IF 23.5 1区化学

Chem Pub Date : 2026-03-31 DOI: 10.1016/j.chempr.2026.103003

Silin Song, Yasu Chen, Chen Zhu

引用次数: 0

Oxygen-atom replacement in non-strained cyclic ethers 非应变环醚中的氧原子置换

IF 23.5 1区化学

Chem Pub Date : 2026-03-30 DOI: 10.1016/j.chempr.2026.103000

Ying-Qi Zhang, Kang Zheng Yap, Shuo-Han Li, Felicia Wan Xin Lim, Ming Joo Koh

引用次数: 0

From absolute barriers to responsiveness: How London dispersion modulates kinetic-thermodynamic relationships 从绝对障碍到响应性：伦敦色散如何调节动力学-热力学关系

IF 23.5 1区化学

Chem Pub Date : 2026-03-30 DOI: 10.1016/j.chempr.2026.103004

Nilangshu Mandal, Guanqi Qiu

{"title":"From absolute barriers to responsiveness: How London dispersion modulates kinetic-thermodynamic relationships","authors":"Nilangshu Mandal, Guanqi Qiu","doi":"10.1016/j.chempr.2026.103004","DOIUrl":"https://doi.org/10.1016/j.chempr.2026.103004","url":null,"abstract":"While London dispersion (LD) is widely recognized for lowering reaction barriers, we show that it also modulates how barriers respond to thermodynamic driving force, representing a conceptual shift from absolute effects to system-level responsiveness. Here we show that LD modulates the Brønsted slope (α), a key measure of kinetic-thermodynamic responsiveness (ΔΔG‡/ΔΔG), revealing effects beyond simple barrier stabilization. Structural analyses further show that LD influences responsiveness both directly and through secondary effects, including changes in geometry and additional non-covalent interactions along the reaction coordinate. By conceptually isolating the thermodynamically independent consequences of LD, we establish dispersion as an active, tunable lever for modulating responsiveness. This reframing enables clearer distinctions between case-specific and systematic effects. We also demonstrate that accounting for this responsiveness is essential for correctly predicting selectivity. More broadly, this work demonstrates how dissecting intuitive outcomes can uncover overlooked causal frameworks governing chemical reactivity.","PeriodicalId":268,"journal":{"name":"Chem","volume":"5 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2026-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147577716","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

Screening, designing, and elucidating anti-dissolving dual atomic sites for highly durable proton exchange membrane fuel cells 高耐久质子交换膜燃料电池抗溶解双原子位的筛选、设计和阐明

IF 23.5 1区化学

Chem Pub Date : 2026-03-30 DOI: 10.1016/j.chempr.2026.103007

Jingwen Wang, Hongye Wang, Linjie Zhao, Yongming Xia, Xian Liang, Lipeng Zhang, Baoguang Mao, Lin Yang, Dong Liu, Yuqin Jiang, Zhengyu Bai, Zhongwei Chen, Chuangang Hu

{"title":"Screening, designing, and elucidating anti-dissolving dual atomic sites for highly durable proton exchange membrane fuel cells","authors":"Jingwen Wang, Hongye Wang, Linjie Zhao, Yongming Xia, Xian Liang, Lipeng Zhang, Baoguang Mao, Lin Yang, Dong Liu, Yuqin Jiang, Zhengyu Bai, Zhongwei Chen, Chuangang Hu","doi":"10.1016/j.chempr.2026.103007","DOIUrl":"https://doi.org/10.1016/j.chempr.2026.103007","url":null,"abstract":"Atomic Fe-based catalysts are promising cathode alternatives to Pt-based materials in proton exchange membrane fuel cells (PEMFCs) toward the oxygen reduction reaction (ORR), yet they suffer from substantial activity degradation during operation. By constructing a novel theoretical descriptor to evaluate the metal dissolution energy (Udiss) and ∗OH adsorption energy (ΔGOH), we transcend the bottleneck of the conventional trial-and-error strategy for Fe-M bimetallic atomic sites (BASs) and screen Cr-Fe as the optimal combination, exhibiting the highest Udiss and suitable ΔGOH for high ORR performance. The developed Cr-Fe BASs in N-doped carbon catalysts exhibit a substantially improved stability in PEMFCs, demonstrating over 55% retention of the initial current (from ca. 410 to 220 mA cm−2) after 210 h, compared with the state-of-the-art Fe single-atom catalysts (SACs). This work provides valuable insights into advancing non-precious metal catalysts for PEMFCs, bringing their commercialization one step closer.","PeriodicalId":268,"journal":{"name":"Chem","volume":"46 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2026-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147586176","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

Regulating the topology and pore size of covalent metal-organic framework for boosting catalytic CO2 conversion 调节共价金属-有机骨架的拓扑结构和孔径以促进催化CO2转化

IF 23.5 1区化学

Chem Pub Date : 2026-03-30 DOI: 10.1016/j.chempr.2026.103006

Xu Chen, Yu-Yang Li, Zhi-Hong Lin, Jing-Yi Song, Ri-Qin Xia, Chuang-Wei Zhou, Yu-Mei Wang, Yu Han, Hai-Long Jiang, Guo-Hong Ning, Dan Li

{"title":"Regulating the topology and pore size of covalent metal-organic framework for boosting catalytic CO2 conversion","authors":"Xu Chen, Yu-Yang Li, Zhi-Hong Lin, Jing-Yi Song, Ri-Qin Xia, Chuang-Wei Zhou, Yu-Mei Wang, Yu Han, Hai-Long Jiang, Guo-Hong Ning, Dan Li","doi":"10.1016/j.chempr.2026.103006","DOIUrl":"https://doi.org/10.1016/j.chempr.2026.103006","url":null,"abstract":"The development of porous materials that serve as low-cost and efficient heterogeneous catalysts for CO2 conversion under dilute conditions is highly desirable yet challenging. Herein, we demonstrated the improvement of the catalytic performance of covalent metal-organic frameworks (CMOFs) for carbon dioxide (CO2) conversion by strategically regulating their topology and pore size—an underexplored approach for MOF catalysts. By modifying pyrazolate ligands, the topology was mediated from a homopore hcb structure to a heteroporous cpt network. Furthermore, varying the length of diamine ligands enabled precise pore-size tuning. Interestingly, heteropore CMOFs exhibited superior CO2 uptake and catalytic activity compared with homopore analogs. Notably, reducing the pore size further strengthened CO2 affinity and boosted catalytic performance in various CO2 conversion reactions. The optimized catalysts also maintained high activity under humid conditions with simulated flue gas. Mechanistic studies involving nuclear magnetic resonance (NMR) monitoring, isotope labeling, density functional theory (DFT), and grand canonical Monte Carlo (GCMC) calculations provide insights into the catalytic process.","PeriodicalId":268,"journal":{"name":"Chem","volume":"52 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2026-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147586175","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

Alcoholysis of nylon 6 waste to ε-caprolactam promoted by phosphoric acid 磷酸促进尼龙6废醇解制ε-己内酰胺的研究

IF 23.5 1区化学

Chem Pub Date : 2026-03-30 DOI: 10.1016/j.chempr.2026.102966

Xianyuan Wu, Rahul Prasad Bangalore Ashok, Xiao Wang, Matthew S. Webber, Anna E. Brenner, Griffin Drake, Joel Miscall, Clarissa Lincoln, Elisabeth Van Roijen, Stefan J. Haugen, Jason S. DesVeaux, Taylor Uekert, Yang Shao-Horn, Shannon S. Stahl, Gregg T. Beckham, Yuriy Román-Leshkov

{"title":"Alcoholysis of nylon 6 waste to ε-caprolactam promoted by phosphoric acid","authors":"Xianyuan Wu, Rahul Prasad Bangalore Ashok, Xiao Wang, Matthew S. Webber, Anna E. Brenner, Griffin Drake, Joel Miscall, Clarissa Lincoln, Elisabeth Van Roijen, Stefan J. Haugen, Jason S. DesVeaux, Taylor Uekert, Yang Shao-Horn, Shannon S. Stahl, Gregg T. Beckham, Yuriy Román-Leshkov","doi":"10.1016/j.chempr.2026.102966","DOIUrl":"https://doi.org/10.1016/j.chempr.2026.102966","url":null,"abstract":"Nylon 6 is widely used in high-performance materials. However, the inherent structural rigidity of nylon 6 inhibits catalytic depolymerization to its monomer, ε-caprolactam. Here, we demonstrate an acid-catalyzed alcoholysis process that depolymerizes nylon 6 to ε-caprolactam, achieving yields up to 74% using n-propanol as solvent and phosphoric acid as catalyst at 220°C for 2 h. We further applied the process to commercial nylon-containing products, demonstrating ε-caprolactam yields of 67% to 76%. Process modeling and techno-economic analysis estimated a minimum selling price of recycled nylon 6 at $1.79/kg, 30% lower than the 5-year average market price of virgin nylon 6. These estimates depend on assumed costs and process performance and may vary with future conditions. Life cycle assessment indicated that nylon 6 produced via alcoholysis can reduce greenhouse gas emissions by up to 63% compared with primary production. Overall, this study demonstrates a facile, cost-effective, and environmentally beneficial process for nylon 6 chemical recycling.","PeriodicalId":268,"journal":{"name":"Chem","volume":"20 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2026-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147586286","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

Trace-water-mediated formamidinium cation anchoring to regulate crystallization of tin-lead perovskite for efficient and stable photovoltaics 痕量水介导的甲脒阳离子锚定调节锡铅钙钛矿结晶的高效和稳定光伏

IF 23.5 1区化学

Chem Pub Date : 2026-03-27 DOI: 10.1016/j.chempr.2026.102964

Weilin Wu, Jiakang Zhang, Mingjun Ma, Mengjiao Lan, Yuanyuan Liao, Cheng Li, Jiahui Cheng, Huijie Cao, Wenjian Yan, Shuming Zhang, Mingzhe Zhu, Zhongmin Zhou

{"title":"Trace-water-mediated formamidinium cation anchoring to regulate crystallization of tin-lead perovskite for efficient and stable photovoltaics","authors":"Weilin Wu, Jiakang Zhang, Mingjun Ma, Mengjiao Lan, Yuanyuan Liao, Cheng Li, Jiahui Cheng, Huijie Cao, Wenjian Yan, Shuming Zhang, Mingzhe Zhu, Zhongmin Zhou","doi":"10.1016/j.chempr.2026.102964","DOIUrl":"https://doi.org/10.1016/j.chempr.2026.102964","url":null,"abstract":"Formamidinium (FA+) effusion and rapid crystallization are two main issues in Sn–Pb perovskite films. Trace amounts of water in the precursor solution catalyze an in situ reaction between benzylamine (BnNH2) and formamidinium iodide (FAI), forming BnFA+ cations. The product retards nucleation and growth during annealing, producing Sn–Pb perovskite films that are more uniform, contain fewer trap states, and exhibit smaller energy offsets with adjacent charge-transport layers. Density functional theory calculations indicate that water creates a proton-shuttle pathway that halves the Gibbs free-energy barrier for intramolecular proton transfer, enabling the early covalent passivation of FA+ sites. In addition, BnFAI shows stronger dissociation and solvation in the mixed solvent, simultaneously reducing both the crystallization rate and Sn2+ oxidation. In situ ultraviolet-visible (UV-vis) measurements reveal a 30% decrease in the crystallization rate constant. As a result, devices incorporating the BnNH2 additive achieve a champion power-conversion efficiency of 24.05% and demonstrate improved shelf and operational stability.","PeriodicalId":268,"journal":{"name":"Chem","volume":"219 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2026-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147519112","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

Aqueous-phase organic photochemistry: Distinct modes and interfaces 水相有机光化学：不同的模式和界面

IF 23.5 1区化学

Chem Pub Date : 2026-03-27 DOI: 10.1016/j.chempr.2026.102962

Xia-Min Jiang, Burkhard König, Ya-Ming Tian

引用次数: 0

Design and organocatalytic enantioselective assembly of axially chiral boracyclohexylidenes and chiral boraspiranes 轴向手性硼环己基醚和手性硼aspiranes的设计和有机催化对映选择性组装

IF 23.5 1区化学

Chem Pub Date : 2026-03-27 DOI: 10.1016/j.chempr.2026.102990

Shuai Wang, Jianbo Liu, Wangyang Li, Ying Li, Yanying Huang, Wenyue Ma, Qiuling Song

引用次数: 0

A metal-ion-linked self-assembled molecular layer as a robust hole-selective contact for perovskite solar cells 金属离子连接的自组装分子层作为钙钛矿太阳能电池的坚固的孔选择接触

IF 23.5 1区化学

Chem Pub Date : 2026-03-27 DOI: 10.1016/j.chempr.2026.102965

Wei Zhou, Wenzhuo Li, Hao Chen, Mingyu Ma, Minyong Du, Junhan Xie, Zhiyi Yao, Chenglong Ge, Haobo Wu, Xin Wen, Yuedong Shi, Chengwu Ouyang, Wenjing Wang, Weixuan Liu, Gaoqi Liu, Hao Liang, Peihong Cheng, Wenjia Zhou, Erkan Aydin, Mingyang Wei, Zhijun Ning

{"title":"A metal-ion-linked self-assembled molecular layer as a robust hole-selective contact for perovskite solar cells","authors":"Wei Zhou, Wenzhuo Li, Hao Chen, Mingyu Ma, Minyong Du, Junhan Xie, Zhiyi Yao, Chenglong Ge, Haobo Wu, Xin Wen, Yuedong Shi, Chengwu Ouyang, Wenjing Wang, Weixuan Liu, Gaoqi Liu, Hao Liang, Peihong Cheng, Wenjia Zhou, Erkan Aydin, Mingyang Wei, Zhijun Ning","doi":"10.1016/j.chempr.2026.102965","DOIUrl":"https://doi.org/10.1016/j.chempr.2026.102965","url":null,"abstract":"Self-assembled monolayers (SAMs) as hole-selective contacts (HSCs) have driven efficiency improvements in inverted perovskite solar cells (PSCs) in recent years. However, their non-uniform coverage on metal oxide electrodes and stress-induced molecular desorption lead to interfacial recombination and compromise device operating stability. Here, we develop a metal-ion-linked self-assembled molecular layer (MiLSAM) as a robust HSC. Through a sequential assembly process, a molecular network with high-valent metal ions as crosslinking nodes is formed, enabling homogeneous substrate coverage and enhanced stability against surface restructuring. Inverted PSCs employing MiLSAM achieved a power conversion efficiency (PCE) of 26.71% (certified 26.46%), while 1 cm2 devices delivered a PCE of 25.75%. Encapsulated devices retained 91% of their initial PCE after 2,000 h near the International Summit on Organic Photovoltaic Stability (ISOS)-D-3 (85°C, 85% RH) and 90% after 1,000 h of maximum power point tracking near ISOS-L-3 (85°C, 50% RH), demonstrating simultaneous gains in efficiency and operational stability.","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2026-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147524523","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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