-
π-Fused Diazocines with Controllable Photoswitching Properties as Molecular Tweezers CCS Chem. (IF 11.2) Pub Date : 2024-04-24 Wei Yuan, Mengjiao Wu, Cheng Qian, Jingjing Guo, Yinglong Wu, Ting He, Haipeng Wei, Xiaokai Chen, Dongdong Wang, Jiawei Liu, Yue Zhao, Shihuai Wang, Jie Yang, Zhongzheng Zhang, Yulan Chen, Yanli Zhao
Diazocines, a type of photoswitch molecules, are distinguished by their unique conformation and photochromic properties. The molecular engineering of diazocines, especially π-extended ones, remains challenging due to limited synthesis methods. Here, we develop three π-fused diazocines ( BAZO-1, BAZO-2 and BAZO-3) via Bischler-Napieralski cyclization. Their isomerizations (Z ⇆ E) are switchable under
-
Lowering *CO Affinity over Cu Nanoparticles for Enhanced Electrochemical CO2 Conversion to Multi-Carbon Products at High Current Density CCS Chem. (IF 11.2) Pub Date : 2024-04-24 Ya Zhang, Qiang Zhou, Xiang-Yu Lu, Xiao-Yu Zhang, Feng Gong, Wei-Yin Sun
Direct electrochemical conversion of CO2 to multi-carbon products over small-sized Cu nanoparticles (NPs) remains a significant challenge due to the strong binding affinity between *CO and Cu sites. Herein, we developed a facile route to synthesize stable Cu NPs with a size of ca. 3.0 nm anchored on ZIF-8 (Cu/ZIF-8) and found that the electronic state of Cu NPs is effectively modulated by ZIF-8, leading
-
In Situ Revelation of the Dynamic Evolution of Molecular Water Oxidation Catalysts CCS Chem. (IF 11.2) Pub Date : 2024-04-22 Qi-Fa Chen, Xianhao Zhang, Jing Shi, Jirui Zhan, Fei Xie, Hong-Tao Zhang, Jintao Deng, Junjie Liu, Meixian Li, Yuanhua Shao, Ming-Tian Zhang
Water oxidation is a crucial reaction in artificial photosynthesis, converting solar energy into chemical energy. Due to the harsh oxidative conditions, the tolerance of water oxidation catalysts is a critical issue. In situ tracking of the dynamic evolution of molecular catalysts is an effective approach to design the sustainable catalytic process. However, there is currently a lack of effective in
-
Boosting CPL and Decagram-Scale Mechanochemistry Synthesis of Atomically Precise Superstructure from Achiral Silver Cluster and Chiral Cyclodextrin CCS Chem. (IF 11.2) Pub Date : 2024-04-22 Tianyang Xu, Sayan Paul, Chengkai Zhang, Mohammad Azam, Bao-Liang Han, Wei-Dan Si, Zhi Wang, Zhi-Yong Gao, Anakuthil Anoop, Chen-Ho Tung, Di Sun
Metal clusters with circularly polarized luminescent (CPL) activity have potential applications in security encoding, encrypted transmission, information storage, etc. However, constructing CPL-active metal clusters on a large scale using self-assemblybased synthetic approaches has been challenging. Herein, we present a collaborative strategy to assemble a chiral cyclic hydrogen-bonding (HB) platform
-
A Golden Touch in the Design of Multifunctional Porphyrin Metallacages: Host–Guest Chemistry for Drug-Target Interactions CCS Chem. (IF 11.2) Pub Date : 2024-04-18 Tamara Rodríguez-Prieto, Darren Wragg, Nicole Heiduk, Mihyun Park, Nicole Strittmatter, Roland A. Fischer, Angela Casini, Guillermo Moreno-Alcántar
The use of three-dimensional self-assembled metallacages (MCgs) as multimodal drug platforms holds great promise. However, the synthesis of MCgs with increased complexity and functionality is a great challenge since understanding of the interaction of MCgs with biological targets is still limited. In this context, this work reports on the integration of a gold(III) porphyrin scaffold into a prismatic
-
An Ultrastable, Easily Scalable and Regenerable Macrocycle-Based Hydrogen-Bonded Organic Framework CCS Chem. (IF 11.2) Pub Date : 2024-04-18 Zhi-Wei Li, Zi-Jun Huang, Ying-Xian Li, Xiaomei Wu, Wen Shi, Yue-Biao Zhang, Xiaomin Ma, Gangfeng Ouyang, Bao-Hui Ye, Gao-Feng Liu, Xiao-Ming Chen
Crystalline porous materials are increasingly significant in synthetic and materials chemistry. Nonetheless, their broad industrial deployment is hampered by challenges in stability, production cost, scalability, and regenerability. Herein, we introduce a one-pot synthetic methodology for fabricating macrocycle-based hydrogen-bonded organic frameworks utilizing commercially available materials. Notably
-
Tetraazahexacene Diimides with Ultralow Lowest Unoccupied Molecular Orbital Levels CCS Chem. (IF 11.2) Pub Date : 2024-04-18 Shuhai Qiu, Li Zhang, Xin Jin, Chengxi Zhao, Junzhi Liu, Da-Hui Qu, Wei Jiang, Zhaohui Wang
Azaacene diimides are expected to possess deep lowest unoccupied molecular orbital (LUMO) levels and narrower bandgaps while maintaining excellent solubility and enhanced stability compared to their parent acenes. However, the synthesis of fully conjugated azaacenes has posed a long-term challenge. In this study, we report a stepwise oxidation approach to successfully synthesize a series of fully conjugated
-
A DNA-programmed Cargo Distributing System in Living Cells CCS Chem. (IF 11.2) Pub Date : 2024-04-12 Yuhan Wei, Yueyue Feng, Xiaoliang Chen, Wenhe Ma, Kaizhe Wang, Qian Li, Jiang Li, Lihua Wang, Chunhai Fan, Ying Zhu
The functionalization of living cells, both internally and externally, transforming them into micromachines with specified functions, holds significant potential in fields such as biosensing, biocomputing, and intelligent theranostics. However, due to the complexity and dynamic nature of living cells, it remains challenging to allocate exogenous functional materials to specific locations within the
-
Near-Frictionless Long-Distance Water Transport in Trees Enabled by Hierarchically Helical Molecular Pumps CCS Chem. (IF 11.2) Pub Date : 2024-04-17 Yanjun Liu, Jialin Zhang, Peiyi Wu
The ascent of water in tall trees has fascinated scientists for over 130 years. However, the microscopic state and dynamic behavior of water within natural and undisturbed trees remain unknown. Here, we employ low-field nuclear magnetic resonance (NMR) to monitor the distribution and movement of water within a living tree in situ, uncovering a counterintuitive water transport process. The hierarchical
-
Adaptive and Dynamic Non-Intertwined Assembly of Rigid and Flexible Rings CCS Chem. (IF 11.2) Pub Date : 2024-04-17 Tao Wang, Xuan He, Jieqiong Xu, Dengke Shen, Liyun Mei, Guoyong Xu, Peifa Wei, Ben Zhong Tang
Biomorphic supramolecular assemblies formed through the collaboration of rigidity and flexibility, akin to bones and ligaments, play a crucial role in constructing advanced functional structures. Non-intertwined ring-ring assemblies that rely on induced fitting between rigid rings and conformationally flexible rings, have emerged as one of the thriving representatives. However, detailing how rigid
-
A Quasi-Solid-State Electrolyte with Semi-Immobilized Solvent-Like Sites for Lithium-Metal Batteries CCS Chem. (IF 11.2) Pub Date : 2024-04-17 Yang Feng, Zhenheng Huang, Ruochen Zhang, Beidou Zhong, Zhonghan Wu, Yanpeng Fan, Zhenhua Yan, Kai Zhang, Jun Chen
Quasi solid-state lithium-metal batteries (QSSLMBs) hold significant promise for enhanced energy density when compared to conventional battery systems. Nevertheless, current QSSLMBs face challenges in lithium dendrites and electrode-electrolyte interfacial side reactions driven by excessive active free solvent molecules. Herein, a metal-organic framework (MOF) with chemically grafted soft multi-ether
-
Electronic Reservoir Regulation Stabling IrOx as Efficient Cathode for Solid-State Zinc-Air Batteries CCS Chem. (IF 11.2) Pub Date : 2024-04-12 Qian Chang, Xinlong Fu, Jingchi Gao, Zhihui Zhang, Yi Wang, Changshui Huang, Yuliang Li
The electrochemical catalysts play an irreplaceable role in the fields of high-performance metal-air batteries, fuel cells and water splitting, and are the source of promoting the high performance of the system. However, a serious drawback is that activity and stability of catalysts are often difficult to maintain at the same time when applied to the electrode. Herein, we present a simple and scalable
-
Electrosynthesis of the Nylon-6 Precursor from Nitrate and Cyclohexanone over a Rutile TiO2 Catalyst CCS Chem. (IF 11.2) Pub Date : 2024-04-15 Lan Luo, Lingxiu Li, Liang Xu, Yifan Yan, Shanshan Zhang, Hua Zhou, Zhenhua Li, Mingfei Shao, Xue Duan
Electrocatalytic reduction of nitrate (NO3−) to valuable organonitrogen compounds beyond ammonia is a promising strategy for mitigating the human-caused unbalance of the global nitrogen cycle. Herein, we present an electrochemical strategy for synthesizing cyclohexanone oxime (CHO), an important feedstock in nylon-6 production through hydrogenative coupling of NO3− and cyclohexanone (CYC) using a rutile
-
Cove-Edged Boron-Doped peri-Acenes via Alkyne-Enabled Cyclization CCS Chem. (IF 11.2) Pub Date : 2024-04-15 Zengming Fan, Yujia Liu, Tianyu Zhang, Yue Wang, Chuandong Dou
Heteroatom-doping of polycyclic aromatic hydrocarbons can alter their electronic structure and thereby produce intriguing physical properties. However, it is very challenging to dope the boron atom into [n,m]peri-acenes due to the difficulty of achieving synthesis due to limitations of the synthetic method. Herein, we disclose implementation of alkyne-enabled cyclization of the organoborane π-system
-
Cationic Spherical Polypeptides with Immunogenic Cell Death Inducing Activity for Oncolytic Immunotherapy CCS Chem. (IF 11.2) Pub Date : 2024-04-15 Zhihui Guo, Tianze Huang, Renyong Yin, Yongchang Tian, Pengqi Wan, Xuan Yi, Gao Li, Peng Zhang, Chunsheng Xiao, Xuesi Chen
Immunogenic cell death (ICD) has gained increasing attention due to its capacity to trigger anticancer immunity. Herein, we report a series of fabricated cationic spherical polypeptides (CSPs) designated CSP-0 to CSP-57, with oncolytic activity and ICD-inducing ability. CSP-57 exerted the optimal broad-spectrum and tumor-cell-selective cytotoxicity by disrupting cell membranes and inducing cell necrosis
-
CO2 Capture in Liquid Phase and Room–Temperature Release and Concentration Using Mechanical Power CCS Chem. (IF 11.2) Pub Date : 2024-04-11 Aimin Li, Yuanchu Liu, Ke Luo, Qing He
Development of advanced materials with high CO2 capture capacity and, inter alia, superior regenerability with low energy consumption (low–temperature CO2 release) remains highly desired yet challenging. Herein, we firstly report the precipitation–involved CO2 capture from ultradilute sources (e.g., exhaled gas and indoor air) and the reversible room–temperature CO2 release accelerated by mechanical
-
Remote Boryl and Alkenyl Radical Migration of Olefin-Bearing Aryl Bromides CCS Chem. (IF 11.2) Pub Date : 2024-04-11 Chaokun Li, Nan Chen, Tangfeng Yao, Chenchen Zhao, Shangteng Liao, Qiuling Song
Compared with well-developed radical aromatic ring migration, heteroatomic radical migration and alkenyl radical migration remain challenging. Herein, a photoinduced remote radical migration reaction based on the aromatic skeleton through tetracoordinate boron species has been developed. In this work, commercially available diboron reagent (B2pin2) or alkenyl boron (alkenylBpin) react with o-bromostyrenes
-
Characterization and Monitoring of Transient Enamine Radical Intermediates in Photoredox/Chiral Primary Amine Synergistic Catalytic Cycle CCS Chem. (IF 11.2) Pub Date : 2024-04-11 Shixue Zhang, Liang Cheng, Jian-Qing Qi, Zongbin Jia, Long Zhang, Lei Jiao, Xingwei Guo, Sanzhong Luo
Enamine-derived radicals are crucial intermediates in singly occupied molecular orbital (SOMO) catalysis. However, observing them directly is elusive and remains a long-standing challenge. Here, an advanced time-resolved electron paramagnetic resonance technique was employed to characterize and monitor the key intermediates in photoredox transformations by primary aminocatalysis on a microsecond timescale
-
Artificial Chlorophyll-like Structure for Photocatalytic CO2 Chemical Fixation CCS Chem. (IF 11.2) Pub Date : 2024-04-11 Lei Li, Wenxiu Liu, Hanghao Ying, Xin He, Shu Shang, Peng Zhang, Xiaodong Zhang, Shuhu Liu, Hui Wang, Yi Xie
In nature, green leaves accomplish photosynthesis via chloroplasts, where the Mg-N4-centered chlorophyll and enzymes undertake light absorption and catalytic reaction, involving CO2 fixation, with the resultant six-carbon compound, respectively. This intriguing phenomenon inspired us to design an artificial photosynthetic system that synergizes these dual attributes, a field that has remained largely
-
Interactional Analysis of Single Mitochondrial Function Directly in Living Cell Reveals the Proton Circuit Decoupling of Mitochondria at the Preliminary Stage of Apoptosis CCS Chem. (IF 11.2) Pub Date : 2024-04-11 Baoguo Wang, Jin Zhu, Tianxiang Wei, Yixin Zhang, Mingyue Li, Zilong Zhang, Tao Gao, Zhihui Dai
Analyzing single organelles within the intricate compartmentalized systems of eukaryotic cells poses significant challenges in biomedical research. Presently, assessment of organelle functions frequently relies on the disjointed application of multiple techniques, resulting in constraints on the promptness and precision of data acquisition. Herein, a dual-nanopore electrochemical biosensor has been
-
A Simple Synthesis of Tetraamino-[60]Fullerene Epoxides as Potential Antitumor Drug Candidates CCS Chem. (IF 11.2) Pub Date : 2024-04-10 Yicheng Lu, Jie Li, Xiaolong Liu, Dan He, Libin Yang, Wei Zhou, Xie Wang, Shanshan Chen, Shiliang Chen, Yating Liu, Xin Wang, Jiao Li, Jiawei Huo, Yang Liu, Zehu Wang, Meihan Liu, Yijun Wang, Yamin Li, Fuwen Zhao, Shumu Li, Jinchao Wei, Jianan Liu, Wei Li, Chunru Wang
Amphiphilic aminated fullerenes have a broad margin of safety and significant antitumor effects. Herein, we develop a simple and versatile synthesis strategy for tetraamino-[60]fullerene epoxide (C60(NR1R2)4O) using C60Cl6 as a precursor, which notably reduces the reaction time to less than 1 h while retaining a high yield of over 80% with both cyclic and linear secondary amine substrates even at the
-
Phosphine-Catalyzed Asymmetric Dearomative [3+2] Annulation Reaction of Benzimidazoles with Cyclopropenones CCS Chem. (IF 11.2) Pub Date : 2024-04-10 Shan-Shan Zhang, Rui-Xiang Wang, Qing Gu, Shu-Li You
A phosphine-catalyzed intermolecular asymmetric dearomatization reaction of benzimidazoles with cyclopropenones has been developed. In the presence of 5 mol % of commercially available chiral phosphine catalyst, the dearomative [3+2] annulation reaction proceeds smoothly to afford the corresponding dearomatized heterocycles in excellent yields (up to 98%) and enantioselectivity (up to 99% ee). Meanwhile
-
Hierarchical On-Surface Synthesis of Two-Dimensional Networks via Multipoint S···N and S···H Bonding CCS Chem. (IF 11.2) Pub Date : 2024-04-10 Chen-Hui Shu, Li-Xia Kang, Shan-shan Wang, Yan He, Ruo-Xi Zhang, Xuelei Su, Ping Yu, Xingguang Li, Pei-Nian Liu
Although electrostatic bonding between chalcogen (Ch) atoms (O, S, Se, and Te) and nitrogen (N) has emerged as a powerful driving force in the fabrication of supramolecular structures; this noncovalent bond has not yet been used to link polymers to form networks. In this study, we took advantage of additive enthalpy in forming multipoint noncovalent bonds to construct a two-dimensional (2D) network
-
High-Porosity, Layered Iridium Oxide as an Efficient, Durable Anode Catalyst for Water Splitting CCS Chem. (IF 11.2) Pub Date : 2024-04-10 Zhoubing Xie, Xiao Liang, Zhenye Kang, Yongcun Zou, Xiyang Wang, Yimin A. Wu, Graham King, Qi Liu, Yalan Huang, Xiao Zhao, Hui Chen, Xiaoxin Zou
Lowering iridium (Ir) loading without sacrificing activity and durability is critical to the future development of proton exchange membrane water electrolyzer (PEMWE). Here, we present the synthesis of iridate-derived, layered iridium oxide microparticles (dubbed p-L-IrO2) with a high open porosity of approximately 74% and their structural advantages for the fabrication of efficient, durable, low-Ir-loading
-
An Ion-Channel-Reconstructed Water/Organic Amphiphilic Quasi-Solid-State Electrolyte for High-Voltage Energy Storage Devices CCS Chem. (IF 11.2) Pub Date : 2024-04-11 Zekai Zhang, Qian He, Hengyi Wang, Changwei Liu, Hongchun Mu, Haiping Su, Xia Han, Honglai Liu, Cheng Lian
Quasi-solid-state electrolytes (QSSE) have garnered significant attention due to combining the dynamic properties of liquid electrolytes and the high safety of solid-state electrolytes. However, the limited electrochemical stability window (ESW) of liquid electrolytes and the low conductivity of the polymer matrix seriously constrain practical application. Herein, an ant-nest electrospun amphiphilic
-
Tailored Interphases Construction for Enhanced Si Anode and Ni-Rich Cathode Performance in Lithium-Ion Batteries CCS Chem. (IF 11.2) Pub Date : 2024-04-11 Yuxiang Huang, Yuchen Ji, Guorui Zheng, Hongbin Cao, Haoyu Xue, Xiangming Yao, Lu Wang, Shiming Chen, Zuwei Yin, Feng Pan, Luyi Yang
As promising candidates for high-energy-density lithium-ion batteries, both silicon (Si) anodes and nickel-rich cathodes face significant challenges due to structural instability arising from interphases. In this study, we introduce tetravinylsilane (TVSi) as a multifunctional electrolyte additive to engineer tailored interphases simultaneously on Si anode and LiNi0.92Mn0.05Co0.03O2 cathode, thereby
-
Regulating Mono/Binuclear Fe Species in Framework Al-Rich Zeolites for Efficient Low-Temperature Alkane Oxidation CCS Chem. (IF 11.2) Pub Date : 2024-04-11 Qiang Zhang, Jialiang Li, Guangyuan He, Junyan Li, Ziyi Chen, Qing Zhang, Chunyu Wang, Guodong Qi, Qiang Wang, Peng Zhang, Jun Xu, Osamu Terasaki, Donghai Mei, Zhongmin Liu, Jihong Yu
Zeolite-encapsulated extra-framework mono/binuclear Fe3+ species present higher catalytic activities compared to clusters and nanoparticles for direct low-temperature alkane oxidation. However, the fine control of mono/binuclear Fe3+ in zeolites is challenging and the reaction mechanism of low-temperature alkane oxidation remains not clearly identified. Different from previous impregnation and ion-exchange
-
Exploration of mixed polyanionic compound for potential high-voltage cathode materials in sodium-ion batteries CCS Chem. (IF 11.2) Pub Date : 2024-04-09 Tianyi Song, Nanzhong Wu, Xiao Zheng, Xinyuan Zhang, Shu Guo, Qi Yan, Wenjiao Yao, Yongbing Tang
Mixed polyanionic compounds are potential cathode materials for sodium-ion batteries. Herein, considering the advantages of the strong inductive effect of sulfate and the diverse, flexible coordination modes of oxalate, we systematically explored mixed sulfate-oxalate systems and obtained three sodium-contained polyanionic compounds. Interestingly, the novel three-dimensional Na2Co(C2O4)(SO4)·xH2O
-
Donor-Acceptor MOFs featuring Tunable Triplet States for Multi-Stimulus Responsive Room-Temperature Charge Transfer Phosphorescence CCS Chem. (IF 11.2) Pub Date : 2024-04-09 Lin Geng, Kai Wang, Rui Sun, Chang-Tai Li, Xiao-Ru Li, Meng Zhang, Mei-Hui Yu, Ze Chang, Xian-He Bu
Room-temperature phosphorescence (RTP) has drawn considerable attention due to its fascinating applications. Herein, we report the achievement of multi-stimulus responsive RTP by utilizing the customizable donor-acceptor (D-A) MOF platform for charge-transfer (CT) based triplet state tuning. A succession of electron-rich donors was introduced into the triazine-based electron-deficient framework ( NKU-Mg-2)
-
A golden touch in the design of multifunctional porphyrin metallacages: Host-guest chemistry for drug-target interactions. CCS Chem. (IF 11.2) Pub Date : 2024-04-03 Tamara Rodríguez-Prieto, Darren Wragg, Nicole Heiduk, Mihyun Park, Nicole Strittmatter, Roland A. Fischer, Angela Casini, Guillermo Moreno-Alcántar
The use of three-dimensional self-assembled metallacages (MCgs) as multimodal drug platforms holds great promise. However, the synthesis of MCgs with increased complexity and functionality is a great challenge, and knowledge of the interaction of MCgs with biological targets is still lacking. In this context, this work reports on the integration of a gold(III) porphyrin scaffold into a prismatic metallacage
-
Identification of Defect Origin and White-Light Emission Tuning of Chalcogenide Quantum Dots Through Pressure Engineering CCS Chem. (IF 11.2) Pub Date : 2024-04-04
CCS Chemistry, Ahead of Print.
-
Asymmetric Nucleophilic Additions Promoted by Quaternary Phosphonium Ion Pair Catalysts CCS Chem. (IF 11.2) Pub Date : 2024-04-04 Lingzhu Chen, Youlin Deng, Tingting Li, Deyu Hu, Xiaoyu Ren, Tianli Wang
Chiral quaternary phosphonium ion pair catalysis showcases a distinctive catalytic and stereoinductive mode arising from the synergy between ionic and noncovalent interactions. Over the recent decades, this methodology has been widely adopted to facilitate enantioselective nucleophilic addition reactions, including conjugate addition, Henry reaction, Mannich reaction, Strecker reaction, and hydrophosphonylation
-
Electrosynthesis of the nylon-6 precursor from nitrate and cyclohexanone over a rutile TiO2 catalyst CCS Chem. (IF 11.2) Pub Date : 2024-04-04 Lan Luo, Lingxiu Li, Liang Xu, Yifan Yan, Shanshan Zhang, Hua Zhou, Zhenhua Li, Mingfei Shao, Xue Duan
Electrocatalytic reduction of nitrate (NO3−) to valuable organonitrogen compounds beyond ammonia is a promising strategy for mitigating the human-caused unbalance of the global nitrogen-cycle. Herein, we present an electrochemical strategy for synthesizing cyclohexanone oxime (CHO), an important feedstock in nylon-6 production, through the hydrogenative coupling of NO3− and cyclohexanone (CYC) using
-
Mass Spectrometry Imaging Reveals the Redox and Metabolic Heterogeneity CCS Chem. (IF 11.2) Pub Date : 2024-04-03 Jing Han, Huihui Liu, Yafeng Li, Junyu Chen, Ke Jia, Lingwei Meng, Caiqiao Xiong, Suming Chen, Zongxiu Nie
CCS Chemistry, Ahead of Print.
-
Author Spotlight CCS Chem. (IF 11.2) Pub Date : 2024-04-02
CCS Chemistry, Volume 6, Issue 4, Page 829-832, April 2024.
-
Cobalt-Catalyzed Electrochemical Enantioselective Reductive Cross-Coupling of Organohalides CCS Chem. (IF 11.2) Pub Date : 2024-04-02 Shi-Shuo Xu, Hui Qiu, Pei-Pei Xie, Zhen-Hua Wang, Xiu Wang, Chao Zheng, Shu-Li You, Tian-Sheng Mei
Transition metal-catalyzed asymmetric reductive coupling of two electrophiles has emerged as a powerful tool for carbon–carbon bond formation; however, the enantioselective reductive cross-coupling of two aryl halides has not been developed and remains a challenge. Herein, we demonstrated the enantioselective reductive cross-coupling of two aryl halides by combining cobalt catalysis with electrochemistry
-
Rare-Earth Metal-Catalyzed Asymmetric Addition/Hydroamidination of Nitriles and Allylamines for the Concise Synthesis of Chiral Imidazolines CCS Chem. (IF 11.2) Pub Date : 2024-04-02 Chenhao Zhu, Yuqiao Zhou, Jing Zhang, Jianfeng Li, Yuxin Zhang, Fei Wang, Xiaoming Feng, Shunxi Dong
Chiral 2-substituted imidazolines are not only privileged scaffolds in many bioactive compounds, but they are also widely used as ligands and catalysts in asymmetric synthesis. However, the synthesis of enantioenriched 2-substituted imidazolines is heavily relied on in step-wise synthetic approaches to chiral diamines under relatively harsh conditions. Herein, we present a highly enantioselective
-
-
Chemical Strategies of Tailoring PEDOT:PSS for Bioelectronic Applications: Synthesis, Processing and Device Fabrication CCS Chem. (IF 11.2) Pub Date : 2024-04-02 Yewei Huang, Lingfeng Tang, Yuanwen Jiang
Poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) has been the most prominent conducting polymer due to its outstanding electrical properties, chemical stability, biocompatibility, and commercial availability. In this mini review, we aim to comprehensively outline the chemical approaches employed in tailoring PEDOT:PSS for bioelectronic applications. We open our discussion by showcasing
-
Rhodium-Catalyzed Asymmetric Trifluoromethoxylation of Racemic Allylic Trichloroacetimidates CCS Chem. (IF 11.2) Pub Date : 2024-03-28 Liyan Wang, Yafeng Si, Yu-Xin Luan, Pingping Tang
A rhodium/diene catalyzed asymmetric allylic trifluoromethoxylation reaction is reported, which afforded chiral trifluoromethoxylated allylic compounds in 52%–97% yields with up to 97% enantiomeric excess. These are the first examples of asymmetric allylic trifluoromethoxylation. The reactions proceed via a dynamic kinetic process that allowed for the use of racemic allylic trichloroacetimidates as
-
Photoelectrochemical Iron-Catalyzed C(sp3)–H Borylation of Alkanes in a Position-Selective Manner CCS Chem. (IF 11.2) Pub Date : 2024-03-28 Wen Wei, Bin Wang, Simon L. Homölle, Jinbin Zhu, Yanjun Li, Tristan von Münchow, Isaac Maksso, Lutz Ackermann
Catalytic C–H borylation is of prime topical importance, since easily available feedstock chemicals can thereby be transformed into valuable transient functional groups in the absence of directing groups. Herein, we disclose an iron-catalyzed C(sp3)–H borylation of simple, non-prefunctionalized alkanes, providing access to value-added products in a single step by means of photoelectrochemistry. The
-
Isoreticular Regulation of Two-Dimensional Redox-Active Covalent Organic Framework Cathodes for Enhanced Lithium-Ion Storage CCS Chem. (IF 11.2) Pub Date : 2024-03-28 Zhangyi Xiong, Liang Gu, Ying Liu, Hao Wang, Le Shi, Xiaowei Wu, Lingmei Liu, Zhijie Chen
A challenge facing scientists is the rational synthesis of highly crystalline covalent organic frameworks (COFs), consisting of both n-type and p-type redox-active units, as cathodes for high-performance lithium-ion batteries (LIBs). Herein, we apply reticular chemistry to regulate a COF platform with the kgm topology via an in-situ postsynthetic oxidation strategy. We integrate both n-type and p-type
-
Expanded Porphyrin Exhibiting Off-Centered Out-of-Plane Coordination to Dysprosium CCS Chem. (IF 11.2) Pub Date : 2024-03-28 Dmitry I. Nazarov, Jorge Labella, Alexey V. Kuzmin, Maxim A. Faraonov, Evgenii N. Ivanov, Salavat S. Khasanov, Tomas Torres, Mikhail K. Islyaikin, Dmitri V. Konarev
The complexation of high-spin lanthanides to porphyrinoids is a powerful strategy for the development of advanced molecular magnets. In this context, the use of expanded porphyrinoids remains elusive since their coordination chemistry is challenging to control. Herein, taking inspiration from on-surface chemistry, we explored the coordination of Dy3+ to a six-membered porphyrinoid, namely, the hemihexaphyrazine
-
Generation of Hydrides or Hydrogen Radicals for Hydrodehalogenation and Deuterodehalogenation of gem-Dihaloalkenes CCS Chem. (IF 11.2) Pub Date : 2024-03-28 Zhe Chang, Cheng-Yu Yao, Wen-Jie Feng, Yi-Fan Zhao, Ru-Ru Qian, Xiao Hu, Yan Li, Deguang Liu, Xi Lu, Yao Fu
Terminal monohaloalkenes are common synthetic fragments used in organic synthesis and are also found in many natural products. Their Z/E stereoisomers are difficult to physically separate, being a persistent difficulty for functional molecular design and synthesis. Herein, we report complementary hydride and hydrogen radical generation pathways to effectuate hydrodehalogenation and deuterodehalogenation
-
Characterization and Monitoring of Transient Enamine Radical Intermediates in Photoredox/Chiral Primary Amine Synergistic Catalysis Cycle CCS Chem. (IF 11.2) Pub Date : 2024-03-28 Shixue Zhang, Liang Cheng, Jian-Qing Qi, Zongbin Jia, Long Zhang, Lei Jiao, Xingwei Guo, Sanzhong Luo
Enamine-derived radicals are crucial intermediates in singly occupied molecular orbital (SOMO) catalysis. However, observing them directly is elusive and remains a long-standing challenge. Here, an advanced time-resolved electron paramagnetic resonance technique is employed to characterize and monitor the key intermediates in photoredox transformations by primary aminocatalysis on a microsecond timescale
-
Intrinsically Stretchable Electroluminescent Materials and Devices CCS Chem. (IF 11.2) Pub Date : 2024-03-23 Wei Liu, Glingna Wang, Sihong Wang
Intrinsically stretchable electroluminescent (EL) devices have emerged as pivotal components with transformative potential in various domains, including wearable technology, medical devices, human–machine interfaces, and communications. This mini-review focuses on the recent progress in the development of intrinsically stretchable EL materials, highlighting milestones and breakthroughs in the field
-
The Smallest Monofluorodiazoethane Reagent and Its [3 + 2] Cycloaddition Reactions CCS Chem. (IF 11.2) Pub Date : 2024-03-23 Xiaodong Tang, Ming-Yue He, Ran Guo, Hao-Nan Liu, Jing Nie, Ilan Marek, Jun-An Ma, Fa-Guang Zhang
Given the widespread applications of fluorinated substances in pharmaceuticals, biology, and materials, the development of fluorine-containing building blocks remains an important topic in organic chemistry. In the repertoire of fluorinated diazo compounds, research on tri- and difluorodiazoethane is well-established, but the lack of synthetic methods has left studies related to monofluorodiazoethane
-
Supramolecular Polymerization of Hydrogen-Bonded Trimers in Bulk and Aqueous Medium CCS Chem. (IF 11.2) Pub Date : 2024-03-23 Freek V. de Graaf, Stef A. H. Jansen, Sandra M. C. Schoenmakers, Bas van Genabeek, Marle E. J. Vleugels, Bart W. L. van den Bersselaar, E. W. Meijer, Ghislaine Vantomme
Synthetic molecules that form functional noncovalent assemblies in water have received much attention for their potential applications as biomaterials. In this work, we introduce a novel water-compatible monomer based on the phthalhydrazide moiety that assembles into hydrogen-bonded trimeric discs. In bulk, the material exhibits a cylindrical nanostructure in the liquid-crystalline phase at elevated
-
Metal Ion-Coordinated Biomolecular Noncovalent Glass with Ceramic-like Mechanics CCS Chem. (IF 11.2) Pub Date : 2024-03-23 Shuai Cao, Wei Fan, Rui Chang, Chengqian Yuan, Xuehai Yan
Glass materials play a vital role in scientific research and engineering applications. Biomolecular noncovalent glasses (BNG), based on amino acids and peptides, have been proposed as the next-generation glass materials to meet the demand of a sustainability and circular economy. However, bulk BNG with remarkable mechanics and tunable photoluminescence are still rare due to the nature of weak noncovalent
-
Organochlorides Mediate Oxidation Reactions Induced by Low Dose Ionizing Radiation CCS Chem. (IF 11.2) Pub Date : 2024-03-23 Juncheng Liu, Tobias G. Brevé, Bing Xu, Peter-Leon Hagedoorn, Antonia G. Denkova, Rienk Eelkema
The controlled release of drugs using local ionizing radiation presents a promising approach for targeted cancer treatment, particularly when applied in concurrent radio-chemotherapy. In these approaches, radiation-generated reactive species often play an important role. However, the reactive species that can be used to trigger release have low yield and lack selectivity. Here, we demonstrate the generation
-
Using BODIPY Unit to Design Molecular Acceptors with Absorption Wavelength of >1000 nm for Organic Photodetectors CCS Chem. (IF 11.2) Pub Date : 2024-03-22 Yinghui Wang, Jiahui Wang, Junhui Miao, Jun Liu, Lixiang Wang
Near-infrared (NIR) organic photodetectors (OPDs) are promising in flexible electronic and imaging sensor applications. However, high-performance NIR-II OPDs with photoresponse wavelength beyond 1000 nm are rare due to the lack of narrow bandgap molecular acceptors. In this work, an A-D-A′-D-A-type molecular acceptor with an onset absorption wavelength of 1150 nm was developed. Its narrow bandgap was
-
Single-Molecule Characterization of van der Waals Contact Between Alkane and Gold CCS Chem. (IF 11.2) Pub Date : 2024-03-22 Hongyu Ju, Jinying Wang, Wangping Liu, Jie Hao, Mengmeng Li, Yanxia Xu, Boyu Wang, Suhang He, Kunrong Mei, Andrew C.-H. Sue, Keqiu Chen, Chuancheng Jia, Xuefeng Guo
Van der Waals (vdW) contact, dominated by weak but ubiquitous vdW interactions, plays a significant role in diverse fields such as supramolecular chemistry, nanotechnology, and surface science. Accurate characterization of vdW contact at the single-molecule level remains challenging. Herein, we combine the scanning tunneling microscope break junction technique with first-principles calculations to
-
Construction of Planar Chiral Ferrocenes by Cobalt-Catalyzed Enantioselective C–H Acyloxylation Enabled by Dual Ligands CCS Chem. (IF 11.2) Pub Date : 2024-03-22 Fan-Rui Huang, Peng Zhang, Qi-Jun Yao, Bing-Feng Shi
Oxy-substituted planar chiral ferrocenes are of great importance in asymmetric synthesis and pharmaceuticals. However, enantioselective C–H activation of ferrocenes that form C–O bonds remains a huge challenge and has not yet been reported. Herein, the asymmetric synthesis of oxy-substituted planar chiral ferrocenes is achieved by cobalt-catalyzed enantioselective dehydrogenative C–H acyloxylation
-
Remote Boryl and Alkenyl Radical Migration of Olefin-bearing Aryl Bromides CCS Chem. (IF 11.2) Pub Date : 2024-03-21 Chaokun Li, Nan Chen, Tangfeng Yao, Chenchen Zhao, Shangteng Liao, Qiuling Song
Compared with the well-developed radical aromatic ring migration, heteroatomic radical migration and alkenyl radical migration remain challenging. Herein, a photo-induced remote radical migration reaction based on the aromatic skeleton through tetracoordinate boron species has been developed. In this work, commercially available diboron reagent (B2pin2) or alkenyl boron (alkenylBpin) react with o-bromostyrenes
-
Identification of Defect Origin and White-light Emission Tuning of Chalcogenide Quantum Dots through Pressure Engineering CCS Chem. (IF 11.2) Pub Date : 2024-03-16 Pengfei Lv, Zhiwei Ma, Jiajia Ning, Guanjun Xiao, Bo Zou
Chalcogenide quantum dots (QDs) are established as promising materials for white-light-emitting applications because of their wide surface defect emission. However, the limited understanding about the origin of defect emission poses challenges in attaining efficient white-light emission. Herein, high pressure is introduced to strengthen the interaction between the different types of ligands and QDs
-
Hierarchical On-surface Synthesis of Two-dimensional Networks via Multipoint S⋯N and S⋯H bonding CCS Chem. (IF 11.2) Pub Date : 2024-03-15 Chen-Hui Shu, Li-Xia Kang, Shan-shan Wang, Yan He, Ruo-Xi Zhang, Xuelei Su, Ping Yu, Xingguang Li, Pei-Nian Liu
Although electrostatic bonding between chalcogen atoms and nitrogen has emerged as a powerful driving force in the fabrication of supramolecular structures, this noncovalent bond has not yet been used to link polymers to form networks. Taking advantage of additive enthalpy in forming multipoint noncovalent bonds, in this study we constructed a two-dimensional (2D) network via the hierarchical on-surface
-
Bioinspired Total Syntheses of Grayanotoxins II/III, Kalmanol, and Rhodomollacetals A–C with Three Distinct Skeletons CCS Chem. (IF 11.2) Pub Date : 2024-03-15 Hao Cheng, Tianhao Ma, Xiao Liu, Yanxing Jia
Grayanane diterpenoids, which have intricate molecular architecture and interesting pharmacological properties, have attracted considerable interest of organic chemists since 1970s. However, the total syntheses of grayanane diterpenoids have been accomplished by only seven groups, which have mainly focused on the same carbon skeleton. Herein, we disclose the bioinspired total syntheses of six grayanane
-
Imidazole-Linked Fully Conjugated Covalent Organic Framework for High-Performance Sodium-Ion Battery CCS Chem. (IF 11.2) Pub Date : 2024-03-15 Lu Liu, Yu Gong, Yifan Tong, Hao Tian, Xubo Wang, Yiming Hu, Shaofeng Huang, Weiwei Huang, Sandeep Sharma, Jingnan Cui, Yinghua Jin, Weitao Gong, Wei Zhang
Covalent organic frameworks (COFs) have garnered increasing attention as promising electrode materials for sodium-ion batteries (SIBs) due to their ordered backbones, uniform pore sizes, and high surface areas. However, they also face challenges, including low capacity, unsatisfactory rate performance, and limited cycling stability, which pose the primary obstacles to their practical use. Herein, a
-
Rhodium-Catalyzed Asymmetric Trifluoromethoxylation of Racemic Allylic Trichloroacetimidates CCS Chem. (IF 11.2) Pub Date : 2024-03-11 Liyan Wang, Yafeng Si, Yu-Xin Luan, Pingping Tang
A rhodium/diene catalyzed asymmetric allylic trifluoromethoxylation reaction is reported, which afforded chiral trifluoromethoxylated allylic compounds in 52–97% yields with up to 97% enantiomeric excess. These are the first examples of asymmetric allylic trifluoromethoxylation. The reactions proceed via a dynamic kinetic process that allowed for the use of racemic allylic trichloroacetimidates as
-
Cobalt-Catalyzed Electrochemical Enantioselective Reductive Cross-Coupling of Organohalides CCS Chem. (IF 11.2) Pub Date : 2024-03-15 Shi-Shuo Xu, Hui Qiu, Pei-Pei Xie, Zhen-Hua Wang, Xiu Wang, Chao Zheng, Shu-Li You, Tian-Sheng Mei
Transition metal-catalyzed asymmetric reductive coupling of two electrophiles has emerged as a powerful tool for carbon-carbon bond formation, however, the enantioselective reduction cross-coupling of two aryl halides has not been developed and remains a challenge. Herein, we demonstrated the enantioselective reductive cross-coupling of two aryl halides by combining cobalt catalysis with electrochemistry