Chinese Chemical Letters最新文献_第3页

Identifying the catalytic active site of durable Ru-based liquid-phase catalyst for acetylene hydrochlorination 耐用钌基液相催化剂乙炔加氢氯化催化活性位点的确定

IF 9.4 1区化学

Chinese Chemical Letters Pub Date : 2025-05-12 DOI: 10.1016/j.cclet.2025.111303

Linfeng Li , Bao Wang , Tiantong Zhang , Xinyuan Wang , Dingqiang Feng , Wei Li , Jiangjiexing Wu , Jinli Zhang

{"title":"Identifying the catalytic active site of durable Ru-based liquid-phase catalyst for acetylene hydrochlorination","authors":"Linfeng Li , Bao Wang , Tiantong Zhang , Xinyuan Wang , Dingqiang Feng , Wei Li , Jiangjiexing Wu , Jinli Zhang","doi":"10.1016/j.cclet.2025.111303","DOIUrl":"10.1016/j.cclet.2025.111303","url":null,"abstract":"<div><div>A comprehensive understanding of the structure and dynamic evolution of catalytic active sites is vital for advancing the study of liquid-phase acetylene hydrochlorination. Here, we successfully developed a Ru-DIPEA/TMS catalyst optimised through systematic composition and condition tuning, demonstrating exceptional performance with 95.5 % C<sub>2</sub>H<sub>2</sub> conversion and sustaining over 91.1 % activity along with nearly 100 % selectivity for VCM during a continuous 900-h test. Using a combination of characterisation techniques, including UV–vis spectroscopy, FT-IR spectroscopy, X-ray photoelectron spectroscopy, single-crystal X-ray diffraction, and X-ray absorption spectroscopy, along with density functional theory (DFT) calculations, the structure and dynamic behaviour of the active sites were thoroughly investigated under the synergistic influence of ligands and HCl. The results revealed that HCl activation induces a significant structural transformation of the active sites, leading to the formation of a hexacoordinate complex, Ru(CO)<sub>2</sub>C<sub>l2</sub>(C<sub>6</sub>H<sub>15</sub>N·HCl)<sub>2</sub>. DFT calculations further elucidated the mechanism underlying active site formation, revealing that an increased electron density around the Ru centre and corresponding changes in its coordination environment play critical roles in enhancing catalyst stability and activity. This study contributes to a deeper understanding of the structural basis of active site evolution during acetylene hydrochlorination, offering both practical insights into industrial applications and foundational knowledge for advancing liquid-phase catalysis.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 10","pages":"Article 111303"},"PeriodicalIF":9.4,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144663057","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}

引用次数: 0

Reinforced nitrogen fixation via synergistic Ru-Ni dual sites 通过协同的Ru-Ni双位点加强固氮

IF 9.4 1区化学

Chinese Chemical Letters Pub Date : 2025-05-09 DOI: 10.1016/j.cclet.2025.111295

Tan Zhang , Zhikai Che , Yuru Song , Jinping Li , Yuhan Sun , Guang Liu

{"title":"Reinforced nitrogen fixation via synergistic Ru-Ni dual sites","authors":"Tan Zhang , Zhikai Che , Yuru Song , Jinping Li , Yuhan Sun , Guang Liu","doi":"10.1016/j.cclet.2025.111295","DOIUrl":"10.1016/j.cclet.2025.111295","url":null,"abstract":"<div><div>The electrocatalytic nitrogen reduction reaction (NRR) is challenging but crucial for the sustainable development of both industry and agriculture. To enhance NRR performance, it is critically important to construct advanced electrocatalysts that offer satisfactory performance containing high activity and selectivity. However, the strong affinity of nitrogen-containing species on the Ru surface resulted in suboptimal NRR activity. Herein, we propose a dual-site catalyst, RuNi, to optimize the binding strength, which leads to superior electrocatalytic performance, achieving a high NH<sub>3</sub> yield rate of 5.07 µg h<sup>-1</sup> cm<sup>-2</sup> at -0.2 V <em>vs.</em> RHE and a Faradaic efficiency (FE) of 26.2 % at -0.1 V <em>vs.</em> RHE in 0.1 mol/L Na<sub>2</sub>SO<sub>4</sub>. Owing to the synergistic interaction between Ru and Ni, a remarkable performance is realized over the RuNi catalyst. In-situ characterization evidenced that hydrogen radicals (H*) on the Ni site of the RuNi catalyst participate in the dissociation of N<sub>2</sub> adsorbed on the Ru site, and theoretical investigations indicated that RuNi reduces the adsorption strength of intermediates. This offers an effective approach to the synthesis of dual-site catalysts for electrocatalytic ammonia synthesis.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 9","pages":"Article 111295"},"PeriodicalIF":9.4,"publicationDate":"2025-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144579313","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}

引用次数: 0

A zinc-nitrate battery for efficient ammonia electrosynthesis and energy output by a high entropy hydroxide catalyst 一种用于高熵氢氧化物催化剂高效氨电合成和能量输出的硝酸锌电池

IF 9.4 1区化学

Chinese Chemical Letters Pub Date : 2025-05-09 DOI: 10.1016/j.cclet.2025.111294

Mingxing Chen, Xue Li, Nian Liu, Zihe Du, Zhitao Wang, Jing Qi

引用次数: 0

Graded nitro-engineering strategy: Tuning surface states and sp² conjugated domains of carbon quantum dots for full-color emission 梯度氮工程策略：调整碳量子点的表面态和sp²共轭畴，用于全彩发射

IF 9.4 1区化学

Chinese Chemical Letters Pub Date : 2025-05-09 DOI: 10.1016/j.cclet.2025.111296

Chunyan Wang , Chen Wei , Hongyang Niu , Ligang Xu , Xue Liu

{"title":"Graded nitro-engineering strategy: Tuning surface states and sp² conjugated domains of carbon quantum dots for full-color emission","authors":"Chunyan Wang , Chen Wei , Hongyang Niu , Ligang Xu , Xue Liu","doi":"10.1016/j.cclet.2025.111296","DOIUrl":"10.1016/j.cclet.2025.111296","url":null,"abstract":"<div><div>Precise control of luminescence in carbon quantum dots (CQDs), from single-color to full-color emission, is crucial for advancing their applications in biomedical imaging and display technologies. While CQDs luminescence is primarily influenced by conjugated domains and surface states, the underlying interaction mechanisms remain poorly understood. This study explores a graded nitro-engineering approach to simultaneously regulate surface states and sp² conjugated domains through nitro (-NO<sub>2</sub>) modulation, enabling comprehensive color tuning. Using <em>o</em>-phenylenediamine (<em>o</em>-PD) as the carbon source and adjusting nitric acid (HNO<sub>3</sub>) concentrations, we synthesized tricolor-emitting nitro-functionalized CQDs (NO₂-CQDs). At lower -NO<sub>2</sub> concentrations, luminescence is mainly influenced by surface states, where the electron-withdrawing effect of -NO<sub>2</sub> enhances <em>π</em>-electron delocalization and stabilizes sp² conjugation. With increasing -NO<sub>2</sub> content, the lowest unoccupied molecular orbital (LUMO) energy level decreases (-2.12 eV to -3.39 eV), resulting in a red-shift in fluorescence. At higher -NO<sub>2</sub> concentrations, luminescence is primarily affected by the sp² conjugated domain, where steric hindrance reduces molecular planarity and conjugation, leading to a blue-shift in fluorescence as the sp² domain size decreases (4.03 nm to 2.83 nm). Combining experimental results with density functional theory (DFT) calculations, we reveal the dual role of -NO₂ in modulating CQDs luminescence, an approach rarely achieved through surface functionalization. This work presents a novel strategy for precise tuning of CQDs luminescence across the visible spectrum.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 10","pages":"Article 111296"},"PeriodicalIF":9.4,"publicationDate":"2025-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144679082","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}

引用次数: 0

Groups 3 and 4 single-site catalysts for olefin-polar monomer copolymerization 烯烃-极性单体共聚的第3和第4基团单位点催化剂

IF 9.4 1区化学

Chinese Chemical Letters Pub Date : 2025-05-09 DOI: 10.1016/j.cclet.2025.111297

Chengkai Li, Guoqiang Fan, Gang Zheng, Rong Gao, Li Liu

{"title":"Groups 3 and 4 single-site catalysts for olefin-polar monomer copolymerization","authors":"Chengkai Li, Guoqiang Fan, Gang Zheng, Rong Gao, Li Liu","doi":"10.1016/j.cclet.2025.111297","DOIUrl":"10.1016/j.cclet.2025.111297","url":null,"abstract":"<div><div>Introducing functional polar groups into polyolefins can significantly improve the material properties, but there are still challenges in achieving this goal, with the core difficulty being that polar groups are prone to interact with metal active species, affecting the efficiency of the copolymerization. With the rapid advancement in catalyst, a variety of copolymerization strategies are developed aimed at producing more versatile polyolefin materials. Although early transition metal catalysts play an indispensable role in the traditional polyolefin industry, their inherent strong oxophilicity becomes a significant constraint in copolymerization involving polar olefins, limiting their application scope. This review summarizes the progress made in recent years in the efficient copolymerization of non-polar olefins with polar comonomers catalyzed by groups 3 and 4 single-site catalysts. We classify the catalysts into four categories, Sc-, Ti-, Zr-, Hf-, based on the type of metal centers, and provide insights into the influence of catalyst structures and the type of comonomers on the copolymerization behavior. The introduction of polar monomers fundamentally improves the comprehensive performance of the products, greatly broadens the application scope of polyolefin materials, and meets the growing market demand for multifunctional and high-performance materials.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 9","pages":"Article 111297"},"PeriodicalIF":9.4,"publicationDate":"2025-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144587881","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}

引用次数: 0

Hierarchical work function programming for optimizing interfacial polarization in electromagnetic wave absorber 电磁波吸收器界面极化优化的分层功函数规划

IF 9.4 1区化学

Chinese Chemical Letters Pub Date : 2025-05-09 DOI: 10.1016/j.cclet.2025.111293

Jinkun Liu , Xuelian Yang , Wenxuan Chen , Pingan Zhu , Guanglei Wu , Jing Zheng , Xu Hou

{"title":"Hierarchical work function programming for optimizing interfacial polarization in electromagnetic wave absorber","authors":"Jinkun Liu , Xuelian Yang , Wenxuan Chen , Pingan Zhu , Guanglei Wu , Jing Zheng , Xu Hou","doi":"10.1016/j.cclet.2025.111293","DOIUrl":"10.1016/j.cclet.2025.111293","url":null,"abstract":"<div><div>The development of next-generation electromagnetic wave (EMW) absorbers requires a shift in interface design. By employing hierarchical work function programming, we propose an approach to tune interfacial polarization dynamics. This method utilizes multi-gradient work functions to guide carrier migration and polarization effectively, thereby enhancing energy dissipation under alternating electromagnetic fields. Here, we constructed a 1T/2H-MoS<sub>2</sub>/PPy/VS<sub>2</sub> composite absorber with integrated gradient interfaces. The composite achieved a powerful absorption (RL<sub>min</sub>) of -58.59 dB at 2.3 mm, and an effective absorption bandwidth (EAB) of 7.44 GHz at 2.5 mm, demonstrating improved broadband absorption. Radar cross-section (RCS) simulations show an EMW loss of -7.2 dB m<sup>2</sup> at 0°, highlighting its potential for stealth and communication applications. This study introduces hierarchical work function programming as a promising strategy in EMW absorber design, contributing to advancements in material performance and functionality.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 10","pages":"Article 111293"},"PeriodicalIF":9.4,"publicationDate":"2025-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144665710","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}

引用次数: 0

P doped Ni3S2 and Ni heterojunction bifunctional catalysts for electrocatalytic 5-hydroxymethylfurfural oxidation coupled hydrogen evolution reaction P掺杂Ni3S2和Ni异质结双功能催化剂电催化5-羟甲基糠醛氧化偶联析氢反应

IF 9.4 1区化学

Chinese Chemical Letters Pub Date : 2025-04-29 DOI: 10.1016/j.cclet.2025.111271

Mengzhao Liu , Jie Yin , Chengjian Wang , Weiji Wang , Yuan Gao , Mengxia Yan , Ping Geng

{"title":"P doped Ni3S2 and Ni heterojunction bifunctional catalysts for electrocatalytic 5-hydroxymethylfurfural oxidation coupled hydrogen evolution reaction","authors":"Mengzhao Liu , Jie Yin , Chengjian Wang , Weiji Wang , Yuan Gao , Mengxia Yan , Ping Geng","doi":"10.1016/j.cclet.2025.111271","DOIUrl":"10.1016/j.cclet.2025.111271","url":null,"abstract":"<div><div>The biomass electrochemical oxidation coupled with hydrogen evolution reaction has received widespread attention due to its carbon-neutral and sustainable properties. The electrosynthesis of 2,5-furanodicarboxylic acid (FDCA) from 5-hydroxymethylfurfural (HMF) oxidation is one of the most promising means for the production of bioplastic monomers. In this work, we constructed a novel P-doped Ni<sub>3</sub>S<sub>2</sub> and Ni heterojunction on nickel foam (P-Ni<sub>3</sub>S<sub>2</sub>/Ni/NF) using electrodeposition methods and thermal sulfuration techniques as a bifunctional catalyst for the simultaneous anodic oxidation of HMF to FDCA (HMFOR) and the cathodic hydrogen evolution reaction (HER). On one hand, the synergistic promotion of P doping and the heterojunction of Ni<sub>3</sub>S<sub>2</sub> and Ni accelerated electron transfer, and on the other hand, the structure of three-dimensional microsphere stacking on NF surface to form macropores enhances the exposure of catalytically active sites. The prepared P-Ni<sub>3</sub>S<sub>2</sub>/Ni/NF exhibited remarkable performance with high HMF conversion (99.2 %), FDCA yield (98.1 %), and Faraday efficiency (98.8 %), and excellent stability with good product selectivity for 7 consecutive cycles, which stands at a higher level than majority of previously published electrocatalysts. Furthermore, P-Ni<sub>3</sub>S<sub>2</sub>/Ni/NF also shows a significant response in HER. By using HMFOR and HER as the anodic reaction and cathodic reaction, respectively, the biomass upgrading and hydrogen production can be carried out simultaneously. The synthesized P-Ni<sub>3</sub>S<sub>2</sub>/Ni/NF only need a voltage of 1.31 V to achieve a current density of 10 mA/cm<sup>2</sup> in a two-electrode system of HMFOR and HER, which is much lower than that of 1.48 V in OER and HER process, thus potentially reducing the cost of this process.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 9","pages":"Article 111271"},"PeriodicalIF":9.4,"publicationDate":"2025-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144579314","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}

引用次数: 0

Rational constructing of Zn0.5Cd0.5S-diethylenetriamine/g-C3N4 S-scheme heterojunction with enhanced photocatalytic H2O2 production 合理构建zn0.5 cd0.5 s -二乙三胺/g- c3n4s方案异质结，增强光催化H2O2产率

IF 9.4 1区化学

Chinese Chemical Letters Pub Date : 2025-04-28 DOI: 10.1016/j.cclet.2025.111272

Zheng Liu , Yuqing Bian , Graham Dawson , Jiawei Zhu , Kai Dai

{"title":"Rational constructing of Zn0.5Cd0.5S-diethylenetriamine/g-C3N4 S-scheme heterojunction with enhanced photocatalytic H2O2 production","authors":"Zheng Liu , Yuqing Bian , Graham Dawson , Jiawei Zhu , Kai Dai","doi":"10.1016/j.cclet.2025.111272","DOIUrl":"10.1016/j.cclet.2025.111272","url":null,"abstract":"<div><div>Photocatalytic hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) production (PHP) offers significant advantages to traditional production methods, including solar energy utilization, mild reaction conditions, environmental friendliness, pollution-free processes, sustainability, and high selectivity. However, despite its potential as a green and sustainable technology, photocatalytic H<sub>2</sub>O<sub>2</sub> production (PHP) is constrained by limited visible light absorption by photocatalysts and the rapid recombination of photogenerated charge carriers, which reduce yield and efficiency. In this study, we synthesized an organic amine constrained Zn<sub>0.5</sub>Cd<sub>0.5</sub>S-DETA/g-C<sub>3</sub>N<sub>4</sub> (ZCS-D/CN) S-scheme heterojunction <em>via</em> a hydrothermal method to enhance PHP. Anchoring ZCS-D on the surface of CN and forming an S-scheme heterojunction effectively prevented ZCS-D agglomeration, modulated the band structure of CN, and enhanced the migration and redox capabilities of photogenerated charge carriers. The optimized heterojunction (ZCS-D/CN) achieved a H<sub>2</sub>O<sub>2</sub> yield of 5124 µmol g<sup>-1</sup> h<sup>-1</sup> in pure H<sub>2</sub>O, significantly outperforming pure CN (24 µmol g<sup>-1</sup> h<sup>-1</sup>) and ZCS-D (4012 µmol g<sup>-1</sup> h<sup>-1</sup>). These results demonstrate that ZCS-D/CN S-scheme heterojunction holds substantial potential for photocatalytic applications, particularly in the efficient production of H<sub>2</sub>O<sub>2</sub>.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 9","pages":"Article 111272"},"PeriodicalIF":9.4,"publicationDate":"2025-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144587087","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}

引用次数: 0

Physicochemical design of magneto-responsive confined interfaces for manipulation of nonmagnetic liquids 操纵非磁性液体的磁响应受限界面的物理化学设计

IF 9.4 1区化学

Chinese Chemical Letters Pub Date : 2025-04-28 DOI: 10.1016/j.cclet.2025.111206

Jing Liu , Ming Li , Jian Zhang , Xinyu Li , Yuqing Zheng , Xu Hou

{"title":"Physicochemical design of magneto-responsive confined interfaces for manipulation of nonmagnetic liquids","authors":"Jing Liu , Ming Li , Jian Zhang , Xinyu Li , Yuqing Zheng , Xu Hou","doi":"10.1016/j.cclet.2025.111206","DOIUrl":"10.1016/j.cclet.2025.111206","url":null,"abstract":"<div><div>Controllable liquid manipulation is of paramount scientific and technological importance in various fields, such as the chemical industry, biomedicine, and agricultural production. Magnetic actuation, characterized by rapid, contactless, and environmentally benign operation, has emerged as a promising approach for precise liquid control. However, conventional magnetic strategies typically govern droplet movement on open surfaces, facing limitations such as restricted liquid volumes, uncertain flow paths, and inevitable evaporation, thereby constraining their broader practical applications. Recently, a variety of magnetic-driven strategies have been developed to dynamically regulate liquids within enclosed spaces, especially through physicochemical mechanisms. These approaches provide efficient control over liquid behavior by leveraging magnetically induced chemical changes, structural deformations, and dragging motions, opening new opportunities for flexible and versatile fluid management. This review explores the design and mechanisms of magneto-responsive confined interfaces for the manipulation of nonmagnetic liquids, highlighting key advancements and potential applications including liquid valves, liquid mixing, liquid flow regulation, and liquid pumping. Finally, the existing challenges and future prospects in this field are presented.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 8","pages":"Article 111206"},"PeriodicalIF":9.4,"publicationDate":"2025-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144229587","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}

引用次数: 0

Dye-stabilized atomically precise copper clusters for enhanced photocatalytic hydrogen evolution 染料稳定原子精确铜簇增强光催化析氢

IF 9.4 1区化学

Chinese Chemical Letters Pub Date : 2025-04-28 DOI: 10.1016/j.cclet.2025.111256

Yan-Ling Li , Yue Xu , Chen-Hong Wang , Rui Wang , Shuang-Quan Zang

{"title":"Dye-stabilized atomically precise copper clusters for enhanced photocatalytic hydrogen evolution","authors":"Yan-Ling Li , Yue Xu , Chen-Hong Wang , Rui Wang , Shuang-Quan Zang","doi":"10.1016/j.cclet.2025.111256","DOIUrl":"10.1016/j.cclet.2025.111256","url":null,"abstract":"<div><div>Metal nanoclusters with well-defined atomic structures offer significant promise in the field of catalysis due to their sub-nanometer size and tunable organic-inorganic hybrid structural features. Herein, we successfully synthesized an 11-core copper(I)-alkynyl nanocluster (Cu<sub>11</sub>), which is stabilized by alkynyl ligands derived from a photosensitive rhodamine dye molecule. Notably, this Cu<sub>11</sub> cluster exhibited excellent photocatalytic hydrogen evolution activity (8.13 mmol g<sup>−1</sup>h<sup>−1</sup>) even in the absence of a mediator and noble metal co-catalyst. Furthermore, when Cu<sub>11</sub> clusters were loaded onto the surface of TiO<sub>2</sub> nanosheets, the resultant Cu<sub>11</sub>@TiO<sub>2</sub> nanocomposites exhibited a significant enhancement in hydrogen evolution efficiency, which is 60 times higher than that of pure TiO<sub>2</sub> nanosheets. The incorporation of Cu<sub>11</sub> clusters within the Cu<sub>11</sub>@TiO<sub>2</sub> effectively inhibits the recombination of photogenerated electrons and holes, thereby accelerating the charge separation and migration in the composite material. This work introduces a novel perspective for designing highly active copper cluster-based photocatalysts.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 10","pages":"Article 111256"},"PeriodicalIF":9.4,"publicationDate":"2025-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144665709","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}

引用次数: 0