splitting","authors":"Entian Cui , Yulian Lu , Zhaoxia Li , Zhilei Chen , Chengyan Ge , Jizhou Jiang","doi":"10.1016/j.cclet.2024.110288","DOIUrl":"10.1016/j.cclet.2024.110288","url":null,"abstract":"<div><div>Photocatalytic overall pure water splitting is a promising method for generating green hydrogen energy under mild conditions. However, this process is often hindered by sluggish electron-hole separation and transport. To address this, a step-scheme (S-scheme) B-doped N-deficient C<sub>3</sub>N<sub>4</sub>/O-doped C<sub>3</sub>N<sub>5</sub> (BN-C<sub>3</sub>N<sub>4</sub>/O-C<sub>3</sub>N<sub>5</sub>) heterojunction with interfacial B-O bonds has been constructed. Utilizing Pt and Co(OH)<sub>2</sub> as co-catalysts, BN-C<sub>3</sub>N<sub>4</sub>/O-C<sub>3</sub>N<sub>5</sub> S-scheme heterojunction demonstrates significantly enhanced photocatalytic activity for overall pure water splitting under visible light, achieving H<sub>2</sub> and O<sub>2</sub> evolution rates of 40.12 and 19.62 µmol/h, respectively. Systematic characterizations and experiments revealed the performance-enhancing effects of the enhanced built-in electric field and the interfacial B-O bonding. Firstly, the strengthened built-in electric field provides sufficient force for rapid interfacial electron transport. Secondly, by reducing the transport energy barrier and transfer distance, the interfacial B-O bonds facilitate rapid recombination of electrons and holes with relatively low redox potential <em>via</em> the S-scheme charge-transfer route, leaving the high-potential electrons and holes available for H<sup>+</sup> reduction and OH<sup>−</sup> oxidation reactions. Overall, the photocatalytic efficiency of BN-C<sub>3</sub>N<sub>4</sub>/O-C<sub>3</sub>N<sub>5</sub> S-scheme heterojunction was significantly improved, making it a promising approach for green hydrogen production through overall pure water splitting.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 1","pages":"Article 110288"},"PeriodicalIF":9.4,"publicationDate":"2024-07-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141850636","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}
Haijun Shen , Yi Qiao , Chun Zhang, Yane Ma, Jialing Chen, Yingying Cao, Wenna Zheng
{"title":"A matrix metalloproteinase-sensitive hydrogel combined with photothermal therapy for transdermal delivery of deferoxamine to accelerate diabetic pressure ulcer healing","authors":"Haijun Shen , Yi Qiao , Chun Zhang, Yane Ma, Jialing Chen, Yingying Cao, Wenna Zheng","doi":"10.1016/j.cclet.2024.110283","DOIUrl":"10.1016/j.cclet.2024.110283","url":null,"abstract":"<div><p>Diabetic pressure ulcers (DPU) are non-healing due to vascular dysfunction and bacterial infection. Early intervention can delay ulcer progression, such as preventing the formation of full-thickness skin defects. Local administration of deferoxamine (DFO) at wound sites has been shown to promote neovascularization and enhance wound healing. However, since DPU skin wounds are not full-thickness defects and DFO is hydrophilic, enhancing its transdermal delivery is crucial for effective treatment. Photothermal ablation of stratum corneum, generated by copper sulfide nanoparticles (CuS NPs) under near-infrared (NIR) light irradiation, is a promising method to improve transdermal drug delivery. Meanwhile, CuS NPs-induced photothermal therapy offers excellent antibacterial performance. In this study, DFO and CuS NPs were incorporated into a matrix metalloproteinase (MMPs)-sensitive hydrogel. This hydrogel promotes cell adhesion and is degraded by cell-secreted MMPs, a process crucial for the controlled release of encapsulated DFO and CuS NPs. Under NIR irradiation, the stratum corneum is disrupted, facilitating transdermal DFO delivery and simultaneously eliminating infected bacteria. As a result, the essential requirements for DPU treatment, “facilitating transdermal DFO delivery, promoting angiogenesis, and inhibiting bacterial infection”, were achieved simultaneously.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"35 12","pages":"Article 110283"},"PeriodicalIF":9.4,"publicationDate":"2024-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141843211","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}
Jumei Zhang , Ziheng Zhang , Gang Li , Hongjin Qiao , Hua Xie , Ling Jiang
{"title":"Ligand-mediated reactivity in CO oxidation of yttrium-nickel monoxide carbonyl complexes","authors":"Jumei Zhang , Ziheng Zhang , Gang Li , Hongjin Qiao , Hua Xie , Ling Jiang","doi":"10.1016/j.cclet.2024.110278","DOIUrl":"10.1016/j.cclet.2024.110278","url":null,"abstract":"<div><div>A series of heteronuclear yttrium-nickel monoxide carbonyl complexes YNiO(CO)<em><sub>n</sub></em><sup>−</sup> (<em>n</em> = 1–5) were generated in a pulsed-laser vaporization source and characterized by mass-selected photoelectron velocity-map spectroscopy combined with theoretical calculations. CO ligand-mediated reactivity in CO oxidation of yttrium-nickel monoxide carbonyl complexes was experimentally and theoretically identified. During the consecutive CO adsorption, a <em>μ</em><sup>2</sup>-O linear structure was most favorable for YNiO(CO)<em><sub>n</sub></em><sup>−</sup> (<em>n</em> = 1, 2), then a structure in which the terminal O was bonded to the Y atom became favored for YNiO(CO)<sub>3</sub><sup>−</sup>, and finally a structure bearing a CO<sub>2</sub> moiety was most favorable for YNiO(CO)<em><sub>n</sub></em><sup>−</sup> (<em>n</em> = 4, 5). Theoretical calculations indicated that the Ni atom acted as an electron acceptor and accumulated electron density at <em>n</em> ≤ 3, and then served as an electron donor along with the Y atom to contribute electron density in the rearrangement that accompanied CO oxidation at <em>n</em> > 3.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 2","pages":"Article 110278"},"PeriodicalIF":9.4,"publicationDate":"2024-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141848145","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":"Boosted solar water oxidation steered by atomically precise alloy nanocluster","authors":"Xian Yan , Huawei Xie , Gao Wu , Fang-Xing Xiao","doi":"10.1016/j.cclet.2024.110279","DOIUrl":"10.1016/j.cclet.2024.110279","url":null,"abstract":"<div><div>Atomically precise metal nanoclusters (NCs) have been deemed as a new generation of metal nanomaterials in the field of solar energy conversion due to their unique atomic stacking manner, quantum confinement effects, light-harvesting capability and multitude of active sites. Nonetheless, wide-spread application of monometallic NCs is blocked by the ultrashort carrier lifespan, uncontrollable charge transport pathway, and light-induced poor stability, impeding the construction of robust and stable metal NC-based photosystems. Herein, we report the fabrication of stable alloy (Au<sub>1-x</sub>Pt<sub>x</sub>) NCs photosystem, for which tailor-made negatively charged <span>l</span>-glutathione (GSH)-capped Au<sub>1-x</sub>Pt<sub>x</sub> NCs as the building blocks are controllably deposited on the BiVO<sub>4</sub> (BVO) by a self-assembly approach for steering enhanced light absorption and interfacial charge transfer over alloy NCs-based photoanodes (Au<sub>1-x</sub>Pt<sub>x</sub>/BVO). The self-assembled Au<sub>1-x</sub>Pt<sub>x</sub>/BVO composite photoanode exhibits the significantly enhanced photoelectrochemical water oxidation performances compared with pristine BVO and Au<sub>x</sub>/BVO photoanodes, which is caused by the Pt atom doping into the Au<sub>x</sub> NCs for elevating photosensitivity and boosting the stability. The synergy of Au and Pt atoms in alloy NCs protects the gold core from rapid oxidation, improving the photostability and accelerating the surface charge transfer kinetics. Our work would significantly inspire ongoing interest in unlocking the charge transport characteristics of atomically precise alloy NCs for solar energy conversion.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 1","pages":"Article 110279"},"PeriodicalIF":9.4,"publicationDate":"2024-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141847930","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}
Guoping Yang , Zhoufu Lin , Xize Zhang , Jiawei Cao , Xuejiao Chen , Yufeng Liu , Xiaoling Lin , Ke Li
{"title":"Assembly of Y(III)-containing antimonotungstates induced by malic acid with catalytic activity for the synthesis of imidazoles","authors":"Guoping Yang , Zhoufu Lin , Xize Zhang , Jiawei Cao , Xuejiao Chen , Yufeng Liu , Xiaoling Lin , Ke Li","doi":"10.1016/j.cclet.2024.110274","DOIUrl":"10.1016/j.cclet.2024.110274","url":null,"abstract":"<div><p>A dimeric Y(III)-containing antimonotungstate [Y<sub>4</sub>(H<sub>2</sub>O)<sub>8</sub>(mal)<sub>2</sub>(OAc)O(Sb<sub>2</sub>W<sup>V</sup><sub>2</sub>W<sup>VI</sup><sub>19</sub>O<sub>72</sub>)<sub>2</sub>]<sup>21−</sup> (<strong>Y<sub>4</sub>mal<sub>2</sub></strong>, H<sub>3</sub>mal = <span>dl</span>-malic acid), resembling a “handshake” configuration, was synthesized and characterized. The polyanion of <strong>Y<sub>4</sub>mal<sub>2</sub></strong> consists of two Dawson-derived {Y<sub>2</sub>Sb<sub>2</sub>W<sub>21</sub>} moieties that are further linked by two mal ligands and one μ<sub>2</sub>-bridging acetate to form an asymmetric polyanion. Notably, the chiral configuration induced by the <span>d</span>- or <span>l</span>-configuration of the mal ligand results in both {Y<sub>2</sub>Sb<sub>2</sub>W<sub>21</sub>} moieties within one polyanion exhibiting identical chirality, leading to the racemate crystallization of <strong>Y<sub>4</sub>mal<sub>2</sub></strong>. Moreover, <strong>Y<sub>4</sub>mal<sub>2</sub></strong> exhibits excellent Lewis acid catalytic activity for environmentally friendly synthesis of imidazoles.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"35 12","pages":"Article 110274"},"PeriodicalIF":9.4,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141841395","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}