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Efficient epoxidation of propylene over non-noble nickel-based catalyst promoted by alkali metals

Science China Chemistry 2024年

作者： Wenqian Li Wanting Li Xinxin Cao Longfei chen Yibo Qin Yanfeng Zhu Yanfei Zhang Gai Miao Lingzhao Kong Jiong Li xinqing chen State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization CAS Key Laboratory of Low-carbon Conversion Science and Engineering Shanghai Advanced Research Institute Chinese Academy of Sciences University of Chinese Academy of Sciences School of Environmental Science and Engineering Suzhou University of Science and Technology Shanghai Synchrotron Radiation Facility Zhangjiang National Lab Shanghai Advanced Research Institute Chinese Academy of Sciences

The application of non-noble metal catalysts in the catalytic direct gas-phase epoxidation of propylene with H2and O2to produce propylene oxide is valuable and *** introduction of alkali metal promoters is one of the effective methods to improve the catalytic activity of ***,a series of alkali metal （Li,Na,K,Rb,and Cs）-promoted Ni/TS-1 catalysts were prepared to deeply understand the effect of alkali metals on the structure-activity relationship for gas-phase epoxidation of *** them,the Na-Ni/TS-1 catalyst exhibits the highest catalytic activity (propylene conversion of 7.35%and POformation rate of 157.9 g h-1kg-1cat) and the best stability （long-term stability exceeding 140 h at 200°C）.X-ray absorption and photoelectron spectroscopy revealed that the electronic structure of Ni can be tuned by the addition of alkali metal ***3-TPD-MS,CO2-TPD-MS,and C3H6-TPD-MS results indicate that the acidity of the catalyst can also be adjusted by the introduction of alkali metal,whereas the Na-Ni/TS-1 catalyst exhibits the strongest C3H6adsorption ***,the suitable acid-base properties,unique electronic properties of Ni species,and the strongest propylene adsorption capacity resulted in improved propylene gas-phase epoxidation activity of Na-Ni/TS-1 *** study not only provides a new strategy for the practical application of nickel-based catalysts in the gas-phase epoxidation of propylene but also provides insights into the promoting effect of alkali metals.

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二氧化碳捕集-转化一体化技术研究进展

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科学通报 2024年第8期69卷 1012-1024页

作者：胡登王星博陈新庆孙楠楠魏伟中国科学院上海高等研究院二氧化碳光子科学建制化研究中心上海201210 中国科学院上海高等研究院中国科学院低碳转化科学与工程重点实验室上海201210

CO_(2)捕集利用与封存(CO_(2)capture,utilization,and storage,CCUS)是一项新兴的、可实现传统化石能源大规模低碳利用的重要技术.然而,传统的CCUS技术成本过高,极大阻碍了其推广和应用.CO_(2)捕集-转化一体化技术是一种在CCUS自身框... 详细信息

CO_(2)捕集利用与封存(CO_(2)capture,utilization,and storage,CCUS)是一项新兴的、可实现传统化石能源大规模低碳利用的重要技术.然而,传统的CCUS技术成本过高,极大阻碍了其推广和应用.CO_(2)捕集-转化一体化技术是一种在CCUS自身框架内发展出的集成型CCUS技术.在该过程中,排放源的CO_(2)被吸收剂或吸附剂捕集后,无须经过高能耗的解吸过程而直接与共反应物进行反应,转化为下游产品,从而有望大幅降低减排成本,是一种全新的高效、低能耗CO_(2)减排技术.本文以CO_(2)捕集-转化一体化技术制备不同产品为出发点,从技术方案、材料构建、反应机理等方面进行综述,分析了一体化技术制备不同产品的研究现状和现存问题,探讨了该类技术的发展趋势.

关键词：碳中和碳捕集碳转化一体化

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Dimensional engineering of covalent organic frameworks derived carbons for electrocatalytic carbon dioxide reduction

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SusMat 2023年第6期3卷 834-842页

作者： Guojuan Liu Xuewen Li Minghao Liu Xiubei Yang Zhuangyan Guo xinqing chen Qing Xu Gaofeng Zeng Yue He CAS Key Laboratory of Low-Carbon Conversion Science and Engineering Shanghai Advanced Research Institute(SARI)Chinese Academy of Sciences(CAS)ShanghaiChina School of Chemical Engineering University of Chinese Academy of SciencesBeijingChina Shanghai Ninth People’s Hospital Shanghai Jiao Tong UniversityShanghaiChina

Covalent organic frameworks(COFs)have been developed as the precursors to construct porous carbons for electrocatalytic ***,the influences of carbon dimensions on the catalytic performance are still *** this work,we have first constructed COF-derived carbons by template-synthesis strategy in different dimensions to catalyze the carbon dioxide reduction(CO_(2)RR).By using different templates,the one-dimensional(1D),two-dimensional(2D),and three-dimensional(3D)COF-derived carbons have been employed to anchor Co-porphyrin to form the Co-N5 sites to catalyze CO_(2)*** 1D catalyst templated by carbon nano tubes presents high binding ability of CO_(2),more defective sites,and higher electronic conductivity,resulting in a higher catalytic activity for CO_(2)and selectivity of CO than 2D and 3D carbon-based *** 1D catalyst delivers the turnover frequency values of 1150 h^(−1)and the FECO of 94.5%at 0.7 V versus RHE,which is significantly better than those of 2D and 3D carbon-based catalysts.

关键词： CO_(2)reduction Co-N_(5)sites covalent organic frameworks dimensional engineering templatesynthesis strategy

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Operando reconstruction towards stable CuI nanodots with favorable facets for selective CO_(2) electroreduction to C2H4

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Science China Chemistry 2023年第6期66卷 1834-1843页

作者： Wenjie Xue Hongxia Liu xinqing chen Xiaoju Yang Ruoou Yang Youwen Liu Minghao Li Xuan Yang Bao Yu Xia Bo You Key Laboratory of Material Chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China School of Chemistry and Chemical Engineering Wuhan Textile UniversityWuhan 430200China Shanghai Advanced Research Institute Chinese Academy of SciencesShanghai 201210China State Key Laboratory of Materials Processing and Die&Mold Technology and School of Materials Science and Engineering Huazhong University of Science and TechnologyWuhan 430074China

Cu-based electrocatalysts with favorable facets and Cu^(+)can boost CO_(2) reduction to valuable multicarbon ***,the inevitable Cu^(+)reduction and the phase evolution usually result in poor ***,we fabricate CuI nanodots with favorable(220)facets and a stable Cu^(+)state,accomplished by operando reconstruction of Cu(OH)_(2) under CO_(2)-and I--containing electrolytes for enhanced CO_(2)-to-C_(2)H_(4) *** X-ray absorption spectroscopy(XAS),in-situ Raman spectroscopy and thermodynamic potential analysis reveal the preferred formation of *** gas electroresponse and density functional theory(DFT)calculations reveal that CO_(2)-related species induce the exposure of the(220)plane of Cu ***,the small size of nanodots enables the adequate contact with I^(-),which guarantees the rapid formation of Cu I instead of the electroreduction to Cu^(0).As a result,the resulting catalysts exhibit a high C2H4 Faradaic efficiency of 72.4%at a large current density of 800 m A cm^(-2) and robust stability for 12 h in a flow *** in-situ ATR-SEIRS spectroscopic characterizations and DFT calculations indicate that the(220)facets and stable Cu^(+) in CuI nanodots synergistically facilitate CO_(2)/*CO adsorption and*CO dimerization.

关键词： CO_(2)reduction reaction cuprous iodide favorable facets halogen electrolyte reconstruction

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Plant-based dietary patterns and risk of esophageal cancer:A prospective cohort study spanning 17 years

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Chinese Journal of Cancer Research 2024年第1期36卷 36-45页

作者： Xiaorui Zhang Feifan He Jiayue Li Ru chen xinqing Li Li Li Fen Liu Shaoming Wang Wenqiang Wei Department of Epidemiology and Health Statistics School of Public HealthBeijing Municipal Key Laboratory of Clinical EpidemiologyCapital Medical UniversityBeijing 100069China National Central Cancer Registry office National Cancer Center/National Clinical Research Center for Cancer/Cancer HospitalChinese Academy of Medical Sciences and Peking Union Medical CollegeBeijing 100021China Department of Cancer Epidemiology National Cancer Center/National Clinical Research Center for Cancer/Cancer HospitalChinese Academy of Medical Sciences and Peking Union Medical CollegeBeijing 100021China

Objective: Plant-based diets have multiple health benefits for cancers;however, little is known about the association between plant-based dietary patterns and esophageal cancer(EC).This study presents an investigation of the prospective associations among three predefined indices of plant-based dietary patterns and the risk of ***: We performed endoscopic screening for 15,709 participants aged 40-69 years from two high-risk areas of China from January 2005 to December 2009 and followed the cohort until December 31, 2022. The overall plant-based diet index(PDI), healthful plant-based diet index(h PDI), and unhealthful plant-based diet index(u PDI), were calculated using survey responses to assess dietary patterns. We applied Cox proportional hazard regression to estimate the multivariable hazard ratios(HRs) and 95% confidence intervals(95% CIs) of EC across 3plant-based diet indices and further stratified the analysis by ***: The final study sample included 15,184 participants in the cohort. During a follow-up of 219,365person-years, 176 patients with EC were identified. When the highest quartile was compared with the lowest quartile, the pooled multivariable-adjusted HR of EC was 0.50(95% CI, 0.32-0.77) for h PDI. In addition, the HR per 10-point increase in the h PDI score was 0.42(95% CI, 0.27-0.66) for ECs. Conversely, u PDI was positively associated with the risk of EC, and the HR was 1.80(95% CI, 1.16-2.82). The HR per 10-point increase in the u PDI score was 1.90(95% CI, 1.26-2.88) for ECs. The associations between these scores and the risk of EC were consistent in most subgroups. These results remained robust in sensitivity ***: A healthy plant-based dietary pattern was associated with a reduced risk of EC. Emphasizing the healthiness and quality of plant-based diets may be important for preventing the development of EC.

关键词： Esophageal cancer diet dietary pattern epidemiology nutrition prospective cohort study

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Identification of potential immune-related mechanisms related to the development of multiple myeloma

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Chinese Medical Journal 2024年第13期137卷 1603-1613页

作者： Yaomei Wang Wenli Zhang Tiandong Li Mengmeng Liu Mengya Gao xinqing Li Yufei chen Yongping Song Wei Li Chunyan Du Fang Wang Lina Liu Department of Hematology The Affiliated Cancer Hospital of Zhengzhou University&Henan Cancer HospitalZhengzhouHenan 450008China The Academy of Medical Science College of MedicalZhengzhou UniversityZhengzhouHenan 450052China College of Public Health Zhengzhou UniversityZhengzhouHenan 450000China Department of Research and Foreign Affairs The Affiliated Cancer Hospital of Zhengzhou University&Henan Cancer HospitalZhengzhouHenan 450008China Department of Clinical Medicine Zhengzhou UniversityZhengzhouHenan 450052China Department of Hematology The First Affiliated Hospital of Zhengzhou UniversityZhengzhouHenan 450052China Laboratory Animal Center School of Medical SciencesZhengzhou UniversityZhengzhouHenan 450052China

Background:Although significant advances have been made in the treatment of multiple myeloma(MM),leading to unprecedented response and survival rates among patients,the majority eventually relapse,and a cure remains *** situation is closely related to an incomplete understanding of the immune microenvironment,especially monocytes/macrophages in patients with treatment-naïve *** aim of this study was to provide insight into the immune microenvironment,especially monocytes/macrophages,in patients with treatment-naïve ***:This study used the single-cell RNA sequencing(scRNA-seq)data of both patients with MM and heathy donors to identify immune cells,including natural killer(NK)cells,T cells,dendritic cells(DCs),and monocytes/*** data and flow cytometry analysis of monocytes/macrophages were used to further examine the effect of monocytes/macrophages in treatment-naïve MM ***:A significant difference was observed between the bone marrow(BM)immune cells of the healthy controls and treatment-naïve MM patients through *** is noteworthy that,through an scRNA-seq data analysis,this study found that interferon(IFN)-induced NK/T cells,terminally differentiated effector memory(TEMRA)cells,T-helper cells characterized by expression of IFN-stimulated genes(ISG^(+)Th cells),IFN-responding exhausted T cells,mannose receptor C-type 1(MRC1)^(+)DCs,IFN-responding DCs,MHCII^(+)DCs,and immunosuppressive monocytes/macrophages were enriched in patients with treatment-naïve ***,transcriptomic data of monocytes/macrophages demonstrated that"don’t eat me"-related genes and IFN-induced genes increase in treatment-naïve MM ***,scRNA-seq,transcriptomic data,and flow cytometry also showed an increased proportion of CD16^(+)monocytes/macrophages and expression level of ***-cell communication analysis indicated that monocytes/macrophages,whose related important signaling pathways include migration i

关键词： Multiple myeloma Monocytes/macrophages Single-cell RNA sequencing Immune cell Microenvironment Bone marrow Molecular characterization

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Preparation of polymer-supported hydrated ferric oxide based on Donnan membrane effect and its application for arsenic removal

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Science China Chemistry 2008年第4期51卷 379-385页

作者： ZHANG QingJian PAN BingCai chen xinqing ZHANG WeiMing PAN BingJun ZHANG QuanXing L.LV X.S.ZHAO State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210093China Department of Chemical and Biomolecular Engineering National University of Singapore10 Kent RidgeSingapore 119260Singapore 不详

In the present study a novel technique was proposed to prepare a polymer-supported hydrated ferric oxide (D201-HFO) based on Donnan membrane effect by using a strongly basic anion exchanger D201 as the host material and FeCl3-HCl-NaCl solution as the reaction environment. D201-HFO was found to exhibit higher capacity for arsenic removal than a commercial sorbent Purolite ArsenX. Furthermore, it presents favorable adsorption selectivity for arsenic removal from aqueous solution, as well as satis- factory kinetics. Fixed-bed column experiments showed that arsenic sorption on D201-HFO could re- sult in concentration of this toxic metalloid element below 10 μg/L, which was the new maximum con- centration limit set recently by the European Commission and imposed by the US EPA and China. Also, the spent D201-HFO is amenable to efficient regeneration by NaOH-NaCl solution.

关键词： hydrated ferrous oxide anion exchanger Donnan membrane effect arsenic sorption

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Novel DNA methylation markers for early detection of gastric cardia adenocarcinoma and esophageal squamous cell carcinoma

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Science China Life Sciences 2024年

作者： Zhiyuan Fan Jiajie Hao Feifan He Hao Jiang Jinwu Wang Minjuan Li xinqing Li Ru chen Wenqiang Wei Office of National Central Cancer Registry National Cancer Center/National Clinical Research Center for Cancer/Cancer HospitalChinese Academy of Medical Sciences and Peking Union Medical College State Key Laboratory of Molecular Oncology Center for Cancer Precision MedicineNational Cancer Center/National Clinical Research Center for Cancer/Cancer HospitalChinese Academy of Medical Sciences and Peking Union Medical College School of Population Medicine and Public Health Chinese Academy of Medical Sciences and Peking Union Medical College Department of Pathology Linzhou Cancer Hospital Department of Orthopedic Surgery Beijing Jishuitan HospitalCapital Medical University Collaborative Innovation Center for Cancer Personalized Medicine Nanjing Medical University

Gastric cardia adenocarcinoma (GCA) and esophageal squamous cell carcinoma (ESCC) present significant health challenges in China,often diagnosed at advanced stages with poor ***,effective biomarkers for early detection remain *** study aimed to integrate methylome and transcriptome data to identify DNA methylation markers for the early detection of GCA and *** the discovery stage,we conducted Infinium MethylationEPIC array analysis on 36 paired GCA and non-tumor adjacent tissues (NAT),identifying differentially methylated CpG sites (DMCs) between GCA/ESCC and NAT through combined analyses of in-house and publicly available *** the validation stage,targeted pyrosequencing and quantitative real-time RT-PCR were performed on paired tumor and NAT samples from 50GCA and 50 ESCC *** the application stage,an independent set of 438 samples,including GCA,ESCC,high-and low-grade dysplasia(HGD/LGD),and normal controls,was tested for selected DMCs using *** analysis validated three GCA-specific,two ESCC-specific,and one tumor-shared DMCs,exhibiting significant hypermethylation and decreased expression of target genes in tumor samples compared with *** these DMCs,we developed a GCA-specific 4-marker panel (cg27284428,cg11798358,cg07880787,and cg00585116) with an area under the receiver operating characteristic curve (AUC) of 0.917,effectively distinguishing between cardia HGD/GCA patients and cardia LGD/normal ***,an ESCC-specific 3-marker panel (cg14633892,cg04415798,and cg00585116)achieved an AUC of 0.865 in distinguishing esophageal HGD/ESCC ***,integrating cg00585116,age,and alcohol consumption yielded a tumor-shared logistic model with good discrimination for two cancer/HGD (AUC,0.767;95%confidence interval,0.720–0.813).The mean AUC of the model after 5-fold cross-validation was *** summary,our study identifies novel DNA methylation markers capable of accurately distinguishing

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丝胶生物吸附剂选择性去除废水中染料的评估(英文)

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Chinese Journal of Chemical Engineering 2012年第3期20卷 426-432页

作者： chen xinqing LAM Koon Fung MAK Shuk Fong CHING Wai Kwong NG Tsz Nok YEUNG King Lun Department of Chemical and Biomolecular Engineering Division of Environment the Hong Kong University of Science and TechnologyHong KongChina

The silk sericin is the main residue in silk production and it is found to be a low cost and efficient *** this study,sericin was characterized with various techniques including SEM(scanning electron microscope),XRD,N2 physisorption,FTIR(Fourier transformed infrared spectroscopy) and XPS(X-ray photoelectron spectroscopy).The nitrogen content of sericin was ca.8.5 mmol·g-1 according to elemental *** adsorp-tion by sericin biosorbent was investigated with the acid yellow(AY),methylene blue(MB) and copper(II) phthalocyanine-3,4'4″4'″-tetrasulfonic acid(CuPc) dyes from *** displayed large capacity for AY and CuPc adsorption with adsorption capacities of respectively 3.1 and 0.35 mmol·g-1,but it did not adsorbed methylene blue *** selectivity is due to the basicity of amide groups in sericin biosorbents.

关键词：生物吸附剂丝胶蛋白染料废水傅里叶变换红外光谱 X射线光电子能谱扫描电子显微镜评估吸附能力

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技术、资本和权力对临床决策的影响机制探究

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医学与哲学 2024年第6期45卷 7-10,18页

作者：仲凤行陈安天张新庆中国中医科学院医学实验中心北京100005 中国医学科学院阜外医院国家心血管病中心北京100037 北京协和医学院人文和社会科学学院北京100730

技术、资本、权力给医学决策带来了双重效应。技术至上观念的行动会忽视人文关怀,资本的逐利性诱发过度医疗,权力的误用、滥用也会削弱临床决策质量。三者间的良性互动能够推进技术的研发和临床应用,提升临床决策的方向和质量。用制度... 详细信息

技术、资本、权力给医学决策带来了双重效应。技术至上观念的行动会忽视人文关怀,资本的逐利性诱发过度医疗,权力的误用、滥用也会削弱临床决策质量。三者间的良性互动能够推进技术的研发和临床应用,提升临床决策的方向和质量。用制度、美德消解资本任性、技术至上与权力滥用;通过构筑道德防线提升认知强自律,健全制度强他律,促成人本临床决策的实现。三条道德防线彼此关联,相互作用,最终实现驾驭资本、技术、权力,促成兼顾道德规范和充分个性化临床决策的顺利实现。

关键词：技术资本权力临床伦理

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