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H* Species Regulation by Mn-Co(OH)2for Efficient Nitrate Electro-reduction in Neutral Solution

Angewandte Chemie 2024年第11期136卷

作者： Shaozhen Liang Xue Teng Heng Xu Prof. Lisong Chen Prof. Jianlin Shi 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 P. R. China Institute of Eco-Chongming Shanghai 202162 P. R. China State Key Laboratory of High-Performance Ceramics and Superfine Microstructures Shanghai Institute of Ceramics Chinese Academy of Sciences Shanghai 200050 P. R. China

During the electrocatalytic NO 3 − reduction reaction (NO 3 − RR) under neutral condition, the activation of H 2 O to generate H* and the inhibition of inter-H* species binding, are critically important but remain challenging for suppressing the non-desirable hydrogen evolution reaction (HER). Here, a Mn-doped Co(OH) 2 (named as Mn-Co(OH) 2 ) has been synthesized by in situ reconstruction in the electrolyte, which is able to dissociate H 2 O molecules but inhibits the binding of H* species between each other owing to the increased interatomic spacing by the Mn-doping. The Mn-Co(OH) 2 electrocatalyst offers a faradaic efficiency (FE) of as high as 98.9±1.7% at −0.6 V vs. the reversible hydrogen electrode (RHE) and an energy efficiency (EE) of 49.90±1.03% for NH 3 production by NO 3 − RR, which are among the highest of the recently reported state-of-the-art catalysts in neutral electrolyte. Moreover, negligible degradation at −200 mA cm −2 has been found for at least 500 h, which is the longest catalytic durations ever reported. This work paves a novel approach for the design and synthesis of efficient NO 3 − RR electrocatalysts.

关键词： Electrocatalytic nitrate reduction Mn-Co(OH)2 nanosheets H* regulation neutral nitrate condition

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Rigidly Locked Pyrene Excimers in Planar Chiral Pyrenophanes for Intense and Stable Circularly Polarized Photoluminescence and Electrochemiluminescence

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Angewandte Chemie 2025年

作者： Lin-Tao Bao Rui-Hua Zhang Xiaoyue Yuan Dr. Xueli Wang Peicong Wu Dr. Xu-Qing Wang Prof. Dr. Jinquan Chen Prof. Dr. Anwei Zhu Prof. Dr. Hai-Bo Yang Prof. Dr. Wei Wang Shanghai Key Laboratory of Green Chemistry and Chemical Processes State Key Laboratory of Petroleum Molecular and Process Engineering School of Chemistry and Molecular Engineering East China Normal University Shanghai 200062 China State Key Laboratory of Precision Spectroscopy East China Normal University Shanghai 200241 China Shanghai Center of Brain-inspired Intelligent Materials and Devices East China Normal University Shanghai 200241 China Shanghai Frontiers Science Center of Molecule Intelligent Syntheses East China Normal University Shanghai 200062 China

Aiming at the construction of novel platforms with excellent performances in both circularly polarized photoluminescence (CP-PL) and electrochemiluminescence (CP-ECL), a new family of pyrenophanes with rigidly locked pyrene dimers and varied bridges has been designed and synthesized. Attributed to densely packed pyrene excimers, the resultant pyrenophanes revealed tunable bridge-dependent emission behaviors, as investigated by femtosecond time-resolved transient absorption spectroscopy. More importantly, all these planar chiral pyrenophanes display strong CP-PL with large dissymmetry factor ( g PL ) values up to 0.034, and such excellent performances remain stable in a wide range of solvents, temperatures, and concentrations. Attractively, the highest g ECL values up to 0.014 reported so far has been achieved for the CP-ECL emissions of the chiral pyrenophanes. Attributed to their unique structural features and outstanding CPL performances, these novel pyrenophanes could serve as promising platforms for both fundamental investigations on pyrene excimers and practical applications such as chiral sensing.

关键词： cyclophanes planar chirality pyrene excimers circularly polarized luminescence electrochemiluminescence

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Electrochemical Responsive Alginate Chains Rendered Sol-to-Gel Gradient Electrolyte towards Practical Ah-level Zinc Metal Pouch Cell

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Angewandte Chemie 2025年

作者： Liheng Zheng Linhui Chang Shiyan Xue Prof. Kangning Zhao Bomian Zhang Prof. Weidong He Feng Tao Jinghao Li Prof. Min Wang Qinyou An Prof. Lei Zhang The Sanya Science and Education Innovation Park of Wuhan University of Technology Sanya 572000 P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China School of Materials Science and Engineering & State Key Laboratory of Advanced Special Steel Shanghai University Shanghai 200444 P. R. China School of Physical Sciences Great Bay University Dongguan 523000 P. R. China Department of Applied Physics The Hong Kong Polytechnic University Hong Kong S.A.R 999077 P. R. China Beijing Key Laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P. R. China

Zinc metal batteries have been considered as an appealing candidate for grid-scale energy storage devices, but are hindered by the instable interface. Herein, we design a sol-to-gel gradient electrolyte through the simultaneous electrochemical deposition of Zn 2+ and alginate. The electrochemical gelation of alginate creates a gradient sol-to-gel interface and enables the high ionic conductivity, where vehicular mechanism dominated transport is maintained in the bulk electrolyte, while a lean-water hydrogel like state is created at the Zn/electrolyte interface to reduce water activity. The electrochemical active alginate undergoes a gelation process to form an egg-shell to confine the Zn 2+ , rendering a 2D growth mode and inhibiting dendrite growth. By taking the advantages of both fast ion transport and stable interface, the full cell based on Zn/VO 2 achieved a stable cycling of 400 cycles at an industrial-level areal capacity of over 4 mAh cm −2 with a capacity retention of 89.25 %. Additionally, we demonstrate the Ah-level pouch cell, which stably operates for over 200 cycles with an almost unity average coulombic efficiency (over 99.90 %). By demonstrating the remarkable performance, our work represents an advancement in zinc metal batteries toward a practical scale and is expected to set a stepping stone for transformative advancements in energy storage technologies.

关键词： Zinc Ion Battery Sol-to-Gel Gradient Electrolyte Confined Deposition Gradient Interphase Pouch Cell

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Construction of BODIPY-based triangular metallacycles with tunable photosensitization efficiency

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Chinese Chemical Letters 2025年

作者： Pei-Pei Jia Yi-Xiong Hu Zhen-Chen Lou Xuelei Ji Xing-Dong Xu Haitao Sun Tongxia Jin Feng Zheng Lin Xu Wuhu Hospital East China Normal University (The Second People's Hospital Wuhu) Wuhu 241001 China State Key Laboratory of Petroleum Molecular & Process Engineering Shanghai Key Laboratory of Green Chemistry and Chemical Processes Shanghai Frontiers Science Center of Molecule Intelligent Syntheses Liwa Institute of Skin Health School of Chemistry and Molecular Engineering East China Normal University Shanghai 200062 China College of New Energy Yulin University Yulin 719000 China Key Laboratory of Special Functional Aggregated Materials of Ministry of Education School of Chemistry and Chemical Engineering National Engineering Research Center for Colloidal Materials Shandong University Ji'nan 250100 China State Key Laboratory of Precision Spectroscopy East China Normal University Shanghai 200241 China

The development of highly effective photosensitizers (PSs) based on supramolecular coordination complexes (SCCs) is highly appealing in supramolecular chemistry, materials science, and biology. SCCs offer promising platforms for incorporating multiple PSs and other functional units into their well-defined structures, allowing for precise control over the number and distribution of these components. In this study, we present an efficient and straightforward method for modulating the photosensitization process of PSs derived from a family of BF 2 -chelated dipyrromethene (BODIPY)-containing Pt(II) metallacycles by varying pre-designed Pt(II) acceptors. By utilizing different Pt(II) acceptors with varying Pt atom configurations and degrees of π-conjugated organic moieties, we observed tunable characteristics in the photosensitization process and singlet oxygen ( 1 O 2 ) generation efficiency of these targeted metallacycles. Furthermore, we successfully conducted the visible-light-driven oxidative coupling of various amines to imines, catalyzed by the prepared metallacycle PSs. This study offers a novel approach for fabricating efficient PSs based on SCCs, featuring tunable photosensitization efficiency and excellent photocatalytic reactivity, while providing new insights into the preparation of effective PSs.

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Syringic acid modulates methyl cellosolve-induced hepatic upregulation of the PI3K-Akt-mTOR pathway and inhibition of p53-Bax-caspase-3-dependent apoptosis in rats

Pharmacological Research - Natural Products

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Pharmacological Research - Natural Products 2024年 2卷

作者： Oluwatobi T. Somade Olukemi A. Osukoya Rasaq T. Onikola Opeyemi Omotoso Basiru O. Ajiboye Babatunji E. Oyinloye Department of Biochemistry College of Biosciences Federal University of Agriculture Abeokuta Nigeria Phytomedicine Biochemical Toxicology and Biotechnology Research Laboratories Department of Biochemistry College of Sciences Afe Babalola University PMB 5454 Ado-Ekiti 360001 Nigeria Key Laboratory of Green Process and Engineering State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 PR China Institute of Drug Research and Development S.E Bogoro Center Afe Babalola University PMB 5454 Ado‑Ekiti 360001 Nigeria Phytomedicine and Molecular Toxicology Research Laboratory Department of Biochemistry Federal University Oye Ekiti Oye Ekiti State Nigeria Biotechnology and Structural Biology (BSB) Group Department of Biochemistry and Microbiology University of Zululand KwaDlangezwa 3886 South Africa

Background Methyl cellosolve (METC) is a widely used industrial solvent due to its amphipathic nature. It is found in household materials such as liquid soaps, dyes, inks, brake fluids, herbicides, etc. This makes exposure in humans incessant and indiscriminate. The PI3K-Akt-mTOR and the intrinsic apoptotic pathways are very important cellular activities. While the former participates in cell growth, proliferation, and survival, the latter coordinates the death of abnormally functional cells, thereby stopping their proliferation. Given that background, we studied the hepatoprotective effect of syringic acid (SA) on METC-induced hepatotoxicity by checking the involvement of the PI3K-Akt-mTOR and apoptotic pathways in male Wistar rats. Methods Thirty (30) rats divided into six groups were used. Rats in group 1 served as control, those in group 2 were administered METC for 30 consecutive days, and those in groups 3, 4, and 5 were treated with 25, 50, and 75 mg/kg body weight of SA respectively also for 30 consecutive days immediately after each day METC administrations, while rats in group 6 received 75 mg/kg body weight of SA only throughout. Results Following analyses, METC-induced activation of the PI3K-Akt pathway and inhibition of apoptosis were marked by a significant elevation in the liver gene expressions of PI3K, Akt, mTOR, PTEN, FoxO1, and TSC2 as well as a significant downregulation in the protein expressions of p53, caspase 3, Bax, and a significant upregulation in Bcl2 protein expression compared with control rats. SA treatment (25 mg/kg only) significantly downregulated the hepatic mTOR, FoxO1, and TSC2 gene expressions, while in addition to mTOR, FoxO1, and TSC2 genes, treatments with 50 and 75 mg/kg significantly downregulated the liver gene expressions of PI3K, Akt, and PTEN compared with METC only exposed rats. For protein expression, all the doses of SA treatment significantly downregulated the liver Bcl2 level (an antiapoptotic protein), while 75 mg

关键词： MDA malondialdehyde PI3K phosphatidyl inositol 3-kinase Akt protein kinase B MTOR mechanistic target of rapamycin PTEN phosphatase and tensin homolog TSC2 tuberous sclerosis complex 2 Bax bcl-2-associated X SOD superoxide dismutase FoxO1 forkhead box protein O1 Bcl-2 b-cell lymphoma 2 ADH alcohol dehydrogenase GSH reduced glutathione 2-MALD 2-methoxyacetaldehyde dehydrogenase 2MAA 2-methoxyacetic acid PIKK PI3K-related kinase MCM modern Chinese medicine RT-PCR reverse transcriptase-polymerase chain reaction ANOVA analysis of variance GST glutathione S-transferase GPCRs G-protein-coupled receptors CAT catalase PDPK1 3-phosphoinositide-dependent protein kinase 1 ILK integrin-linked kinase P53 tumor suppressor protein SD standard deviation MTORC2 mammalian target of rapamycin complex 2 DNA-PK DNA-dependent protein kinase T2DM type 2 diabetes mellitus GPx glutathione peroxidase PIP2 phosphatidyl inositol-4,5-diphosphate Apaf1 apoptotic protease activating factor 1 PIP3 phosphatidyl inositol-3,4,5-triphosphate Cyt c cytochrome-c AST aspartate aminotransferase AR aldose reductase ALT alanine aminotransferase Apoptosis Cell growth Cell survival Methyl cellosolve Syringic acid

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灭活口蹄疫病毒颗粒的稳定、纯化和递送新策略:二价过渡金属离子的独特作用

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中国预防兽医学报 2021年第5期43卷 573-573页

作者： LIN XUAN YANG YAN-LI SONG YAN-MIN [a]State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing PR China [b]University of Chinese Academy of Sciences Beijing PR China University of Kentucky College of Medicine

灭活口蹄疫病毒(FMDV 146S)疫苗是目前预防口蹄疫(FMD)最有效的产品。作为抗原的146S的颗粒结构完整性是保证疫苗的免疫活性的关键。然而,146S在高温或微酸性环境,甚至是低温保存时均容易裂解失活。如何保持146S的结构稳定,是FMD疫苗生... 详细信息

灭活口蹄疫病毒(FMDV 146S)疫苗是目前预防口蹄疫(FMD)最有效的产品。作为抗原的146S的颗粒结构完整性是保证疫苗的免疫活性的关键。然而,146S在高温或微酸性环境,甚至是低温保存时均容易裂解失活。如何保持146S的结构稳定,是FMD疫苗生产和储存应用的最大挑战。大量前期研究结果已证实,146S的裂解起始于病毒衣壳相邻的五聚体亚基交界处,而亚基交界处的大量组氨酸在酸性环境中质子化产生的电荷排斥,是导致146S耐酸稳定性差的关键因素之一,因此以往的研究中通常采取去除或替换掉组氨酸的策略来提高其稳定性。

关键词：口蹄疫病毒病毒衣壳低温保存疫苗生产过渡金属离子微酸性酸性环境灭活

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Microporous Polymer Membranes: Molecular Stents Enhanced Solvent-Accessibility for Organic Solvent Transport

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Advanced science (Weinheim, Baden-Wurttemberg, Germany) 2025年 e16748页

作者： Shuang Guo Chuanjie Fang Jiaqi Li Xiaohe Wang Weilin Feng Hukang Guo Ming Xie Yongbing Zhuang Young Moo Lee Liping Zhu MOE Key Laboratory of Macromolecular Synthesis and Functionalization MOE Engineering Research Center of Membrane and Water Treatment Technology Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 China. Department of Polymer Science and Engineering Department of Chemical Engineering University of Bath Bath BA2 7AY UK. State Key Laboratory of Biochemical Engineering Institute of Process Engineering University of Chinese Academy of Sciences Chinese Academy of Sciences Beijing 100190 China. Department of Energy Engineering College of Engineering Hanyang University Seoul 04763 South Korea.

Microporous polymer membranes with high solvent permeability are pivotal for upgrading molecular separations in organic solvents, but this remains challenging due to numerous sub-0.4 nm ultra-micropores resulting from local tight packing, which limit solvent-accessibility. Herein, a microporous polyimide with high intrinsic free volume [PI-TB-NDI, naphthalenediimide (NDI) and Tröger's base (TB)] is synthesized for organic solvent nanofiltration. The resulting polymer showed high free volume because of fused aromatic rings and a twisted structure. Aromatic rings enhanced solvent resistance due to strong molecular interaction, but increased detrimental local tight packing as well. To suppress local tight packing without compromising the molecular interactions vital for stability, an ortho-methyl group is deliberately introduced onto the TB unit to increase both intra- and inter-molecular steric hindrance, imparting an H-shaped TB-NDI-TB molecular stent. On the introduction of ortho-methyl groups, the sub-0.4 nm ultra-micropores are enlarged to ultra-micropores (0.6-0.7 nm) to give the membrane with rich solvent-accessible sub-nanochannels. This resulted in an unprecedented enhancement of solvent permeability, with ethanol permeability 2-8 times greater than that of state-of-the-art polymer membranes with similar selectivity. These findings advance the design strategy of microporous membranes with well-tailored free volume without post-treatments, enabling upscaling and efficient separation of precious species in organic solvents.

关键词： free volume microporous polymer membranes molecular stents organic solvent transport

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Bilateral Unsymmetrical Disulfurating Reagent Design for Polysulfide Construction

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Angewandte Chemie 2024年第37期136卷

作者： Qing Yu XiangJin Zhang Xuefeng Jiang Hainan Institute of East China Normal University State Key Laboratory of Petroleum Molecular & Process Engineering Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular Engineering East China Normal University Shanghai 200062 P.R. China School of Chemistry and Chemical Engineering Henan Normal University Xinxiang Henan 453007 P.R. China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic Chemistry Chinese Academy of Sciences 345 Lingling Road Shanghai 200032 P. R. China

Polysulfides are significant compounds in life science, pharmaceutical science, and materials science. Therefore, polysulfide construction is in great demand. The controllable sequential installation of groups on both ends of a S−S motif faces an enormous challenge owing to the reversible nature of the covalent S−S bond. A library was established with two divergent mask groups for bilateral unsymmetrical disulfurating reagents (R 1 O−SS−SO 2 R 2 ). Sequential coupling with preferential activation of the S−SO 2 bond (37.6 kcal/mol) and controllable activation of the S−O bond (54.8 kcal/mol) in the presence of the S−S bond (62.0 kcal/mol) enabled successive reactions at each end of the S−S motif to afford unsymmetrical disulfides and trisulfides, even for the cross-linkage of natural products, pharmaceuticals, peptides, and a protein (bovine serum albumin).

关键词： Disulfurating reagents Disulfuration Disulfides Copper catalysis Protein modification

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3D bioprinting for cell culture and tissue fabrication

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Bio-Design and Manufacturing 2018年第1期1卷 45-61页

作者： Honglei Jian Meiyue Wang Shengtao Wang Anhe Wang Shuo Bai State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China

Three-dimensional （3D） bioprinting is a computer-assisted technology which precisely controls spatial position of biomaterials, growth factors and living cells, offering unprecedented possibility to bridge the gap between structurally mimic tissue constructs and functional tissues or organoids. We briefly focus on diverse bioinks used in the recent progresses of biofabrication and 3D bioprinting of various tissue architectures including blood vessel, bone, cartilage, skin, heart, liver and nerve systems. This paper provides readers a guideline with the conjunction between bioinks and the targeted tissue or organ types in structuration and final functionalization of these tissue analogues. The challenges and perspectives in 3D bioprinting field are also illustrated.

关键词： 3D bioprinting Bioink Cell culture Tissue fabrication Organoid

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Carbonation Impact on the Stabilization of Heavy Metals in Carbon-rich Geopolymers Based on Gasification Slag and Fly Ash

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Environmental Pollution 2025年

作者： Qingbai Chen Yuchi Chen Jin Kang Fangyuan Chen State Key Laboratory of Separation Membranes and Membrane Processes School of Environmental Science and Engineering Tiangong University Tianjin 300387 PR China Key Laboratory for Green Chemical Process of Ministry of Education School of Chemistry and Environmental Engineering Wuhan Institute of Technology Wuhan 430074 PR China Hubei Provincial Academy of Eco-environment Sciences (Provincial Ecological Environment Engineering Assessment Center) Wuhan 430072 China School of Chemical and Environmental Engineering Wuhan Polytechnic University Wuhan 430023 PR China

Carbonization is a common phenomenon that occurs when carbon-rich geopolymers engages in heavy metals’ stabilization. The carbonation impact on the stabilization effect remains controversy. This study investigates the carbonation course and the relative migration and transportation of heavy metals in carbon-rich geopolymer with different type of ions. The results revealed that the synthesized calcite or other carbonates can disrupt the dense layered structure and increase the porosity of geopolymer with the higher content of cationic heavy metals. Zn, Cr and Cu are transformed into migratable state, resulting in increased leaching amounts of 31.8%, 1333.3%, and 2529.0%, respectively. For the geopolymer with higher content of CrO 4 2- or AsO 4 3- , the release rate of both heavy metal cations and anions is significantly reduced with carbonation. These oxyanions with tetrahedral structures participate themselves in geopolymerization, leading to the formation of covalent bond with CO 2 by substitution of AlO 4 tetrahedron. By this, an extra addition of K 2 HPO 4 (at P/Al ratio of 0.1) will inhibit the capillary diffusion of CO 3 2- and the releasing of heavy metals. The research establishes a mechanism relationship between carbonation course and heavy metals’ leaching, and provides a practical approach for diminishing the negative impact on geopolymer stabilization.

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