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Molecular detection of pancreatic neoplasia: Current status and future promise

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World Journal of Gastroenterology 2015年第40期21卷 11387-11395页

作者： Shounak Majumder Suresh T Chari david a ahlquist Division of Gastroenterology and Hepatology Mayo ClinicRochesterMN 55905United States

Pancreatic cancer is usually diagnosed at an advanced stage and curative resection is feasible in only a small minority of patients at the time of diagnosis. Diagnosis at an early stage is unequivocally associated with better long-term survival. Several candidate molecular markers for early detection are currently under investigation in different phases of discovery and validation. Recent advances in the technology for whole genome,methylome,ribonucleome,and proteome interrogation has enabled rapid advancements in the field of biomarker discovery. In this review we discuss the current status of molecular markers for detection of pancreatic cancer in blood,pancreatic cyst fluid,pancreatic juice and stool and briefly highlight some promising preliminary results of new approaches that have the potential of advancing this field in the near future.

关键词： Early detection of cancer Sensitivity and specific

Dual-ionic imidazolium salts to promote synthesis of cyclic carbonates at atmospheric pressure

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Green Energy & Environment 2022年第6期7卷 1327-1339页

作者： Tengfei Wang Danning Zheng Beibei An Yi Liu Tiegang Ren HansÅgren Li Wang Jinglai Zhang Mårten S.G.ahlquist Henan Engineering Research Center of Green Anticorrosion Technology for Magnesium Alloys Henan UniversityKaifengHenan475004China Henan Engineering Research Center of Corrosion and Protection for Magnesium Alloys Henan UniversityKaifengHenan475004China College of Chemistry and Chemical Engineering Henan UniversityKaifengHenan475004China Department of Theoretical Chemistry&Biology School of BiotechnologyKTH Royal Institute of Technology10691 StockholmSweden

Novel dual-ionic imidazolium salts are shown to display excellent catalytic activity for cycloaddition of carbon dioxide and epoxides under room temperature and atmospheric pressure(0.1 MPa)without any solvent and co-catalyst leading to 96.1%product *** can be reused five times to keep the product yield over 90%.These intriguing results are attributed to a new reaction mechanism,which is supported by theoretical calculations along with the measurements of ^(13)C NMR spectrum and Fourier transform infrared spectroscopy(FT-IR).The excellent catalytic activity can be traced to a CO_(2)-philic group along with an electrophilic hydrogen *** work shows that incorporation of CO_(2)-philic group is an feasible pathway to develop the new efficient ionic liquids.

关键词： Dual-ionic imidazolium salts CO_(2)-Philic group New mechanism Room temperature Atmospheric pressure

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Tuning the O–O bond formation pathways of molecular water oxidation catalysts on electrode surfaces via second coordination sphere engineering

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Chinese Journal of Catalysis 2021年第3期42卷 460-469页

作者： Qiming Zhuo Shaoqi Zhan Lele Duan Chang Liu Xiujuan Wu Mårten S.G.ahlquist Fusheng Li Licheng Sun State Key Laboratory of Fine Chemicals Institute of Artificial PhotosynthesisDUT-KTH Joint Education and Research Centre on Molecular DevicesInstitute for Energy Science and TechnologyDalian University of TechnologyDalian 116024LiaoningChina Department of Theoretical Chemistry and Biology School of Engineering Sciences in ChemistryBiotechnology and HealthKTH Royal Institute of TechnologyStockholm 10691Sweden Department of Chemistry and Shenzhen Grubbs Institute Southern University of Science and Technology(SUSTech)Shenzhen 518055GuangdongChina Department of Chemistry School of Engineering Sciences in ChemistryBiotechnology and HealthKTH Royal Institute of TechnologyStockholm 10044Sweden

A molecular [Ru(bda)]-type(bda = 2,2’-bipyridine-6,6’-dicarboxylate) water oxidation catalyst with 4-vinylpyridine as the axial ligand(Complex 1) was immobilized or co-immobilized with 1-(trifluoromethyl)-4-vinylbenzene(3 F) or styrene(St) blocking units on the surface of glassy carbon(GC) electrodes by electrochemical polymerization, in order to prepare the corresponding poly-1@GC, poly-1+P3 F@GC, and poly-1+PSt@GC functional electrodes. Kinetic measurements of the electrode surface reaction revealed that [Ru(bda)] triggers the O–O bond formation via(1) the radical coupling interaction between the two metallo-oxyl radicals(I2 M) in the homo-coupling polymer(poly-1), and(2) the water nucleophilic attack(WNA) pathway in poly-1+P3 F and poly-1+PSt copolymers. The comparison of the three electrodes revealed that the second coordination sphere of the water oxidation catalysts plays vital roles in stabilizing their reaction intermediates, tuning the O–O bond formation pathways and improving the water oxidation reaction kinetics without changing the first coordination structures.

关键词： Water oxidation catalyst Second coordination sphere Dipole moment O-O bond formation Reaction kinetics

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Switching O-O bond formation mechanism between WNA and I2M pathways by modifying the Ru-bda backbone ligands of water-oxidation catalysts

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Journal of Energy Chemistry 2021年第3期30卷 815-821页

作者： Biaobiao Zhang Shaoqi Zhan Tianqi Liu Linqin Wang A.Ken Inge Lele Duan Brian J.J.Timmer Oleksandr Kravchenko Fei Li Marten S.G.ahlquist Licheng Sun Department of Chemistry KTH Royal Institute of Technology10044 StockholmSweden Department of Theoretical Chemistry&Biology School of Engineering Sciences in Chemistry Biotechnology and HealthKTH Royal Institute of Technology10691 StockholmSweden Department of Materials and Environmental Chemistry Stockholm University10691 StockholmSweden Department of Chemistry Southern University of Science and Technology(SUSTech)Shenzhen 518055GuangdongChina State Key Laboratory of Fine Chemicals Institute of Artificial PhotosynthesisDUT–KTH Joint Education and Research Center on Molecular DevicesDalian University of Technology(DUT)Dalian 116024LiaoningChina

Understanding the seven coordination and O-O coupling pathway of the distinguished Ru-bda catalysts is essential for the development of next generation efficient water-oxidation catalysts based on earthabundant *** work reports the synthesis,characterization and catalytic properties of a monomeric ruthenium catalyst Ru-bnda(H2 bnda=2,2’-bi(nicotinic acid)-6,6’-dicarboxylic acid)featuring steric hindrance and enhanced hydrophilicity on the *** experimental evidence with systematic density functional theory calculations on the Ru-bnda and related catalysts Ru-bda(H_(2)bda=2,2’-bipyridine-6,6’-dicarboxylic acid),Ru-pda(H_(2)pda=1,10-phenanthroline-2,9-dicarboxylic acid),and Ru-biqa(H_(2)biqa=(1,1’-biisoquinoline)-3,3’-dicarboxylic acid),we emphasized that seven coordination clearly determines presence of Ru^(Ⅴ)=O with high spin density on the ORu^(Ⅴ)=O atom,*** with radical properties,which is one of the necessary conditions for reacting through the O-O coupling ***,an additional factor to make the condition sufficient is the favorable intermolecular faceto-face interaction for the generation of the pre-reactive[Ru^(Ⅴ)=O…O=Ru^(Ⅴ)],which may be significantly influenced by the secondary coordination *** work provides a new understanding of the structure-activity relationship of water-oxidation catalysts and their potential to adopt I2M pathway for O-O bond formation.

关键词： Water oxidation Oxygen evolution Ruthenium O-O bond formation

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Isolation and Identification of Pseudo Seven-Coordinate Ru(Ⅲ)Intermediate Completing the Catalytic Cycle of Ru-bda Type of Water Oxidation Catalysts

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CCS Chemistry 2022年第7期4卷 2481-2490页

作者： Tianqi Liu Ge Li Nannan Shen Linqin Wang Brian J.J.Timmer Shengyang Zhou Biaobiao Zhang Alexander Kravchenko Bo Xu Marten S.G.ahlquist Licheng Sun Department of Chemistry School of Engineering Sciences in ChemistryBiotechnologyand HealthKTH Royal Institute of TechnologyStockholm 10044 Department of Theoretical Chemistry and Biology School of Engineering Sciences in ChemistryBiotechnologyand HealthKTH Royal Institute of TechnologyStockholm 10691 State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhou 215123 Center of Artificial Photosynthesis for Solar Fuels School of ScienceWestlake UniversityHangzhou 310024 Nanotechnology and Functional Materials Department of Materials Sciences and EngineeringThe Angstrom LaboratoryUppsala UniversityUppsala 75103 Institute of Artificial Photosynthesis(IAP) State Key Laboratory of Fine ChemicalsDalian University of Technology(DUT)Dalian 116024

Isolation of RuⅢ-bda(17-electron specie)complex with an aqua ligand(2-electron donor)is challenging due to violation of the 18-electron *** considerable efforts have been dedicated to mechanistic studies of water oxidation by the Ru-bda family,the structure and initial formation of the Ru^(Ⅲ)-bda aqua complex are still ***,we challenge this often overlooked step by designing a pocketshape Ru-based complex *** computational studies showed that 1 possesses the crucial hydrophobicity at the Ru^(V)(O)state as well as similar probability of access of terminal O to solvent water molecules when compared with classic Ru-bda *** characterization of single-crystal structures at the Ru^(Ⅱ) and Ru^(Ⅲ) states,a pseudo seven-coordinate“ready-togo”aqua ligand with Ru^(Ⅲ)…O distance of 3.62A was *** aqua ligand was also found to be part of a formed hydrogen-bonding network,providing a good indication of how the Ru^(Ⅲ)-OH_(2)complex is formed.

关键词： Ru-bda water oxidation pseudo seven-coordinate Ru^(Ⅲ)-OH_(2)intermediate water preorganization

Switching the O-O Bond Formation Pathways of Ru-pda Water Oxidation Catalyst by Third Coordination Sphere Engineering

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Research 2021年第1期2021卷 1343-1353页

作者： Yingzheng Li Shaoqi Zhan Lianpeng Tong Wenlong Li Yilong Zhao Ziqi Zhao Chang Liu Mårten S.G.ahlquist Fusheng Li Licheng Sun State Key Laboratory of Fine Chemicals Institute of Artificial PhotosynthesisDUT-KTH Joint Education and Research Centre on Molecular DevicesDalian University of TechnologyDalian 116024China Department of Theoretical Chemistry and Biology School of Engineering Sciences in Chemistry Biotechnology and HealthKTH Royal Institute of Technology10691 StockholmSweden Department of Chemistry University of CaliforniaRiversideCalifornia 92521USA School of Chemistry and Chemical Engineering/Institute of Clean Energy and Materials Guangzhou UniversityNo.230 Wai Huan Xi RoadHigher Education Mega CenterGuangzhou 510006China Department of Chemistry School of Engineering Sciences in ChemistryBiotechnology and HealthKTH Royal Institute of Technology10044 StockholmSweden Center of Artificial Photosynthesis for Solar Fuels School of ScienceWestlake University310024 HangzhouChina

Water oxidation is a vital anodic reaction for renewable fuel generation via electrochemical-and photoelectrochemical-driven water splitting or CO_(2)*** complexes,such as Ru-bda family,have been shown as highly efficient wateroxidation catalysts(WOCs),particularly when they undergo a bimolecular O-O bond formation *** this study,a novel Ru(pda)-type(pda^(2–)=1,10-phenanthroline-2,9-dicarboxylate)molecular WOC with 4-vinylpyridine axial ligands was immobilized on the glassy carbon electrode surface by electrochemical *** kinetic studies revealed that this homocoupling polymer catalyzes water oxidation through a bimolecular radical coupling pathway,where interaction between two Ru(pda)–oxyl moieties(I2M)forms the O-O *** calculated barrier of the I2M pathway by densityfunctional theory(DFT)is significantly lower than the barrier of a water nucleophilic attack(WNA)*** using this polymerization strategy,the Ru centers are brought closer in the distance,and the O-O bond formation pathway by the Ru(pda)catalyst is switched from WNA in a homogeneous molecular catalytic system to I2M in the polymerized film,providing some deep insights into the importance of third coordination sphere engineering of the water oxidation catalyst.

关键词： coupling closer Oxidation

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粪便隐血试验在检测结直肠癌中的应用

国际消化病杂志 1986年第2期 98-99页

作者： ahlquist DA ,Beart RW Jr ,邝耀麟

结直肠癌的病因仍未明了.因此,尚不可能作一级预防,即去除诱发的影响.生存率的提高有赖于二级预防,即检出可治疗的癌前病变或早期病变,为此需对危险人群定期进行普查筛选.结直肠癌是可筛选的疾病,原因为:1.常见病,美国约20人中可有1人... 详细信息

结直肠癌的病因仍未明了.因此,尚不可能作一级预防,即去除诱发的影响.生存率的提高有赖于二级预防,即检出可治疗的癌前病变或早期病变,为此需对危险人群定期进行普查筛选.结直肠癌是可筛选的疾病,原因为:1.常见病,美国约20人中可有1人患结肠癌.2.严重性,如不治疗大多致死.3.大多数病例的症状前期长.病人可有癌前腺瘤或早期病变数年而无症状.4.早期诊断和治疗预后良好.筛选所得病例经手术治疗后5年生存率在90%以上,有症状的病例则低于50%.

关键词：粪便隐血试验血红素叶琳萤光敏感性特异性肠道结直肠癌免疫化学反应血红蛋白含量