Chem最新文献_第6页

Recycling homocarbon backbone polymers toward a circular materials economy

IF 19.1 1区化学

Chem Pub Date : 2025-03-13 DOI: 10.1016/j.chempr.2024.102406

Jie Zheng , Zhuang Mao Png , Xin Yi Oh , Huanning Zuo , Zibiao Li

{"title":"Recycling homocarbon backbone polymers toward a circular materials economy","authors":"Jie Zheng , Zhuang Mao Png , Xin Yi Oh , Huanning Zuo , Zibiao Li","doi":"10.1016/j.chempr.2024.102406","DOIUrl":"10.1016/j.chempr.2024.102406","url":null,"abstract":"<div><div>Global plastic waste has reached a critical level, posing serious hazards to ecosystems and human health because of its persistent presence in landfills, oceans, and natural environments. Unlike heteroatom-backbone polymers, which feature a heterochain structure, homocarbon backbone polymers with nonpolar C–C backbones exhibit unprecedented durability and resistance to environmental factors, making them less prone to degradation. Consequently, the conversion of such plastic waste into valuable chemicals via chemical recycling presents a crucial solution to address the issues stemming from plastic waste. This review aims to summarize the latest developments in the closed-loop recycling and upcycling of homocarbon backbone polymers with a specific focus on the conversion of waste plastics into their original monomers and/or value-added chemicals through bio-, thermo-, and photocatalysis, which promotes a circular economy. Notably, the development of highly active catalysts and related depolymerization systems accelerates the evolution of plastic degradation and enhances product controllability, rendering the recycling of plastic waste feasible and affordable.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 3","pages":"Article 102406"},"PeriodicalIF":19.1,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375294","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

Excited-state protonation and reduction enable the umpolung Birch reduction of naphthalenes 激发态质子化和还原使萘的umpolung Birch 还原成为可能

IF 19.1 1区化学

Chem Pub Date : 2025-03-13 DOI: 10.1016/j.chempr.2024.10.009

Javier Corpas , Eva Rivera-Chao , Enrique M. Arpa , Miguel Gomez-Mendoza , Yuri Katayama , Victor A. de la Peña O’Shea , Céline Bouchel , Clément Jacob , Pierre-Georges Echeverria , Alessandro Ruffoni , Daniele Leonori

{"title":"Excited-state protonation and reduction enable the umpolung Birch reduction of naphthalenes","authors":"Javier Corpas , Eva Rivera-Chao , Enrique M. Arpa , Miguel Gomez-Mendoza , Yuri Katayama , Victor A. de la Peña O’Shea , Céline Bouchel , Clément Jacob , Pierre-Georges Echeverria , Alessandro Ruffoni , Daniele Leonori","doi":"10.1016/j.chempr.2024.10.009","DOIUrl":"10.1016/j.chempr.2024.10.009","url":null,"abstract":"<div><div>The Birch reaction is a classical process used for the partial reduction of aromatics into non-conjugated cyclohexadienes that can be further functionalized. This strategy and its more modern variants are all based on an initial single-electron transfer event converting the arene into the corresponding radical anion for either protonation or hydrogen-atom transfer. Herein, we demonstrate an umpolung approach where the aromatic is first protonated to its corresponding carbocation and then reduced using the Lewis acid-base complex Et<sub>3</sub>N−BH<sub>3</sub>. This strategy requires aromatic photoexcitation so that protonation is favored by charge-transfer and driven by excited-state antiaromaticity relief. This means that aromatic excited-state basicity rather than ground-state redox potential needs to be considered when approaching reaction development. The mild conditions and the avoidance of strong reductants have enabled tolerance of functionalities generally not compatible under standard Birch conditions.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 3","pages":"Article 102342"},"PeriodicalIF":19.1,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142684996","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Cluster-based redox-responsive super-atomic MRI contrast agents 基于簇的氧化还原反应超原子核磁共振成像造影剂

IF 19.1 1区化学

Chem Pub Date : 2025-03-13 DOI: 10.1016/j.chempr.2024.09.029

Alexandros A. Kitos , Raúl Castañeda , Zachary J. Comeau , Niki Mavragani , Nicholas D. Calvert , Alexia Kirby , Francisco M. Martinez-Santiesteban , Peter J. Pallister , Timothy J. Scholl , Muralee Murugesu , Adam J. Shuhendler , Jaclyn L. Brusso

{"title":"Cluster-based redox-responsive super-atomic MRI contrast agents","authors":"Alexandros A. Kitos , Raúl Castañeda , Zachary J. Comeau , Niki Mavragani , Nicholas D. Calvert , Alexia Kirby , Francisco M. Martinez-Santiesteban , Peter J. Pallister , Timothy J. Scholl , Muralee Murugesu , Adam J. Shuhendler , Jaclyn L. Brusso","doi":"10.1016/j.chempr.2024.09.029","DOIUrl":"10.1016/j.chempr.2024.09.029","url":null,"abstract":"<div><div>Transition metal molecular clusters hold great promise as magnetic resonance imaging (MRI) probes, where careful chemical design can afford control over the size, shape, and total spin state of the contrast agent (CA). Although such clusters can act as a single entity, exhibiting advanced <em>in situ</em> reactivity to key diagnostic biomolecules, their dissociation/speciation in biological media hinders their potential as MRI CAs. To resolve this, the <em>N</em>-2-pyrimidylimidoyl-2-pyrimidylamidine chelate was employed to selectively bind 3d metal ions, forming highly stable mixed-metal clusters. Through spectroscopic, electrochemical, and magnetic analysis, along with <em>in vitro</em> and <em>in vivo</em> studies, the application of iron and manganese homo- and heterometallic complexes as MRI CAs capable of mapping tumor redox status through a simple <em>T</em><sub>1</sub>w/<em>T</em><sub>2</sub>w ratiometric approach was demonstrated. The use of heteropolynuclear 3d super-atomic complexes suitable for semi-quantitative <em>in vivo</em> MRI of tissue redox status opens new avenues for non-invasive characterization of biochemical microenvironments by MRI.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 3","pages":"Article 102330"},"PeriodicalIF":19.1,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452210","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

Interfacial solvation-structure effects of molecularly dispersed CoPc catalysts on CO2 electrochemical conversion

IF 19.1 1区化学

Chem Pub Date : 2025-03-13 DOI: 10.1016/j.chempr.2025.102458

Ning Han , Xianqiang Xiong , Mohamed Noufal , Bo Weng , Alain R. Puente-Santiago

引用次数: 0

Next-generation de novo luciferases: How artificial intelligence is improving its own designs at light speed

IF 19.1 1区化学

Chem Pub Date : 2025-03-13 DOI: 10.1016/j.chempr.2025.102491

Yosta de Stigter , Maarten Merkx

引用次数: 0

Structural stability of a bent tetra(amino)tetraborane ring across four charge states

IF 19.1 1区化学

Chem Pub Date : 2025-03-13 DOI: 10.1016/j.chempr.2024.10.005

Eva Beck , Ivo Krummenacher , Thomas Kupfer , Maximilian Dietz , Maximilian Michel , Kai Hammond , Holger Braunschweig

引用次数: 0

A roadmap toward the synthesis of life

IF 19.1 1区化学

Chem Pub Date : 2025-03-13 DOI: 10.1016/j.chempr.2024.102399

Christine M.E. Kriebisch , Olga Bantysh , Lorena Baranda Pellejero , Andrea Belluati , Eva Bertosin , Kun Dai , Maria de Roy , Hailin Fu , Nicola Galvanetto , Julianne M. Gibbs , Samuel Santhosh Gomez , Gaetano Granatelli , Alessandra Griffo , Maria Guix , Cenk Onur Gurdap , Johannes Harth-Kitzerow , Ivar S. Haugerud , Gregor Häfner , Pranay Jaiswal , Sadaf Javed , Job Boekhoven

{"title":"A roadmap toward the synthesis of life","authors":"Christine M.E. Kriebisch , Olga Bantysh , Lorena Baranda Pellejero , Andrea Belluati , Eva Bertosin , Kun Dai , Maria de Roy , Hailin Fu , Nicola Galvanetto , Julianne M. Gibbs , Samuel Santhosh Gomez , Gaetano Granatelli , Alessandra Griffo , Maria Guix , Cenk Onur Gurdap , Johannes Harth-Kitzerow , Ivar S. Haugerud , Gregor Häfner , Pranay Jaiswal , Sadaf Javed , Job Boekhoven","doi":"10.1016/j.chempr.2024.102399","DOIUrl":"10.1016/j.chempr.2024.102399","url":null,"abstract":"<div><div>The synthesis of life from non-living matter has captivated and divided scientists for centuries. This bold goal aims at unraveling the fundamental principles of life and leveraging its unique features, such as its resilience, sustainability, and ability to evolve. Synthetic life represents more than an academic milestone—it has the potential to revolutionize biotechnology, medicine, and materials science. Although the fields of synthetic biology, systems chemistry, and biophysics have made great strides toward synthetic life, progress has been hindered by social, philosophical, and technical challenges, such as vague goals, misaligned interdisciplinary efforts, and incompletely addressing public and ethical concerns. Our perspective offers a roadmap toward the synthesis of life based on discussions during a 2-week workshop with scientists from around the globe.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 3","pages":"Article 102399"},"PeriodicalIF":19.1,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143192477","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Borohydride oxidation-water reduction fuel cells advanced by local hydroxyl enrichment-inhibited borohydride hydrolysis on Cu(0) sites 通过局部羟基富集抑制铜（0）位上的硼氢化物水解推进硼氢化物氧化-水还原燃料电池的发展

IF 19.1 1区化学

Chem Pub Date : 2025-03-13 DOI: 10.1016/j.chempr.2024.09.030

Libo Zhu , Chang Chen , Tiantian Wu , Xu Yu , Han Tian , Fantao Kong , Ziwei Chang , Wenshu Luo , Xiangzhi Cui , Jianlin Shi

{"title":"Borohydride oxidation-water reduction fuel cells advanced by local hydroxyl enrichment-inhibited borohydride hydrolysis on Cu(0) sites","authors":"Libo Zhu , Chang Chen , Tiantian Wu , Xu Yu , Han Tian , Fantao Kong , Ziwei Chang , Wenshu Luo , Xiangzhi Cui , Jianlin Shi","doi":"10.1016/j.chempr.2024.09.030","DOIUrl":"10.1016/j.chempr.2024.09.030","url":null,"abstract":"<div><div>A promising fuel cell using the acidic hydrogen evolution reaction (HER) instead of kinetically sluggish oxygen reduction reaction to couple with the borohydride oxidation reaction (BOR) has been established. This BOR-HER fuel cell (BHFC) has achieved the concurrent electricity generation and hydrogen production. To catalyze HER/BOR, a copper (Cu)-doped cobalt phosphide nanosheet grown on Cu foam (Cu–CoP/CF) was developed, which exhibits significantly inhibited competitive NaBH<sub>4</sub> hydrolysis during BOR, along with excellent HER performance and stability over 700 h. Specifically, the Cu(0), <em>in situ</em> formed on the surface of Cu–CoP/CF, plays a decisive role in creating an OH<sup>−</sup>-enriched local environment, resulting in significantly inhibited borohydride hydrolysis but greatly enhanced BOR selectivity of up to 85%, as well as the reduced thermodynamic barrier of BOR. The assembled BHFC equipped with Cu–CoP/CF is capable of generating a high power density of 114 mW cm<sup>−2</sup> and concurrently producing hydrogen at a rate of at least 40 mol h<sup>−1</sup> m<sup>−2</sup> at cathode.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 3","pages":"Article 102331"},"PeriodicalIF":19.1,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452039","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

Synthesis of securingine B enables photoresponsive materials design 合成 securingine B 可实现光致发光材料的设计

IF 19.1 1区化学

Chem Pub Date : 2025-03-13 DOI: 10.1016/j.chempr.2024.10.003

Sangbin Park , Gyumin Kang , Wantae Kim , Sieun Jeon , Myung-Kun Chung , Hee-Seung Lee , Dong Ki Yoon , Sunkyu Han

{"title":"Synthesis of securingine B enables photoresponsive materials design","authors":"Sangbin Park , Gyumin Kang , Wantae Kim , Sieun Jeon , Myung-Kun Chung , Hee-Seung Lee , Dong Ki Yoon , Sunkyu Han","doi":"10.1016/j.chempr.2024.10.003","DOIUrl":"10.1016/j.chempr.2024.10.003","url":null,"abstract":"<div><div>In general, natural products exist in their most thermodynamically stable form. Therefore, final stage-reaction conditions leading to thermodynamic equilibrium often facilitate the production of the desired natural products. On the other hand, syntheses of contra-thermodynamic natural products pose greater challenges, as the thermodynamic bias should be overcome. Herein, we present the synthesis of contra-thermodynamic securinega alkaloid securingine B, derived from the more thermodynamically stable isomer secu’amamine D. Harnessing the disparity in triplet energy between two natural products, we have established a photochemical equilibrium favoring securingine B. Conversely, secu’amamine D was reformed from securingine B under thermodynamic equilibrium conditions. Inspired by these observations, we devised a novel type of photoswitching platform by introducing a push-pull system to the securinega framework. By leveraging this new photoswitching scaffold, we have developed a securingine B-inspired photochromic material and, subsequently, exploited it as a photoresponsive chiral dopant.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 3","pages":"Article 102336"},"PeriodicalIF":19.1,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142556281","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

Direct production of o-xylene from six-component BTEXs using a channel-pore interconnected metal-organic framework 利用槽孔互连金属有机框架从六组分 BTEX 直接生产邻二甲苯

IF 19.1 1区化学

Chem Pub Date : 2025-03-13 DOI: 10.1016/j.chempr.2024.10.006

Xiao-Jing Xie , Heng Zeng , Yong-Liang Huang , Ying Wang , Qi-Yun Cao , Weigang Lu , Dan Li

{"title":"Direct production of o-xylene from six-component BTEXs using a channel-pore interconnected metal-organic framework","authors":"Xiao-Jing Xie , Heng Zeng , Yong-Liang Huang , Ying Wang , Qi-Yun Cao , Weigang Lu , Dan Li","doi":"10.1016/j.chempr.2024.10.006","DOIUrl":"10.1016/j.chempr.2024.10.006","url":null,"abstract":"<div><div>Metal-organic frameworks (MOFs) with precisely controlled pore dimensions have greatly enriched the versatility of molecular sieving materials. Here, we report a channel-pore interconnected MOF (JNU-2) for direct production of <em>o</em>-xylene from six-component BTEXs (benzene, toluene, ethylbenzene, <em>o</em>-xylene, <em>m</em>-xylene, and <em>p</em>-xylene) in a single adsorption process. Individual adsorption measurements show complete exclusion of <em>o</em>-xylene and benchmark adsorption of other BTEXs. Competitive adsorption studies reveal record-high adsorption selectivity of other BTEXs over <em>o</em>-xylene. Vapor-phase breakthrough experiments verify its superior separation potential for sieving <em>o</em>-xylene from BTEXs. We further demonstrate <em>o</em>-xylene purification by simply soaking JNU-2 (10 g) in BTEXs (18 mL, 90% <em>o</em>-xylene) at room temperature, realizing an average of 15.2 mL of <em>o</em>-xylene (99.5%+ purity, 94% recovery) for 10 cycles. Considering its exceptional stability, JNU-2 may have great promise for energy-efficient <em>o</em>-xylene separation from BTEXs.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 3","pages":"Article 102339"},"PeriodicalIF":19.1,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142562007","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