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协同光电及热效应实现铜光阴极上等离激元催化高效硝酸根还原反应

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Chinese Journal of Catalysis 2024年第7期62卷 219-230页

作者：陈振霖薛静武磊党昆籍宏伟陈春城章宇超赵进才中国科学院化学研究所光化学重点实验室北京分子科学国家研究中心北京100190 中国科学院大学北京100049

近年来,电催化硝酸根还原反应(NO_(3)RR)已经成为水处理和合成氨领域的研究热点.相比于传统的电催化剂,等离激元辅助的电催化反应通过将太阳能和电化学偏压同时施加到金属纳米结构上,在实现高效太阳能到化学能转化领域展现出了巨大潜力... 详细信息

近年来,电催化硝酸根还原反应(NO_(3)RR)已经成为水处理和合成氨领域的研究热点.相比于传统的电催化剂,等离激元辅助的电催化反应通过将太阳能和电化学偏压同时施加到金属纳米结构上,在实现高效太阳能到化学能转化领域展现出了巨大潜力.然而,目前有关等离激元辅助NO_(3)RR的文献报道较少,已有的研究主要集中于利用金(Au)纳米结构的等离激元效应辅助增强NO_(3)RR.但Au对NO_(3)RR的本征电催化活性很差,这导致在等离激元辅助NO_(3)RR领域,氨的产率和法拉第效率难以令人满意.此外,对于等离激元辅助NO_(3)RR的机理研究不深入,例如如何区分等离激元产生的光电效应和光热效应对NO_(3)RR的影响,以及等离激元激发的金属纳米结构是如何影响NO_(3)RR过程等问题都尚未解决.因此,有必要采取有效的策略来深入探究等离激元辅助NO_(3)RR的内在机制,从而进一步提高其催化性能.铜(Cu)作为一种高效的硝酸根还原电催化剂,同时是一种典型的具有等离激元效应的金属材料.然而,目前关于利用Cu的等离激元效应辅助增强NO_(3)RR的报道很少.本文报道了利用Cu纳米线(CuNWs)的等离激元效应辅助增强NO_(3)RR性能.在等离激元激发条件下,CuNWs展现出较好的NO_(3)RR催化性能.在协同的光电和热效应的作用下,与暗态常温条件相比,催化性能提升了近2倍.经过400次循环伏安测试,CuNWs光阴极的电流密度仅下降到初始值的88%,而在黑暗条件下,CuNWs光阴极催化NO_(3)RR的电流密度则下降了43%.这表明光照同时显著提升了CuNWs催化NO_(3)RR的稳定性.产物分析结果表明,在-0.2到-0.4 V(相对于可逆氢电极)的宽电势范围内,CuNWs光阴极实现了接近100%的氨法拉第效率,并取得了较高的氨产率,超过了之前大多数报道的等离激元辅助Au催化剂的NO_(3)RR性能.通过活化能实验、微分电流实验以及升温实验,区分了等离激元激发产生的光电效应以及光热效应对NO_(3)RR的影响.通过原位拉曼光谱、在线差分电化学质谱以及原位电化学红外光谱技术,确定了CuNWs光阴极NO_(3)RR过程中的活性相及反应中间体.密度泛函理论计算结果表明,氨的脱附是NO_(3)RR的决速步.光生电子可以通过电子跃迁激发脱附机制促进氨的脱附从而抑制了氨在Cu表面的累积,弱化了氨对CuNWs光阴极的毒化作用.同时,光热效应也显著提升了NO_(3)RR的反应速率.因此,等离激元激发产生的光电和光热效应协同促进了NO_(3)RR性能,提高了CuNWs光阴极的活性与稳定性.将该策略拓展到其它Cu纳米材料上,同样展现出较好的等离激元促进效果.综上,本文提出了利用Cu的等离激元效应辅助增强电催化NO_(3)RR性能的策略,并验证了该策略在其它Cu纳米材料上的适用性.深入的机理研究揭示了同时耦合太阳能、电能以及热能对进一步提升NO_(3)RR性能的巨大潜力.

关键词：铜光阴极等离激元辅助电催化剂光电效应光热效应硝酸根还原反应

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固相自养-异养反硝化脱氮同步去除微污染物

中国环境科学 2024年第3期44卷 1265-1277页

作者：曹阳刘彩虹陈子惟刘乾亮何强重庆大学环境与生态学院三峡库区生态环境教育部重点实验室重庆400044 哈尔滨理工大学化学与环境工程学院黑龙江哈尔滨150040

针对固相反硝化体系,以聚己内酯复合花生壳(PCL/PS)的固体碳源为基底,耦合以S和Fe O主导的自养反硝化,构建新型多功能碳源,考察其对典型微污染物(Cr(Ⅵ)、ClO_(4)^(-)、BPA、NPX)与硝酸盐的同步降解效能,探究自养异养共存的反硝化体系... 详细信息

针对固相反硝化体系,以聚己内酯复合花生壳(PCL/PS)的固体碳源为基底,耦合以S和Fe O主导的自养反硝化,构建新型多功能碳源,考察其对典型微污染物(Cr(Ⅵ)、ClO_(4)^(-)、BPA、NPX)与硝酸盐的同步降解效能,探究自养异养共存的反硝化体系内微生物群落特征及微观作用机制.结果表明,PCL/PS异养反硝化体系具有更好的反硝化脱氮和同步去除Cr(Ⅵ)、BPA性能,对NO_(3)^(-)-N、Cr(Ⅵ)的去除率分别为94%、92%,对NO_(3)^(-)-N、BPA的去除率均可达99%以上;PCL/PS同时耦合Fe O和S的体系反硝化脱氮同步去除ClO_(4)^(-)、NPX性能良好且稳定,在反硝化率均维持90%的基础上,对NO_(3)^(-)-N、ClO_(4)^(-)的去除率分别达90%、96%,对NO_(3)^(-)-N、NPX的去除率分别达96%、99%;固体碳源种类不同,其对微污染物降解去除的选择性也不同.测序结果表明,耦合自养反硝化后,反应体系内微生物多样性和丰富度均有所提高,Clostridium_sensu_strito、Lactococcus和Prevotella是4个固体碳源体系中影响污染物去除性能的主要优势菌属.

关键词：固体碳源自养反硝化微污染物同步去除

Numerical Analysis of the Influence of the Impinging Distance on the Scouring Efficiency of Submerged Jets

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Fluid Dynamics & Materials Processing 2024年第2期20卷 429-445页

作者： Hao chen Xianbin Teng Zhibin Zhang Faxin Zhu Jie Wang Zhaohao Zhang School of Naval Architecture and Maritime Zhejiang Ocean UniversityZhoushan316022China School of Marine Engineering Guangzhou Maritime UniversityGuangzhou510725China

Water jet technology is widely used in submerged buried pipes as a non-traditional trenching process,often invol-ving a complex sediment *** important adjustable and inﬂuential engineering variable in this technol-ogy is represented by the impinging *** this study,the FLOW-3D software was used to simulate the jet scouring of sand beds in a submerged *** particular,four sets of experimental conditions were con-sidered to discern the relationship between the maximum scour depth and mass and the impinging *** shown by the results,a critical impinging distance h0 exists by which the static scour depth can be maximized;the scour mass ratio between dynamic and static conditions decreases as the impinging distance ***,the proﬁle contours are similar when the erosion parameter Ec is in the range 0.35

关键词： Submerged jet impinging distance numerical simulation scour depth scour proﬁle

Noise-Tolerant ZNN-Based Data-Driven Iterative Learning Control for Discrete Nonaffine Nonlinear MIMO Repetitive Systems

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Hexacyanoferrate as the Electrochemical Probe for 2-Mercaptobenzothiazole Modified Gold Electrode

自动化学报（英文版） 2024年第2期

作者： Yunfeng Hu Chong Zhang Bo Wang jing Zhao Xun Gong Jinwu Gao hong chen

来源：博看期刊评论

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博看期刊

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Chemical Research in Chinese Universities 1999年第2期15卷 30-35页

作者： XU jing-juan FANG Hui-qun chen hong-yuan Department of Chemistry the State Key Laboratory of Coordination ChemistryNanjing UniversityNanjing210093

A gold electrode covered with selfassembled monolayers of 2mercaptobenzothiazole(Au/MBT)has been developed and its electrochemical characteristics have been investigated in *** hexacyanoferrate as the electrochemical probe for studying the characteristics of the MBT monolayer film,the results,obtained by *** spectroscopy technique,show that the electron transfer of hexacyanoferrate()on Au|MBT in higher pH media was more difficult than that obtained in H2SO4 medium or on a bare gold *** electrochemical reversibility of Fe(CN)3-6/Fe(CN)4-6 changed with pH of the solution due to the proton and deproton states of N atom of *** relationship between the coverage of MBT on Au surface or pH and the apparent heterogeneous rate constant was derived and *** double layer capacitance of Au|MBT is(76455)F/*** characteristic frequency was dependent on the pH of the solution.

关键词： Mercaptobenzothiazole Selfassembly Resistance Capacitance

Optimization design and experiment of the variable differential gear train planting mechanism

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International Journal of Agricultural and Biological Engineering 2024年第2期17卷 85-93页

作者： Xiong Zhao Ziwei Liu Yuanwu Jia Xingxiao Ma Pengfei Zhang Jianneng chen School of Mechanical Engineering Zhejiang Sci-Tech UniversityHangzhou 310018China Xi’an International University Engineering College Xi’an 710077China Hangzhou Vocational&Technical College Hangzhou 310018China

In order to improve the adaptability of the planting mechanism for different plant spacings,a variable differential gear train planting mechanism based on precise pose and trajectory control was proposed by combining the open chain 2R rod group and the variable differential gear *** to the pose requirements of receiving seedling point,transporting seedling point and planting point,three precise pose points of constrained planting trajectory were *** the three-position motion generation structural synthesis method,combined with computer-aided optimization design software,a set of mechanism parameters that meet the planting requirements were *** on the optimized mechanism parameters,by only changing the coordinates of two trajectory shape control points,three planting trajectories with key point position information adapted to 300 mm,400 mm and 500 mm plant spacing were obtained by interpolation,and three pairs of total transmission ratio of three groups of variable differential gear trains were *** distributing the total transmission ratio of the mechanism,the fixed axis gear train and the differential gear train are *** fixed axis gear train included a pair of non-circular gear pairs and a pair of positive gear pairs,which were convenient for disassembly and *** former drives the sun gear at variable speed,and the latter drives the planet carrier at uniform *** on this structure,the transmission ratio of the positive gear pair is-1,and the transmission ratio of the differential gear train is *** sub-transmission ratio of the single-stage non-circular gear pair was calculated and the pitch curves of three pairs of noncircular gears were *** pairs of non-circular gear pairs with different transmission ratios were replaced in turn and three sets of planting mechanisms were modeled in three *** virtual prototype motion simulation was completed by ADAMS software,and the p

关键词： plant spacing planting mechanism variable differential gear train precise pose trajectory control parameter optimization

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子宫颈鳞状上皮内病变的影响因素分析

中国实用妇科与产科杂志 2024年第2期40卷 239-243页

作者：沈兰陈爱红钱爱萍浙江中医药大学滨江学院附属江南医院浙江杭州311201

目的探讨高危型人乳头瘤病毒(HR-HPV)感染、阴道微生态对子宫颈鳞状上皮内病变的影响。方法选取2019年1月至2023年1月浙江中医药大学滨江学院附属江南医院收治的CIN患者124例作为研究组,按子宫颈病变级别分成两组,子宫颈高级别鳞状上皮... 详细信息

目的探讨高危型人乳头瘤病毒(HR-HPV)感染、阴道微生态对子宫颈鳞状上皮内病变的影响。方法选取2019年1月至2023年1月浙江中医药大学滨江学院附属江南医院收治的CIN患者124例作为研究组,按子宫颈病变级别分成两组,子宫颈高级别鳞状上皮内病变(HSIL)组62例,子宫颈低级别鳞状上皮内病变(LSIL)组65例,选取同期入院进行常规体检(阴道分泌物微生态和人乳头瘤病毒基因分型检测)子宫颈正常的健康体检者107例作为对照组,比较3组的临床资料、阴道微生态情况和炎症细胞因子水平,利用logistic回归模型分析HR-HPV感染对阴道微生态的影响。结果3组之间HPV感染、细菌性阴道病(BV)、外阴阴道假丝酵母菌病(VVC)、肿瘤坏死因子-α(TNF-α)、白细胞介素(IL)-2、IL-4、干扰素-γ(IFN-γ)、首次性生活年龄小于20岁、初孕年龄<20岁、HPV感染、阴道微生态(BV、VVC)异常、菌群多样性异常对比差异有统计学意义(P<0.05)。将影响HSIL、LSIL发生的各单因素(P<0.05)再次纳入logistic回归分析,得出影响HSIL、LSIL的多因素指标。结果发现,HPV感染、阴道微生态(BV、VVC)异常是影响LSIL发生的独立危险因素(P<0.05);首次性生活年龄、HPV感染、菌群多样性异常、阴道微生态[BV、阴道毛滴虫病(TV)、VVC]、白细胞计数(WBC)是影响HSIL发生的独立危险因素(P<0.05)。结论HPV感染、炎性因子表达异常、阴道微生态异常是影响LSIL发生的危险因素。HPV感染、首次性生活年龄、菌群多样性异常、白细胞计数是导致HSIL发生的危险因素。

关键词：子宫颈上皮内瘤变高危型人乳头瘤病毒阴道微生态

异质结构CoCrFeNiW高熵合金的拉伸性能和强化行为

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Transactions of Nonferrous Metals Society of China 2024年第3期34卷 890-904页

作者：高雪峰陈峣任浩秦刚周启文陈瑞润郭景杰哈尔滨工业大学金属精密热加工国家重点实验室哈尔滨150001 沈阳工业大学材料科学与工程学院沈阳110870

采用真空电弧熔炼方法制备Co_(30)Cr_(30)(FeNi)_(40-x)W_(x)(x=0~8%(摩尔分数),分别简化为HWO~HW8)高熵合金。研究铸态和退火态合金的显微组织和拉伸性能。结果表明,HW2和HW4具有单一的FCC相。随着W含量和退火温度的增加,细小粒状μ相... 详细信息

采用真空电弧熔炼方法制备Co_(30)Cr_(30)(FeNi)_(40-x)W_(x)(x=0~8%(摩尔分数),分别简化为HWO~HW8)高熵合金。研究铸态和退火态合金的显微组织和拉伸性能。结果表明,HW2和HW4具有单一的FCC相。随着W含量和退火温度的增加,细小粒状μ相的面积分数增加且分散在FCC基体中。软FCC基体和硬μ相构成应变不相容的异质结构。随着W含量从0增加到8%(摩尔分数),屈服强度和抗拉强度分别从278和629 MPa提高到530和839 MPa,应变维持在33%。退火后的HW8表现出优异的屈服强度(810 MPa)和抗拉强度(1087 MPa)。屈服强度的提高归因于固溶、沉淀和背应力强化。异质结构中产生的背应力强化作用诱导高硬化行为,在提高抗拉强度和塑性方面发挥着主导作用。

关键词：高熵合金异质结构拉伸性能应变硬化强化机制

Crossroads:Pathogenic role and therapeutic targets of neutrophil extracellular traps in rheumatoid arthritis

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BIOCELL 2024年第1期48卷 9-19页

作者： YANG LI JIAN LIU YUEDI HU chenGZHI CONG YIMING chen QIAO ZHOU Department of Rheumatology The First Affiliated Hospital of Anhui University of Chinese MedicineHefei230031China First Clinical Medical School Anhui University of Chinese MedicineHefei230031China Institute of Rheumatology Anhui Academy of Chinese MedicineHefei230031China

Rheumatoid arthritis(RA)is a prevalent autoimmune disease whose main features include chronic synovial inflammation,bone destruction,and joint *** are often considered to be the first responders to inflammation and are a key presence in the inflammatory milieu of *** extracellular traps(NETs),a meshwork of DNA-histone complexes and proteins released by activated neutrophils,are widely involved in the pathophysiology of autoimmune diseases,especially RA,in addition to playing a key role in the neutrophil innate immune *** have been found to be an important source of citrullinated autoantigen antibodies and inflammatory factor release,which can activate RA synovial fibroblasts(FLS)and cause joint *** article reviews the role of NETs in the pathophysiology of RA,demonstrating the application of multiple molecules with various therapies,with a view to informing the discovery and development of novel biomarkers and therapeutic targets for RA.

关键词： Rheumatoid arthritis Neutrophil extracellular traps Review