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Metallo-Supramolecular Helicates as Surface-Enhanced Raman Scattering (SERS) Substrates with High Tailorability

Angewandte Chemie 2024年第2期137卷

作者： Bo Song Zhonghui Zhang Dr. Weitao Dou Dr. Xiaoli Zhao Yanfei Niu Prof. Chen Wang Chunchun Li Prof. Jonathan R. Nitschke Prof. Yang Tian Prof. Hai-Bo Yang Prof. Lin Xu State Key Laboratory of Molecular & Process Engineering Shanghai Key Laboratory of Green Chemistry and Chemical Processes Shanghai Frontiers Science Center of Molecule Intelligent Syntheses School of Chemistry and Molecular Engineering East China Normal University Shanghai 200062 China Institute of Photochemistry and Photofunctional Materials University of Shanghai for Science and Technology 516 Jungong Road Shanghai 200093 P. R. China Yusuf Hamied Department of Chemistry University of Cambridge Lensfield Road Cambridge CB2 1EW United Kingdom

The exploration of novel functionalized supramolecular coordination complexes (SCCs) can enable new applications in domains that include purification and sensing. In this study, employing a coordination-driven self-assembly strategy, we designed and prepared a series of benzochalcogenodiazole-based metallohelicates as high-efficiency charge-transfer surface-enhanced Raman scattering (SERS) substrates, expanding the range of applications for these metallohelicates. Through structural modifications, including the substitution of single heteroatoms on ligands, replacement of coordinating metals, and alteration of ligand framework linkages, the Raman performance of these metallohelicates as substrates were systematically optimized. Notably, the SERS enhancement factors (EFs) of the metallohelicate-based SERS substrates were significantly enhanced to levels as high as 1.03×10 7 , which rivals the EFs of noble metals devoid of “hot spots”. Additionally, the underlying Raman enhancement mechanisms of these metallohelicates have been investigated through a combination of control experiments and theoretical calculations. This study not only demonstrates the utility of metallohelicates as SERS substrates but also offers insights and materials for the development of high-efficiency new charge-transfer SERS substrates.

关键词： Supramolecular Chemistry Coordination-driven Self-assembly Metallacages Surface-Enhanced Raman Scattering Benzothiadiazole

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Lattice Strain engineering Boosts CO2Electroreduction to C2+Products

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Angewandte Chemie 2024年第38期136卷

作者： Jiapeng Jiao Xinchen Kang Jiahao Yang Shuaiqiang Jia Xiao Chen Yaguang Peng Chunjun Chen Xueqing Xing Zhongjun Chen Mingyuan He Haihong Wu Buxing Han Shanghai Key Laboratory of Green Chemistry and Chemical Processes State Key Laboratory of Petroleum Molecular & Process Engineering School of Chemistry and Molecular Engineering East China Normal University Shanghai 200062 China Institute of Eco-Chongming Chongming District Shanghai 202162 China Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Centre for Excellence in Molecular Sciences Centre for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China School of Chemistry and Chemical Engineering University of Chinese Academy of Sciences Beijing 100049 China Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China

Regulating the binding effect between the surface of an electrode material and reaction intermediates is essential in highly efficient CO 2 electro-reduction to produce high-value multicarbon (C 2+ ) compounds. Theoretical study reveals that lattice tensile strain in single-component Cu catalysts can reduce the dipole–dipole repulsion between *CO intermediates and promotes *OH adsorption, and the high *CO and *OH coverage decreases the energy barrier for C−C coupling. In this work, Cu catalysts with varying lattice tensile strain were fabricated by electro-reducing CuO precursors with different crystallinity, without adding any extra components. The as-prepared single-component Cu catalysts were used for CO 2 electro-reduction, and it is discovered that the lattice tensile strain in Cu could enhance the Faradaic efficiency (FE) of C 2+ products effectively. Especially, the as-prepared Cu TPA catalyst with high lattice tensile strain achieves a FE C2+ of 90.9 % at −1.25 V vs. RHE with a partial current density of 486.1 mA cm −2 .

关键词： CO2 electro-reduction lattice strain multicarbon products single-component Cu

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Advances in immunoPET/SPECT imaging: The role of Fab and F(ab′) 2 fragments in theranostics

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Acta Pharmaceutica Sinica B 2025年

作者： Wenpeng Huang Jingwei Zhou Yanchen Liu Yihan Yang Rachel J. Saladin Jessica C. Hsu Weibo Cai Lei Kang Department of Nuclear Medicine Peking University First Hospital Beijing 100034 China Department of Plastic and Reconstructive Surgery Shanghai Ninth People’s Hospital Shanghai Jiao Tong University School of Medicine Shanghai 200011 China State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Science Beijing 100190 China Departments of Radiology and Medical Physics University of Wisconsin - Madison Madison WI 53705 USA

With the advent of precision medicine and personalized treatment, targeted therapies have become pivotal in oncology. Noninvasive molecular imaging, especially immunoPET/SPECT, plays a crucial role in refining cancer diagnostics and treatment monitoring by visualizing biological processes at the molecular level. This review explores the dynamic field of immunoPET/SPECT imaging using Fab and F(ab′) 2 fragments, characterized by advantageous pharmacokinetics and swift clearance from the bloodstream, making them suitable for same-day imaging procedures. We examine contemporary strategies for radiolabeling these fragments with PET and SPECT radionuclides and discuss potential advancements and the challenges anticipated in the further development of Fab and F(ab′) 2 fragments. Despite the complexities involved in their development, these fragments hold significant promise for advanceing personalized cancer treatment. keys to this advancement are innovative radiolabeling techniques, site-specific conjugation chemistries, and short-lived radionuclides, all of which are crucial for overcoming existing limitations and enhancing the clinical utility of these imaging agents. As research progresses, Fab and F(ab′) 2 fragments are expected to become central to the future of cancer diagnostics and therapeutic monitoring, thereby improving patient management and contributing significantly to the evolution of personalized medicine.

关键词： ImmunoPET ImmunoSPECT Fab F(ab′) 2 Antibody fragment Molecular imaging Therapy Diagnostics

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Corrigendum to “Efficient recovery of bio-based 1,2,4-butanetriol by using boronic acid anionic reactive extraction” [Sep. Purif. Technol. 255 (2021) 117728]

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Separation and Purification Technology 2021年 274卷

作者： Qiyu Meng Jiemiao Yu Liangrong Yang Yanqing Li Mo Xian Huizhou Liu CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Biochemical Engineering Chinese Academy of Sciences Beijing 100190 China School of Chemical Engineering University of Chinese Academy of Sciences Beijing 100049 China CAS Key Laboratory of Biobased Materials Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Sciences Qingdao 266101 China

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Selective electroreduction of carbon dioxide to ethylene over stable iodide-induced asymmetric copper sites within a metal-organic polyhedron

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Science Bulletin 2025年

作者： Yaguang Peng Yinlin Chen Zi Wang Yaoyu Yin Jiangnan Li Huanyan Liu Jiapeng Jiao Wenling Zhao Ran Duan Pei Zhang Jiahao Yang Hengan Wang Xueqing Xing Zhimin Liu Sihai Yang Xinchen Kang Buxing Han Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Centre for Excellence in Molecular Sciences Centre for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China Department of Chemistry The University of Manchester Manchester M13 9PL UK School of Chemistry University of Chinese Academy of Sciences Beijing 100049 China Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular Engineering Peking University Beijing 100871 China Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China Shanghai Key Laboratory of Green Chemistry and Chemical Processes State Key Laboratory of Petroleum Molecular & Process Engineering School of Chemistry and Molecular Engineering East China Normal University Shanghai 200062 China

Porous Cu-based metal-organic compounds have attracted increasing attention for CO 2 electroreduction due to their well-defined porous structures and abundant metal sites. However, the classical {Cu 2 }-paddlewheel moieties within these materials often show poor electrochemical stability, leading to structural degradation during CO 2 electroreduction. Here, we report a strategy to generate stable {Cu(II)·Cu(I)} active sites by iodide species in a Cu-based metal-organic polyhedron, Cu-TCBB (TCBB=1,3,5-tris(4′-carboxybiphenyl-2-yl)benzene), to not only promote C 2 H 4 production but also clarify the real active sites of {Cu 2 }-paddlewheel-based materials during CO 2 electroreduction. Cu-TCBB exhibits a high Faradaic efficiency (FE) of 73.1% towards C 2 H 4 at −1.1 V vs. reversible hydrogen electrode (RHE) in 0.1 mol L −1 CsI aqueous solution, outperforming all porous metal-organic compounds to date. The presence of iodide-induced {Cu(II)·Cu(I)} sites was verified through in situ synchrotron X-ray diffraction and absorption spectroscopy, electron paramagnetic resonance spectroscopy, coupled with modelling, shedding light on the mechanism of CO 2 electroreduction over unique {Cu(II)·Cu(I)} sites.

关键词： Metal-organic polyhedron CO 2 electroreduction Ethylene {Cu(II)·Cu(I)} sites

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Correction: Efficient transformation of CO2 to cyclic carbonates using bifunctional protic ionic liquids under mild conditions

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green Chemistry 2021年第22期23卷 9179-9179页

作者： Xianglei Meng Zhaoyang Ju Suojiang Zhang Xiaodong Liang Nicolas von Solms Xiaochun Zhang Xiangping Zhang Beijing Key Laboratory of Ionic Liquids Clean Process Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 People's Republic of China Department of Chemical and Biochemical Engineering Center for Energy Resources Engineering (CERE) Technical University of Denmark Kgs. Lyngby Denmark School of Chemical Engineering University of Chinese Academy of Sciences Beijing 100049 China

Correction for ‘Efficient transformation of CO2 to cyclic carbonates using bifunctional protic ionic liquids under mild conditions’ by Xianglei Meng et al., green Chem., 2019, 21, 3456–3463, DOI: 10.1039/C9GC01165J.

Correction for ‘Efficient transformation of CO₂ to cyclic carbonates using bifunctional protic ionic liquids under mild conditions’ by Xianglei Meng et al., green Chem., 2019, 21, 3456–3463, DOI: 10.1039/C9GC01165J.

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MOF-based high-entropy-alloy evaporator featuring enhanced interband transitions for efficient solar steam and green electricity generation

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Chemical engineering Journal 2025年 517卷

作者： Chenyang Dai Jia-Han Zhang Cheng-Yu He Rongrong Dai Likun Pan Yusuke Yamauchi Jing Zhang Zhengtong Li Xingtao Xu Marine Science and Technology College Zhejiang Ocean University Zhoushan 316022 China Electronic-Photonic Smart Sensing Device R&D Team Inner Mongolia Key Laboratory of Intelligent Communication and Sensing and Signal Processing School of Electronic Information Engineering Inner Mongolia University Hohhot 010021 China Research Center of Resource Chemistry and Energy Materials State Key Laboratory of Solid Lubrication Lanzhou Institute of Chemical Physics Chinese Academy of Sciences Lanzhou China Shanghai Key Laboratory of Magnetic Resonance School of Physics and Electronic Science East China Normal University Shanghai 200026 China Department of Materials Process Engineering Graduate School of Engineering Nagoya University Nagoya 464-8603 Japan Australian Institute for Bioengineering and Nanotechnology (AIBN) The University of Queensland Brisbane QLD 4072 Australia Department of Chemical and Biomolecular Engineering Yonsei University 50 Yonsei-ro Seodaemun-gu Seoul 03722 South Korea Ningbo Key Laboratory of Green Petrochemical Carbon Emission Reduction Technology and Equipment Zhejiang Institute of Tianjin University Ningbo Zhejiang 315201 China State Key Laboratory of Hydrology-Water Resources and Hydraulic Engineering Yangtze Institute for Conservation and Development Hohai University Nanjing 210098 China

Photothermal materials exhibiting broadband optical absorption and high energy efficiency are highly sought after in the field of solar-driven evaporation. Herein, we present a novel photothermal material derived from polymetallic metal–organic frameworks (MOFs) through a d - d interband transition ( d - d IBT) engineering strategy. This approach enables comprehensive occupation of electronic states within ±4 eV relative to the Fermi level through 3d transition metal coordination, achieving an exceptional average solar absorption efficiency of over 97 % across the full solar spectrum (250–2500 nm). This breakthrough effectively overcomes the inherent wide bandgap limitation of MOFs that traditionally restricts their full-spectrum solar utilization. Leveraging its remarkable broadband sunlight harvesting capacity and ultrafast localized heating performance, this evaporator engineered with high-entropy alloy nanoparticles, achieves an evaporation efficiency surpassing 95% under one sun irradiation while maintaining a high evaporation rate of 2.80 kg m −2 h −1 . Moreover, this evaporator demonstrates exceptional desalination efficiency even with high-salinity seawater (20 wt%), while the waste heat generated during operation can be strategically repurposed to produce green electricity, enhancing its sustainability profile. Thus, the FeCoNiMnCuAlZn high-entropy alloy nanoparticle-based photothermal evaporator offers innovative solutions for addressing the scarcity of clean water resources and the need for green energy.

关键词： green electricity generation High-entropy alloys Interband transition Metal–organic frameworks Solar steam generator

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Meshfree simulation of multiphase flows with SPH family methods

arXiv

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arXiv 2020年

作者： Chen, Feiguo State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China Innovation Academy for Green Manufacture Chinese Academy of Sciences Beijing100190 China

With meshfree and fully Lagrangian features of particle methods, smoothed particle hydrodynamics (SPH) is suitable to achieve high-accurate simulations of multiphase flows with large interfacial deformations, discontinuities, and multi- physics. In this review, the basic concept of SPH is first briefly introduced. Then, various implementations of SPH in regard to multiphase flow simulations are summarized and discussed. Some problems associated with SPH simulations of multiphase flows are suggested as requiring attention. Copyright © 2020, The Authors. All rights reserved.

关键词： Hydrodynamics

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Cover Feature: Understanding Electric Field-Dependent Structure Variation of Functional Ionic Liquids at the Electrode Interface (ChemElectroChem 9/2021)

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ChemElectroChem 2021年第9期8卷

作者： Jingyu Qin Mi Wang Prof. Yanlei Wang Chenlu Wang Yumiao Lu Feng Huo Prof. Hongyan He Beijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex Systems CAS Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China University of Chinese Academy of Sciences Beijing 100049 China Innovation Academy for Green Manufacture Chinese Academy of Sciences Beijing 100190 China

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Porphyrin/Ionic-Liquid Co-assembly Polymorphism Controlled by Liquid–Liquid Phase Separation

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Angewandte Chemie 2020年第40期132卷

作者： Yuan C. Yang M. Ren X. Zou Q. Yan X. State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China School of Chemical Engineering University of Chinese Academy of Sciences Beijing 100049 China Center for Mesoscience Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China

Understanding and controlling multicomponent co-assembly is of primary importance in different fields, such as materials fabrication, pharmaceutical polymorphism, and supramolecular polymerization, but these aspects have been a long-standing challenge. Herein, we discover that liquid–liquid phase separation (LLPS) into ion-cluster-rich and ion-cluster-poor liquid phases is the first step prior to co-assembly nucleation based on a model system of water-soluble porphyrin and ionic liquids. The LLPS-formed droplets serve as the nucleation precursors, which determine the resulting structures and properties of co-assemblies. Co-assembly polymorphism and tunable supramolecular phase transition behaviors can be achieved by regulating the intermolecular interactions at the LLPS stage. These findings elucidate the key role of LLPS in multicomponent co-assembly evolution and enable it to be an effective strategy to control co-assembly polymorphism as well as supramolecular phase transitions. © 2020 Wiley-VCH GmbH

关键词： co-assembly ionic liquids liquid–liquid phase separation nucleation porphyrin

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