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Boosting hydrocarbon conversion via Cu-doping induced oxygen vacancies on CeO2 in CO2 electroreduction

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Journal of Energy chemistry 2025年第1期100卷 66-76页

作者： Lei Xue Tong Shi Chenhui Han Heng Zhang Fenrong Liu Haorun Li Yan Wang Xiaojun Gu Shanghong Zeng Inner Mongolia Key Laboratory of chemistry and Physics of Rare Earth Materials School of Chemistry and Chemical Engineering Inner Mongolia University State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences Institute of Catalysis Department of Chemistry Zhejiang University National Key Laboratory of Baiyunobo Rare Earth Resource research and Comprehensive Utilization Baotou Research Institute of Rare Earths

Conversion of CO2back to hydrocarbons is the most direct way of closing the“carbon cycle”,and its significance is further enlarged if this process is driven by renewable energies such as ***,precisely controlling the product selectivity towards hydrocarbons against the competitive hydrogen evolution remains challenging,especially for Cu-based ***,we report a novel defect engineering strategy,by which Cu-doping-induced oxygen vacancies on CeO2nanorods were effectively created,with adjustable vacancy/Cu *** resulting optimum catalyst shows up to 79% catalytic current density to hydrocarbons （excluding CO）,with 49% faradaic efficiency to *** and density functional theory unveil that the ratio between oxygen vacancy and Cu affects significantly the formation of*CHO and activation of H2O,which leads to the following deep hydrogenation to *** findings may spur new insights for designing and developing more controllable chemical process relevant to CO2utilization.

关键词： Nanorods

Trinuclear gold-catalyzed site-selective alkylation of peptides

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Science China chemistry 2025年第1期 249-256页

作者： Qing-Yun Fang Chengyihan Gu Yinghan Chen Wencheng Yan Yong Liang Weipeng Li Chengjian Zhu Jie Han Jin Xie State Key Laboratory of Coordination chemistry Jiangsu Key Laboratory of Advanced Organic Materials Chemistry and Biomedicine Innovation Center (Chem BIC) School of Chemistry and Chemical Engineering Nanjing University Green Catalysis Center College of Chemistry Zhengzhou University State Key Laboratory of natural Medicines China Pharmaceutical University

Selective modification of peptides has always been a challenging issue. The selective alkylation of peptides can alter the biological activity and physical properties of molecules, and it has gained significant research interest. We herein disclose an intriguing gold-catalyzed alkylation of peptides using bench-stable unactivated alkyl bromides under photoredox catalysis. A wide range of structurally diverse primary, secondary and tertiary alkyl bromides serve as effective coupling partners to precisely connect with the α-C(sp3)–H in glycine residue of peptides. This protocol demonstrates an exceptionally broad scope for alkyl halides and excellent tolerance for a wide range of useful functional groups. A series of relay transformations to construct cyclic peptides, to proceed click reaction and to realize peptide fluorescence labeling further enhance its synthetic practicality. In addition, mechanistic studies and density functional theory(DFT) calculations reveal an inner-sphere and subsequent outersphere single electron transfer(SET) mechanism.

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Inhibiting ceramide synthase 5 expression in microglia decreases neuroinflammation after spinal cord injury

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Neural Regeneration research 2025年第10期20卷 2955-2968页

作者： Wei Zhang Yubao Lu Ruoqi Shen Yingjie Wu Chenrui Liu Xingxing Fang Liangming Zhang Bin Liu Limin Rong Department of Spine Surgery The Third Affiliated HospitalSun Yat-sen UniversityGuangzhouGuangdong ProvinceChina National Medical products Administration(NMPA)Key Laboratory for Quality research and Evaluation of Cell products GuangzhouGuangdong ProvinceChina Guangdong Provincial Center for Quality Control of Minimally Invasive Spine Surgery GuangzhouGuangdong ProvinceChina Guangdong Provincial Center for Engineering and Technology research of Minimally Invasive Spine Surgery GuangzhouGuangdong ProvinceChina

Microglia,the resident monocyte of the central nervous system,play a crucial role in the response to spinal cord ***,the precise mechanism remains *** investigate the molecular mechanisms by which microglia regulate the neuroinflammatory response to spinal cord injury,we performed single-cell RNA sequencing dataset analysis,focusing on changes in microglial *** found that the MG1 subpopulation emerged in the acute/subacute phase of spinal cord injury and expressed genes related to cell pyroptosis,sphingomyelin metabolism,and neuroinflammation at high ***,we established a mouse model of contusive injury and performed intrathecal injection of siRNA and molecular inhibitors to validate the role of ceramide synthase 5 in the neuroinflammatory responses and pyroptosis after spinal cord ***,we established a PC12-BV2 cell co-culture system and found that ceramide synthase 5 and pyroptosis-associated proteins were highly expressed to induce the apoptosis of neuron *** ceramide synthase 5 expression in a mouse model of spinal cord injury effectively reduced ***,ceramide synthase 5-induced pyroptosis was dependent on activation of the NLRP3 signaling *** ceramide synthase 5 expression in microglia in vivo reduced neuronal apoptosis and promoted recovery of neurological ***2g7 formed a“bridge”between sphingolipid metabolism and ceramide synthase 5-mediated cell death by inhibiting the NLRP3 signaling ***,these findings suggest that inhibiting ceramide synthase 5 expression in microglia after spinal cord injury effectively suppressed microglial pyroptosis mediated by NLRP3,thereby exerting neuroprotective effects.

关键词： ceramide synthase 5 gasdermin D microglia neuroinflammation NLRP3 nuclear factor kappa B Pla2g7 pyroptosis sphingomyelin metabolism spinal cord injury

维普期刊数据库

Imidazolium-based ionic polymers for fast and efficient anion-exchange driven capture of Cr2O72-

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Science China chemistry 2025年

作者： Yishou Wang Xiaonan Yuan Xingxing Gou Xiatian Song Xiaogang Wang Ling Guo Yanfeng Liu Chengfang Qiao Chunsheng Zhou Yingfeng Han Shaanxi Key Laboratory of Comprehensive Utilization of Tailings Resources Shaanxi Engineering Research Center for Mineral Resources Clean & Efficient Conversion and New Materials College of Chemical Engineering and Modern Materials Shangluo University Key Laboratory of Synthetic and natural Functional Molecule chemistry of the Ministry of Education Xi'an Key Laboratory of Functional Supramolecular Structure and Materials College of Chemistry and Materials Science Northwest University

The pervasive issue of chromium（VI） contamination,particularly in dichromate (Cr2O2-7),resulting from unchecked industrial growth and inadequate waste management,remains a pressing concern that demands immediate and dedicated ***,we present two novel imidazolium-based ionic polymers （ImIPs）.The ImIPs boast a highly cationic structure rich in bromide（Br-） ions and exhibit remarkable porosity,facilitating the easy exchange of these ions for chromate (Cr2O2-7) through anion *** unique combination leads to exceptional performance,including a high adsorption capacity （423 mg/g）,rapid adsorption rate (75 mg g-1min-1),and a broad operational pH range （2–12）.Moreover,our material demonstrates remarkable reusability,maintaining its efficacy even after 10 cycles without significant loss of *** mechanistic studies underscore the role of ion-exchange chemistry in effectively removing dichromate by the presented ImIPs,providing strong evidence for their suitability as a robust solution to address the ongoing challenges in water *** findings represent a crucial step in developing advanced materials for tackling chromium（VI） pollution.

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Status and prospects for symmetric organic redox flow batteries

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Journal of Energy chemistry 2025年第1期100卷 125-143页

作者： Md Al Raihan C.Adam Dyker Department of chemistry University of New Brunswick

As environmental concerns from fossil fuel consumption intensify, large-scale energy storage becomes imperative for the integration of renewable sources like wind, hydro, and solar with the electrical *** flow batteries, particularly those employing organic molecules, are positioned as a key technology for this purpose. This review explores the growing field of symmetric organic redox flow batteries(ORFBs) within this context. Unlike traditional asymmetric designs based on unique active materials for each electrode, symmetric ORFBs involve a single bipolar species for both electrodes. This review highlights the benefits of a symmetric design, and categorizes five distinct classes of organic bipolar molecules used in both aqueous and non-aqueous solvents. By providing a comprehensive overview of their cell cycling and performance characteristics, the strengths and weaknesses of the diverse categories of bipolar molecules are highlighted for both solvent systems, as are opportunities for future development. This should guide new research directions and advance the development of practical symmetric ORFBs.

关键词： Redox flow battery Symmetric battery Organic battery Aqueous electrolyte Non-aqueous electrolyte

High-performance poly(aromatic pyridine) copolymers with crown ether moieties for high temperature polymer electrolyte membrane fuel cells

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Science China chemistry 2025年

作者： Qian Wang Songhao Zhao Yunpeng Guo Wei Wei Lele Wang Jingshuai Yang Department of chemistry College of Sciences Northeastern University Institute of Metal research Chinese Academy of Sciences

This study concentrates on the development of high temperature polymer electrolyte membranes（HT-PEMs）, which are essential components for HT-PEM fuel cells（HT-PEMFCs）. Although the phosphoric acid（PA）-doped polybenzimidazole（PBI） has been regarded as the successful HT-PEM, this system still suffers from several challenges, including the use of carcinogenic monomers, complex synthesis procedures, and poor solubility in organic solvents. To develop more cost-effective, readily synthesized and high-performance alternatives, this study employs a simply superacid-catalyzed Friedel-Crafts reaction to synthesize a series of poly（triphenyl-co-dibenzo-18-crown-6 pyridine） copolymers, denoted as P(TPx%-co-CEy%), using ptriphenyl, dibenzo-18-crown-6 and 4-acetylpyridine as monomers. The copolymerized hydrophilic and bulky crown ether unites introduce large free volumes and multiple interaction sites with PA molecules, as elucidated by theoretical *** microphase separation structures are formed as confirmed by atomic force microscope（AFM）, transmission electron microscopy（TEM） and small-angle X-ray scattering（SAXS）. Thus P(TPx%-co-CEy%) membranes exhibit excellent PA absorption and proton conduction abilities. For example, after immersing in 85 wt% PA at 30 °C, the P(TP91%-co-CE9%) membrane achieves a PA doping content of 205% and a high conductivity of 0.138 S cm-1at 180 °C, while maintaining a tensile strength of 7.5 MPa at room temperature. Without humidification and backpressure, the peak power density of an H2-O2cell equipped with P(TP91%-co-CE9%)/205%PA reaches nearly 1200 mW cm-2, representing one of the highest performances reported for PA-doped HT-PEMs to date. This work demonstrates the enormous potential of poly（triphenyl-co-crown ether pyridine） membranes in the HT-PEMFC applications.

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Deciphering fungal metabolon coupling tandem inverse-electrondemand Diels-Alder reaction and semipinacol rearrangement for the biosynthesis of spiro polycyclic alkaloids

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Science China chemistry 2025年第01期 288-296页

作者： Shuai Liu Wen-Qiang Xu Ying-Tong Di Man-Cheng Tang Ding-Kang Chen Ming-Ming Cao Yao-Wen Chang Hong-Yu Tang Chun-Mao Yuan Jun-Bo Yang Zhi-Li Zuo Han Guo Zi-Fei Xu Ying Zeng Yun-Dong Wu Xiao-Jiang Hao Key Laboratory of Phytochemistry and natural Medicines (Chinese Academy of Sciences) Kunming Institute of Botany Chinese Academy of Sciences University of Chinese Academy of Sciences Lab of Computational chemistry and Drug Design State Key Laboratory of Chemical Oncogenomics Peking University Shenzhen Graduate School Shenzhen Bay Laboratory State Key Laboratory of Microbial Metabolism School of Life Sciences & Biotechnology Shanghai Jiao Tong University State Key Laboratory of Functions and Applications of Medicinal Plants Guizhou Medical University Molecular Biology Experimental Center Germplasm Bank of Wild Species in Southwest China Kunming Institute of Botany Chinese Academy of Sciences Yunnan Key Laboratory for Wild Plant Resources Kunming Institute of Botany Chinese Academy of Sciences research unit of Chemical Biology of natural Anti-Virus products Chinese Academy of Medical Sciences

In the intricate process of natural product biosynthesis, a metabolon can enhance metabolic flux by associating sequential enzymes. A fungal metabolon, comprising of flavin-dependent monooxygenase Spe F and P450 monooxygenase Spe G, is identified in the biosynthesis of spiro polycyclic alkaloids(+)-notoamide B and its diastereomer(+)-versicolamide B. Using notoamide E as a substance, Spe F/Spe G metabolon can control the stereoselectivity of its 2,3-epoxidation, followed by hydrogen atom ion at C-17 to generate reactive epoxide tau-m A with dienyl iminium unit. Subsequently,(+)-notoamide B and(+)-versicolamide B are produced via tandem nonenzymatic inverse-electron-demand Diels-Alder reaction and semipinacol rearrangement. This provides the first example of metabolon in the biosynthesis of spiro-prenylated indole alkaloids.

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Breaking the structural symmetry of active sites in zeolite imidazolate framework for enhanced CO2 photoreduction

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Science China chemistry 2025年

作者： Yupeng Han Yayu Yan Qiaohong Li Xin Wu Fei Wang Jian Zhang State Key Laboratory of Structural chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences University of Chinese Academy of Sciences College of chemistry Fuzhou University

Adjusting the structure and composition of active sites is a highly effective method for activating linear ***, precise control of interfacial chemistry within molecular-scale environments presents a significant challenge in heterogeneous catalysis. In our study, we present symmetry-broken Mo-O-Co triple-atom active sites within the hybrid zeolite imidazole framework HZIF-CoMo. These sites disrupt the electronic balance and create a weak built-in electric field, thus promoting photocatalytic CO2reduction. The CO yield over HZIF-CoMo is improved to 3.1 mmol g-1h-1, which is over four times higher than the parent cobalt-imidazole framework MAF-6-Co. Both experimental and theoretical studies indicate that electronic modulation through the symmetry-breaking Mo-O-Co moiety acts as an organizing knob to accelerate charge separation and result in more carriers participating in the catalytic reaction. This work provides important insights into optimizing site-related electronic structures for targeted photocatalytic reactions.

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CaH2-promoted activity of Ni-carbonate interface for CO2 methanation

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Journal of Energy chemistry 2025年第1期100卷 522-532页

作者： Jin-Peng Wang Guo-Cui Mao Hui-Lin Jiang Bao-Xia Dong Yun-Lei Teng School of chemistry and Chemical Engineering Yangzhou University

Transition metal-carbonate interfaces often act as active sites in heterogeneous catalytic *** interface between transition metal and metal carbonate exhibits a dynamic equilibrium during the CO2hydrogenation reaction,involving surface carbonate hydrogenation and ***,there have been few reports on engineering the activity of the interface between transition metal and alkaline earth metal carbonate for catalytic *** work demonstrated that the incorporation of CaH2in Ni/CaCO3enhances the CO2methanation activity of the *** CO2conversion for Ni/CaH2-CaCO3reached 68.5%at 400°C,which was much higher than that of the Ni/CaCO3（31.6%） and Ni/CaH2-CaO （42.4%） ***,the Ni/CaH2-CaCO3catalysts remained stable during the stability test for 24 h at 400°C and 8 *** research revealed that CaH2played a crucial role in promoting the activity of the Ni-carbonate interface for ***2could modify the electronic structure of Ni and tune the structural properties of CaCO3to generate medium basic sites （OH groups）,which are favorable for the activation of H2and ***-situ Fourier transform infrared spectroscopy （FTIR） analysis combined with density functional theory calculations demonstrated that CO2activation occurs at the hydroxyl group （OH） on the CaH2-modified Ni-carbonate surface,leading to the formation of CO3H****,our study has confirmed that CO2methanation over the Ni/CaH2-CaCO3catalysts proceeds via the formate pathway.

关键词： CO 2 methanation Metal hydride Ni catalysts Carbonate Metal-carbonate interface