IF 23.5 1区化学

Chem Pub Date : 2026-04-15 DOI: 10.1016/j.chempr.2026.103025

Wen Wang, Xinyuan Zhao, Qi Li, Yue Zhang, Qifan Wang, Yao Xie, Fangyu Ren, Shengli Hou, Bin Zhao

{"title":"Bimetallic synergistic catalysis in MOFs toward transforming CO2 into carbonates with a record turnover number","authors":"Wen Wang, Xinyuan Zhao, Qi Li, Yue Zhang, Qifan Wang, Yao Xie, Fangyu Ren, Shengli Hou, Bin Zhao","doi":"10.1016/j.chempr.2026.103025","DOIUrl":"https://doi.org/10.1016/j.chempr.2026.103025","url":null,"abstract":"The synthesis of asymmetric carbonates from renewable CO2 is important for sustainable chemistry but often suffers from low efficiency, harsh reaction conditions, and noble metal catalysts. Achieving this efficient transformation under mild conditions by non-noble metal catalysts remains a great challenge. Herein, a framework {[In3(μ3-O)(H2O)Cu4(CPT)4I2]⋅(NO3)⋅1.5H2O⋅3DMF}n (CuIn-CPT, CPT = 3,5-bis(4′-carboxyphenyl)-1,2,4-triazole) was synthesized, assembled from a [Cu12In18] nanocage with multiple CuI and InIII Lewis acid sites, and it exhibits good thermal and chemical stabilities. It achieves up to 98% yield in multicomponent reactions of CO2, propargyl alcohols, and primary alcohols without solvent under mild conditions, with a record turnover number of 4,844—ten times higher than top Ag-based catalysts—and excellent recyclability over 10 cycles. Density functional theory (DFT) calculations and mechanistic studies confirm that the synergistic effect between [Cu4] and [In3] clusters enhances catalytic efficiency. This work provides an inspiration for developing efficient non-noble metal heterogeneous catalysts in CO2 conversion.","PeriodicalId":268,"journal":{"name":"Chem","volume":"323 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2026-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147709289","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

Programming extracellular protein fate with peptide chimeras 利用肽嵌合体编程细胞外蛋白命运

IF 23.5 1区化学

Chem Pub Date : 2026-04-14 DOI: 10.1016/j.chempr.2026.103040

Jun Liao, Zhiqiang Lin, Chuang Liu

引用次数: 0

Predict the ceiling 预测天花板

IF 23.5 1区化学

Chem Pub Date : 2026-04-14 DOI: 10.1016/j.chempr.2026.102970

Xiaoyu Xie, Rong Tong

引用次数: 0

Integrated transient chromophores for efficient photo-induced radiofluorination 集成瞬态发色团用于有效的光诱导放射性氟化

IF 19.6 1区化学

Chem Pub Date : 2026-04-09 Epub Date: 2026-03-04 DOI: 10.1016/j.chempr.2025.102908

Zhengbo Zhu , Chia-Yu Huang , Richard W. Russell , Peyton Kinon , Xinrui Ma , Yifan Mao , Xuedan Wu , Zhanhong Wu , David A. Nicewicz , Zibo Li

{"title":"Integrated transient chromophores for efficient photo-induced radiofluorination","authors":"Zhengbo Zhu , Chia-Yu Huang , Richard W. Russell , Peyton Kinon , Xinrui Ma , Yifan Mao , Xuedan Wu , Zhanhong Wu , David A. Nicewicz , Zibo Li","doi":"10.1016/j.chempr.2025.102908","DOIUrl":"10.1016/j.chempr.2025.102908","url":null,"abstract":"<div><div>Photoredox catalysis has emerged as a powerful tool in organic synthesis, enabling substrate activation via visible light in the presence of an external photocatalyst. However, reliance on bimolecular interactions between the photoexcited catalyst and substrate limits efficiency, a critical drawback for applications such as radiolabeling. To address this challenge, we report a molecular design strategy that bypasses this constraint by integrating a transient chromophore directly into the substrate. This approach eliminates diffusion-dependent activation, achieving highly efficient transformations through a self-correcting mechanism: reactive intermediates either engage nucleophilic addition or revert to the ground state via decay, minimizing side reactions. The transient chromophore additionally acts as a charged leaving group, enabling facile purification of the neutral labeled product. We demonstrate this strategy in radiofluorination reactions, achieving superior yields and simplicity compared with conventional photoredox methods. Its utility is highlighted by the synthesis of positron emission tomography (PET) tracers for oncology, neurology, and cardiology.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 4","pages":"Article 102908"},"PeriodicalIF":19.6,"publicationDate":"2026-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147360101","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

Improving productivity and stability for CO2 hydrogenation by using pincer-ligated Mn complexes with hemilabile ligands 利用半可溶配体螯合Mn配合物提高CO2加氢效率和稳定性

IF 19.6 1区化学

Chem Pub Date : 2026-04-09 Epub Date: 2026-01-05 DOI: 10.1016/j.chempr.2025.102833

Justin C. Wedal , Kyler B. Virtue , Wesley H. Bernskoetter , Nilay Hazari , Brandon Q. Mercado , Nicole Piekut

{"title":"Improving productivity and stability for CO2 hydrogenation by using pincer-ligated Mn complexes with hemilabile ligands","authors":"Justin C. Wedal , Kyler B. Virtue , Wesley H. Bernskoetter , Nilay Hazari , Brandon Q. Mercado , Nicole Piekut","doi":"10.1016/j.chempr.2025.102833","DOIUrl":"10.1016/j.chempr.2025.102833","url":null,"abstract":"<div><div>Pincer ligands are widely used to support transition-metal catalysts, but first-row systems often deactivate too quickly for widespread use. Here, pincer ligands bearing an additional hemilabile donor were designed to stabilize Mn catalysts for CO2 hydrogenation to formate. Ligands of the type (RCH2CH2)N(CH2CH2PiPr2)2 (iPrPNRP; R = OMe, CH2OMe, NMe2, PiPr2) were synthesized and coordinated to Mn to form complexes of the type (iPrPNRP)Mn(CO)2H. Their performance was compared with that of {MeN(CH2CH2PiPr2)2}Mn(CO)2H, which lacks a pendant donor. The pendant donor identity and arm length strongly influenced catalytic activity, but all pendant-arm-containing systems extended catalyst lifetime. Notably, (iPrPNCH2OMeP)Mn(CO)2H achieved turnover frequencies of 158,000 h−1 and turnover numbers of 838,000, exceeding most state-of-the-art catalysts. Mechanistic studies revealed that hemilabile coordination enhances stability by avoiding deactivation, although excessive binding can lead to inactive states. This work demonstrates that hemilabile donors dramatically improve pincer-based Mn catalysts and provides design principles for broader applications.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 4","pages":"Article 102833"},"PeriodicalIF":19.6,"publicationDate":"2026-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147636777","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 critical assessment of fluorescent probes as cellular reporters for thioredoxin system enzyme activities 荧光探针作为硫氧还蛋白系统酶活性的细胞报告者的关键评估

IF 19.6 1区化学

Chem Pub Date : 2026-04-09 Epub Date: 2026-02-02 DOI: 10.1016/j.chempr.2025.102868

Karoline C. Scholzen , Lukas Zeisel , Elias S.J. Arnér

引用次数: 0

Highly selective and efficient uranium recovery by size-sieving porous aromatic frameworks with rigidly functionalized windows 高选择性和高效的铀回收的大小筛选多孔芳香框架与刚性功能化窗口

IF 19.6 1区化学

Chem Pub Date : 2026-04-09 Epub Date: 2025-11-05 DOI: 10.1016/j.chempr.2025.102814

Lei Cui , Wanning Wu , Ethan R. Pezoulas , Jiangtao Jia , Zheng Bian , Jeffrey R. Long , Guangshan Zhu

{"title":"Highly selective and efficient uranium recovery by size-sieving porous aromatic frameworks with rigidly functionalized windows","authors":"Lei Cui , Wanning Wu , Ethan R. Pezoulas , Jiangtao Jia , Zheng Bian , Jeffrey R. Long , Guangshan Zhu","doi":"10.1016/j.chempr.2025.102814","DOIUrl":"10.1016/j.chempr.2025.102814","url":null,"abstract":"<div><div>Implementing marine uranium extraction is crucial for maintaining a continuous supply of fuel for nuclear reactors. Many adsorbents leverage oxime or amidoxime functional groups to bind uranyl ions, but the competitive adsorption of orthovanadate inhibits their practical application. Despite the high affinity of these ligands for binding both uranyl and orthovanadate, the different steric profiles of the two ions could be leveraged for their separation. Here, porous aromatic frameworks (PAFs) functionalized with oxime and amidoxime groups (PAF-1-O and PAF-1-AO) were synthesized and tested for their size-sieving capabilities. In both materials, the narrow pore size and rigid nature of the framework lead to the exclusion of the larger orthovanadate ions, whereas the smaller uranyl ions penetrate the framework and are readily adsorbed by the binding groups. In a binary mixture of uranyl and orthovanadate ions (∼2 mg L−1 each), PAF-1-O and PAF-1-AO both exhibit near-perfect adsorption selectivity for uranyl. In an unmodified sample of seawater, PAF-1-AO reached a uranium-adsorption capacity of 11.5 mg g−1 within 28 days and a record uranium-to-vanadium (U/V) selectivity of 243. The sieving-based selectivity exhibited by these PAF materials offers a promising new prospect for the extraction of uranium from seawater.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 4","pages":"Article 102814"},"PeriodicalIF":19.6,"publicationDate":"2026-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145441721","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

Breaking ampere-level current density limitations in multi-carbon products through crystal facet engineering 通过晶面工程突破多碳产品的电流密度限制

IF 19.6 1区化学

Chem Pub Date : 2026-04-09 Epub Date: 2025-11-20 DOI: 10.1016/j.chempr.2025.102824

Xi Cao , Yan Liu , Rui Yu , Yan Yang , Ang Li , Xinyang Li , Junjie Mao

{"title":"Breaking ampere-level current density limitations in multi-carbon products through crystal facet engineering","authors":"Xi Cao , Yan Liu , Rui Yu , Yan Yang , Ang Li , Xinyang Li , Junjie Mao","doi":"10.1016/j.chempr.2025.102824","DOIUrl":"10.1016/j.chempr.2025.102824","url":null,"abstract":"<div><div>The structural regulation of copper-based catalysts is an effective strategy for realizing the electroreduction of carbon dioxide to multi-carbon (C2+) products. However, the complexity of product distribution and reaction pathways limits the achievable ampere-level current densities for C2+ products. Herein, a crystal facet engineering strategy was developed to delicately balance the protonation processes, enabling the selective formation of C2+ products at ampere-level current densities. The balance between proton activation, ∗CO formation, and C–C coupling was achieved by the in situ generation of defect sites and the control of the Cu(111)/Cu(100) ratio, overcoming current density limitations. Notably, the optimized catalyst sustained a Faradaic efficiency (FE) for C2+ products exceeding 80%, with current density increasing from 0.4 to 1.7 A cm−2 and a yield of 4.29 mmol h−1cm−2 in a flow cell. In a large-scale membrane electrode assembly, an industrial current of 15 A maintained 80% FE, achieving a yield of 39 mmol h−1.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 4","pages":"Article 102824"},"PeriodicalIF":19.6,"publicationDate":"2026-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145554871","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

Chelation logic in a horseshoe ligand design for durable 2D perovskites 持久二维钙钛矿马蹄配体设计中的螯合逻辑

IF 19.6 1区化学

Chem Pub Date : 2026-04-09 Epub Date: 2026-03-26 DOI: 10.1016/j.chempr.2026.103028

Mercouri G. Kanatzidis

引用次数: 0

(R)evolutionary energy-storage density: Dewar pyrimidones inspired by nature (R)进化能量储存密度：杜瓦嘧啶类灵感来自大自然

IF 19.6 1区化学

Chem Pub Date : 2026-04-09 Epub Date: 2026-03-30 DOI: 10.1016/j.chempr.2026.103031

Sarah Plutzar , Lorette Fernandez , Rebecca J. Salthouse , Pedro Ferreira , Liang Fei , Vitor A.S. Almodovar , Jacob L. Elholm , Kasper Moth-Poulsen

引用次数: 0

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