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Combination of Copper-Catalyzed Multicomponent Cascade with 12π Electrocyclization Constructing Perifused Cycle 铜催化多组分级联与 12π 电环化相结合构建外溢循环
IF 11.2 1区 化学
CCS Chemistry Pub Date : 2024-08-16 DOI: 10.31635/ccschem.024.202404453
{"title":"Combination of Copper-Catalyzed Multicomponent Cascade with 12π Electrocyclization Constructing Perifused Cycle","authors":"","doi":"10.31635/ccschem.024.202404453","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404453","url":null,"abstract":"CCS Chemistry, Ahead of Print.<br/>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"9 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2024-08-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141994643","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
Ultrastable Ruthenium-Based Electrocatalysts for Hydrogen Oxidation Reaction in High-Temperature Polymer Electrolyte Membrane Fuel Cells 用于高温聚合物电解质膜燃料电池中氢氧化反应的超稳定钌基电催化剂
IF 11.2 1区 化学
CCS Chemistry Pub Date : 2024-08-13 DOI: 10.31635/ccschem.024.202404436
Miaoyu Li, Pupu Yang, Wenjie Lv, Qie Liu, Yujie Wu, Shiqian Du, Gen Huang, Zuyao Jiang, Jingjing Wang, Yabin Xu, Yangyang Zhou, Shanfu Lu, Li Tao, Shuangyin Wang
{"title":"Ultrastable Ruthenium-Based Electrocatalysts for Hydrogen Oxidation Reaction in High-Temperature Polymer Electrolyte Membrane Fuel Cells","authors":"Miaoyu Li, Pupu Yang, Wenjie Lv, Qie Liu, Yujie Wu, Shiqian Du, Gen Huang, Zuyao Jiang, Jingjing Wang, Yabin Xu, Yangyang Zhou, Shanfu Lu, Li Tao, Shuangyin Wang","doi":"10.31635/ccschem.024.202404436","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404436","url":null,"abstract":"<p>Ruthenium (Ru) is a promising electrocatalyst for hydrogen oxidation reaction (HOR) due to the similar metal hydrogen bond energy to Pt. However, Ru is easily deactivated or dissolved under an oxidation potential, which makes it unavailable in proton exchange membrane fuel cells. In this work, ultrastable Ru-based electrocatalysts for HOR in high-temperature polymer electrolyte membrane fuel cells (HT-PEMFCs) were developed by Mo doping. Under the operation conditions of HT-PEMFCs, thermal reduction inhibited the production of amorphous Ru oxide (RuO<sub>2</sub>) in the Ru-based electrocatalysts during the HOR. Mo doping significantly improved the stability of the electrocatalyst by decreasing the reduction temperature of RuO<sub>2</sub> and accelerating the HOR by reducing the adsorption of H*. RuMo/C exhibited excellent HOR activity at high temperatures due to thermal reduction inhibition of electrooxidation; the fabricated HT-PEMFCs exhibited long-term stability and a 1050 mW cm<sup>−2</sup> peak power density, comparable to the commercial Pt catalyst. This work provides a novel strategy for designing electrocatalysts by combining material intrinsic properties and work conditions, which could promote the development of advanced electrocatalysts for HT-PEMFCs.</p>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"24 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142225317","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
Integrating Pd(I) Atoms in Schottky Junctions for Visible-Light-Driven Urea Production from Ambient Nitrogenous Species and CO 2 在肖特基结中整合钯（I）原子，利用可见光驱动环境含氮物质和 CO 2 生产尿素
IF 11.2 1区 化学
CCS Chemistry Pub Date : 2024-08-13 DOI: 10.31635/ccschem.024.202404490
Wei-Yao Hu, Qi-Yuan Li, Dong Xu, Peng Gao, Pan-Zhe Qiao, Dong Li, Si-Yuan Xia, Xiu Lin, Jie-Sheng Chen, Xin-Hao Li
{"title":"Integrating Pd(I) Atoms in Schottky Junctions for Visible-Light-Driven Urea Production from Ambient Nitrogenous Species and CO 2","authors":"Wei-Yao Hu, Qi-Yuan Li, Dong Xu, Peng Gao, Pan-Zhe Qiao, Dong Li, Si-Yuan Xia, Xiu Lin, Jie-Sheng Chen, Xin-Hao Li","doi":"10.31635/ccschem.024.202404490","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404490","url":null,"abstract":"<p>The mass production of urea, the most widely used agricultural fertilizer, usually relies on energy- and carbon-intensive processes. The light-driven synthesis path has great potential for more sustainable techniques to produce urea from abundant naturally occurring resources, but this method suffers from the use of pure CO<sub>2</sub> and high-energy-driven forces (high temperature or ultraviolet light). Herein, we present a mild photocatalytic pathway for urea production from diverse nitrogenous species (such as NO<sub>3</sub><sup>−</sup>, NH<sub>3</sub>, and N<sub>2</sub>) and diluted CO<sub>2</sub> using visible light. We designed a palladium (Pd)-doped Schottky heterojunction, composed of graphene and titanium dioxide, as an effective photocatalyst to achieve on-farm urea generation. With the injection of visible-light-generated hot electrons from graphene to TiO<sub>2</sub>, the as-integrated Pd(I) centers with a special oxidation state of +1.36 in the TiO<sub>2</sub> lattice can initiate the universal reaction path of cascade reduction of NO<sub>3</sub><sup>−</sup>/N<sub>2</sub> to NH<sub>3</sub> and resulting C–N coupling of CO<sub>2</sub> with as-formed or added NH<sub>3</sub> to transform diverse nitrogenous species and CO<sub>2</sub> into urea. The urea yield over the <i>at.</i>-Pd@TiO<sub>2</sub>/Gr photocatalyst is 1.62 mmol g<sup>−1</sup> h<sup>−1</sup> under visible-light irradiation with an apparent quantum yield of 1.05% at 400 nm and 0.39% even at 700 nm.</p>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"80 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142198474","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
Room-Temperature Self-Healing Glassy Thermosetting Polymers via Defective Network Design 通过缺陷网络设计实现室温自愈合玻璃态热固性聚合物
IF 11.2 1区 化学
CCS Chemistry Pub Date : 2024-08-06 DOI: 10.31635/ccschem.024.202404486
Hao Wang, Biqiang Jin, Haitao Wu, Changcheng Wang, Jinrong Wu
{"title":"Room-Temperature Self-Healing Glassy Thermosetting Polymers via Defective Network Design","authors":"Hao Wang, Biqiang Jin, Haitao Wu, Changcheng Wang, Jinrong Wu","doi":"10.31635/ccschem.024.202404486","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404486","url":null,"abstract":"<p>Glassy thermosetting polymers, which possess excellent mechanical properties, structural stability, and solvent resistance, cannot be healed and recycled due to the irreversible crosslinking network. Covalent adaptive networks could address these drawbacks, as their chemical networks are able to shuffle dynamic covalent bonds through exchange reactions, which nevertheless need high temperature or solvent assistance. Here we report a room-temperature self-healing glassy thermoset enabled by designing a disulfide-bond and H-bond hybridized network carrying abundant dangling chains, which are commonly known as network “defects.” However, the “defects” do not plasticize the polymer, as they are bound to network chains through H-bonds. Therefore, the polymer possesses high modulus and strength at room temperature. Importantly, the “defects” can drive the metathesis reaction of disulfide bonds and the rearrangement of H-bonds in the glassy state, enabling the thermosetting network to self-heal at and even below room temperature.</p>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"40 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2024-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141899870","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
Surface-Mediated Catalytic Dechlorination and Spin-State Modulation of ClFePc on Au(111) 金（111）上 ClFePc 的表面介导催化脱氯和自旋态调制
IF 11.2 1区 化学
CCS Chemistry Pub Date : 2024-08-06 DOI: 10.31635/ccschem.024.202404417
Jie Li, Chenyang Yuan, Yang He, Zhen Xu, Haoyang Pan, Shuai Lu, Yudi Wang, Mingjun Zhong, Xin Li, Shimin Hou, Qian Shen, Kai Wu, Yajie Zhang, Song Gao, , YongFeng Wang
{"title":"Surface-Mediated Catalytic Dechlorination and Spin-State Modulation of ClFePc on Au(111)","authors":"Jie Li, Chenyang Yuan, Yang He, Zhen Xu, Haoyang Pan, Shuai Lu, Yudi Wang, Mingjun Zhong, Xin Li, Shimin Hou, Qian Shen, Kai Wu, Yajie Zhang, Song Gao, , YongFeng Wang","doi":"10.31635/ccschem.024.202404417","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404417","url":null,"abstract":"<p>Interactions between molecules and surfaces are crucial in modern surface science. In particular, surfaces catalyze molecular reactions and modulate molecular spin states. In this article, we investigate the adsorption behaviors and electronic structures of chloro-iron phthalocyanine (ClFePc) on Au(111). Combining ultrahigh vacuum scanning tunneling microscopy experiments with density functional theory calculations, we found indications of surface-catalyzed dechlorination. Our findings reveal that the adsorption behavior of ClFePc is determined by its adsorption direction. ClFePc in the Cl-up (Cl pointing to the vacuum) configuration exhibits stable adsorption on the Au(111) surface. Conversely, the Cl-down (Cl pointing to the substrate) configuration is unstable, resulting in the dissociation of the Cl–Fe bond due to interactions with the Au(111) surface. Through scanning tunneling spectroscopy analysis, we further investigate the Kondo resonance features and spin characteristics. Notably, following dechlorination, the spin-state transitions from <i>S</i> = 3/2 to 1. This study provides profound insights into the surface-molecule interaction and its application in modulating magnetic properties.</p>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"21 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2024-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141899869","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
Leveraging Adsorption Kinetics and Thermodynamics in a Channel-Pore Interconnected Metal–Organic Framework for Stepwise Splitting Hexanes 利用通道-孔隙互连金属有机框架中的吸附动力学和热力学原理逐步拆分己烷
IF 11.2 1区 化学
CCS Chemistry Pub Date : 2024-08-06 DOI: 10.31635/ccschem.024.202404180
{"title":"Leveraging Adsorption Kinetics and Thermodynamics in a Channel-Pore Interconnected Metal–Organic Framework for Stepwise Splitting Hexanes","authors":"","doi":"10.31635/ccschem.024.202404180","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404180","url":null,"abstract":"CCS Chemistry, Ahead of Print.<br/>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"17 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2024-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141899710","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
Twenty-Step Total Synthesis of (+)-Phorbol 二十步全合成 (+)-Phorbol
IF 11.2 1区 化学
CCS Chemistry Pub Date : 2024-08-06 DOI: 10.31635/ccschem.024.202404505
{"title":"Twenty-Step Total Synthesis of (+)-Phorbol","authors":"","doi":"10.31635/ccschem.024.202404505","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404505","url":null,"abstract":"CCS Chemistry, Ahead of Print.<br/>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"38 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2024-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141899865","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
Efficient N-Trifluoromethylation of Amines with Carbon Disulfide and Silver Fluoride as Reagents 以二硫化碳和氟化银为试剂高效进行胺的 N-三氟甲基化反应
IF 11.2 1区 化学
CCS Chemistry Pub Date : 2024-08-06 DOI: 10.31635/ccschem.024.202404432
Haixia Song, Qin Wang, Xiaoying Wang, Yinbin Zhang, Xin-Hua Duan, Mingyou Hu
{"title":"Efficient N-Trifluoromethylation of Amines with Carbon Disulfide and Silver Fluoride as Reagents","authors":"Haixia Song, Qin Wang, Xiaoying Wang, Yinbin Zhang, Xin-Hua Duan, Mingyou Hu","doi":"10.31635/ccschem.024.202404432","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404432","url":null,"abstract":"<p>The installation of a trifluoromethyl group onto a nitrogen atom can effectively modulate the basicity of amines owing to the strong electron-withdrawing effect of fluorine. Nevertheless, efficient and operationally simple methods for <i>N</i>-trifluoromethylation of amines are yet to be developed. This protocol involves the use of readily available secondary amines as starting materials, along with CS<sub>2</sub> and AgF as the <i>N</i>-trifluoromethylation reagents, enabling the target molecules to be synthesized in a single step. The versatility of our method was demonstrated by successfully synthesizing <i>N,N</i>-dialkyl and <i>N</i>-(hetero)aromatic <i>N</i>-CF<sub>3</sub>-containing compounds with various substituents. Moreover, this methodology has been successfully applied to the late-stage modification of complex bioactive molecules, facilitating the synthesis of <i>N</i>-CF<sub>3</sub> drug bioisosteres and <i>N</i>-CF<sub>3</sub>-tailored amino acids, which would broadly stimulate the drug discovery of <i>N</i>-CF<sub>3</sub> containing molecules.</p>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"75 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2024-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141899868","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
Molecular Bowls Protecting Guests from Oxidation 保护客人免受氧化的分子碗
IF 11.2 1区 化学
CCS Chemistry Pub Date : 2024-08-06 DOI: 10.31635/ccschem.024.202404512
Yating Wu, Yueyan Kuang, Shuai Fang, Chenqi Ge, Hua Tang, Jizeng Sun, Shaoying Huang, Simon Duttwyler, Xufeng Lin, Hao Li
{"title":"Molecular Bowls Protecting Guests from Oxidation","authors":"Yating Wu, Yueyan Kuang, Shuai Fang, Chenqi Ge, Hua Tang, Jizeng Sun, Shaoying Huang, Simon Duttwyler, Xufeng Lin, Hao Li","doi":"10.31635/ccschem.024.202404512","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404512","url":null,"abstract":"<p>Two structurally analogous self-assembled bowl-shaped hosts were obtained in close to quantitative yields via hydrazone condensation in acidic aqueous media, where the dynamic nature of hydrazone bonds was activated. Each bowl bears nine positive charges, endowing it with good water solubility. The bowls can thus take advantage of the hydrophobic effect and/or electrostatic forces to recognize neutral or anionic guests. Upon being accommodated within the host cavity, an anthracene derivative was protected from UV-stimulated oxidation.</p>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"83 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2024-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141899866","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
Author Spotlight 作者聚焦
IF 11.2 1区 化学
CCS Chemistry Pub Date : 2024-08-01 DOI: 10.31635/ccschem.024.202400720ed2
{"title":"Author Spotlight","authors":"","doi":"10.31635/ccschem.024.202400720ed2","DOIUrl":"https://doi.org/10.31635/ccschem.024.202400720ed2","url":null,"abstract":"CCS Chemistry, Volume 6, Issue 8, Page 1840-1843, August 2024.<br/>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"14 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141884706","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
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