Chemistry - A European Journal最新文献_第9页

Origins of Catalysis in Non-Heme Fe(II)/2-Oxoglutarate-Dependent Histone Lysine Demethylase KDM4A with Differently Methylated Histone H3 Peptides. 非血红蛋白 Fe(II)/2-Oxoglutarate 依赖性组蛋白赖氨酸去甲基化酶 KDM4A 在不同甲基化组蛋白 H3 肽中的催化起源

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-01-14 Epub Date: 2024-11-18 DOI: 10.1002/chem.202403989

Sudheesh Devadas, Midhun George Thomas, Simahudeen Bathir Jaber Sathik Rifayee, Bhargav Varada, Walter White, Ethan Sommer, Kylin Campbell, Christopher J Schofield, Christo Z Christov

{"title":"Origins of Catalysis in Non-Heme Fe(II)/2-Oxoglutarate-Dependent Histone Lysine Demethylase KDM4A with Differently Methylated Histone H3 Peptides.","authors":"Sudheesh Devadas, Midhun George Thomas, Simahudeen Bathir Jaber Sathik Rifayee, Bhargav Varada, Walter White, Ethan Sommer, Kylin Campbell, Christopher J Schofield, Christo Z Christov","doi":"10.1002/chem.202403989","DOIUrl":"10.1002/chem.202403989","url":null,"abstract":"Histone lysine demethylase 4 A (KDM4A), a non-heme Fe(II)/2-oxoglutarate (2OG) dependent oxygenase that catalyzes the demethylation of tri-methylated lysine residues at the 9, 27, and 36 positions of histone H3 (H3 K9me3, H3 K27me3, and H3 K36me3). These methylated residues show contrasting transcriptional roles; therefore, understanding KDM4A's catalytic mechanisms with these substrates is essential to explain the factors that control the different sequence-dependent demethylations. In this study, we use molecular dynamics (MD)-based combined quantum mechanics/molecular mechanics (QM/MM) methods to investigate determinants of KDM4A catalysis with H3 K9me3, H3 K27me3 and H3 K36me3 substrates. In KDM4A-H3(5-14)K9me3 and KDM4A-H3(23-32)K27me3 ferryl complexes, the O-H distance positively correlates with the activation barrier of the rate-limiting step, however in the KDM4A-H3(32-41)K36me3, no direct one-to-one relationship was found implying that the synergistic effects between the geometric parameters, second sphere interactions and the intrinsic electric field contribute for the effective catalysis for this substrate. The intrinsic electric field along the Fe-O bond changes between the three complexes and shows a positive correlation with the HAT activation barrier, suggesting that modulating electric field can be used for fine engineering KDM catalysis with a specific substrate. The results reveal how KDM4A uses a combination of strategies to enable near equally efficient demethylation of different H3Kme3 residues.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202403989"},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142563396","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Copper Nanoclusters Imparted Metalloporphyrin Based Metal-Organic Frameworks for Enhanced CO₂ Electroreduction. 基于金属卟啉的铜纳米簇金属有机框架用于增强二氧化碳电还原。

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-01-14 Epub Date: 2024-11-19 DOI: 10.1002/chem.202403231

Qian Wang, Bangli Feng, Yan Rong, Danxuan Pan, Mingfu Ye, Zhifeng Xin, Yifa Chen

{"title":"Copper Nanoclusters Imparted Metalloporphyrin Based Metal-Organic Frameworks for Enhanced CO2 Electroreduction.","authors":"Qian Wang, Bangli Feng, Yan Rong, Danxuan Pan, Mingfu Ye, Zhifeng Xin, Yifa Chen","doi":"10.1002/chem.202403231","DOIUrl":"10.1002/chem.202403231","url":null,"abstract":"Strategies that can introduce catalytic auxiliary into electrocatalysts to boost the performance of electrocatalytic CO2 reduction reaction (CO2RR) are meaningful in exploring hybrid electrocatalytic systems. Here, a series of hybrid electrocatalysts (Cu NCs@MOF-545-M, M=Fe, Co and Ni) have been prepared by assembly Cu NCs with MOF-545-M (M=Fe, Co and Ni) and successfully applied in electrocatalytic CO2RR. In the obtained MOF-545-M (M=Fe, Co and Ni), the integration of Cu NCs with MOF-545-M (M=Fe, Co and Ni) can create a hybrid electrocatalytic system that enhances the charge transfer efficiency and electrocatalytic CO2RR activity. Specifically, the optimal Cu NCs@MOF-545-Co presents remarkable FECO over a wide potential range (-0.7 V to -1.0 V), high CO generation rate (8.2 mol m-2 h-1) and excellent maximum energy efficiency (69 %, -0.7 V), which is superior to Cu NCs and MOF-545-Co, and represented to be one of the best performances to date. This work demonstrates a facile approach to significantly improve the FECO by loading metal nanoclusters into MOFs, providing a valuable reference for future studies on hybridization strategies to enhance the performance of electrocatalysts.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202403231"},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142542331","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

An Efficient Bifunctional Core-Shell ZIF-90@ZIF-67 Composite as a Stable Pickering Interfacial Catalyst for the Deacetalization-Knoevenagel Tandem Reaction. 一种高效的双功能核壳 ZIF-90@ZIF-67 复合材料，作为脱乙酰化-Knoevenagel 串联反应的稳定皮克林界面催化剂。

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-01-14 Epub Date: 2024-11-18 DOI: 10.1002/chem.202403363

Wei Liu, Yu-Qing Zhang, Zhen-Lin Dong, Zi-Xuan Chen, Lei Li, Xin-Yuan Zhao, Yang Wu, Yu-Yang Zhang

引用次数: 0

Recent Advances in NIR-Switchable Multi-Redox Systems Based on Organic Molecules. 基于有机分子的近红外可开关多重氧化还原系统的最新进展。

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-01-14 Epub Date: 2024-11-22 DOI: 10.1002/chem.202403273

Takashi Harimoto, Yusuke Ishigaki

{"title":"Recent Advances in NIR-Switchable Multi-Redox Systems Based on Organic Molecules.","authors":"Takashi Harimoto, Yusuke Ishigaki","doi":"10.1002/chem.202403273","DOIUrl":"10.1002/chem.202403273","url":null,"abstract":"Electrochromic systems capable of switching absorption in the near-infrared (NIR) region (750-2500 nm) are attractive from the viewpoint of applications for material and life science, and thus several examples have been reported to date. In general, the development of organic-based systems is needed to reduce the environmental impact and improve biocompatibility. Although extending the switchable spectral range is crucial for the application of organic electrochromic molecules, the switching of NIR absorption based on redox interconversion is still a challenging issue regarding reversibility and durability during interconversion. To overcome this potential instability, the introduction of heteroatoms into the molecular backbone and/or π-extension could be useful strategies in terms of effective delocalization of charge and spin in the corresponding redox states. In this review, we focus on redox-active well-defined small molecules that enable ON/OFF switching of NIR absorption based on precise control of the redox states, and present recent studies on their intrinsic electrochemical and spectroscopic properties and/or structural characterization of their charged states.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202403273"},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142581230","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Highly Active and Stable Cu-Cd Bimetallic Oxides for Enhanced Electrochemical CO₂ Reduction. 用于增强电化学二氧化碳还原的高活性、高稳定性铜镉双金属氧化物。

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-01-14 Epub Date: 2024-11-25 DOI: 10.1002/chem.202403261

Guoliang Mei, Yanling Zhai, Weiwei Guo, Doudou Liu, Zijian Fang, Guixian Xie, Zongxia Duan, Xianzhen Lang, Zhijun Zhu, Xiaoquan Lu, Jianguo Tang

{"title":"Highly Active and Stable Cu-Cd Bimetallic Oxides for Enhanced Electrochemical CO2 Reduction.","authors":"Guoliang Mei, Yanling Zhai, Weiwei Guo, Doudou Liu, Zijian Fang, Guixian Xie, Zongxia Duan, Xianzhen Lang, Zhijun Zhu, Xiaoquan Lu, Jianguo Tang","doi":"10.1002/chem.202403261","DOIUrl":"10.1002/chem.202403261","url":null,"abstract":"Electrochemical reduction of carbon dioxide (CO2) can produce value-added chemicals such as carbon monoxide (CO) and multicarbon (C2+). However, the complex reaction pathways of CO2 electro-reduction reaction (CO2RR) greatly limit the product selectivity and conversion efficiency. Herein, the Cu-Cd bimetallic oxides catalyst was designed and applied for the CO2RR. The optimized 4.73 %Cd-CuO exhibits remarkable electrocatalytic CO2RR activity for selective CO production in H-cell using 0.5 M 1-butyl-3-methylimidazolium hexafluorophosphate ([Bmim]PF6)/MeCN as electrolyte. The Faradaic efficiency of CO (FE(CO)) can be maintained above 90 % over a wide potential range of -2.0 to -2.4 V vs. Ag/Ag+. Particularly, the catalyst achieves an impressive FE(CO) of 96.3 % with a current density of 60.7 mA cm-2 at -2.2 V vs. Ag/Ag+. Furthermore, scaling up the 4.73 %Cd-CuO catalyst into a flow cell can reach 56.64 % FE of C2+ products (ethylene, ethanol and n-propanol) with a current density as high as 600 mA cm-2 steadily. The excellent CO2RR performance of the as-synthesized 4.73 %Cd-CuO can be mainly attributed to the introduction of CdO to improve the ability of CuO to activate CO2, the electronic interactions between Cu and Cd can boost the activation and conversion the key intermediates of CO2RR and ensure the continuous stability of the 4.73 %Cd-CuO in electrolysis process.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202403261"},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142613213","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Tandem Electroreduction of CO₂ to C2+ Products Based on M-SACs/Cu Catalysts.

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-01-14 Epub Date: 2024-12-12 DOI: 10.1002/chem.202403297

Qizhe He, Ting-Ting Li

{"title":"Tandem Electroreduction of CO2 to C2+ Products Based on M-SACs/Cu Catalysts.","authors":"Qizhe He, Ting-Ting Li","doi":"10.1002/chem.202403297","DOIUrl":"10.1002/chem.202403297","url":null,"abstract":"Electrochemical CO2 reduction reaction (ECO2RR) is considered a highly promising method to produce high-value chemicals and fuels, contributing significantly the artificial carbon balance. Plenty catalysts can facilitate the conversion of CO2 into mono-carbon (C1) products. Among these catalysts, Cu species exhibit a distinct role in the formation of multi-carbon (C2+) products characterized by enhanced energy density. However, the limited selectivity of C2+ products, along with the inferior stability, and high overpotential demonstrated by single-component Cu catalysts, hinders their applicability in industrial-scale production. The implementation of a tandem strategy, which involves coupling the CO2-to-CO pathway using Ag, Au, metal single-atom catalysts (M-SACs), etc., with the CO-to-C2+ conversion on Cu, represents a novel approach for the efficient generation of C2+ products. Given the high cost and restricted availability of noble metals, M-SACs have attracted substantial interest in tandem systems due to their cost-effectiveness and efficient atom utilization. The systematic analysis of the design principles and structure-activity relationship is essential for the advancement of M-SACs/Cu-based tandem catalysts. Here we first introduce various prevalent design strategies of M-SACs/Cu-based tandem catalysts for ECO2RR and then systematically summarize the latest advancements of M-SACs/Cu-based tandem system, encompassing metal-organic frameworks/Cu (MOFs/Cu), covalent organic frameworks/Cu (COFs/Cu), and nitrogen-doped carbon support transition metal single atomic materials/Cu (M-N-C/Cu). Lastly, we discuss the challenges and opportunities with the design and construction of M-SACs/Cu-based tandem catalysis for ECO2RR.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202403297"},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142778777","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Photogeneration and Direct Observation of a 2H-phosphirene and a Closed-shell Singlet Arylphosphenium Ion.

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-01-14 Epub Date: 2024-12-23 DOI: 10.1002/chem.202402494

Zi-Gang Lu, David Lee Phillips, Ming-De Li

{"title":"Photogeneration and Direct Observation of a 2H-phosphirene and a Closed-shell Singlet Arylphosphenium Ion.","authors":"Zi-Gang Lu, David Lee Phillips, Ming-De Li","doi":"10.1002/chem.202402494","DOIUrl":"10.1002/chem.202402494","url":null,"abstract":"Phosphenium ions are highly reactive species with the formula of RR'P+. Although phosphenium ions were proposed as the invaluable intermediates of various important chemical processes, the methods to generate and characterize them were very limited. In this study, a novel photoprecursor to give rise to the arylphosphenium ions, 1-(naphthalen-2-yl)phosphirane, was synthesized and investigated by femtosecond to nanosecond transient absorption spectroscopies, photoproduct analysis, and density functional theory calculations. Subsequent to photoexcitation, the S1 state of the photoprecursor of interest is populated from the higher excited states, accompanied by the generation of an unexpected 2H-phosphirene, 7bH-naphtho[1,2-b]phosphirene. After that, the resulted 2H-phosphirene is protonated by H2O in the solvent to generate the naphthalen-2-yl(hydryl)phosphenium ion, which can be attacked by H2O and oxidized by O2 to give naphthalen-2-ylphosphinic acid as the major final product. The presence of these transient species is supported by density functional theory calculation and control experiments with different solvents. This study provides an understanding of the reactivity of arylphosphenium ions as well as 2H-phosphirenes, and provides a novel method to generate and characterize these reactive species, which may help to further reveal their reactivity and explore their chemistry and use in a range of applications.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202402494"},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142764997","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Non-alternant Benzodifluoranthene Tetraimides from 7,8,9,10-Fluoranthene Diimides: Synthesis, Structure, and Optical-Limiting Properties. 从 7,8,9,10-氟蒽二酰亚胺制备非替代性苯并二氟蒽四酰亚胺：合成、结构和光学限制特性。

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-01-14 Epub Date: 2024-11-19 DOI: 10.1002/chem.202403332

Hanwen Qin, Lingli Zhao, Liping Zheng, Zhipeng Ma, Miaoli Liao, Jibin Sun, Chenghua Sun, Huajie Chen

{"title":"Non-alternant Benzodifluoranthene Tetraimides from 7,8,9,10-Fluoranthene Diimides: Synthesis, Structure, and Optical-Limiting Properties.","authors":"Hanwen Qin, Lingli Zhao, Liping Zheng, Zhipeng Ma, Miaoli Liao, Jibin Sun, Chenghua Sun, Huajie Chen","doi":"10.1002/chem.202403332","DOIUrl":"10.1002/chem.202403332","url":null,"abstract":"A novel tetraimide-functionalized non-alternant π-conjugated system, namely, benzodifluoranthene tetraimides (BDFTI), has been designed and synthesized through highly efficient UV-photocyclization of a vinyl-bridged fluoranthene diimide dimer (i. e., FDI-V). The synthesis of FDI-V starts from a straightforward three-step route to produce novel 7,8,9,10-fluoranthene diimide (FDIs) building-blocks, followed by nearly complete bromination and then Stille-coupling reaction to give the desired dimer. The analysis by X-ray crystallography confirms a near-coplanar geometry for FDIs, while BDFTI shows a U-shaped and distorted backbone configuration proven by theoretical optimizations. The tetraimide BDFTI exhibits several advantages over the FDI cores, including an extended absorption band and a red-shift in photoluminescence spectra. This enhancement can be attributed to the presence of additional electron-deficient imide units, which promotes increased intramolecular charge transfer and improved electron affinity. All the imides show a local aromatic characteristic owing to the incorporation of pentagon rings in the π-frameworks. The fully fused BDFTI exhibits nonlinear optical properties as analyzed by the open-aperture Z-scan technique, demonstrating superior optical-limiting performance compared to vinyl-bridged FDI-V. The versatile UV-photocyclization chemistries provide a pathway for developing complex and unique multiimide-functionalized π-conjugated systems, paving the way for creating high-performance optical-limiting materials.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202403332"},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142542337","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 Photolockable Polyaromatic Capsule Designed via Regiochemical Substitution. 通过 Regiochemical Substitution 设计的光锁定聚芳香族胶囊。

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-01-14 Epub Date: 2024-12-13 DOI: 10.1002/chem.202403703

Lorenzo Catti, Shiina Yasugami, Shinji Aoyama, Natsuki Kishida, Michito Yoshizawa

{"title":"A Photolockable Polyaromatic Capsule Designed via Regiochemical Substitution.","authors":"Lorenzo Catti, Shiina Yasugami, Shinji Aoyama, Natsuki Kishida, Michito Yoshizawa","doi":"10.1002/chem.202403703","DOIUrl":"10.1002/chem.202403703","url":null,"abstract":"Photocontrol over host frameworks is an elegant way to manipulate host-guest composites, yet the majority of previous systems suffer from long irradiation time and narrow guest scope, and are restricted to intramolecular photoreactions in organic solvents. Herein we present a photolockable polyaromatic capsule with high guest binding abilities in water. The capsule assembles from bent amphiphiles featuring two 2-subsutituted anthracene panels, which shows high stability against dilution and undergoes intermolecular [4+4] photo-oligomerization upon short light irradiation (<10 min). The photolocked capsule provides a roughly spherical framework, with an average, core diameter of ~3 nm, composed of amphiphilic oligomers (e. g., trimer). The new capsule shows improved host ability (up to 10-fold) in water toward various hydrophobic compounds (e. g., organic and metal-complex dyes), as compared with an analogous, non-photolockable capsule with 9-subsutituted anthracene panels. In addition, the resultant dye-loaded capsules are also successfully photolocked via short irradiation with high retention of the bound dyes.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202403703"},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142724357","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Programing Green Light-Responsive Hydrogels: from Photo-Weakening to Photo-unresponsiveness and Photo-Strengthening.

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-01-14 DOI: 10.1002/chem.202404360

Saskia Frank, Seraphine Wegner

{"title":"Programing Green Light-Responsive Hydrogels: from Photo-Weakening to Photo-unresponsiveness and Photo-Strengthening.","authors":"Saskia Frank, Seraphine Wegner","doi":"10.1002/chem.202404360","DOIUrl":"https://doi.org/10.1002/chem.202404360","url":null,"abstract":"Light-responsive hydrogels are highly valued for their dynamic mechanical properties and biocompatibility. In this study, we present a hydrogel system that can either soften or strengthen on green light exposure, or remain unresponsive to light, depending on the addition of adenosyl cobalamin (AdoCbl) and Co2+. These protein-based hydrogels were formed using genetically encoded SpyTag-SpyCatcher chemistry and included green light-sensitive CarHc protein domains. As previously reported, these hydrogels formed in the dark with the addition of AdoCbl, due to the tetramerization of the CarHc domains. Under green light exposure, the CarHc tetramers disassembled, leading to a rapid transition from gel to sol. Interestingly, we discovered that an excess of AdoCbl leads to photo-strengthening rather than photo-weakening. This occurred because light exposure induces interchain crosslinks between AdoCbl and poly-histidine tags (His6-tags) of the proteins. Furthermore, incorporating Co2+ ions enhanced hydrogel stiffness by coordinating to His6-tags. This not only suppressed photo-weakening but also promoted photo-strengthening behaviour. These findings highlight the role of His6-tags in photochemical crosslinking with excess AdoCbl and in coordination to Co2+ ions, providing a novel strategy for designing tuneable, light responsiveness in materials.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202404360"},"PeriodicalIF":3.9,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142976978","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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