IF 23.5 1区化学

Chem Pub Date : 2025-04-17 DOI: 10.1016/j.chempr.2025.102533

Yanmei Huang, Ying Gao, Bin Zhang

{"title":"Interfacial water regulation for water-participating electrocatalytic hydrogenation reactions","authors":"Yanmei Huang, Ying Gao, Bin Zhang","doi":"10.1016/j.chempr.2025.102533","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102533","url":null,"abstract":"Electrocatalytic hydrogenation of abundant feedstocks to value-added products using water as the hydrogen source offers promising alternatives to traditional methods. At the electrode-electrolyte interface, water molecules not only act as active hydrogen sources but also facilitate mass transport via hydrogen-bond networks. The configuration, orientation, and distribution of interfacial water molecules are directly related to the connectivity of the hydrogen-bond network, thereby directly determining the hydrogenation efficiency. A fundamental understanding of interfacial water dynamics and the development of precise modulation strategies are key to advancing electrochemical hydrogenation. This perspective systematically discusses three dominant strategies—namely, manipulating the local electric field, engineering surface modifications/electrolyte additives, and tuning solvated-cation interactions—to regulate the properties of interfacial water and enhance the corresponding hydrogenation performance. Finally, we highlight critical issues for future research aimed at better controlling interfacial water dynamics to enhance the performance of electrocatalytic hydrogenation and other water-participating reactions.","PeriodicalId":268,"journal":{"name":"Chem","volume":"22 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143841944","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

Biosynthesis of nitrile-containing amino acids for rapid protein conjugation and fluorogenic labeling 含腈氨基酸的生物合成，用于快速蛋白质偶联和荧光标记

IF 23.5 1区化学

Chem Pub Date : 2025-04-17 DOI: 10.1016/j.chempr.2025.102573

Yu Hu, Mengxi Zhang, Han Xiao

引用次数: 0

Challenges and perspectives for the perovskite module research 过氧化物模块研究的挑战和前景

IF 23.5 1区化学

Chem Pub Date : 2025-04-16 DOI: 10.1016/j.chempr.2025.102542

Runda Li, Libing Yao, Jingyi Sun, Zengyi Sun, Kai Zhang, Jingjing Xue, Rui Wang

引用次数: 0

Practical flow battery diagnostics enabled by chemically mediated monitoring 通过化学介导监测实现实用的液流电池诊断技术

IF 23.5 1区化学

Chem Pub Date : 2025-04-16 DOI: 10.1016/j.chempr.2025.102543

Mark E. Carrington, Loh Min Yi, Erlendur Jónsson, Clare P. Grey

引用次数: 0

One-dimensional lead halide perovskite quantum ribbons with controllable edge terminations and ribbon widths 具有可控制边缘端点和能带宽度的一维卤化铅钙钛矿量子带

IF 23.5 1区化学

Chem Pub Date : 2025-04-15 DOI: 10.1016/j.chempr.2025.102548

Xiaofan Jiang, Mingyuan Li, Yu Tao, Meng Zhang, Xinyu Li, Tianhao Zhang, Jiazhen Gu, Guangsheng Bai, Nanlong Zheng, Xuan Zhao, Huilong Hong, Leyang Jin, Xu Huang, Sanli Xu, Yan Guan, Chen Li, Wenkai Zhang, Yongping Fu

{"title":"One-dimensional lead halide perovskite quantum ribbons with controllable edge terminations and ribbon widths","authors":"Xiaofan Jiang, Mingyuan Li, Yu Tao, Meng Zhang, Xinyu Li, Tianhao Zhang, Jiazhen Gu, Guangsheng Bai, Nanlong Zheng, Xuan Zhao, Huilong Hong, Leyang Jin, Xu Huang, Sanli Xu, Yan Guan, Chen Li, Wenkai Zhang, Yongping Fu","doi":"10.1016/j.chempr.2025.102548","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102548","url":null,"abstract":"One-dimensional (1D) halide perovskite quantum ribbons, featuring 1D corner-sharing octahedral networks, are promising for optoelectronics and photonics due to quantum confinement in two dimensions. However, the rational design of 1D perovskites remains challenging, and existing materials with narrow ribbon widths predominantly form self-trapped excitons, which limit their potential applications. Here, we synthesize 30 1D perovskites with controllable ribbon widths and edge octahedra terminations by organic cation engineering. We observe the absence of self-trapped excitons as the ribbon width increases up to four octahedra, alongside the ability to modulate their optoelectronic properties by tailoring the edge terminations. The 1D free excitons result in in-plane anisotropic photoluminescence (PL) emission with polarization degree reaching 60%. Moreover, we observe robust exciton-photon coupling with Rabi splitting energies up to 800 meV, which is significantly larger than those of three-dimensional (3D) and two-dimensional (2D) perovskites, demonstrating a class of 1D quantum materials for advanced optoelectronics and photonics.","PeriodicalId":268,"journal":{"name":"Chem","volume":"136 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832147","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

Atomic-resolution imaging as a mechanistic tool for studying single-site heterogeneous catalysis 原子分辨率成像作为研究单位点多相催化的机制工具

IF 23.5 1区化学

Chem Pub Date : 2025-04-11 DOI: 10.1016/j.chempr.2025.102541

Yosi Kratish, Yiqi Liu, Jiaqi Li, Anusheela Das, Leighton O. Jones, Amol Agarwal, Qing Ma, Michael J. Bedzyk, George C. Schatz, Takayuki Nakamuro, Eiichi Nakamura, Tobin J. Marks

{"title":"Atomic-resolution imaging as a mechanistic tool for studying single-site heterogeneous catalysis","authors":"Yosi Kratish, Yiqi Liu, Jiaqi Li, Anusheela Das, Leighton O. Jones, Amol Agarwal, Qing Ma, Michael J. Bedzyk, George C. Schatz, Takayuki Nakamuro, Eiichi Nakamura, Tobin J. Marks","doi":"10.1016/j.chempr.2025.102541","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102541","url":null,"abstract":"Heterogeneous catalysts dominate the chemical industry but, unlike homogeneous catalysts, typically feature diverse, incompletely defined active sites. Thus, describing their structure-activity relationships remains challenging. In contrast, molecularly defined single-site heterogeneous catalysts (SSHCs) are poised to address these challenges and provide new avenues for catalysis research and development. The present study explores eco-friendly H<sub>2</sub> production mediated by discrete MoO<sub>2</sub> sites supported on carbon nanohorns (CNHs) and active for alcohol dehydrogenation. Although informative, detailed extended X-ray absorption fine structure (EXAFS), X-ray absorption near-edge structure (XANES), X-ray photoelectron spectroscopy (XPS,) kinetic measurements, and density functional theory (DFT) analysis alone cannot provide a full molecular picture of the reaction pathway. Here, using single-molecule atomic-resolution time-resolved electron microscopy (SMART-EM), we propose the identification of four key catalytic intermediates anchored to CNHs and uncover a new reaction pathway involving alkoxide/hemiacetal equilibration and acetal oligomerization. These intermediates are inferred through a combination of theory and SMART-EM, showcasing the potential of SMART-EM as a complementary tool for exploring mechanistic hypotheses in catalysis.","PeriodicalId":268,"journal":{"name":"Chem","volume":"108 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143820116","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

Circumventing the activity-selectivity trade-off: Pt-Fe-Pt active sites for selective heterogeneous hydrogenation of crotonaldehyde 规避活性-选择性权衡：巴豆醛选择性异相氢化的铂-铁-铂活性位点

IF 23.5 1区化学

Chem Pub Date : 2025-04-11 DOI: 10.1016/j.chempr.2024.102405

Hongchen Yang, Xiangwen Liu, Dingsheng Wang

引用次数: 0

Hybrid photoanodes based on surface-bound host-guest molecular assemblies 基于表面结合主客体分子组装的杂化光阳极

IF 19.1 1区化学

Chem Pub Date : 2025-04-10 DOI: 10.1016/j.chempr.2024.11.003

Jiaxuan Wang , Daokuan Li , Xiaona Li , Guoquan Liu , Yong Zhu , Licheng Sun , Fei Li

{"title":"Hybrid photoanodes based on surface-bound host-guest molecular assemblies","authors":"Jiaxuan Wang , Daokuan Li , Xiaona Li , Guoquan Liu , Yong Zhu , Licheng Sun , Fei Li","doi":"10.1016/j.chempr.2024.11.003","DOIUrl":"10.1016/j.chempr.2024.11.003","url":null,"abstract":"<div><div>In artificial photosynthesis, molecule/semiconductor hybrids combine the merits of the high activity of molecular catalysts and the high stability of semiconductor light absorbers. We report here a host-guest strategy for hybrid photoanode fabrication, where phosphonate-derivatized cyclodextrins (p-CDs) as hosts were anchored on the surface of a tungsten oxide (WO<sub>3</sub>) film, and molecular catalysts as guests were self-encapsulated into the cavities of p-CDs in either aqueous or organic media. By choosing an admantanyl cobaloxime complex (<strong>Co1</strong>) as a molecular water oxidation catalyst, the resulting WO<sub>3</sub>|p-CD|<strong>Co1</strong> photoanode exhibited high photoelectrochemical (PEC) activity and stability for water oxidation due to the unexpected efficient charge separation and the strong affinity between p-CD and catalyst. In addition, the WO<sub>3</sub>|p-CD was identified to be a versatile platform for catalyst loading, when a 4-hydroxy-2,2,6,6-tetramethylpiperidine 1-oxyl (TEMPO) derivative was employed as the guest molecule, the conversion yield of PEC alcohol oxidation to aldehyde was dramatically increased.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 4","pages":"Article 102365"},"PeriodicalIF":19.1,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793789","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

Beyond natural synthesis via solar-decoupled biohybrid photosynthetic system 超越自然合成通过太阳解耦的生物杂交光合系统

IF 19.1 1区化学

Chem Pub Date : 2025-04-10 DOI: 10.1016/j.chempr.2024.11.019

Na Chen , Jing Xi , Tianpei He , Ruichen Shen , Rui Zhao , Haoming Chi , Jia Yao , Na Du , Lilei Yu , Yun Zhang , Tianyou Peng , Tiangang Liu , Quan Yuan

{"title":"Beyond natural synthesis via solar-decoupled biohybrid photosynthetic system","authors":"Na Chen , Jing Xi , Tianpei He , Ruichen Shen , Rui Zhao , Haoming Chi , Jia Yao , Na Du , Lilei Yu , Yun Zhang , Tianyou Peng , Tiangang Liu , Quan Yuan","doi":"10.1016/j.chempr.2024.11.019","DOIUrl":"10.1016/j.chempr.2024.11.019","url":null,"abstract":"<div><div>Inspired by the solar energy storage process during photosynthesis, we report herein a solar-decoupled photosynthetic biohybrid strategy through integrating a persistent photocatalyst with photoautotrophic microbes for sustainable and all-weather biomanufacturing, allowing for overcoming the intrinsic intermittent nature of solar energy availability by introducing energy storage and release processes. The results demonstrate that the apparent photo conversion efficiency (APCE) for of the persistent catalyst/<em>R</em>. <em>palustris</em> hybrid system reaches 8.30%, much higher than the 4.36% observed in bare <em>R. palustris</em>. Additionally, the proposed solar-decoupled biohybrid strategy not only shows considerable potential in coupling the practical power plant for the capture and utilization of CO<sub>2</sub> from the flue gas but also exhibits universal applicability in different photosynthetic microorganisms. This concept-proving research offers new ideas to extend photocatalysis reactions without <em>in situ</em> irradiation and could pave new ways for sustainable solar energy utilization as well as biomanufacturing in space, where solar energy might be limited.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 4","pages":"Article 102381"},"PeriodicalIF":19.1,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142917917","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

Strained diradicaloids for σ-bond-insertion reactions: A breakthrough in drug discovery 用于σ键插入反应的张力双根碱：药物发现的一个突破

IF 19.1 1区化学

Chem Pub Date : 2025-04-10 DOI: 10.1016/j.chempr.2025.102524

Yoshio Barrera , Florian F. Mulks

引用次数: 0

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