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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

Cobalamin-dependent radical S-adenosyl-L-methionine protein functions with a partner to successively methylate tricyclic indole alkaloid for chuangxinmycin maturation and derivatization

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Science China Chemistry 2025年第1期68卷 308-316页

作者： Sili Wang Jiancheng Huang Yanan Du Wei Huang Yufeng xue Xiaokun xu Guannan zhong Yuanyuan Shi Bin Hong Xiaoying Bian Wen Liu State Key Laboratory of Chemical Biology Shanghai Institute of Organic Chemistry University of Chinese Academy of SciencesChinese Academy of Sciences State Key Laboratory of Microbial Technology Shandong University National Health Commission (NHC) Key Laboratory of Biotechnology for Microbial Drugs Institute of Medicinal BiotechnologyChinese Academy of Medical Science & Peking Union Medical College

Cobalamin(Cbl)-dependent radical S-adenosyl-L-methionine(SAM) proteins constitute the largest collection of the radical SAM superfamily that has hundreds of thousands of individual members. Many of these proteins are involved in the biosynthesis of pharmaceutically important natural products to catalyze chemically demanding reactions. In the biosynthetic pathway of chuangxinmycin(CXM), a unique indole alkaloid antibiotic with potent anti-infective activity, functionalization of the characteristic thiopyrano[4,3,2-cd]indole scaffold by regio-and stereoselective C3-methylation is believed to rely on a Cbl-dependent radical process, which, however, remained to be reconstituted biochemically. We here report the dissection of this enzymatic process, which requires the incorporation of Cxm8, a Cbl-dependent radical SAM protein, with Cxm9, a DUF5825family protein that shares no homology to any proteins of known functions. Cxm8 and Cxm9 function together by forming an unexpected heterodimeric complex that selectively catalyzes C3-methylation of the tricyclic indole-S-hetero ring system in a successive manner, achieving CXM and a recently identified, C3-dimethylated congener. Detailed biochemical characterization,isotope labeling, structural simulation and bioinformatics analysis rationalized the catalysis of the Cxm8/Cxm9 complex and particularly the necessity of the DUF5825 protein for C3-methylase activity. This is the first example that a Cbl-dependent protein acts with a partner to exhibit radical SAM activity.

关键词： cbl-dependent radical SAM protein biosynthesis chuangxinmycin stereoselective methylation

Constructing 2D bismuth-based heterostructure for highly efficient photocatalytic CO2 reduction

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Tungsten 2025年第1期7卷 71-79页

作者： Ruo-Hang xu Hao-Yu Jiang Dan-Dan Cui Kun-Rong Du Hong-Run Zhang Sheng-Jie xu Ya-Qi Li Zhi-zhen Ren Liang Wang Wei-Chang Hao Yi Du School of Physics and BUAA-UOW Joint Research Centre Beihang University Shenzhen Institute of Beihang University Centre for Catalysis and Clean Energy School of Environment and Science Griffith University

Reforming carbon dioxide（CO2） into fuels and valuable chemicals using solar energy holds significant potential for emission reduction and addressing energy supply *** recombination of photocarriers remains a major obstacle,however,to enhancing solar energy conversion efficiency in the photocatalytic reaction *** two-dimensional materials,constructing heterogeneous structures has emerged as an effective strategy to enhance the separation of photoexcited carriers by leveraging the internal electric field at the heterogeneous ***,we present a facile strategy for preparing Bi4NbO8Br/Bi2WO6plate-on-plate Z-scheme junctions with a strong internal electric field by in situ *** unique heterostructure facilitates efficient separation and transport of photoexcited charges by harnessing the internal electric field induced by chemical bonding at the lateral ***,the Bi4NbO8Br/Bi2WO6heterostructure exhibits enhanced CO2photoreduction properties,along with a CO yield rate of approximately 35 μmol·g-1·h-1under full light *** work offers novel insights into the synthesis of unique hetero structures intended to enhance the efficiency of photocatalytic CO2reduction.

关键词： Bi4NbO8Br/Bi2WO6 CO2 reduction Heterostructures Photocatalysts

Inhibitory gamma-aminobutyric acidergic neurons in the anterior cingulate cortex participate in the comorbidity of pain and emotion

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Neural Regeneration Research 2025年第10期20卷 2838-2854页

作者： Lu Guan Mengting Qiu Na Li zhengxiang Zhou Ru Ye Liyan zhong Yashuang xu Junhui Ren Yi Liang Xiaomei Shao Jianqiao Fang Junfan Fang Junying Du Department of Neurobiology and Acupuncture Research Third School of Clinical MedicineZhejiang Chinese Medical UniversityHangzhouZhejiang ProvinceChina Key Laboratory for Research of Acupuncture Treatment and Transformation of Emotional Diseases Third School of Clinical MedicineZhejiang Chinese Medical UniversityHangzhouZhejiang ProvinceChina Fuchun Community Health Service Center of Fuyang District HangzhouZhejiang ProvinceChina

Pain is often comorbid with emotional disorders such as anxiety and *** of the anterior cingulate cortex has been implicated in pain and pain-related negative emotions that arise from impairments in inhibitory gamma-aminobutyric acid *** review primarily aims to outline the main circuitry(including the input and output connectivity)of the anterior cingulate cortex and classification and functions of different gamma-aminobutyric acidergic neurons;it also describes the neurotransmitters/neuromodulators affecting these neurons,their intercommunication with other neurons,and their importance in mental comorbidities associated with chronic pain *** understanding on their role in pain-related mental comorbidities may facilitate the development of more effective treatments for these ***,the mechanisms that regulate gamma-aminobutyric acidergic systems remain *** is also unclear as to whether the mechanisms are presynaptic or *** exploration of the complexities of this system may reveal new pathways for research and drug development.

关键词： anterior cingulate cortex anxiety chronic pain circuit communication comorbidity depression gamma-aminobutyric acidergic neurons parvalbumin neurons synaptic transmission

Impregnating photo-stable gold precursor onto uncalcined TS-1 to boost catalytic hydro-oxidation of propane

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Science China Chemistry 2025年

作者： Zhihua Zhang Erchuan Yang Fan Liu Kesheng xu Yuxia zhong Jinwei Sun Shudong Shi xuezhi Duan Xinggui Zhou State Key Laboratory of Chemical Engineering East China University of Science and Technology

Immobilizing highly dispersed Au nanoparticles onto titanium silicalite-1 (TS-1) by a simple impregnation method under light is still a challenging *** this work,a high photostable Au precursor protected by thiol ligands was firstly synthesized,and the as-prepared Au precursor displayed excellent stability under light for over 30 days,while the Au precursor without thiol ligands formed precipitates after just 2 h under ***,the Au precursor protected by thiol ligands was immobilized on the external surface of uncalcined TS-1 (i.e.,TS-1-B) by the incipient wetness impregnation method (IWI method) to prepare Au/TS-1-B *** activity of as-prepared Au/TS-1-B catalyst in the hydro-oxidation of propane to acetone was 1.4 times higher than that of the catalyst prepared by the deposition-precipitation urea method (DPU method).The structures of the Au/TS-1-B catalysts prepared by different methods were analyzed by multiple *** to the Au/TS-1-B catalyst prepared by the DPU method,the Au/TS-1-B catalyst synthesized by the IWI method exhibited a narrower size distribution of Au nanoparticles and had more small Au particles (<2 nm),which is the main reason for its superior ***,the effects of gold loadings,reaction temperature and Si/Ti molar ratio on the catalytic performance of the Au/TS-1-B catalyst prepared by the IWI method were also *** addition,the Au/TS-1-B catalyst prepared by the IWI method also exhibited excellent stability for over 140 h.

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Palladium installed copper-organic framework for C–C coupling reactions

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Science China Chemistry 2025年

作者： Yu-Mei Wang Mei-Xia Tao Kai-Ming Mo xu Chen Shu-Hua zhong Elena S Shubina Guo-Hong Ning Dan Li College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Supramolecular Coordination ChemistryJinan University A.N.Nesmeyanov Institute of Organoelement Compounds Russian Academy of Sciences

The formation of C–C bonds is a crucial aspect of organic synthesis. Synthesists' long-term objective is to identify novel catalysts to optimize reaction systems based on traditional transition metal catalysis. This study explores the synthesis and catalytic potential of palladium-installed covalent metal-organic frameworks(CMOFs) based on copper cyclic trinuclear units(Cu-CTUs). By incorporating palladium ions into the imine-based framework JNM-7 through a straightforward immersion method, we achieved a notable enhancement in catalytic activity for critical C–C coupling reactions, including C–H arylation and Sonogashira cross-coupling. The resulting JNM-7-Pd demonstrated remarkable stability and recyclability, maintaining its efficiency over at least three cycles without any decline in efficiency.

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从网络角度研究元胡止痛胶囊治疗头痛与痛经的分子作用机制

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中国新药杂志 2016年第20期25卷 2323-2330页

作者：张新庄柯志鹏李娜曹亮王振中萧伟徐筱杰江苏康缘药业股份有限公司中药制药新技术国家重点实验室连云港222001 北京大学化学与分子工程学院北京100871

目的:研究元胡止痛胶囊治疗头痛和痛经的药效物质和分子作用机制。方法:采用分子对接、分子-靶蛋白网络特征分析以及靶蛋白-生物通路信息挖掘的方法研究元胡止痛胶囊中分子与靶蛋白的相互作用。结果:分子对接与网络分析发现元胡止痛胶... 详细信息

目的:研究元胡止痛胶囊治疗头痛和痛经的药效物质和分子作用机制。方法:采用分子对接、分子-靶蛋白网络特征分析以及靶蛋白-生物通路信息挖掘的方法研究元胡止痛胶囊中分子与靶蛋白的相互作用。结果:分子对接与网络分析发现元胡止痛胶囊中有63个活性成分,且大部分具有良好的生物利用度和血脑屏障通透性,其中Coptisine,Protopine,Berberine等17个为其主要活性成分,可通过与Glu A2,i NOS,AKR1C2,ROCK1等28个靶蛋白相互作用,一方面降低疼痛信号的感知和传递,另一方面调控血管/子宫平滑肌的舒张与收缩,进而达到缓解疼痛的治疗作用。结论:通过数据分析确定了元胡止痛胶囊止痛的分子作用机制和主要活性成分,有助于减少后续药效物质基础和分子作用机制实验研究的盲目性。

关键词：疼痛分子描述符中药白芷网络药理学

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特大型钢结构整体顶推平移技术

施工技术 2004年第11期33卷 23-25页

作者：王云飞崔振中许勇倪洪革上海市机械施工公司上海200072

结合重庆江北机场新航站楼钢结构安装工程,介绍整体顶推平移技术的原理、工艺、技术创新及应用效益。

关键词：空间钢结构整体顶推平移计算机控制

C-X-C chemokine receptor type 5+CD8+T cells as immune regulators in hepatitis Be antigen-positive chronic hepatitis B under interferonalpha treatment

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World Journal of Gastroenterology 2025年第3期31卷 73-83页

作者： zhen-Yu xu zhong-Shang Dai Guo-zhong Gong Min Zhang Department of Infectious Diseases Second Xiangya HospitalCentral South UniversityChangsha 410011Hunan ProvinceChina Institute of Hepatology and Department of Infectious Diseases The Second Xiangya HospitalCentral South UniversityChangsha 410011Hunan ProvinceChina

BACKGROUND C-X-C chemokine receptor type 5(CXCR5)+CD8+T cells represent a unique immune subset with dual roles,functioning as cytotoxic cells in persistent viral infections while promoting B cell *** their importance,the specific role of CXCR5+CD8+T cells in chronic hepatitis B(CHB),particularly during interferon-alpha(IFN-α)treatment,is not fully *** study aims to elucidate the relationship between CXCR5+CD8+T cells and sustained serologic response(SR)in patients undergoing 48 weeks of pegylated IFN-α(peg-IFN-α)treatment for *** To elucidate the relationship between CXCR5+CD8+T cells and sustained SR in patients undergoing 48 weeks of peg-IFN-αtreatment for *** This study enrolled 60 patients with hepatitis Be antigen(HBeAg)-positive CHB undergoing 48 weeks of peg-IFN-α*** were assessed for eligibility based on criteria such as persistent HBsAg-positive status for at least six months,HBeAb-negative,hepatitis B virus DNA levels exceeding 2×104 copies/mL,and alanine aminotransferase(ALT)levels between 2 and 10 times the upper limit of *** samples were collected at baseline and at weeks 12,24,48,and a 24-week treatment-free follow-up(week 72)to measure serum interleukin(IL)-21 concentration via ELISA and to analyze CXCR5 and programmed death-ligand 1(PD-L1)expression on CD8+T cells by flow cytometry,CXCR5 is a chemokine receptor that directs immune cells to specific tissues,while PD-L1 is a protein that regulates immune responses by inhibiting T cell *** Patients with CHB exhibited significantly lower levels of circulating CXCR5+CD8+T cells compared to healthy controls(P<0.01).Notably,CXCR5+CD8+T cells were prominently expressed in patients who achieved sustained SR compared to non-SR(NSR).A significant correlation was observed between CXCR5 and PD-L1 expression(r=-0.189,P=0.002).However,there was no significant correlation between serum IL-21 levels and CXCR5+CD8+lymphocytes(r=-0.03,P=0.62

关键词： C-X-C chemokine receptor type 5 Programmed death-ligand 1 Interleukin-21 Pegylated interferon-alpha Chronic hepatitis B