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A generalized formula for two-dimensional diffusion of CO in graphene nanoslits with different Pt loadings
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作者 Chenglong Qiu Yinbin Wang +5 位作者 yuejin li Xiang Sun Guilin Zhuang Zihao Yao Shengwei Deng Jianguo Wang 《Green Energy & Environment》 SCIE CSCD 2020年第3期322-332,共11页
Catalytic performance of supported metal catalysts not only depends on the reactivity of metal,but also the adsorption and diffusion properties of gas molecules which are usually affected by many factors,such as tempe... Catalytic performance of supported metal catalysts not only depends on the reactivity of metal,but also the adsorption and diffusion properties of gas molecules which are usually affected by many factors,such as temperature,pressure,properties of metal clusters and substrates,etc.To explore the impact of each of these macroscopic factors,we simulated the movement of CO molecules confined in graphene nanoslits with or without supported Pt nanoparticles.The results of molecular dynamics simulations show that the diffusion of gas molecules is accelerated with high temperature,low pressure or low surface-atom number of supported metals.Notably,the supported metal nanoparticles greatly affect the gas diffusion due to the adsorption of gas molecules.Furthermore,to bridge a quantitative relationship between microscopic simulation and macroscopic properties,a generalized formula is derived from the simulation data to calculate the diffusion coefficient.This work helps to advise the diffusion modulation of gas molecules via structural design of catalysts and regulation of reaction conditions. 展开更多
关键词 Gas diffusion Graphene nanoslits Supported Pt nanoparticles Molecular dynamics simulation
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Hydrothermally stable metal oxide-zeolite composite catalysts for low-temperature NO_(x) reduction with improved N_(2) selectivity
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作者 lijun Yan Shiqi Chen +5 位作者 Penglu Wang Xiangyu liu Lupeng Han Tingting Yan yuejin li Dengsong Zhang 《Chinese Chemical Letters》 SCIE CAS CSCD 2024年第6期515-523,共9页
Development of hydrothermally stable,low-temperature catalysts for controlling nitrogen oxides emissions from mobile sources remains an urgent challenge.We have prepared a metal oxide-zeolite composite catalyst by dep... Development of hydrothermally stable,low-temperature catalysts for controlling nitrogen oxides emissions from mobile sources remains an urgent challenge.We have prepared a metal oxide-zeolite composite catalyst by depositing Mn active species on a mixture support of CeO_(2)/Al_(2)O_(3) and ZSM-5.This composite catalyst is hydrothermally stable and shows improved low-temperature SCR activity and significantly reduced N_(2)O formation than the corresponding metal oxide catalyst.Comparing with a Cu-CHA catalyst,the composite catalyst has a faster response to NH_(3) injection and less NH_(3) slip.Our characterization results reveal that such an oxide-zeolite composite catalyst contains more acidic sites and Mn^(3+)species as a result of oxide-zeolite interaction,and this interaction leads to the generation of more NH_(4)^(+)species bound to the Br?nsted acid sites and more reactive NOxspecies absorbed on the Mn sites.Herein,we report our mechanistic understanding of the oxide-zeolite composite catalyst and its molecular pathway for improving the low-temperature activity and N_(2) selectivity for NH_(3)-SCR reaction.Practically,this work may provide an alternative methodology for low-temperature NO_(x) control from diesel vehicles. 展开更多
关键词 Selective catalytic reduction Mn-based catalysts Hydrothermal stability N_(2) selectivity
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部分氧化碳化硅提高钯催化氧还原反应性能 被引量:1
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作者 李晶 孙翔 +3 位作者 段永正 贾冬梅 李跃金 王建国 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第6期963-970,共8页
燃料电池具有能量转换效率高的优点,是能量转换与储存的高效器件之一.目前,燃料电池阴极氧还原反应(ORR)动力学缓慢,并且催化ORR大量使用铂碳(Pt/C)催化剂,由于Pt储量少,价格高,载体碳材料易发生碳蚀导致催化剂稳定性降低,限制了其进一... 燃料电池具有能量转换效率高的优点,是能量转换与储存的高效器件之一.目前,燃料电池阴极氧还原反应(ORR)动力学缓慢,并且催化ORR大量使用铂碳(Pt/C)催化剂,由于Pt储量少,价格高,载体碳材料易发生碳蚀导致催化剂稳定性降低,限制了其进一步商业化应用.钯(Pd)与Pt为同族元素,具有相似的电子结构和化学性质,其储量是Pt的50倍,同时,Pd具有良好的抗甲醇毒性和抗一氧化碳毒性,因此,被视为燃料电池中阴极Pt催化剂的潜在替代品.但商用Pd/C催化剂的ORR活性较Pt/C差,因此,大量的研究工作集中在提高Pd基ORR催化剂的活性方面:将Pd与具有3d轨道的金属形成合金或将Pd负载到不同的载体上.通过选择合适的载体影响Pd的电子结构,从而提高催化剂活性和稳定性,是一种较简单的、有利于规模化生产Pd基ORR催化剂的方法.碳化硅(SiC)具有良好的电化学稳定性、热稳定性、机械强度和较强的供电子能力,可被用作ORR的金属催化剂载体.然而,由于金属与SiC作用较弱,需要制备特殊形貌的SiC或将SiC表面改性;通常,这些SiC基载体的制备过程复杂并且成本高.而在有氧条件下制备、保存或使用SiC时,其表面不可避免地被氧化,这种在温和条件下生成的表面具有含氧官能团的SiC,由于制备过程简便,可以大规模生产,且与金属有强的相互作用,是一种很有前景的ORR的Pd基催化剂载体.对于用于替代Pt基催化剂的负载型Pd基ORR催化剂的开发和大规模制造来说,对载体表面改性的深入了解是一个重要并且具有挑战性的课题.目前尚未发现关于SiC表面的含氧基团对ORR性能影响的报道.因此,详细考察SiC载体上含氧基团在ORR中的作用对于理解、设计和开发具有优异ORR性能的SiC负载催化剂至关重要.本文采用沉积沉淀法在表面部分氧化的碳化硅(O-SiC)均匀负载了平均直径为5.2 nm的Pd纳米颗粒.与20 wt%商业Pt/C相比,制备的2.5 wt%Pd/O-SiC催化剂显示出较好的ORR活性(半波电位正向移动10 mV),较好的稳定性(10 h后,电流密度损失3.5%vs.34.9%),和较高的抗甲醇毒性.结构表征及密度泛函理论(DFT)计算结果表明,与Pd/C相比,Pd/O-SiC具有优异的ORR性能主要是由于O-SiC载体对Pd纳米颗粒具有电子调控作用,使Pd带负电.富电子Pd增强了ORR关键中间体OOH的吸附,降低了反应的吉布斯自由能,从而提高了ORR活性.另外,O-SiC载体对Pd纳米颗粒具有大的结合能和较好的SiC稳定性,增强了Pd/O-SiC催化剂的抗甲醇毒性及稳定性.DFT计算结果表明,SiC表面部分氧化后,仍保持对Pd的较高结合能,同时大幅增强了催化剂对中间体的吸附,降低了ORR关键电化学步骤吉布斯自由能,从而提高了氧还原性能.因此,本工作明确了SiC表面氧化的作用,同时提供了一种简易大规模制备高效负载型铂基替代ORR催化剂的策略. 展开更多
关键词 碳化硅 表面氧化 氧还原反应 密度泛函理论 电荷转移 富电钯
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Removal atrazine using two anion-exchange resins supported nanohydrous metal-oxide particle
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作者 Dongmei Jia Aimin li +2 位作者 Changhai li Guoxia liu yuejin li 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2017年第2期180-186,共7页
Hydrous iron oxide and hydrous aluminum oxide were loaded successfully onto a polymeric adsorbent(D301) to modify adsorbing materials(HIOD301 and HAOD301). The adsorptive equilibrium of atrazine was investigated in an... Hydrous iron oxide and hydrous aluminum oxide were loaded successfully onto a polymeric adsorbent(D301) to modify adsorbing materials(HIOD301 and HAOD301). The adsorptive equilibrium of atrazine was investigated in an aquatic environment using HIOD301 and HAOD301 under different experimental conditions. The results indicated that both HIOD301 and HAOD301 showed good adsorption capacities for atrazine at p H 4. The Langmuir and Freundlich isotherm equations were used to study the interactions between the adsorbate and adsorbent.The adsorption kinetics of atrazine at different concentrations was well described in terms of a pseudosecond-order equation in regard to the correlation coefficients and adsorption capacity. The removal percentages of atrazine for HIOD301 and HAOD301 were still more than 95% in the presence of sodium chloride. 展开更多
关键词 阴离子交换树脂 莠去津 氧化物粒子 金属 阿特拉津 二阶方程 水合氧化铝 水合氧化铁
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The prevalence of soil transmitted helminths and its infuential factors in Shandong Province, China: an analysis of surveillance data from 2016 to 2020 被引量:1
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作者 Yan Xu Yongbin Wang +5 位作者 Longjiang Wang Xiangli Kong Ge Yan yuejin li Cancan Bu Benguang Zhang 《Infectious Diseases of Poverty》 SCIE CAS CSCD 2023年第3期97-98,共2页
Background Soil-transmitted helminths(STHs)were previously endemic in Shandong Province,China.This study aimed to analyze the STHs prevalence trend and the natural,social,and human cognitive and behavioural factors in... Background Soil-transmitted helminths(STHs)were previously endemic in Shandong Province,China.This study aimed to analyze the STHs prevalence trend and the natural,social,and human cognitive and behavioural factors infuencing the discrepancies between high and low infection levels from 2016 to 2020 in Shandong Province in eastern China.Methods STHs surveillance data of Shandong Province from 2016 to 2020 were obtained from China Information Management System for Prevention and Control of Parasitic Diseases.STHs infections were detected by modifed Kato–Katz method.Comprehensive information on the natural and social factors,STHs-related knowledge and behaviours were collected through questionnaire surveys.Retrospective spatial scan analysis was performed using SaTScan v10.1 to evaluate any identifed spatial clusters of STHs infection for statistical signifcance and Bayes discriminant analysis was used to discriminate the high or low infection groups of the villages.Results In total,72,160 participants were involved in our survey from 2016 to 2020.The overall STHs prevalence rate was 1.13%,with the eastern region of Shandong Province having the highest rate(2.02%).The predominant species was T.trichiura,with the prevalence rate of 0.99%and the≥70-year age group possessed the highest rate of 2.21%.The STHs prevalence rate showed an annual linear downward trend from 2016 to 2020(χ_(trend)^(2) =127.600,P<0.001).Respondents aged≥60 years had the lowest awareness level of STHs-related prevention knowledge(all P<0.05),and were the most likely to adopt the practice of fertilizing with fresh stool(χ^(2)=28.354,P<0.001).Furthermore,the southern region demonstrated the highest temperature and rainfall level and the lowest GNP and annual net income per capita(all P<0.05).Conclusions There is a remarkable declining in STHs prevalence in Shandong Province from 2016 to 2020.However,the prevalence rates of STHs especially T.trichiura in the southern and eastern regions were still high,and the elderly were more susceptible to be infected with STHs owning to their low awareness level of STHS-related prevention knowledge and high adoption rate of dangerous production and living behaviours.Integrated approaches of health education,environment improvement and behaviour change should be strengthened to obtain a further reduction of STHs prevalence in China. 展开更多
关键词 Soil-transmitted helminths SURVEILLANCE PREVALENCE Influential factor Shandong Province China
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