Junchen Peng , Zhongyuan Guo , Dandan Dong, Yusheng Lu, Bao Wang, Fangjie Lu, Chaofeng Huang, Bin Dai
{"title":"Cu0/Cuδ+ site construction and its catalytic role in acetylene hydrochlorination","authors":"Junchen Peng , Zhongyuan Guo , Dandan Dong, Yusheng Lu, Bao Wang, Fangjie Lu, Chaofeng Huang, Bin Dai","doi":"10.1016/j.cclet.2025.111208","DOIUrl":"10.1016/j.cclet.2025.111208","url":null,"abstract":"<div><div>In view of the dearth of active components and the unsatisfactory dispersion of Cu-based catalysts, it is imperative to undertake a detailed investigation of catalysts with enhanced catalytic performance. In order to achieve a balance between the catalytic activity and stability in the reaction process, a series of P-atom doped Cu<sup>0</sup>/Cu<sup>δ+</sup> binary Cu-based catalysts were prepared by means of heteroatom introduction and heat treatment. The introduction of P enhanced the stability of Cu during heat treatment, thereby inhibiting the excessive agglomeration of Cu. The structure of the Cu<sup>0</sup>/Cu<sup>δ+</sup> binary catalyst was modified through heat treatment and HCl activation, and the relationship between its structure and catalytic activity was subsequently investigated. The activation process of HCl facilitated the conversion of the Cu<sup>0</sup> state to the Cu-Cl state and augmented the valence state of Cu. The valence modulation of the Cu site by HCl during the reaction prevented the over-reduction of the Cu site by acetylene and enhanced the stability of the catalyst. The 3Cu/5CuP/AC-800 catalyst was operated for 50 h without significant deactivation under the reaction conditions of <em>T</em> = 180 °C, V(HCl)/V(C<sub>2</sub>H<sub>2</sub>) = 1.15 and <em>GHSV</em>(C<sub>2</sub>H<sub>2</sub>) = 180 h<sup>-1</sup>. This design strategy provides a novel reference point for further studies of CuCl<sub>2</sub> based catalysts for acetylene hydrochlorination.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 8","pages":"Article 111208"},"PeriodicalIF":9.4,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144223662","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":"Controlling the extent of nanoparticle occlusion within calcite crystals via surface chemistry engineering","authors":"Xia Sun, Zixian Liang, Jiahao Zhang, Boxiang Peng, Bing Yu, Pei Liu, Biao Xiong, Jizhuang Wang, Yin Ning","doi":"10.1016/j.cclet.2025.111205","DOIUrl":"10.1016/j.cclet.2025.111205","url":null,"abstract":"<div><div>Directly occluding polymer nanoparticles into growing host crystals provides a versatile pathway for synthesizing polymer-inorganic composite crystals, where guest nanoparticles are distributed within the crystal matrix. However, systematically controlling the extent of nanoparticle occlusion within a host crystal remains a significant challenge. In this study, we employ a one-step, soap-free emulsion polymerization method to synthesize polyethyleneimine-functionalized poly(<em>tert</em>‑butyl methacrylate) (PtBMA/PEI) nanoparticles. These cationic nanoparticles are subsequently modified using formaldehyde to systematically tune the content of surface amine group <em>via</em> the Eschweiler-Clarke reaction. This approach yields a series of model nanoparticles that allow us to investigate how surface chemistry influences the extent of nanoparticle occlusion within calcite crystals. Our findings reveal that the extent of nanoparticle occlusion within calcite crystals is proportional to the surface amine group content. This study offers a new design rule for creating composite crystals with tailored compositions through a nanoparticle occlusion strategy.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 9","pages":"Article 111205"},"PeriodicalIF":9.4,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144587494","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}
Ze-Hong Zheng, Mu-Qiu Chen, Jin Zhou, Jie Wang, Yan-Rong Wei, Cheng Peng, Gu Zhan, Qian-Qian Yang, Bo Han
{"title":"Diverse synthesis of bridged bicyclo[3.2.1]octa-2,6-diene and tricyclo[3.2.1.02,7] oct-3-ene frameworks via stepwise cascade reactions","authors":"Ze-Hong Zheng, Mu-Qiu Chen, Jin Zhou, Jie Wang, Yan-Rong Wei, Cheng Peng, Gu Zhan, Qian-Qian Yang, Bo Han","doi":"10.1016/j.cclet.2025.111202","DOIUrl":"10.1016/j.cclet.2025.111202","url":null,"abstract":"<div><div>Strained bridged rings bicyclo[3.2.1]octane and tricyclo[3.2.1.0<sup>2,7</sup>]octane are prevalent in natural products known for their significant biological activities. However, strategies for efficiently synthesizing these complex frameworks from simple starting materials <em>via de novo</em> synthesis remain underexplored. This article presents an efficient strategy that combines phosphine catalysis and photocatalysis to execute a stepwise tandem reaction involving allenoates and α-cyano cinnamaldehydes, including [3 + 2] cyclization, [5 + 2] cyclization, acyl transfer, and decarboxylation reactions, synthesizing a series of functional bicyclo[3.2.1]octa-2,6-diene and tricyclo[3.2.1.0<sup>2,7</sup>]oct‑3-ene skeleton derivatives with excellent chemoselectivity demonstrated throughout the process. Meanwhile, the reaction can also be performed <em>via</em> a one-pot, scalable phosphine/photocatalytic cascade process, efficiently yielding the bridged products which can serve as versatile intermediates for further applications.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 12","pages":"Article 111202"},"PeriodicalIF":8.9,"publicationDate":"2025-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145107643","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":"Stabilizing Cu2+ in perovskite via A-site modulation for efficient CO2 electrocatalysis to CH4","authors":"Yuhan Zheng, Yunzhen Jia, Xuelei Lang, Dazhong Zhong, Jinping Li, Qiang Zhao","doi":"10.1016/j.cclet.2025.111193","DOIUrl":"10.1016/j.cclet.2025.111193","url":null,"abstract":"<div><div>Cu<sup>2+</sup> in copper-based catalysts can facilitate the hydrogenation of the CH<sub>4</sub> production pathway <em>via</em> the electrochemical carbon dioxide reduction reaction (ECRR). However, Cu<sup>2+</sup> species in copper oxides are unstable and have been revealed to reduce to Cu<sup>0</sup> under the applied cathodic potential. In this work, we reported an A-site modulation strategy to stabilize Cu<sup>2+</sup> in perovskite for efficient ECRR to CH<sub>4</sub>. After the introduction of Ca<sup>2+</sup> in La<sub>2</sub>CuO<sub>4</sub>, the obtained LaCa<sub>0.4</sub>CuO<sub>3-</sub><em><sub>δ</sub></em> is stable during ECRR. We achieved a 59.6 % ± 3.8 % CH<sub>4</sub> faradaic efficiency at -1.30 V <em>versus</em> reversible hydrogen electrode in H-cell and a partial current density of 155.0 mA/cm<sup>2</sup> in membrane electrode assembly. DFT calculations and <em>in situ</em> Raman spectroscopy show that Cu<sup>2+</sup> facilitates the hydrogenation of *CH<sub>2</sub>O to *CH<sub>3</sub>O and the further production of CH<sub>4</sub>. This work introduces an efficient strategy to stabilize Cu<sup>2+</sup> and provides an understanding of Cu<sup>2+</sup> in promoting ECRR to CH<sub>4</sub>.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 8","pages":"Article 111193"},"PeriodicalIF":9.4,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144223661","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}
Zenggang Lin , Peng Zhang , Yuzhu Yang , Weisheng Liu
{"title":"Multilevel stimulus-responsive smart organic afterglow materials beyond crystal limitations: Aqueous-phase dual emission afterglow and upconversion afterglow under ultra-wide range excitation","authors":"Zenggang Lin , Peng Zhang , Yuzhu Yang , Weisheng Liu","doi":"10.1016/j.cclet.2025.111194","DOIUrl":"10.1016/j.cclet.2025.111194","url":null,"abstract":"<div><div>Organic afterglow materials hold significant potential for applications in information storage, anti-counterfeiting, and biological imaging. However, studies on afterglow materials capable of ultra-wide range excitation and emission simultaneously are limited. To enhance the practicality of strong emission single-component organic afterglow systems, overcoming the constraints of crystalline or other rigid environments is essential. We have developed solid-state dual-persistent thermally activated delayed fluorescence (TADF) and room temperature phosphorescence (RTP) emissions spanning yellow to red under visible light excitation, utilizing a single-molecule terminal group regulation strategy. The RTP lifetime extends from 4.19 ms to 399.70 ms. These afterglow materials exhibit an ultra-wide absorption range from 200 nm to 800 nm, rendering them capable of being excited by both sunlight simulator and near-infrared radiation. The upconversion phosphorescence lifetime under 808 nm excitation reaches 13.72 μs. The double persistent emission of these compounds is temperature-sensitive. Moreover, following grinding or heat treatment, accompanied by extensive afterglow color conversion due to planarization of excited state conformations and additional efficient <em>k</em><sub>RISC</sub> generation. In addition, the amorphous state post melt annealing facilitates the afterglow transition from yellow to green. Crucially, these compounds also maintain stable ultra-long afterglow emission in aqueous and acid-base environments. Overall, we have successfully developed a series of single-component intelligent luminescent materials that demonstrate significant benefits, including dual TADF and RTP emissions, adjustable afterglow lifetimes, a broad range of excitation and emission wavelengths, multi-modal luminescence not restricted to crystalline states, and robust afterglow performance in challenging environments, setting the stage for the practical deployment of afterglow materials in engineering applications, the upconversion afterglow emission also holds promising potential for applications in the field of biological imaging.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 9","pages":"Article 111194"},"PeriodicalIF":9.4,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144587088","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}
Peng Wang , Guanyu Zhao , Yicai Pan , Yujing Li , Chenxi Fu , Shipeng Sun , Junqi Gai , Jinping Mu , Xue Bai , Xiaohui Li , Jinfeng Sun , Xiaodong Shi , Rui He
{"title":"Dual-salt electrolyte strategy enables stable interface reaction and high-performance lithium-ion batteries at low temperature","authors":"Peng Wang , Guanyu Zhao , Yicai Pan , Yujing Li , Chenxi Fu , Shipeng Sun , Junqi Gai , Jinping Mu , Xue Bai , Xiaohui Li , Jinfeng Sun , Xiaodong Shi , Rui He","doi":"10.1016/j.cclet.2025.111190","DOIUrl":"10.1016/j.cclet.2025.111190","url":null,"abstract":"<div><div>Lithium-ion batteries (LIBs) are increasingly required to operate under harsh conditions, particularly at low-temperature condition. Developing novel electrolytes is a facile and effective approach to elevate the electrochemical performances of LIBs at low temperature. Herein, a dual-salt electrolyte consisting of (lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) and lithium difluoro(oxalato)borate (LiODFB)) is proposed to regulate the solvation structure of Li<sup>+</sup> ions and improve the reaction kinetics under low temperature. Based on the comprehensive electrochemical tests and theoretical computations, the introduction of LiODFB component not only effectively benefits the formation of cathode electrolyte interface (CEI) layer on the surface of LiFePO<sub>4</sub> electrode, but also inhibits the chemical corrosion effect of LiTFSI-containing electrolytes on Al foil. As expected, the optimized Li||LiFePO₄ cells can display high reversible capacity of 117.0 mAh/g after 100 cycles at -20 °C. This work provides both theoretical basis and experimental guidance for the rational design of low-temperature resistant electrolytes.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 11","pages":"Article 111190"},"PeriodicalIF":8.9,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144879829","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}
Gaojing Yang , Zhimeng Hao , Chun Fang , Wen Zhang , Xia-hui Zhang , Yuyu Li , Zhenhua Yan , Zhiyuan Wang , Tao Sun , Xiaofei Yang , Fei Wang , Chengzhi Zhang , Hongchang Jin , Shuaifeng Lou , Nan Chen , Yiju Li , Jia-Yan Liang , Le Yang , Shouyi Yuan , Jin Niu , Jianmin Ma
{"title":"Research progress and perspectives on rechargeable batteries","authors":"Gaojing Yang , Zhimeng Hao , Chun Fang , Wen Zhang , Xia-hui Zhang , Yuyu Li , Zhenhua Yan , Zhiyuan Wang , Tao Sun , Xiaofei Yang , Fei Wang , Chengzhi Zhang , Hongchang Jin , Shuaifeng Lou , Nan Chen , Yiju Li , Jia-Yan Liang , Le Yang , Shouyi Yuan , Jin Niu , Jianmin Ma","doi":"10.1016/j.cclet.2025.111185","DOIUrl":"10.1016/j.cclet.2025.111185","url":null,"abstract":"<div><div>Energy storage plays a critical role in sustainable development, with secondary batteries serving as vital technologies for efficient energy conversion and utilization. This review provides a comprehensive summary of recent advancements across various battery systems, including lithium-ion, sodium-ion, potassium-ion, and multivalent metal-ion batteries such as magnesium, zinc, calcium, and aluminum. Emerging technologies, including dual-ion, redox flow, and anion batteries, are also discussed. Particular attention is given to alkali metal rechargeable systems, such as lithium-sulfur, lithium-air, sodium-sulfur, sodium-selenium, potassium-sulfur, potassium-selenium, potassium-air, and zinc-air batteries, which have shown significant promise for high-energy applications. The optimization of key components—cathodes, anodes, electrolytes, and interfaces—is extensively analyzed, supported by advanced characterization techniques like time-of-flight secondary ion mass spectrometry (TOF-SIMS), synchrotron radiation, nuclear magnetic resonance (NMR), and <em>in-situ</em> spectroscopy. Moreover, sustainable strategies for recycling spent batteries, including pyrometallurgy, hydrometallurgy, and direct recycling, are critically evaluated to mitigate environmental impacts and resource scarcity. This review not only highlights the latest technological breakthroughs but also identifies key challenges in reaction mechanisms, material design, system integration, and waste battery recycling, and presents a roadmap for advancing high-performance and sustainable battery technologies.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 10","pages":"Article 111185"},"PeriodicalIF":8.9,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144780341","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}
Jingyuan Luo , Liping Wu , Jinxi Yan , Xintong Lv , Yuqi Luo , Wei Jiang , Zhiqiang Xiong , Anqi Ni , Chongbo Liu , Renchao Che
{"title":"Radar-stealth and thermal-insulating MOF-derived cellulose-carbon aerogels for broadband electromagnetic wave absorption","authors":"Jingyuan Luo , Liping Wu , Jinxi Yan , Xintong Lv , Yuqi Luo , Wei Jiang , Zhiqiang Xiong , Anqi Ni , Chongbo Liu , Renchao Che","doi":"10.1016/j.cclet.2025.111065","DOIUrl":"10.1016/j.cclet.2025.111065","url":null,"abstract":"<div><div>Considering the challenges posed by severe electromagnetic wave pollution and escalating international tensions, there is a critical need to develop advanced electromagnetic wave absorbing (EMWA) materials that integrate radar stealth and thermal insulation capabilities. In this study, we have synthesized three-dimensional (3D) porous composites comprising V<sub>2</sub>O<sub>3</sub> nanoparticles embedded in <em>Juncus effusus</em> cellulose-derived carbon aerogels (VCA) using a self-templating method followed by high-temperature pyrolysis. The V<sub>2</sub>O<sub>3</sub> nanoparticles possess a 3D V-V framework and a relatively narrow bandgap, facilitating the Mott transition for enhanced conductivity. Furthermore, their uniform dispersion on hollow carbon tubes of <em>Juncus effusus</em> promotes efficient electron transfer and creates numerous heterogeneous interfaces. Consequently, VCA-2 demonstrates outstanding EMWA performance, achieving a minimum reflection loss of −63.92 dB at a matching thickness of 2.0 mm and a maximum effective absorption bandwidth of 8.24 GHz at a thickness of 2.44 mm, covering nearly half of the tested frequency range. Additionally, the radar cross-section reduction reaches a peak value of 29.40 dB m<sup>2</sup>, underscoring the excellent radar stealth capabilities of the material. In summary, VCA exhibits exceptional EMWA, radar stealth, and thermal insulation properties, highlighting its potential for multifunctional applications in EMWA material development.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 7","pages":"Article 111065"},"PeriodicalIF":9.4,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143934734","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}
Wenjuan Liu , Shanshan Zhang , Yu Wang , Bin Fang , Weirui Wang , Shujing Song , Tomohiro Hakozaki
{"title":"Three-channel imaging reveals the comprehensive protein modifications and their impact on skin appearance induced by multiple stimuli","authors":"Wenjuan Liu , Shanshan Zhang , Yu Wang , Bin Fang , Weirui Wang , Shujing Song , Tomohiro Hakozaki","doi":"10.1016/j.cclet.2025.111182","DOIUrl":"10.1016/j.cclet.2025.111182","url":null,"abstract":"<div><div>Protein damage repair and prevention are important objectives in skin care industry. Skin protein damage or modifications such as glycation, carbonylation or oxidation, have a significant impact on its function, therefore directly influencing various skin functions or properties including skin appearance. However, there is a lack of comprehensive methods to visualize and assess the protein damage. In this article, we present a three-channel imaging approach to simultaneously visualize and quantitatively evaluate protein oxidation, protein glycation and carbonylation in a full-thickness skin model. We successfully visualized and quantified the impact of the multiple stimuli (ultraviolet radiation A (UVA) and/or methylglyoxal) as well as treatment effect of positive control (vitamins C and E) with this method. Our findings indicate that multiple stimuli exhibit synergistic effects on protein damage. Furthermore, we evaluated a unique combination of skin care ingredients which demonstrated an excellent efficacy in resisting protein damage. Further research revealed that three ingredients of the combination upregulate autophagy in cells, which may contribute to remove damaged proteins and maintain protein quality homeostasis. This method provides a holistic assessment of protein damages and can be employed to evaluate the impact of various stimuli or to assess the efficacy of skin care ingredients in mitigating such damage.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 6","pages":"Article 111182"},"PeriodicalIF":9.4,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143845134","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}