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Small modifications of endo-functionalized cavities lead to large changes in molecular interaction in water

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Science China Chemistry 2025年第1期68卷 369-376页

作者： Song-Meng Wang Hao Nian Yan-Fang Wang Li-Shuo Zheng Yu-Tao Zheng Yi-Wei Dong Liping Huang Xiaoping Wang Wei Jiang Liu-Pan Yang Department of Chemistry Southern University of Science and Technology School of Chemistry and Pharmaceutical Sciences State Key Laboratory for Chemistry and Molecular Engineering of Medicinal ResourcesGuangxi Normal University School of Pharmaceutical Science Hengyang Medical School University of South China

Studying molecular recognition in aqueous environments is crucial for understanding biological processes. Herein, we present a series of N-doped endo-functionalized anthracene-based cavities by introducing inward-directed pyridine units. The subtle modifications can significantly affect the binding properties of these receptors, which is similar to the mutations in biological systems. Combining theoretical calculations and molecular recognition experiments demonstrated that these “mutations” have an impact on the hydrophobicity and charge distribution of the hosts, consequently significantly influencing molecular *** is crucial for understanding the intricate mechanisms of molecular-level interactions in biological receptors.

关键词： host-guest interaction hydrophobic effect endo-functionalized cavity mutation pyridine

Upcycling of polyethylene terephthalate to1,4-cyclohexanedimethanol in water

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Science China Chemistry 2025年

作者： Shuhui Fang Zhiwen Gao Xinrui Shi Min Zhang Wei Zhang Yue Liu State Key laboratory of Petroleum molecular & Process Engineering Shanghai Key Laboratory of Green Chemistry and Chemical ProcessesSchool of Chemistry and Molecular Engineering East China Normal University Engineering Center for Sustainable Carbon Science and Technology East China Normal University Institute of Eco-Chongming

The recycling of waste polyethylene terephthalate（PET）, an extensively used polymer as plastic and fiber materials, has become an urgent topic due to the rapid generation and accumulation of plastic waste into the environment. Current chemical recycling approaches to depolymerize and convert PET into 1,4-cyclohexanedimethanol（CHDM）, an important chemical in the production of advanced polyesters, predominantly use organic solvents, such as alcohols or dioxane. Herein, we developed an environmentally friendly and economically viable pathway for converting PET to CHDM using water as the solvent. In this process, PET is sequentially hydrolyzed in water, hydrogenated to 1,4-cyclohexane dicarboxylic acid（CHDA）, and then reduced to CHDM. The PET conversion rate is self-enhanced in aqueous medium via acid-catalyzed hydrolysis by the generated CHDA intermediate. A Pd-based catalyst（e.g., Pd/C） selectively hydrogenates the arene ring of the PET monomer, terephthalic acid intermediate, and a Ru-Sn/C bimetallic catalyst reduces its COOH to CH2OH group. At optimized reaction conditions, a complete conversion of PET and 80.1% yield of CHDM are obtained. Alternatively, this approach can also efficiently produce CHDA from PET, with a yield up to 86.4%.

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Mainchain conformation ordering self-assembly tailored room temperature phosphorescence emission

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Science China Chemistry 2025年第1期68卷 329-336页

作者： Yuzhu Li Yumeng Gao Feng Tian Yu Wang Yuan Yao Shaoliang Lin Xiang Ma Binbin Xu Shanghai Key laboratory of Advanced Polymeric Materials Key Laboratory for Ultrafine Materials of Ministry of Education School of Materials Science and Engineering East China University of Science and Technology Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences Key laboratory for Advance Materials and Feringa Noble Prize Scientist Joint Research Centre Frontiers Science for Materiobiology and Dynamic Chemistry School of Chemistry and Molecular Engineering East China University of Science & Technology

Developing organic room-temperature phosphorescence （RTP） materials with a wide range of tunable-emission is significant in expanding the applications of RTP ***,we rationally designed amphiphilic alternating copolymers poly(1,2-bis（4-alkoxyphenyl）ethane-1,2-dione-alt-（ethylene glycol）x)(P（Bz-alt-EGx）) that combined the advantage of alternating benzil and EGxskeleton,and tunable mainchain *** a mainchain conformation ordering assembly （COA） process,P（Bz-alt-EGx） self-assembled into well-defined platelets,and such assemblies emitted blue RTP at ca.425 nm due to the ordered folded-chain conformation and confined *** contrast,traditional self-assembly （TA） of P（Bz-alt-EGx） obtained less ordered aggregates,such as asymmetric worms,vesicles,and rod-like *** resultant less ordered aggregates exhibited yellow-green RTP at ca.550 *** wide-tuning RTP emission in solution （between blue and yellow-green,over125 nm） is realized using the P（Bz-alt-EGx） alternating copolymers under the treatment of different self-assembly *** study uncovers a new strategy to tailor the RTP emission through different self-assembly pathways and holds great promise for the fabrication of advanced optical materials.

关键词： self-assembly conformation ordering alternating copolymer phosphorescence emission

Nanoscale and hollow inorganic sulfide@porous organic network doped intelligent hydrogels for accelerating diabetes wound therapeutics

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Science China Chemistry 2025年

作者： Yanhong Li Qiang Zhang Quanbo Wang Junping Wang Xiaomei Zhang Caixia Yin School of Chemistry and Chemical Engineering Shandong University Key laboratory of Chemical Biology and molecular Engineering of Ministry of Education Shanxi University

Diabetic wound healing remains a major challenge due to the excess hyperglycemia microenvironment,massively bacterial infections,macrophage dysfunction,and persistent *** comprehensively solve these problems,novel multifunctional materials are highly ***,a versatile and intelligent hydrogel (Cu2S@FePPOPTPM@GOx@Gel) is ***2S@FePPOPTPM@GOx with hollow morphology and controllable size was rationally designed and fabricated by using Cu2S nanocubes as a template,followed by in situ growth of FePPOPTPMand loading glucose oxidase （GOx）,*** infection occurs,the Schiff base bonds in Cu2S@FePPOPTPM@GOx@Gel can controllably release Cu2S@FePPOPTPM@GOx based on its excellent dynamic pH-responsiveness,thereby synergically reducing blood glucose levels and killing bacteria achieved relying on the excellent catalytic activity of GOx towards glucose and its promoted peroxidelike activity of *** experiments on diabetic wound model in vivo demonstrated that Cu2S@FePPOPTPM@GOx@Gel promoted wound healing and skin regeneration,which was attributed to its antibacterial properties,alleviating inflammation,stimulating vascular regeneration,and encouraging M2 polarization of *** work provides a novel strategy for the construction of a microenvironment-responsive and antibiotics-free drug delivery platform to treat diabetic wounds,as well as broad prospects of nanomaterials in the clinical treatment of chronic wounds.

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Recent progress on photoactive nonprecious transition-metal complexes

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Science China Chemistry 2025年第1期68卷 46-95页

作者： Zhong-Liang Gong Hong-Jie Zhang Yan Cheng Jianxun Liu Yuhan Ai Yaqin Li Zhihui Feng Qiong Zhang Shaolong Gong Yong Chen Chang-Jiang Yao Yuan-Yuan Zhu Liang-Jin Xu Yu-Wu Zhong CAS Key laboratory of Photochemistry Institute of Chemistry Chinese Academy of Sciences State Key laboratory of Structural Cemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences School of Chemistry and Chemical Engineering Anhui Key Laboratory of Advanced Catalytic Materials and Reaction EngineeringHefei University of Technology State Key laboratory of Explosion Science and Safety Protection School of Mechatronical Engineering Beijing Institute of Technology College of Chemistry and molecular Sciences Hubei Key Lab on Organic and Polymeric Optoelectronic Materials Wuhan University School of Chemistry and Chemical Engineering Anhui University Key laboratory of Photochemical Conversion and Optoelectronic Materials & CAS-HKU Joint laboratory on New Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences

Photoactive complexes of nonprecious transition metals, mainly including those in the first-row and partially the second-row of the Periodic table of elements, have received increasing attention in view of their low cost and long-term sustainability. They are recognized as promising alternatives to noble transition metal complex congeners that have been extensively studied in optoelectronic devices, artificial photosynthesis, photocatalysis, biodiagnostics, and therapeutics, etc. This review is devoted to a comprehensive summary on the classical and recent advances on photoactive nonprecious transition metal complexes, including photoactive Zr, V, Cr, Mo, and W complexes, Mn complexes and hybrids, Fe, Co, Ni, and Cu complexes, and Zn and Cd complexes and hybrids. A particular focus is given on the molecular design, modulation of photophysical and photochemical properties, and applications of the representative and lately-developed nonprecious metal complexes. In addition, a perspective on the future development in this field is provided at the end of this review.

关键词： photoactive metal complexes earth-abundant metals nonprecious metal complexes luminescence photochemistry

Investigations of liquid-liquid transitions in metallic melts by fast differential scanning calorimetry

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Science China(Physics,Mechanics & Astronomy) 2025年

作者： Qi Cheng Yonghao Sun Weihua Wang Beijing National laboratory for molecular Sciences College of Chemistry and Molecular Engineering Peking University School of Physics and Electronic Information Anhui Normal University Institute of Physics Chinese Academy of Sciences Songshan Lake Materials Lab

Liquid-liquid transition in metallic melts is an intriguing phenomenon often confused with liquid-liquid separation, oxidation or precipitation. Here, we employ a state-of-the-art ultrafast chip-based differential scanning calorimeter to investigate the thermal behavior of six metallic melts, ranging from unary to quinary systems, at temperatures above their liquidus. Calorimetric signals of liquid-liquid transition vary across systems: Sn melts showed no direct endothermic or exothermic events, though liquid-liquid transition influenced solidification and melting temperatures, while Yb-Zn melts exhibited an exothermic peak during cooling,indicating liquid-liquid transition. Thermal signals in other systems including Li, Pd-Ni-P, Yb-Mg-Zn-Cu and Au-Ag-Pd-Cu-Si,are primarily driven by compositional changes. Our in-situ analysis provides new insights into the structural and compositional evolution of metallic melts, offering significant implications for the design and processing of novel materials.

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Boosting Oxygen Evolution Reaction Performance on NiFe‑Based Catalysts Through d‑Orbital Hybridization

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Nano-Micro Letters 2025年第1期17卷 281-292页

作者： Xing Wang Wei Pi Sheng Hu Haifeng Bao Na Yao Wei Luo State Key laboratory of New Textile Materials and Advanced Processing Technology Key Laboratory of New Textile Materials and Applications of Hubei ProvinceSchool of Materials Science and EngineeringWuhan Textile UniversityWuhan 430200People’s Republic of China College of Chemistry and molecular Sciences Wuhan UniversityWuhan 430072People’s Republic of China

Anion-exchange membrane water electrolyzers(AEMWEs)for green hydrogen production have received intensive attention due to their feasibility of using earth-abundant NiFe-based *** introducing a third metal into NiFe-based catalysts to construct asymmetrical M-NiFe units,the d-orbital and electronic structures can be adjusted,which is an important strategy to achieve sufficient oxygen evolution reaction(OER)performance in ***,the ternary NiFeM(M:La,Mo)catalysts featured with distinct M-NiFe units and varying d-orbitals are reported in this *** and theoretical calculation results reveal that the doping of La leads to optimized hybridization between d orbital in NiFeM and 2p in oxygen,resulting in enhanced adsorption strength of oxygen intermediates,and reduced rate-determining step energy barrier,which is responsible for the enhanced OER *** critically,the obtained NiFeLa catalyst only requires 1.58 V to reach 1 A cm^(−2) in an anion exchange membrane electrolyzer and demonstrates excellent long-term stability of up to 600 h.

关键词： NiFe-based catalysts d-orbital coupling Oxygen evolution reaction Anion exchange membrane electrolyzer

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Ca2+ cation-mediated microenvironment for electrochemical hydrodimerization of furfural

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Science China Chemistry 2025年

作者： Wei Du Shuangshuang Cha Can Lei Mengxin Qu Zhongqiang Deng Ming Gong Xinhe Bao Department of Chemistry and Shanghai Key laboratory of molecular Catalysis and Innovative Materials Fudan University State Key laboratory of Catalysis National Laboratory for Clean Energy Collaborative Innovation Center of Chemistry for Energy Materials Dalian Institute of Chemical Physics Chinese Academy of Sciences

Furfural is one of the most important biomass-based platform molecules as sustainable precursors for chemicals and fuels. The electrochemical hydrodimerization of furfural can generate hydrofuroin, which is a promising precursor for gasoline or jet ***, steering the selectivity toward hydrodimerization under near-neutral conditions that suppress polymerization and disproportionation of furfural remains challenging. Herein, we discovered that tuning the electrolyte cations could be an effective and alternative strategy for modulating furfural reduction to the traditional electrocatalyst design. Under the optimal Ca2+cations,hydrofuroin yield could be much improved from other cations with hydrofuroin selectivity of 95.5%. The systematic characterization of the ion-centered double layer reflected the suitable sizes and charges of hydrated Ca2+for suppressing the hydrogen evolution reaction from activation of surrounding water molecules as well as encouraging furfural accumulation via non-covalent interaction for directing the electron transfer to furfurals. Ions with smaller or larger sizes can either activate local water molecules or form a crowded ionic interface that casts an adverse effect on furfural enrichment. This work not only presents an effective strategy for facilitating biomass valorization via hydrodimerization but also emphasizes the essential role of the ion-centered microenvironment for steering the electrocatalytic pathways.

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Electrochemical conversion of methane to bridge the gap in the artificial carbon cycle

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Journal of Energy Chemistry 2025年第1期100卷 286-308页

作者： Yuhao Peng Yuefeng Song Ihar Razanau Juanxiu Xiao Wei Xiao Di Hu Guoxiong Wang College of Chemistry and molecular Sciences Hubei Key Laboratory of Electrochemical Power Sources Wuhan University State Key laboratory of Catalysis Dalian National Laboratory for Clean Energy iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Dalian Institute of Chemical Physics Chinese Academy of Sciences laboratory of Physical-Chemical Technologies SSPA Scientific and Practical Materials Research Centre of NAS of Belarus State Key laboratory of Marine Resources Utilization in South China Sea Collaborative Innovation Center of Marine Science and Technology School of Marine Science and Engineering Hainan University Department of Chemical and Environmental Engineering University of Nottingham Ningbo China

Methane, an abundant one-carbon（C1） resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO2emissions and coke deposition. Electrochemical conversion of methane（ECM） using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO2emission.

关键词： Activation energy