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CdS纳米棒/含Ni多钨氧酸盐光催化苯硫酚氧化偶联耦合制氢
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作者 任梦真 刘天府 +5 位作者 董媛媛 李正 杨嘉新 刁振恒 吕红金 杨国昱 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第6期312-321,共10页
二硫化物是生物和药学有机分子合成的重要中间体,并已广泛用于蛋白质功能化、药物传递系统和智能材料等领域.然而,在传统的合成策略中,常使用昂贵或者有毒的有机氧化剂,这不仅增加了合成成本并造成环境污染,而且合成过程中容易出现选择... 二硫化物是生物和药学有机分子合成的重要中间体,并已广泛用于蛋白质功能化、药物传递系统和智能材料等领域.然而,在传统的合成策略中,常使用昂贵或者有毒的有机氧化剂,这不仅增加了合成成本并造成环境污染,而且合成过程中容易出现选择性差、过度氧化等问题.光催化硫醇/硫酚氧化偶联生成二硫化物是一种环境友好的生产路线,但存在催化活性低以及光生载流子不完全利用等问题.因此,开发一种环境友好、成本低廉以及光生电子-空穴高效利用的光催化体系,用于催化硫醇/硫酚氧化偶联并耦合制氢,具有重要的基础研究意义和潜在应用价值.本文构筑了一种Ni_(4)P_(2)/CdS耦合光催化体系,该耦合体系由硫化镉纳米棒(CdS NRs)和含镍的多钨酸盐(Na_(6)K_(4)[Ni_(4)(H_(2)O)_(2)(PW_(9)O_(34))_(2)]·32H_(2)O,简称Ni_(4)P_(2))组成.在光催化氧化4-甲氧基苯硫酚(4-MTP)偶联生成二硫化物的同时,能够释放出氢气,并展现出较好的反应活性.反应4 h后,4-MTP的转化率高达98.39%,二硫化物的选择性为95.0%,二硫化物的收率达24.45μmol,H_(2)的收率为25.96μmol.该耦合体系还展现出了良好的普适性,以–NH_(2),–C_(2)H_(5),–CH_(3),–Cl和–F作为取代基,取代4-甲氧基苯硫酚中的甲氧基并作为底物进行反应,生成相应二硫化物的选择性均超过97%.透射电子显微镜(TEM)和高分辨率X射线光电子能谱(XPS)结果表明,CdS NRs在反应前后形貌保持不变,稳定性较好.X射线光电子能谱表征发现,反应后的CdS NRs表面没有检测到Ni元素的XPS信号峰,说明Ni_(4)P_(2)催化剂附着在CdS NRs的表面,并且能够在反应过程中保持分子的完整性.红外光谱进一步证实了析氢催化剂Ni_(4)P_(2)催化剂的稳定性.此外,荧光光谱、寿命衰减以及光电流测试等系列实验结果表明,CdS NRs与Ni_(4)P_(2)之间存在协同作用,Ni_(4)P_(2)的存在明显地促进光生电子-空穴对的分离和迁移.通过一系列对比实验,证实了可见光在反应中的必要性,以及电子和空穴在反应过程中的关键作用.通过顺磁共振(EPR)检测到了•SC_(6)H_(4)(OCH_(3))自由基中间体的存在,证实了偶联产物是通过硫中心自由基生成的.EPR测试还显示,加入Ni_(4)P_(2)催化剂后,自由基中间体信号增强,进一步验证了Ni_(4)P_(2)可以促进光生电子-空穴对的分离和迁移.基于上述实验和表征结果,我们提出了以下反应机理:在可见光的照射下,4-MTP被空穴氧化脱氢,生成•SC_(6)H_(4)(OCH_(3))自由基.随后,两个•SC_(6)H_(4)(OCH_(3))自由基偶联生成二硫化物.同时,Ni_(4)P_(2)捕获活性氢物种,促进了氢气的析出,最终实现了4-MTP氧化偶联生成二硫化物并耦合制氢的光催化循环.综上所述,本研究成功构筑了Ni_(4)P_(2)/CdS光催化反应体系,实现了有机底物4-MTP的氧化增值与催化制氢的耦合反应.该体系不仅显示出良好的催化活性,还具备较好的稳定性和普适性,为太阳能驱动下的化学转化提供了有效的途径,并为太阳能的可持续利用提供了参考. 展开更多
关键词 脱氢偶联 多金属氧酸盐 硫化镉 析氢 光催化
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基于全直径岩心二维核磁共振测量的低阻油层评价方法
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作者 白莎 石玉江 +5 位作者 李思 淑华 李新 赵建斌 刘鹏 董元媛 《国外测井技术》 2024年第2期32-39,2,共9页
河套盆地临河组砂岩储层中油层类型多样,低阻油层普遍存在,油层识别难度大。本文通过室内柱塞样岩心离心状态、饱和状态测量核磁T谱,结合测井资料及油水分析,明确河套盆地临河组砂岩低阻油层主要成因;根据移动式全直径岩心核磁共振Ti一T... 河套盆地临河组砂岩储层中油层类型多样,低阻油层普遍存在,油层识别难度大。本文通过室内柱塞样岩心离心状态、饱和状态测量核磁T谱,结合测井资料及油水分析,明确河套盆地临河组砂岩低阻油层主要成因;根据移动式全直径岩心核磁共振Ti一T,现场测量数据,分析不同流体组分T1-T,图谱特征,明确典型油层、低阻油层、水层孔隙流体组分分布特征规律,确定二维核磁TI-T,图谱中油水信号的分布特征;同时,根据低阻油信号在二维核磁Ti-T,图谱中的分布特征建立含油饱和度计算模型,实现低阻油层含油性定量评价;形成了基于全直径岩心二维核磁共振测量的低阻油层评价方法,该方法在河套盆地规模化应用,效果显著。 展开更多
关键词 全直径岩心 二维核磁共振 低阻油层 流体识别 含油性定量评价
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A Low-Complexity Signal Detection Utilizing AOR Iterative Method for Massive MIMO Systems 被引量:2
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作者 Zhenyu Zhang Xiaoming Dai +2 位作者 yuanyuan dong Xiyuan Wang Tong Liu 《China Communications》 SCIE CSCD 2017年第11期269-278,共10页
Massive multiple-input multiple-output(MIMO) system is capable of substantially improving the spectral efficiency as well as the capacity of wireless networks relying on equipping a large number of antenna elements at... Massive multiple-input multiple-output(MIMO) system is capable of substantially improving the spectral efficiency as well as the capacity of wireless networks relying on equipping a large number of antenna elements at the base stations. However, the excessively high computational complexity of the signal detection in massive MIMO systems imposes a significant challenge for practical hardware implementations. In this paper, we propose a novel minimum mean square error(MMSE) signal detection using the accelerated overrelaxation(AOR) iterative method without complicated matrix inversion, which is capable of reducing the overall complexity of the classical MMSE algorithm by an order of magnitude. Simulation results show that the proposed AOR-based method can approach the conventional MMSE signal detection with significant complexity reduction. 展开更多
关键词 massive multiple-input multiple-output(MIMO) accelerated overrelaxation(AOR) iterative method minimum mean square error(MMSE) convergence complexity
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Effects of Photosynthetic Bacteria-enhanced Biological Floc Replacement Diets on Tilapia Growth,Water Environment and Water Microbial Diversity
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作者 yuanyuan dong Limin FAN +4 位作者 Liping QIU Dandan LI Lu QIN Xinxu dong Jiazhang CHEN 《Agricultural Biotechnology》 CAS 2020年第5期73-79,82,共8页
With Oreochromis niloticus as the object of study,glucose was added as a carbon source to promote the formation of the biological flocs for replacing part of the feed,and three gradients were set up,namely Group A(all... With Oreochromis niloticus as the object of study,glucose was added as a carbon source to promote the formation of the biological flocs for replacing part of the feed,and three gradients were set up,namely Group A(all feed),Group B(replacement of 10%feed)and Group C(replacement of 20%feed),so as to explore the effects of photosynthetic bacteria-enhanced biological flocs on tilapia growth and water environment conditions.Meanwhile,the Biolog-ECO technology was applied to study the changes of microbial carbon metabolism diversity in aquaculture water.The results showed that the utilization of microbial carbon sources under different feed replacement gradients increased with the extension of the culture time.The overall performance was in order of 10%replacement>all feed>20%feed replacement.A suitable replacement rate could not only enhance the overall utilization of carbon sources by water microorganisms,but also save culture costs.The principal component analysis showed that the carbon source metabolism of the water microbial communities under different feed replacement gradients was significantly different.Specifically,polysaccharides,esters and amino acids were the preferred carbon sources of water microbes,while the utilization of amines and acids was low. 展开更多
关键词 Photosynthetic bacteria Biological floc Bait substitute Microbial community TILAPIA
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Investigation into the roles of interfacial H_(2)O structure in catalytic oxidation of HCHO and CO over CuMnO_(2) catalysts
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作者 Chunyan Ma Jushuang Pan +4 位作者 Cheng Chen yuanyuan dong Feng Yao Fengbang Wang Maoyong Song 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2024年第3期310-320,共11页
The rapid deactivation of cost-effective MnO_(2)-based catalysts in humid air limits their application in practice,and the identification of the role of water in an oxidation process is significant for developing wate... The rapid deactivation of cost-effective MnO_(2)-based catalysts in humid air limits their application in practice,and the identification of the role of water in an oxidation process is significant for developing water-resistant MnO_(2)-based catalysts.Here,CuMnO_(2)showed a20.3%HCHO conversion in 10 hr at room temperature in humid air with relative humidity of 40%,but deactivated in 3 hr in dry air.The excellent activity and stability of HCHO oxidation in humid air were attributed to the positive effect of H_(2)O on HCHO oxidation to the H_(2)O-HOCH_(2)OH supermolecule assemblies via hydrogen bonds formed on CuMnO_(2).H_(2)O-HOCH_(2)OH supermolecule assemblies tend to be oxidized to carbonate,which is further oxidized to CO_(2).Furthermore,CuMnO_(2)exhibited a much poorer activity of CO oxidation in humid air,but the CO conversion was still 100%in 10 hr in dry air.H_(2)O showed a competitive adsorption effect to CO on CuMnO_(2).CuMnO_(2)could be applied in HCHO elimination in humid air and CO elimination in dry air. 展开更多
关键词 H_(2)O-HOCH_(2)OH supermolecule HCHO oxidation Humid air CuMnO_(2) CO oxidation
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Prevalence and factors associated with pentavalent vaccination:a cross-sectional study in Southern China 被引量:1
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作者 Jianing Xu Yujie Cui +5 位作者 Chuican Huang yuanyuan dong Yunting Zhang Lichun Fan Guohong Li Fan Jiang 《Infectious Diseases of Poverty》 SCIE CAS CSCD 2023年第5期32-44,共13页
Background Immunization is one of the most far-reaching and cost-effective strategies for promoting good health and saving lives.A complex immunization schedule,however,may be burdensome to parents and lead to reduced... Background Immunization is one of the most far-reaching and cost-effective strategies for promoting good health and saving lives.A complex immunization schedule,however,may be burdensome to parents and lead to reduced vaccine compliance and completion.Thus,it is critical to develop combination vaccines to reduce the number of injections and simplify the immunization schedule.This study aimed to investigate the current status of the pentavalent diphtheria-tetanus-acellular pertussis inactivated poliomyelitis andHaemophilus influenzae type B conjugate(DTaP-IPV/Hib)vaccination in Southern China as well as explore the factors in the general population associated with uptake and the differences between urban and rural populations.Methods A cross-sectional study was conducted with recently enrolled kindergarten students in Hainan Province between December 2022 and January 2023.The study employed a stratified multistage cluster random sampling method.Information regarding the demographic characteristics and factors that influence decisions were collected from the caregivers of children via an online questionnaire.Multivariate logistic regression was used to determine the factors associated with the status of DTap-IPV/Hib vaccinations.Results Of the 4818 valid responses,95.3%of children were aged 3-4 years,and 2856(59.3%)held ruralhukou.Coverage rates of the DTaP-IPV/Hib vaccine,from 1 to 4 doses,were 24.4%,20.7%,18.5%,and 16.0%,respectively.Caregivers who are concerned about vaccine efficacy[adjusted odds ratio(aOR)=1.53,95%confidence interval(CI):1.30-1.79],the manufacturer(aOR=2.05,95%CI:1.69-2.49),and a simple immunization schedule(aOR=1.26,95%CI:1.04-1.54)are factors associated with a higher likelihood of vaccinating children against DTaP-IPV/Hib.In addition,caregivers in urban areas showed more concern about the vaccine price(P=0.010)and immunization schedule(P=0.022)in regard to vaccinating children.Conclusions The DTaP-IPV/Hib vaccine coverage rate in Hainan Province remains low.Factors such as lower socioeconomic status,cultural beliefs,concerns about vaccine safety,and cost may hinder caregivers from vaccinating their children.Further measures,such as health education campaigns to raise knowledge and awareness,and encouragement of domestic vaccine innovation,which would reduce out-of-pocket costs,could be implemented to improve the coverage of DTap-IPV/Hib vaccination. 展开更多
关键词 Early child development Pentavalent Diphtheria-tetanus-acellular pertussis inactivated poliomyelitis and Haemophilus influenzae type B vaccine Vaccination coverage Influencing factor China
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Heterojunction-Type Photocatalytic System Based on Inorganic Halide Perovskite CsPbBr3 被引量:4
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作者 Enbo Zhu Yizhou Zhao +4 位作者 Yi Dai Qiuhe Wang yuanyuan dong Qi Chen Yujing Li 《Chinese Journal of Chemistry》 SCIE CAS CSCD 2020年第12期1718-1722,共5页
of main observation and conclusion The heterojunction-type structure has shown significant merits in tuning the optical properties and carrier physics.Inspired by the excellent absorption capability of halide perovski... of main observation and conclusion The heterojunction-type structure has shown significant merits in tuning the optical properties and carrier physics.Inspired by the excellent absorption capability of halide perovskite materials for visible light,a series of CsPbBr3/TiO2 heterojunction-type photocatalysts with various all-inorganic-perovskite/TiO2 ratios are successfully fabricated by the ligand-assisted reprecipitation(LARP)method.The heterojunction structure extends the light absorption of TiO2 with good chemical and structural stability.A Pb-O interaction at the CsPbBr3/TiO2 interface is observed by the XPS and confirmed by the TRPL showing improved interface carrier transport and stability.The heterojunction-type catalyst shows drastically enhanced photocatalytic activity towards the direct oxidation of toluene with 02 molecule,as an important reaction for organic chemical synthesis.The optimized sample shows an activity of 2356μmol·g^-1·h^-1 at 75℃,4 times of that of the naked CsPbBr3 nanocrystals,and 3 times of that of the bare TiO2.Based on the investigation with trapping agents,a reaction mechanism is hence proposed suggesting that the photo-generated hole may be involved in the rate-limiting step.This work demonstrates the potential of inorganic halide perovskite-based heterojunction structure for photocatalytic applications. 展开更多
关键词 stability. synthesis. PEROVSKITE
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Influence of crystalline phase of Li-AI-O oxides on the activity of Wacker-type catalysts in dimethyl carbonate synthesis 被引量:3
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作者 Yadong GE yuanyuan dong +3 位作者 Shengping WANG Yujun ZHAO Jing LV Xinbin MA 《Frontiers of Chemical Science and Engineering》 CAS CSCD 2012年第4期415-422,共8页
The catalysts supported on LiA1508 (spinel) for vapor phase synthesis of dimethyl carbonate (DMC) from methyl nitrite (MN) have been studied. Their catalytic activities on supports prepared by different methods ... The catalysts supported on LiA1508 (spinel) for vapor phase synthesis of dimethyl carbonate (DMC) from methyl nitrite (MN) have been studied. Their catalytic activities on supports prepared by different methods were evaluated in a continuous reactor. The samples were characterized by powder X-ray diffraction, N2 adsorption-desorption isotherms, fourier transform infrared spectroscopy and temperature-programmed reduction of H2. Li/A1 molar ratio and calcination temperature greatly influence the structure of crystalline phase of Li-AI-O oxides. Desirable LiAIsO8 (spinel) was formed at 800℃, while LiA1508 (primitive cube) formed at 900℃ is undesirable for the reaction. A high Li/A1 molar ratio, which was related with LiA102, also slowed the reaction rate. The electron transfer ability and the interaction with active component are the important properties of the spinel-based supports. The CuC12-PdC12/LiAIsO8 (spinel) with better electron transfer ability and low Pd2+ reduction temperature exhibited a better catalytic ability. 展开更多
关键词 Wacker-type catalyst dimethyl carbonate methyl nitrite SPINEL
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CdTe/CdSe-sensitized photocathode coupling with Ni-substituted polyoxometalate catalyst for photoelectrochemical generation of hydrogen
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作者 Junhao Zhang Mo Zhang +4 位作者 yuanyuan dong Congcong Bai Yeqin Feng Le Jiao Hongjin Lv 《Nano Research》 SCIE EI CSCD 2022年第2期1347-1354,共8页
In terms of photoelectrochemical(PEC)hydrogen evolution,substantial challenge still remains regarding the controllable fabrication of quantum dots(QDs)-sensitized photocathodes with enhanced visible-light absorption,e... In terms of photoelectrochemical(PEC)hydrogen evolution,substantial challenge still remains regarding the controllable fabrication of quantum dots(QDs)-sensitized photocathodes with enhanced visible-light absorption,efficient charge carrier separation,and directional migration at the electrode interface.In this work,the CdTe/CdSe QDs-sensitized photocathodes were delicately constructed on p-type NiO-coated indium tin oxide(ITO)electrodes by spin-coating approach.The resulting co-sensitized photocathode exhibits a favorable pseudo-Type Ⅱ energetic band alignment that combines the advantages of strong light absorption of constituent QDs as well as the effective and oriented charge separation and migration.Upon green LED light illumination,the photogenerated electrons could be effectively transferred to a tetra-nickel-substituted polyoxometalate catalyst for hydrogen production while photogenerated holes will be scavenged at the NiO/ITO electrode.Under minimally optimized conditions,the pseudo-Type Ⅱ CdTe/CdSe-sensrtized photocathode yields a photcx:urrent density of over 100 pA/cm^(2) and a Faradaic efficiency of〜100%,which is among one of the most efficient QDs-based photocathode systems coupling with Ni-substituted polyoxometalate catalyst for photoelectrochemical hydrogen generation. 展开更多
关键词 POLYOXOMETALATES quantum dots-sensitized photocathode favorable energetic gradient photoelectrochemical water splitting hydrogen generation
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