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Iron Atom-Cluster Strategy Synthesis of Hierarchically Porous Fe-N-C Catalysts for Proton Exchange Membrane Fuel Cells
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作者 Wenhao Qiu Qing Han +1 位作者 xiaogang yu Zhonghua Xiang 《Transactions of Tianjin University》 EI CAS 2023年第6期453-461,共9页
Developing nonprecious metal-nitrogen-doped carbon(M-N-C)catalysts with high activity and stability is critical to their widespread use in fuel cells;however,these catalysts still face considerable challenges.Herein,a... Developing nonprecious metal-nitrogen-doped carbon(M-N-C)catalysts with high activity and stability is critical to their widespread use in fuel cells;however,these catalysts still face considerable challenges.Herein,a novel iron atom-cluster strategy for the synthesis of iron-based N-C catalyst comprising Fe nanoparticles(Fe NPs)surrounded by Fe-N_(x) sites is developed for oxygen reduction reactions in an acidic fuel cell.Iron oxide NPs were incorporated into zeolitic imidazolate framework-8(ZIF-8)-derived carbon materials and pyrolyzed at high temperatures using NaCl as a modifi er to produce Fe NPs and Fe-N_(x) composite active sites.The half-wave potential of the optimized Fe_(NP)/FeNC-NaCl material was substantially improved to 0.81 V.Furthermore,even after 15,000 cycles,the half-wave potential of the catalyst remained essentially unchanged.As a cathode catalyst for fuel cells,it realized a high peak power density of 436 mW/cm^(2)under a practical H_(2)-air atmosphere.Therefore,this study presents a new approach for designing and synthesizing electrocatalytic materials with high catalytic activity and stability. 展开更多
关键词 Oxygen reduction reaction Fuel cell Fe-N-doped carbon IRON ATOM CLUSTERS PYROLYSIS synthesis
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卟啉修饰的光阴极用于光电催化二氧化碳还原(英文) 被引量:3
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作者 董亚鹏 聂融 +4 位作者 王继贤 于晓刚 涂鹏程 陈加藏 景欢旺 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第8期1222-1230,共9页
将二氧化碳有效地转化为高附加值化学品是人类的梦想,尤其是通过光电催化实现该过程更加令人期待.本文报道了一种新的人工光合成体系,它是由金属卟啉配合物修饰的二氧化钛光电阴极以及羟基氧化铁和羟基氧化镍修饰的钒酸铋光电阳极构成,... 将二氧化碳有效地转化为高附加值化学品是人类的梦想,尤其是通过光电催化实现该过程更加令人期待.本文报道了一种新的人工光合成体系,它是由金属卟啉配合物修饰的二氧化钛光电阴极以及羟基氧化铁和羟基氧化镍修饰的钒酸铋光电阳极构成,电解液是0.1 M碳酸氢钠水溶液.该体系在有硅太阳电池供电和一个标准太阳下工作.在外加电压为-0.6V时,甲醇是光电池的唯一产物,同时放出氧气;生成甲醇的速率是55.5 μM h^–1 cm^–2.当外加电压大于-0.75 V时,光电催化电池有氢气生成.卟啉和金属卟啉按照文献合成并命名为Dx,即D1 (meso-tetra-p-carboxyphenylporphyrin), D2 (CoTCPP), D3 (NiTCPP),D4 (CuTCPP),和D5 (PdTCPP).制备电极时,首先将P25粉涂覆在FTO玻璃上,然后经胺丙基三乙基硅烷(APTES)修饰,再与Dx反应生成酰胺键,从而实现卟啉染料与TiO2半导体材料的共价键键合,制备的系列电极记为Dx@TiO2.对卟啉和金属卟啉进行了紫外吸收、发射光谱(PL)、核磁共振和电化学循环伏安测试等检测,以及简单的DFT计算.对制备的光电阴极进行了红外光谱、固体紫外和电化学交流阻抗测试,计算了电极的Mott-Schottky曲线,得到了电极材料的平带电位,对于n型半导体,一般认为是近似的导带电位(CB).所有电极的CB电位均高于-0.56 V,高于甲醇生成需要的电位-0.38 V.经过卟啉修饰的电极材料,其能带结构发生了根本变化,由TiO2锐钛矿的3.2 eV降低到了2.37-2.73 eV. SEM及其元素分布彩色图表明所需元素都均匀分布在电极表面.电化学线性伏安扫描图表明,在光照条件下电流的提升是能带修饰和降低的结果.最好的光电阴极在光电还原电池D3@TiO2|NaHCO3|BiVO4中,-0.6 V条件下,一个标准太阳光照射2 h,生成甲醇的光量子效率用500 nm光子估算为0.92%,达到了自然界植物光合作用效率的2倍.循环实验表明,光电阴极经过4次2 h照射后仍有约50%的催化效力,性能的减弱主要来自卟啉作为光敏剂的消耗.在这一新的光电催化二氧化碳还原系统中,由于卟啉修饰的TiO2半导体材料表面构筑了合适的3D结构空间、敏化剂和催化剂,形成了对天然植物细胞和Calvin循环的有效模拟,因而提高了人工光合成的效率.同位素标记实验(13CO2)证实了产物甲醇来自CO2气体.与文献报道的卟啉催化体系相比,本文新催化体系的主要产物是甲醇而不是CO,而且新催化体系的效率是文献报道的80-500倍. 展开更多
关键词 人工光合成 二氧化碳还原 光电催化 金属卟啉配合物 二氧化钛
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Logistics Regression Analysis between TCM Constitution Types of Patients with Hypertension,Insomnia and ABPM,PSQI 被引量:2
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作者 xiaogang yu Qingsheng WANG +2 位作者 Erdan XIN yujun LU Yingdong LI 《Medicinal Plant》 CAS 2022年第2期44-49,54,共7页
[Objectives]The research aimed to explore the distribution characteristics of TCM constitution types of patients with hypertension and insomnia,and study the clinical characteristics of patients with different constit... [Objectives]The research aimed to explore the distribution characteristics of TCM constitution types of patients with hypertension and insomnia,and study the clinical characteristics of patients with different constitutions,in order to provide new ideas for the treatment of patients with hypertension and insomnia.[Methods]Cross sectional observation method was used,and 420 patients with hypertension and insomnia were selected.Required information was collected,and the constitution type of traditional Chinese medicine was determined,and relevant data were recorded.SPSS and Logistic regression analysis method were used to explore the correlation between the distribution of TCM constitution types and gender,age,24 h-SBP,24 h-DBP,24 h-BPV,PSQI score,etc.[Results]Among 420 patients,the proportion of gentleness constitution was the most,and others in turn were Qi deficiency constitution>Yang deficiency constitution>phlegm dampness constitution>Qi stagnation constitution>Yin deficiency constitution>blood stasis constitution>damp heat constitution>special constitution.Among male patients,the proportion of gentleness constitution was the most.Among female patients,the proportion of Qi deficiency constitution was the most.In each constitution,the proportion of men and women was different,and the difference in gentleness constitution,Qi deficiency constitution and Yin deficiency constitution had statistical significance(P<0.05).The proportion of gentleness constitution for young and middle-aged patients was the most,while elderly patients with Qi deficiency constitution was the most.There was difference in the distribution of TCM constitution in different age groups,and the difference had statistical significance(P<0.05).Compared with the patients with gentleness constitution,the patients with Qi deficiency constitution,Yang deficiency constitution,Yin deficiency constitution,damp heat constitution,blood stasis constitution and Qi stagnation constitution had different differences in terms of age,24 h-SBP,24 h-DBP,24 h-BPV and PSQI score,and there was statistical significance(P<0.05).Except damp heat constitution,blood stasis constitution and special constitution,other constitutions had certain correlation with age,24 h-SBP,24 h-DBP,24 h-BPV and PSQI score.[Conclusions]TCM constitution types of patients with hypertension and insomnia were dominant by gentleness constitution,Qi deficiency constitution and Yang deficiency constitution.The distribution of TCM constitution in different gender and age groups was different,and different TCM constitution was related to ABPM and PSQI. 展开更多
关键词 Hypertension with insomnia Constitution of traditional Chinese medicine ABPM PSQI Logistics regression analysis
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Secondary reduction strategy synthesis of Pt-Co nanoparticle catalysts towards boosting the activity of proton exchange membrane fuel cells
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作者 Bolong Yang xiaogang yu +1 位作者 Jingkui Hou Zhonghua Xiang 《Particuology》 SCIE EI CAS CSCD 2023年第8期18-26,共9页
Based on the volcanic relationship between catalytic activity and key adsorption energies,Pt-Co alloy materials have been widely studied as cathode oxygen reduction reaction(ORR)catalysts in proton exchange membrane f... Based on the volcanic relationship between catalytic activity and key adsorption energies,Pt-Co alloy materials have been widely studied as cathode oxygen reduction reaction(ORR)catalysts in proton exchange membrane fuel cells(PEMFCs)due to their higher active surface area and adjustable D-band energy levels compared to Pt/C.However,how to balance the alloying degree and ORR performance of Pt-Co catalyst remains a great challenge.Herein,we first synthesized a well-dispersed Pt/Co/C precursor by using a mild dimethylamine borane(DMAB)as the reducing agent.The precursor was calcined at high temperature under H_(2)/Ar mixed gas by a secondary reduction strategy to obtain an ordered Pt_(3)Co intermetallic compound nanoparticle catalyst with a high degree of alloying.The optimization of elec-tronic structure due to Pt-Co alloying and the strong metal-carrier interaction ensure the high kinetic activity of the cell membrane electrode.Additionally,the high degree of graphitization increases the electrical conductivity during the reaction.As a result,the activity and stability of the catalyst were significantly improved,with a half-wave potential as high as 0.87 V,which decreased by only 20 mV after 10000 potential cycles.Single-cell tests further validate the high intrinsic activity of the ordered Pt_(3)Co catalyst with mass activity up to 0.67 A mg_(pt)^(-1),exceeding the United States Department of Energy(US DOE)standard(0.44 A mg_(pt)^(-1)),and a rated power of 5.93 W mg_(pt)^(-1). 展开更多
关键词 Ordered Pt3Co nanoparticle Low platinum catalyst Secondary reduction strategy Oxygen reduction reaction Proton exchange membrane fuel cells
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磷掺杂提升三氧化钨导带用于高效二氧化碳还原 被引量:1
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作者 于晓刚 魏艳 +2 位作者 陈云 王继贤 景欢旺 《科学通报》 EI CAS CSCD 北大核心 2021年第7期825-832,共8页
光电催化还原二氧化碳是一种环境友好的高效方法,可将过量排放的CO_(2)转化为燃料与化学品,减少温室效应并存储太阳能为化学能.本研究设计制备了新型磷掺杂的WO_(3)催化剂,并将其用于CO_(2)和水转化为碳基化学品.通过X射线粉末衍射(XRD)... 光电催化还原二氧化碳是一种环境友好的高效方法,可将过量排放的CO_(2)转化为燃料与化学品,减少温室效应并存储太阳能为化学能.本研究设计制备了新型磷掺杂的WO_(3)催化剂,并将其用于CO_(2)和水转化为碳基化学品.通过X射线粉末衍射(XRD)、X射线光电子能谱(XPS)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、顺磁共振(EPR)等证实了新型催化剂的成功制备;通过紫外可见(UV-vis)、线性扫描伏安曲线(LSV)、莫特-肖特基(Mott-Schottky)和电化学交流阻抗谱(EIS)表征了其光电性能.结果表明,随着P掺杂量的增加,其导带位置从WO_(3)的-0.13 V升高到30-P样品的-0.54 V,增强了其对CO_(2)的还原能力;所有样品X-P比纯WO_(3)有更高的活性,其中15-P电极还原CO_(2)的活性最高,其光电池的表观光量子效率为0.4%,与植物的光合作用相当,且导带位置越高越有利于甲酸和乙酸产物的生成,而相对较低的导带更有利于乙醇的生成.同时,氧空位对反应的正影响也通过设计H_(2)O_(2)猝灭实验进行了验证. 展开更多
关键词 半导体 三氧化钨 能带 掺杂 二氧化碳还原 光电催化
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