Angewandte Chemie International Edition最新文献

High-Performance Electron Acceptors Containing Transition Metals

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-25 DOI: 10.1002/anie.202504616

Zheng Xu, Shuhui Ding, Wendi Shi, Wenkai Zhao, Xiangjian Cao, Zhaoyang Yao, Yaxiao Guo, Guankui Long, Chenxi Li, Xiangjian Wan, Yongsheng Chen

引用次数: 0

Cooperative Redox Reactions Encoded by Two Gene Clusters Enable Intermolecular Cycloaddition Cascade for the Formation of Meroaspochalasins

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-25 DOI: 10.1002/anie.202502766

Pengkun Li, Jie Meng, Xiaotian Zhang, Xiaopeng Zhang, Yonghao Ye, Yunpeng Zhao, Xuenian Huang, Ziou Zha, Zhenhua Guan, Suitian Lai, Zhe Chen, Zengwei Luo, Jianping Wang, Chunmei Chen, Junjun Liu, Lianghu Gu, Yuhui Sun, Shuming Li, Hucheng Zhu, Ying Ye, Yuan Zhou, Yonghui Zhang

{"title":"Cooperative Redox Reactions Encoded by Two Gene Clusters Enable Intermolecular Cycloaddition Cascade for the Formation of Meroaspochalasins","authors":"Pengkun Li, Jie Meng, Xiaotian Zhang, Xiaopeng Zhang, Yonghao Ye, Yunpeng Zhao, Xuenian Huang, Ziou Zha, Zhenhua Guan, Suitian Lai, Zhe Chen, Zengwei Luo, Jianping Wang, Chunmei Chen, Junjun Liu, Lianghu Gu, Yuhui Sun, Shuming Li, Hucheng Zhu, Ying Ye, Yuan Zhou, Yonghui Zhang","doi":"10.1002/anie.202502766","DOIUrl":"https://doi.org/10.1002/anie.202502766","url":null,"abstract":"Meroaspochalasins (mAPOs) are a group of intricate heteromers comprising two distinct subunits, dienophile aspochalasin and diene isobenzofuran, of which the biosynthetic mechanism is of great interest yet unrevealed. In this study, two independent biosynthetic gene clusters (BGCs), flas and epi, being responsible for the biosynthesis of aspochalasin B (7) and pre-diene hemiacetal 21 (or 26), respectively, were identified in the filamentous fungus Aspergillusflavipes. In vivo and in vitro studies proved that a flavin adenine dinucleotide (FAD)-dependent oxidase FlasF in the flas cluster catalyzes the crucial oxidation to generate diverse aspochalasin monomers, particularly the dienophile 7. Interactive reduction catalyzed by the short-chain alcohol dehydrogenase/reductase (SDR) FlasG and endogenous NADPH further increases the complexity of this anabolic network. The cytochrome P450 enzyme EpiC and SDR enzyme EpiD in the epi cluster collaboratively catalyze the formation of pre-diene 21 (or 26), which can spontaneously dehydrate to yield a diene, leading to the non-enzymatic cascade of [4π + 2π] Diels-Alder and formal [5π + 2π] cycloaddition reaction to generate mAPO dimers and trimer progressively. Moreover, the FAD-dependent oxidase EpiG catalyzes the hydroxylation at the C3 position of the diene as a critical step in the formation of mAPO trimers.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"61 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695149","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

Revealing Collaborative Effects of Binary Additives on Regulating Precursor Crystallization toward Highly Efficient Perovskite Solar Cells

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-25 DOI: 10.1002/anie.202424910

Shaoyu Geng, Song Zhang, Nan Shen, Geping Qu, Haojiang Shen, Jiayu Hu, Jie Yang, Yeming Jin, Ya Li, Ruirui Cao, Huayang Li, Zhitao Shen, Zong-Xiang Xu, Shi Chen, Alex K.-Y. Jen

{"title":"Revealing Collaborative Effects of Binary Additives on Regulating Precursor Crystallization toward Highly Efficient Perovskite Solar Cells","authors":"Shaoyu Geng, Song Zhang, Nan Shen, Geping Qu, Haojiang Shen, Jiayu Hu, Jie Yang, Yeming Jin, Ya Li, Ruirui Cao, Huayang Li, Zhitao Shen, Zong-Xiang Xu, Shi Chen, Alex K.-Y. Jen","doi":"10.1002/anie.202424910","DOIUrl":"https://doi.org/10.1002/anie.202424910","url":null,"abstract":"Fabricating high-quality perovskite layers with large grains and low defect density is essential for achieving high-performance solar cells. Considering the significant advancements made in additive engineering for optimizing perovskite crystallization using single additive, exploring the collaborative effect of dual additives on precursor for perovskite crystallization may be an effective way for further advancing device performance. Herein, a binary additives strategy is proposed, where PMAI and 2PACz are introduced into the precursor. Compared with the precursor with no additives or a single additive, the use of dual additives more effectively cleaves edge-shared Pb-I octahedra to expedite the transformation from PbI2 to PbI3- complexes as prenucleation clusters, and produces much larger colloidal particles with accelerated nucleation. Concurrently, the crystallization in both spin-coating and annealing processes is significantly retarded due to the stronger interaction between perovskite and binary additives with more functional groups. Benefiting from such rapid nucleation and slow crystallization, high-quality perovskite layer with larger-sized crystals and fewer defects is formed, resulting in mitigated micro-strain, enhanced charge extraction, and suppressed non-radiative recombination. Consequently, the device with dual additives could achieve an impressive efficiency of 26.05% (certified 25.49%) and retained 90% of its initial efficiency after 1200 hours of maximum power point tracking.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"21 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695239","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

Isolation of a Square Pyramidal Bis(amidophenolate)-supported As(III)-Cation: Coordination-Induced Electromerism at As

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-25 DOI: 10.1002/anie.202501439

Simon B. H. Karnbrock, Jan F. Köster, Christopher Golz, Ricardo A. Mata, Manuel Alcarazo

引用次数: 0

A Light-driven Electrochromic Materials-Based Nanomotor for H2S-Controlled Drug Release in Synergistic Cancer Chemotherapy Immunotherapy.

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-25 DOI: 10.1002/anie.202503297

Luyan Wu, Xiang Cao, Yusuke Ishigaki, Qiang Tong, Fangqi Yang, Huihui Lin, Takanori Suzuki, Quli Fan

{"title":"A Light-driven Electrochromic Materials-Based Nanomotor for H2S-Controlled Drug Release in Synergistic Cancer Chemotherapy Immunotherapy.","authors":"Luyan Wu, Xiang Cao, Yusuke Ishigaki, Qiang Tong, Fangqi Yang, Huihui Lin, Takanori Suzuki, Quli Fan","doi":"10.1002/anie.202503297","DOIUrl":"https://doi.org/10.1002/anie.202503297","url":null,"abstract":"Nanomotors hold tremendous potential for drug delivery. However, current nanomotors face limitations that compromise efficiency of drug utilization, including the use of inorganic materials with suboptimal soft interface and biocompatibility, uncontrollable drug release, insufficient directional control and slow movement speeds. Herein, we present a novel near-infrared (NIR) light-driven porous unsymmetric nanomotor with ultrafast motion, which utilizes hydrogen sulfide (H2S)-responsive cationic organic π-electron structure-based electrochromic material (F12+) for the payload and controlled release of anionic anticancer drugs, enabling synergistic cancer chemotherapy and immunotherapy. We demonstrate that the nanomotor can precisely target tumors driven by thermophoresis, tumor-targeting peptide (RGD) and H2S (highly expressed in tumors and acted as chemoattractants), which induces chemotactic behavior to guide nanomotors into tumors. Once in the tumors, the cationic F12+ is reduced to the diene F2 upon reaction with H2S, activating the nanomotor’s NIR fluorescence for real-time monitoring of drug delivery and release in vivo. Upon exposure to H2S, the nanomotor undergoes disassembly due to the disruption of electrostatic interactions between the anionic anticancer drugs and the cationic F12+, leading to the precise and controlled drug release, ensuring uniform distribution across the tumor. This innovative strategy would open avenues for delivering mRNA vaccines or other anionic drugs.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"39 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695863","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

Multi-Dimensional Ni@TiN/CNT Heterostructure with Tandem Catalysis for Efficient Electrochemical Nitrite Reduction to Ammonia

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-25 DOI: 10.1002/anie.202501578

Zhijie Cui, Pengwei Zhao, Honghai Wang, Chunli Li, Wenchao Peng, Jiapeng Liu

{"title":"Multi-Dimensional Ni@TiN/CNT Heterostructure with Tandem Catalysis for Efficient Electrochemical Nitrite Reduction to Ammonia","authors":"Zhijie Cui, Pengwei Zhao, Honghai Wang, Chunli Li, Wenchao Peng, Jiapeng Liu","doi":"10.1002/anie.202501578","DOIUrl":"https://doi.org/10.1002/anie.202501578","url":null,"abstract":"Electrochemical nitrite reduction reaction (NO2RR) is considered as a sustainable ammonia (NH3) synthesis strategy. However, there are still significant challenges in designing efficient NO2RR catalysts. Here, carbon nanotube (CNT) encapsulated Ni nanoparticles (NPs) loaded on MXene-derived TiN (Ni@TiN/CNT) heterostructure is constructed by combining molten salt etching strategy and chemical vapor deposition. Ni@TiN/CNT exhibits excellent NH3 yield rate (15.6 mg h−1 mgcat.−1), Faradaic efficiency (95.6%) and record cycle stability (NO2RR performance is virtually unattenuated after 60 cycles) at −0.7 V versus reversible hydrogen electrode (vs. RHE). In addition, the Zn-nitrite battery with Ni@TiN/CNT as the cathode shows high power density (9.6 mW cm−2) and NH3 synthesis performance. Combining validation experiments and density functional theory calculations reveal that Ni@TiN/CNT follows the tandem catalytic mechanism. The TiN site preferentially adsorbs and activates NO2−, while the Ni site provides abundant active hydrogen for the subsequent reduction process. Meanwhile, the chainmail structure of CNT prevents the oxidation and leaching of active sites, thereby significantly enhancing the stability of Ni@TiN/CNT. This work provides a new inspiration for the preparation of durable and efficient NO2RR electrocatalysts with tandem catalytic sites.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"96 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695143","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

Anode Engineering with pH-neutral Conjugated Polyelectrolyte Enabling over 19% Efficiency in Organic Solar Cells

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-25 DOI: 10.1002/anie.202504085

Yao Tong, Luxin Feng, jiayu Li, Heng Liu, Cunbin An, Shouke Yan, Bowei Xu

{"title":"Anode Engineering with pH-neutral Conjugated Polyelectrolyte Enabling over 19% Efficiency in Organic Solar Cells","authors":"Yao Tong, Luxin Feng, jiayu Li, Heng Liu, Cunbin An, Shouke Yan, Bowei Xu","doi":"10.1002/anie.202504085","DOIUrl":"https://doi.org/10.1002/anie.202504085","url":null,"abstract":"The lack of effective hole-transporting layers (HTLs) materials has become a significant bottleneck in the advancement of organic solar cells (OSCs). Particularly, to obtain sufficient doping property, most HTLs have to be used by mixing with substantial amounts of acid, which causes serious corrosion problems. Herein, by optimizing molecular conformation, we designed and synthesized two conjugated polyelectrolytes (CPEs) that exhibited superior hole-transporting capability without involving the addition of acid. The PEP-BT features a planar conjugated backbone constructed from non-fused segment, which leads to an enhanced doping effect, highly ordered molecular arrangement and reduced π-π stacking from 4.13 Å to 3.85 Å. These contributed to the outstanding hole collection performance of polyoxometalate-doped PEP-BT:POM while maintaining a neutral pH. The binary OSC showed a photovoltaic efficiency of 19.16%, demonstrating an unprecedented example that a CPE-based HTL can provide a photovoltaic efficiency exceeding 19% in OSCs. Moreover, as an another evidence of high-performance HTL, the organic light-emitting diode by incorporating PEP-BT:POM exhibited a superior luminous efficiency to the reference device, along with a decrease of 0.4 V for turn-on voltage. The results from this work demonstrates the great potential of CPEs as high-performance HTL materials.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"71 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695148","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

Cl3Al-PH3 is a Weak Lewis Pair Allowing the Synthesis of Sterically Highly Hindered Primary and Secondary Alkyl Phosphanes

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-25 DOI: 10.1002/anie.202501656

Hansjörg Grützmacher, Jan Oswald, Csilla Fekete, Matt Baker, Mark Bispinghoff, Paul G. Pringle, Norbert Weferling, Zoltan Benkő

引用次数: 0

Outside Back Cover: DNA Framework-Ensembled Aptamers Enhance Fluid Stability in Circulating Tumor Cells Capture for Tumor Treatment Evaluation

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-25 DOI: 10.1002/anie.202506102

Yirong Chen, Fan Li, Shuyang Zhang, Feng Liu, Chenzhou Mao, Min Li, Jinhua Jiang, Yueyue Zhang, Chunhai Fan, Xiaolei Zuo

引用次数: 0

Cascaded Metalation of Two-Dimensional Covalent Organic Frameworks for Boosting Electrochemical CO Reduction

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-25 DOI: 10.1002/anie.202505461

Qianfeng Gu, Yinger Xin, Mingzi Sun, Hexiang Zhang, Anchun Tang, Yanwei Zhao, Zihao Chen, Yun Song, Tuoya Naren, Lei Zhang, Jinghang Wu, Xin Wang, Fangyuan Kang, Yang Yang Li, Fu-Rong Chen, Chubin Wan, Bolong Huang, Ruquan Ye, Qichun Zhang

{"title":"Cascaded Metalation of Two-Dimensional Covalent Organic Frameworks for Boosting Electrochemical CO Reduction","authors":"Qianfeng Gu, Yinger Xin, Mingzi Sun, Hexiang Zhang, Anchun Tang, Yanwei Zhao, Zihao Chen, Yun Song, Tuoya Naren, Lei Zhang, Jinghang Wu, Xin Wang, Fangyuan Kang, Yang Yang Li, Fu-Rong Chen, Chubin Wan, Bolong Huang, Ruquan Ye, Qichun Zhang","doi":"10.1002/anie.202505461","DOIUrl":"https://doi.org/10.1002/anie.202505461","url":null,"abstract":"Carbon monoxide reduction reaction (CORR) to yield value-added methanol entails the delicate design of catalysts due to the large overpotential of this reaction. Especially, achieving precise modification of electrocatalysts while preserving the periodic alignment of active sites to optimize performance remains a significant challenge. Here, we report the cascaded metalation of phthalocyanine-based COFs for selective reduction of CO to methanol. After implanting the secondary metal (Ni), CityU-35 achieves a Faradaic efficiency (FE) of 48.4% at -0.85 V vs. RHE, surpassing that of CityU-34 (2.1%) with only Co atoms. The enhanced methanol production originates from the optimization of electronic structure with improved *CO adsorption, which is substantiated by the spectroscopic shift in UV and X-ray photoelectron spectroscopy and a stronger *CO signal in the in-situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS). Theoretical calculations have demonstrated that the cascaded metalation with the introduction of secondary Ni sites in CityU-35 not only improves the adsorption towards *CO intermediates but also supplies a fast generation of protons for the hydrogenation of *CO towards CH3OH. The optimized electronic structures with synergistic effects between Co and Ni sites after cascaded metalation reduce the energy barriers and improve the overall electroactivity.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"57 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695142","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