Angewandte Chemie (International ed. in English)最新文献_第9页

Ni-Mediated High-Spin Iron(III) for Boosting Electrocatalytic NO to Oxime Conversion. 镍介导的高自旋铁（III）促进电催化NO转化为肟。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-10 DOI: 10.1002/anie.202515660

Runan Xiang, Jiawei Kang, Lu Zhang, Xupeng Qin, Peisen Liao, Sijia Zhan, Qinghua Liu, Zheng Liu, Song Gao, Guangqin Li

{"title":"Ni-Mediated High-Spin Iron(III) for Boosting Electrocatalytic NO to Oxime Conversion.","authors":"Runan Xiang, Jiawei Kang, Lu Zhang, Xupeng Qin, Peisen Liao, Sijia Zhan, Qinghua Liu, Zheng Liu, Song Gao, Guangqin Li","doi":"10.1002/anie.202515660","DOIUrl":"https://doi.org/10.1002/anie.202515660","url":null,"abstract":"Oximes serve as indispensable intermediates in synthetic chemistry, owing to their distinctive C═N─OH structure, conferring highly versatile reactivity. Synthesis of oxime via the electrochemical method has potential advantages, accompanied by the upgrading of industrialization. Herein, we propose a novel strategy by introducing nickel (Ni) mediation to obtain high-spin iron (Fe)(III) in phthalocyanine structure for synthesizing glyoxylate oxime via electrocatalytic nitric oxide (NO) coupling with keto acid. The optimized pFeNiPc catalyst achieved a Faradaic efficiency of 84.3% and a long-term stability for glyoxylate oxime electrosynthesis. Moreover, the oxime could be directly cyclized to synthesize a gram-level agrochemical isoxazoline molecule. The enriched amounts of high-spin Fe(III) sites promote the accumulation of NO on the catalyst surface and further accelerate reduction, which enables the efficient adsorption-conversion of NO to oxime. This work devises an innovative strategy to selectively engineer the activation of catalytic sites by tailoring electronic configuration and presents a method to facilitate NO valorization in organonitrogen synthesis.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202515660"},"PeriodicalIF":16.9,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145034465","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Temperature-Driven Conformational Switching of Binaphthalene-Based Tetraimidazolium Macrocycles to Enhance Sequence-Selective Recognition of Dinucleotides in Water. 温度驱动的双萘基四咪唑大环构象开关增强对水中二核苷酸的序列选择性识别。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-10 DOI: 10.1002/anie.202516534

Tianci He, Mengxin Huo, Pingxia Wang, Haoyang Huo, Ting Yang, Fan Cao, Lingyu Zhao, Yanxia Yang, Lin Cheng, Liping Cao

{"title":"Temperature-Driven Conformational Switching of Binaphthalene-Based Tetraimidazolium Macrocycles to Enhance Sequence-Selective Recognition of Dinucleotides in Water.","authors":"Tianci He, Mengxin Huo, Pingxia Wang, Haoyang Huo, Ting Yang, Fan Cao, Lingyu Zhao, Yanxia Yang, Lin Cheng, Liping Cao","doi":"10.1002/anie.202516534","DOIUrl":"https://doi.org/10.1002/anie.202516534","url":null,"abstract":"Developing artificial hosts with temperature-driven conformational switching behaviors facilitates our understanding of the temperature-dependent allostery and adaptation mechanisms in natural recognition systems. Herein, we report the design and synthesis of three pairs of water-soluble, enantiomeric binaphthalene-based tetraimidazolium macrocycles (SS/RR-1•4Cl- - SS/RR-3•4Cl-) as artificial hosts for exploring sequence-selective recognition of dinucleotides in aqueous media. Owing to the reversible rotational conformation of axially chiral binaphthyl units, SS-1•4Cl- demonstrates the conformational switching, converting from cis-conformation (SS-1cis) to trans-conformation (SS-1trans) by increasing temperature, thereby causing the recognition cavity to transition from a closed to an open state. Given its ability for temperature-driven conformational switching, SS-1•4Cl- exhibits temperature-cooperative enhanced binding behavior with d(TpA), with association constants (Ka) increasing to ∼106 M-1 at 323 K, up from ∼104 M-1 at 288 K. In contrast, its affinity for other dinucleotides, including d(ApT), d(GpC), and d(CpG), decreases to varying extents with increasing temperature. As a result, SS-1•4Cl-, with an ability of temperature-driven conformational switching, achieves an unexpected sequence-selective recognition for the sequence-complementary dinucleotide pair d(TpA) and d(ApT), with high sequence selectivity factors (Krel = Ka[d(TpA)]/Ka[d(ApT)]) reaching up to ∼118.8 at 323 K, increased from ∼1.1 at 288 K, in water.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202516534"},"PeriodicalIF":16.9,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145034492","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Heavyweight Champion: Caesium Diorganophosphides Outperform Lighter Congeners in the Catalytic Hydrophosphination of Alkenes and Alkynes. 重量级冠军：重有机磷化铯在烯烃和炔的催化氢磷化反应中优于较轻的同系物。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-10 DOI: 10.1002/anie.202516376

Felix Krämer, Michelle H Crabbe, Israel Fernández, Robert E Mulvey

{"title":"Heavyweight Champion: Caesium Diorganophosphides Outperform Lighter Congeners in the Catalytic Hydrophosphination of Alkenes and Alkynes.","authors":"Felix Krämer, Michelle H Crabbe, Israel Fernández, Robert E Mulvey","doi":"10.1002/anie.202516376","DOIUrl":"https://doi.org/10.1002/anie.202516376","url":null,"abstract":"We present a study of the ability of our recently reported well-defined crown ether-coordinated alkali metal phosphides 1AM to catalyze hydrophosphination (HP) of alkynes and alkenes. In a comparative study including reaction monitoring by 1H NMR spectroscopy, we show that the activity of caesium compound 1Cs greatly exceeds that of its lighter congeners, enabling us to solve some reported challenges of catalytic hydrophosphination. Through the rarely used application of dialkyl phosphines, we were able to produce trialkyl phosphines from HP of styrene derivatives and activated as well as non-activated alkynes by catalytic HP with nBu2PH and tBu2PH. Using tBuPhPH, P-chiral products were obtained, still in racemic mixtures showcasing this system's potential. We also proved the method is suited for preparing unsymmetrical ethylene-bridged bisphosphines by HP of Ph2P(vinyl) isolable in high yields. These advances hint that well-defined organocaesium compounds could make a long-term impact in chemistry.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202516376"},"PeriodicalIF":16.9,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145035062","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Spin Frustration Determines the Stability and Reactivity of Metal-Organic Frameworks with Triangular Iron(III)-Oxo Clusters. 具有三角形铁(III)-氧簇的金属-有机骨架的自旋受挫性决定了其稳定性和反应性。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-09 DOI: 10.1002/anie.202514014

Patrick Lechner, Gaurab Ganguly, Michael J Sahre, Georg Kresse, Johannes C B Dietschreit, Leticia González

{"title":"Spin Frustration Determines the Stability and Reactivity of Metal-Organic Frameworks with Triangular Iron(III)-Oxo Clusters.","authors":"Patrick Lechner, Gaurab Ganguly, Michael J Sahre, Georg Kresse, Johannes C B Dietschreit, Leticia González","doi":"10.1002/anie.202514014","DOIUrl":"https://doi.org/10.1002/anie.202514014","url":null,"abstract":"Density functional theory (DFT) is the standard approach for modeling MIL-101(Fe) and related Fe-based metal-organic frameworks, typically assuming a ferromagnetic high-spin configuration. However, this widely adopted approach overlooks a key electronic feature: Spin frustration in the triangular <math> <semantics> <mrow><msub><mi>Fe</mi> <mn>3</mn></msub> <mrow><mo>(</mo></mrow> <msub><mi>μ</mi> <mn>3</mn></msub> </mrow> <annotation>${rm Fe}_{3}(mu _{3}$</annotation></semantics> </math> -O) nodes. Using flip-spin, broken-symmetry DFT, we identify the true ground state as an antiferromagnetic <math> <semantics><mrow><mn>2</mn> <mi>S</mi> <mo>+</mo> <mn>1</mn> <mo>=</mo> <mn>6</mn></mrow> <annotation>$2S+1=6$</annotation></semantics> </math> state that standard DFT fails to capture. We demonstrate that neglecting spin frustration in MIL-101(Fe) leads to structural distortions, incorrect energetics, and misleading predictions of stability and reactivity. By explicitly accounting for spin frustration, we recover the correct structure and rationalize the temperature-dependent <math> <semantics><msub><mi>N</mi> <mn>2</mn></msub> <annotation>${rm N}_{2}$</annotation></semantics> </math> and CO binding. Spin frustration enhances <math> <semantics><msub><mi>N</mi> <mn>2</mn></msub> <annotation>${rm N}_{2}$</annotation></semantics> </math> fixation at room temperature, while its loss upon partial <math> <semantics><msup><mi>Fe</mi> <mi>III</mi></msup> <annotation>${rm Fe}^{mathrm {III}}$</annotation></semantics> </math> reduction suppresses this activity but promotes CO adsorption via <math><semantics><mi>π</mi> <annotation>$pi$</annotation></semantics> </math> -backbonding. These findings challenge current computational conventions and highlight spin frustration as a critical electronic feature in these frameworks.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202514014"},"PeriodicalIF":16.9,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145031591","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Controlling the Regioselectivity of Topochemical Reduction Reactions Through Sequential Anion Insertion and Extraction. 通过序贯阴离子插入和提取控制拓扑化学还原反应的区域选择性。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-09 DOI: 10.1002/anie.202514045

Romain Wernert, Bodoo Batnaran, Michael A Hayward

{"title":"Controlling the Regioselectivity of Topochemical Reduction Reactions Through Sequential Anion Insertion and Extraction.","authors":"Romain Wernert, Bodoo Batnaran, Michael A Hayward","doi":"10.1002/anie.202514045","DOIUrl":"https://doi.org/10.1002/anie.202514045","url":null,"abstract":"Topochemical reduction of the n = 2 Ruddlesden-Popper oxide, LaSr2CoRuO7, yields LaSr2CoRuO5.3, a phase containing (Co/Ru)O4 squares which share corners to form 1D infinite double-chains. In contrast, fluorination of LaSr2CoRuO7 yields the oxyfluoride LaSr2CoRuO5.5F3.5, which can then be reduced to form LaSr2CoRuO4.5F1.5. This reduced oxyfluoride is almost isoelectronic with LaSr2CoRuO5.3, but LaSr2CoRuO4.5F1.5 has a crystal structure in which the (Co/Ru)O4 squares are connected into 2D infinite sheets. Thus, by following a fluorinate-then-reduce reaction scheme, the regiochemistry of topochemical reduction reactions can be modified, and compounds with different transition-metal-centre interconnectivity can be prepared. Both LaSr2CoRuO5.3 and LaSr2CoRuO4.5F1.5 adopt glassy magnetic states at low temperature, but the magnetic interactions present in LaSr2CoRuO5.3 appear to be significantly stronger than those in LaSr2CoRuO4.5F1.5, attributable to the differing dimensionality of the transition-metal connectivity. The structural features of LaSr2CoRuO5.5F3.5 that modify the regioselectivity of the topochemical reduction reaction appear to be common to many fluorinated Ruddlesden-Popper oxides, suggesting this fluorinate-then-reduce strategy could be used to prepare a range of \"infinite-layer\" reduced phases which cannot be made by direct reduction of Ruddlesden-Popper oxide precursors.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202514045"},"PeriodicalIF":16.9,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145031589","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Hetero-Hydrazone Photoswitches. Hetero-Hydrazone光电开关。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-09 DOI: 10.1002/anie.202515136

Daniil Sosnin, Syed Ali Abbas Abedi, Mohammad Izadyar, Yağmur Ünal, Xiaogang Liu, Ivan Aprahamian

{"title":"Hetero-Hydrazone Photoswitches.","authors":"Daniil Sosnin, Syed Ali Abbas Abedi, Mohammad Izadyar, Yağmur Ünal, Xiaogang Liu, Ivan Aprahamian","doi":"10.1002/anie.202515136","DOIUrl":"https://doi.org/10.1002/anie.202515136","url":null,"abstract":"The fine-tuning of the (photo)physical properties of molecular photoswitches remains an active area of research, and recently, the incorporation of heterocycles into photoswitch scaffolds has emerged as an effective strategy in this vein. To assess the influence that heterocyclic rings have on hydrazone-based systems, we synthesized a series of photoswitches and examined the impact that heterocycles have on the switching efficiency. TD-DFT calculations and structure-property analyses revealed that heterocycles with basic nitrogen and secondary hydrogen-bonding sites (e.g., imidazole) show poor switching efficiency and undergo thermal back-isomerization via an unusual mechanism involving tautomerization followed by rotation, resulting in fast thermal isomerization rates (i.e., half-lives of seconds to minutes). In contrast, less basic heterocycles such as benzoxazole and benzothiazole favor an inversion pathway, leading to improved bistability. Hydrazones lacking secondary hydrogen-bonding sites, on the other hand, exhibit significantly enhanced photostationary states, improved quantum yields, and red-shifted activation wavelengths compared to their 1st-generation phenyl-based analogs. These results showcase the importance of heterocycle basicity and electron-donating ability, in addition to secondary H-binding sites on photoswitching efficiency, features that are not fully elaborated on in other heterocycle-containing switches. These findings, based on the 2nd generation hydrazone switches, establish key design principles for tuning the bistability and efficiency of such photoswitches.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202515136"},"PeriodicalIF":16.9,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145031571","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Visible Light-Driven Membrane-Bound Compartment for Precise Regulation of Enzyme Activity. 用于酶活性精确调控的可见光驱动膜结合隔室。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-09 DOI: 10.1002/anie.202513676

Zilu Li, Jialiang Wang, Hao Zhuo, Qiushi Li, Qingqing Huang, Chenjue Tang, Wei Zhai, Yang Liu, Yu Zhao

{"title":"Visible Light-Driven Membrane-Bound Compartment for Precise Regulation of Enzyme Activity.","authors":"Zilu Li, Jialiang Wang, Hao Zhuo, Qiushi Li, Qingqing Huang, Chenjue Tang, Wei Zhai, Yang Liu, Yu Zhao","doi":"10.1002/anie.202513676","DOIUrl":"https://doi.org/10.1002/anie.202513676","url":null,"abstract":"Photo-responsive systems provide a powerful tool to reversibly regulate enzyme activity. However, inhibitor-based strategies, though widely used, are often restricted to specific enzymes. Noninhibitor strategies, such as enzyme surface modification or genetic mutation, often compromise structural integrity or residual activity. Inspired by the gating mechanisms of biological membranes, we reported a visible light-driven membrane-bound compartment system constructed from phenylazothiazole gated lipids and phospholipids. In this design, phenylazothiazole lipids undergo reversible isomerization between trans and cis configurations under alternating purple and green light, generating continuous nanomechanical motions that transiently enhance membrane permeability. This dynamic gating behavior enables substrate diffusion across the membrane under light exposure and allows the activity of encapsulated enzymes to be switched on and off in a noninvasive, temporally defined manner. This system requires no chemical modification or mutagenesis, thus preserving the native structure and activity of encapsulated enzymes. Beyond binary regulation, precise modulation of the irradiation pattern permits graded control over enzyme activity, offering an advanced level of functional tunability. Using carbonic anhydrase, catalase, and glucose oxidase as models, we demonstrate that enzyme activity can be reversibly and quantitatively regulated via programmable light inputs. This strategy offers a broadly applicable and biocompatible platform for spatiotemporal enzyme regulation.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202513676"},"PeriodicalIF":16.9,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145031512","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

On-Target Photoassembly of Pyronin Dyes for Super-Resolution Microscopy. 超分辨显微镜中Pyronin染料的靶光组装。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-09 DOI: 10.1002/anie.202506894

Gergely Knorr, Mariano L Bossi, Stefan W Hell

{"title":"On-Target Photoassembly of Pyronin Dyes for Super-Resolution Microscopy.","authors":"Gergely Knorr, Mariano L Bossi, Stefan W Hell","doi":"10.1002/anie.202506894","DOIUrl":"https://doi.org/10.1002/anie.202506894","url":null,"abstract":"Controlled photoactivation is an auspicious and emerging approach in super-resolution microscopy, offering virtually zero background signal from the marker prior to activation. Pyronins are well-established fluorophores, but due to their inherent intercalating tendency towards nucleic acids, their use has been mostly avoided in super-resolution microscopy. Here, we describe a new class of diaryl ether and diaryl silane molecules that upon photoactivation close into fluorescent (silicon-)pyronins and term them Pyronin Upon Light Irradiation (PULI). This concept exploits the outstanding photophysical properties of pyronins (bright, photostable, and optimal spectral features for standard microscopes), while overcoming their major drawback (intrinsic affinity of accumulating in the nucleus and around RNA) for the design of fluorescent markers for imaging applications. Furthermore, we also demonstrate that this approach is applicable to their Si-bridged analogues, extending this family of photoactivatable molecules to the far-red regime. The versatility of our approach was also highlighted by tagging diverse biological targets in cells and visualizing them using advanced super-resolution microscopy techniques, such as PALM, STED, and MINFLUX.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202506894"},"PeriodicalIF":16.9,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145031552","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Changing Self-Assembly Through Degradation: Phenyl Vinyl Ketone Polymer Nanoparticles Under Light. 通过降解改变自组装：光下苯基乙烯基酮聚合物纳米颗粒。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-08 DOI: 10.1002/anie.202514545

M A Sachini N Weerasinghe, Parker Anthony McBeth, Michelle C Mancini, Dominik Konkolewicz

{"title":"Changing Self-Assembly Through Degradation: Phenyl Vinyl Ketone Polymer Nanoparticles Under Light.","authors":"M A Sachini N Weerasinghe, Parker Anthony McBeth, Michelle C Mancini, Dominik Konkolewicz","doi":"10.1002/anie.202514545","DOIUrl":"https://doi.org/10.1002/anie.202514545","url":null,"abstract":"Photodegradable nanoparticles with sphere, worm, and vesicle morphologies were synthesized following polymerization induced self-assembly (PISA), incorporating a photoresponsive phenyl vinyl ketone (PVK) block and a nonphoto responsive 2-hydroxypropyl methacrylamide (HPMA) block. The photodegradation of nanoparticles under UV revealed that the initial shapes of sphere and vesicle particles are retained even until 7 h and after 24 h of photo-induced degradation, respectively, despite a significant reduction in molecular weight (Mn). This could be due to the assembly of degraded PVK fragments in the hydrophobic region, maintaining the relative hydrophilic to hydrophobic ratio. However, worm nanoparticles exhibited a fast morphology reversal after 2 min of degradation, yielding sphere nanoparticles. Therefore, photo responsive PVK nanoparticles with morphology and conversion-dependent degradation behavior were explored. Furthermore, undegraded and degraded nanoparticle coatings exhibited different surface properties, determined by contact angle measurements, with both morphology and degradation impacting the surface properties. Finally, the PVK nanoparticles could encapsulate molecules and release them upon degradation. Therefore, this study can ultimately be applied to numerous fields due to the potential uses of degradable polymers in various material systems, especially for the controlled release of agrochemicals, cleaning agents, or antifungal agents, as well as to enable surface modifications upon degradation.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202514545"},"PeriodicalIF":16.9,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145025048","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Electrochemistry-Accelerated Water-Gas Shift Reaction on IrN₄-RhN₄ Dual Sites Catalysts for Efficient Hydrogen Production. IrN4-RhN4双位催化剂上的电化学加速水气转换反应高效制氢。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-04 DOI: 10.1002/anie.202517292

Qie Liu, Liyuan Gong, Jingjing Wang, Luyao Ma, Yandong Wu, Yu-Cheng Huang, Ta Thi Thuy Nga, Yabin Xu, Zuyao Jiang, Shiqian Du, Hongjing Zhong, Yanjing Wang, Miaoyu Li, Chung-Li Dong, Guobin Wen, Li Tao, Shuangyin Wang

{"title":"Electrochemistry-Accelerated Water-Gas Shift Reaction on IrN4-RhN4 Dual Sites Catalysts for Efficient Hydrogen Production.","authors":"Qie Liu, Liyuan Gong, Jingjing Wang, Luyao Ma, Yandong Wu, Yu-Cheng Huang, Ta Thi Thuy Nga, Yabin Xu, Zuyao Jiang, Shiqian Du, Hongjing Zhong, Yanjing Wang, Miaoyu Li, Chung-Li Dong, Guobin Wen, Li Tao, Shuangyin Wang","doi":"10.1002/anie.202517292","DOIUrl":"https://doi.org/10.1002/anie.202517292","url":null,"abstract":"The water-gas shift reaction (WGSR) is crucial to the hydrogen economy, which is hampered by the harsh conditions and complicated purification process. In this work, the spatially separated efficient CO conversion and high-purity H2 production are realized by electrochemistry-accelerated water-gas shift reaction (WGSR) with IrN4-RhN4 dual sites single atom catalysts (IrRh-NC) in high-temperature polymer-electrolyte-membrane electrolyzer. In this reaction, the Ir single atoms in the catalysts can rapidly dissociate H2O at an extremely low potential to supply abundant *OH, which ensures the *OH groups bind to the spontaneously adsorbed *CO on neighboring Rh sites to further accelerate CO conversion. What's more, the elevated temperatures (120-300 °C) maintain water in the gaseous state during the reaction, thus greatly facilitating mass transfer of the reactants CO and H2O within the reactor. Employing IrRh-NC as the anodic catalyst, the electrolyzer achieves superior CO catalytic performance (424 mA cm-2 at 0.4 V) and high purity (99.9%) H2 production (3.2 ml min-1), surpassing the performance of particle catalysts. This work illuminates the tantalizing possibility for sustainable hydrogen economic development.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202517292"},"PeriodicalIF":16.9,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145002716","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0