IF 19.1 1区化学

Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.10.017

Niklas Sülzner

引用次数: 0

Self-activated energy release cascade from anthracene-based solid-state molecular solar thermal energy storage systems 蒽基固态分子太阳能热储存系统的自激活能量释放级联

IF 19.1 1区化学

Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.06.033

Subhayan Chakraborty , Han P.Q. Nguyen , Junichi Usuba , Ji Yong Choi , Zhenhuan Sun , Cijil Raju , Gustavo Sigelmann , Qianfeng Qiu , Sungwon Cho , Stephanie M. Tenney , Katherine E. Shulenberger , Klaus Schmidt-Rohr , Jihye Park , Grace G.D. Han

{"title":"Self-activated energy release cascade from anthracene-based solid-state molecular solar thermal energy storage systems","authors":"Subhayan Chakraborty , Han P.Q. Nguyen , Junichi Usuba , Ji Yong Choi , Zhenhuan Sun , Cijil Raju , Gustavo Sigelmann , Qianfeng Qiu , Sungwon Cho , Stephanie M. Tenney , Katherine E. Shulenberger , Klaus Schmidt-Rohr , Jihye Park , Grace G.D. Han","doi":"10.1016/j.chempr.2024.06.033","DOIUrl":"10.1016/j.chempr.2024.06.033","url":null,"abstract":"<div><div>We introduce donor-acceptor substituted anthracenes as effective molecular solar thermal energy storage compounds that operate exclusively in the solid state. The donor-acceptor anthracenes undergo a visible light-induced [4+4] cycloaddition reaction, producing metastable cycloadducts—dianthracenes with quaternary carbons—and storing photon energy. The triggered cycloreversion of dianthracenes to anthracenes discharges the stored energy as heat in the order of 100 kJ/mol (200 J/g). The series of compounds displays remarkable self-heating, or cascading heat release, upon the initial triggering. Such self-activated energy release is enabled by the large energy storage in dianthracenes, low activation energy for their thermal reversion, and effective heat transfer to unreacted molecules in the solid state. This process mirroring the self-ignition of fossil fuels opens up opportunities to use dianthracenes as effective and renewable solid-state fuels that can release energy rapidly and completely upon initial activation.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3309-3322"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141746613","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 skeletally diverse library of bioactive natural-product-like compounds enabled by late-stage P450-catalyzed oxyfunctionalization 通过后期 P450 催化氧官能化作用，建立一个骨架多样化的生物活性天然产物类化合物库

IF 19.1 1区化学

Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.08.003

Andrew R. Bortz , John M. Bennett , Rudi Fasan

{"title":"A skeletally diverse library of bioactive natural-product-like compounds enabled by late-stage P450-catalyzed oxyfunctionalization","authors":"Andrew R. Bortz , John M. Bennett , Rudi Fasan","doi":"10.1016/j.chempr.2024.08.003","DOIUrl":"10.1016/j.chempr.2024.08.003","url":null,"abstract":"<div><div>Natural products have historically represented a major source of therapeutics and small-molecule probes for interrogating biological systems. Here, we describe the design and implementation of P450-mediated chemoenzymatic diversity-oriented synthesis (CeDOS), a strategy in which selective, regiodivergent P450-catalyzed oxyfunctionalizations are leveraged as key steps for enabling the skeletal rearrangement and diversification of a parent compound. Using this strategy and plant-derived parthenolide as the parent molecule, a structurally diverse library of over 50 unprecedented natural-product-like scaffolds was generated via divergent chemoenzymatic routes. Importantly, several members of this CeDOS library were found to exhibit notable cytotoxicity against human cancer cells as well as diversified anticancer activity profiles. This work demonstrates the power of CeDOS as a strategy for directing the construction and discovery of novel bioactive molecules, and it offers a blueprint for the broader application of this approach toward the creation and exploration of natural-product-like chemical libraries.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3488-3502"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142138190","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 high-throughput workflow to analyze sequence-conformation relationships and explore hydrophobic patterning in disordered peptoids 分析序列构象关系和探索无序蛋白胨疏水模式的高通量工作流程

IF 19.1 1区化学

Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.07.025

Erin C. Day , Supraja S. Chittari , Keila C. Cunha , Roy J. Zhao , James N. Dodds , Delaney C. Davis , Erin S. Baker , Rebecca B. Berlow , Joan-Emma Shea , Rishikesh U. Kulkarni , Abigail S. Knight

{"title":"A high-throughput workflow to analyze sequence-conformation relationships and explore hydrophobic patterning in disordered peptoids","authors":"Erin C. Day , Supraja S. Chittari , Keila C. Cunha , Roy J. Zhao , James N. Dodds , Delaney C. Davis , Erin S. Baker , Rebecca B. Berlow , Joan-Emma Shea , Rishikesh U. Kulkarni , Abigail S. Knight","doi":"10.1016/j.chempr.2024.07.025","DOIUrl":"10.1016/j.chempr.2024.07.025","url":null,"abstract":"<div><div>Understanding how a macromolecule’s primary sequence governs its conformational landscape is crucial for elucidating its function, yet these design principles are still emerging for macromolecules with intrinsic disorder. Herein, we introduce a high-throughput workflow that implements a practical colorimetric conformational assay, introduces a semi-automated sequencing protocol using matrix-assisted laser desorption/ionization and tandem mass spectrometry (MALDI-MS/MS), and develops a generalizable sequence-structure algorithm. Using a model system of 20mer peptidomimetics containing polar glycine and hydrophobic <em>N</em>-butylglycine residues, we identified nine classifications of conformational disorder and isolated 122 unique sequences across varied compositions and conformations. Conformational distributions of three compositionally identical library sequences were corroborated through atomistic simulations and ion mobility spectrometry coupled with liquid chromatography. A data-driven strategy was developed using existing sequence variables and data-derived “motifs” to inform a machine-learning algorithm toward conformation prediction. This multifaceted approach enhances our understanding of sequence-conformation relationships and offers a powerful tool for accelerating the discovery of materials with conformational control.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3444-3458"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142142935","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

Nanocellulose: New horizons in organic chemistry and beyond 纳米纤维素：有机化学及其他领域的新视野

IF 19.1 1区化学

Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.09.007

Sayad Doobary , Varvara Apostolopoulou-Kalkavoura , Aji P. Mathew , Berit Olofsson

引用次数: 0

Deuteration of arenes in pharmaceuticals via photoinduced solvated electrons 通过光诱导溶电子使药物中的炔烃发生氘化反应

IF 19.1 1区化学

Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.06.029

Yi Tao , Cuihua Jin , Chuanwang Liu , Jiawei Bu , Ling Yue , Xipan Li , Kangjiang Liang , Chengfeng Xia

引用次数: 0

Charge delocalization and global aromaticity in a partially fused 12-porphyrin nanoring 部分融合的 12-卟啉纳米中的电荷析出和全局芳香性

IF 19.1 1区化学

Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.06.034

Sebastian M. Kopp , Henrik Gotfredsen , Janko Hergenhahn , Arnau Rodríguez-Rubio , Jie-Ren Deng , He Zhu , Wojciech Stawski , Harry L. Anderson

{"title":"Charge delocalization and global aromaticity in a partially fused 12-porphyrin nanoring","authors":"Sebastian M. Kopp , Henrik Gotfredsen , Janko Hergenhahn , Arnau Rodríguez-Rubio , Jie-Ren Deng , He Zhu , Wojciech Stawski , Harry L. Anderson","doi":"10.1016/j.chempr.2024.06.034","DOIUrl":"10.1016/j.chempr.2024.06.034","url":null,"abstract":"<div><div>Aromatic and antiaromatic ring currents can reveal global electronic delocalization around the circumference of <em>π</em>-conjugated macrocycles, although these phenomena are poorly understood in large rings. Here, we present the template-directed synthesis of a fully <em>π</em>-conjugated cyclic porphyrin 12-mer consisting of six <em>β</em>,<em>meso</em>,<em>β</em>-edge-fused porphyrin dimers connected by six butadiyne bridges. The lowest energy <em>π</em>-<em>π</em>∗ absorption band of this partially fused nanoring is shifted far into the NIR, confirming strong <em>π</em>-conjugation around the circumference of the macrocycle. Investigation of the oxidized and reduced nanoring-template complex by <sup>1</sup>H and <sup>19</sup>F NMR spectroscopy demonstrates the presence of coherent global (anti)aromatic ring currents, consistent with DFT calculations. The stronger <em>π</em>-conjugation enables global charge delocalization even at low levels of oxidation or reduction. These findings open new avenues for the engineering of cyclic molecular wires.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3410-3427"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141754427","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

Advancements in cost-effective direct air capture technology 具有成本效益的直接空气捕获技术的进步

IF 19.1 1区化学

Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.09.025

Mihrimah Ozkan, Saeb Besarati, Christopher Gordon, Gaël Gobaille-Shaw, Noah McQueen

{"title":"Advancements in cost-effective direct air capture technology","authors":"Mihrimah Ozkan, Saeb Besarati, Christopher Gordon, Gaël Gobaille-Shaw, Noah McQueen","doi":"10.1016/j.chempr.2024.09.025","DOIUrl":"10.1016/j.chempr.2024.09.025","url":null,"abstract":"<div><div>Advancements in cost-effective direct air capture (DAC) technology have become critical in addressing climate change, with a particular emphasis on energy and cost reductions. Recent innovations have significantly decreased the energy requirements of DAC systems. In collaboration with experts from industry leaders such as Climeworks, Carbon Capture, Mission Zero, and Heirloom, the latest developments highlight DAC technology’s potential to become a viable and sustainable solution for large-scale CO₂ removal. These advancements include reductions in energy consumption to as low as 1,055 kWh per ton of CO₂ through electrochemical methods and strategic integration of renewable energy sources like geothermal power. Additionally, economies of scale achieved through bulk purchasing and streamlined manufacturing processes have lowered DAC modules’ per-unit cost. Financial incentives and supportive policies, such as the 45Q tax credit in the United States, enhance the economic feasibility of these technologies. These innovations underscore the substantial contributions of DAC technology to global climate change mitigation efforts, making it a promising solution for achieving significant reductions in atmospheric CO₂ levels.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3261-3265"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142662853","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

Dynamic vertical triplet energies: Understanding and predicting triplet energy transfer 动态垂直三重能：了解和预测三重能传递

IF 19.1 1区化学

Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.07.001

Mihai V. Popescu , Robert S. Paton

引用次数: 0

Cooperative hydrogenation catalysis at a constrained gallylene-nickel(0) interface 受约束的镓-镍（0）界面上的协同氢化催化作用

IF 23.5 1区化学

Chem Pub Date : 2024-11-13 DOI: 10.1016/j.chempr.2024.10.016

Till L. Kalkuhl, Israel Fernández, Terrance J. Hadlington

引用次数: 0

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