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双层石墨烯层间限域CO氧化反应的密度泛函研究 被引量:1
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作者 崔树稳 李璐 +1 位作者 魏连甲 钱萍 《物理学报》 SCIE EI CAS CSCD 北大核心 2019年第21期280-287,共8页
利用密度泛函理论,研究了双层石墨烯层间一氧化碳(CO)与氧(O)的氧化反应,获得了双层石墨烯层间距与反应能垒的定量关系.计算结果表明反应初态、过渡态、末态体系总能以及反应能垒对层间距离变化敏感:随着层间距的逐渐缩小,反应能垒逐渐... 利用密度泛函理论,研究了双层石墨烯层间一氧化碳(CO)与氧(O)的氧化反应,获得了双层石墨烯层间距与反应能垒的定量关系.计算结果表明反应初态、过渡态、末态体系总能以及反应能垒对层间距离变化敏感:随着层间距的逐渐缩小,反应能垒逐渐增加.因此,改变双层石墨烯层间间距可以实现反应能垒的原子级调控.通过差分电荷密度分析体系的电子结构,发现当双层石墨烯层间距较小时,过渡态O—C=O中碳原子与石墨烯上下层中的碳原子之间有明显的电荷堆积,出现sp轨道杂化,导致二者相互作用增强,在z轴方向受到束缚力,难以与吸附在石墨烯表面的氧原子形成较弱的O—C键,阻碍了过渡态O—C=O的形成.通过调控双层石墨烯间距,可以降低一氧化碳氧化反应能垒.该研究可为石墨烯的应用以及新型碳基插层复合材料的制备提供一定的理论支撑. 展开更多
关键词 石墨烯 限域反应 密度泛函理论 反应能垒
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Robust MOF-253-derived N-doped carbon confinement of Pt single nanocrystal electrocatalysts for oxygen evolution reaction 被引量:1
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作者 Hellen Gabriela Rivera Monestel Ibrahim Saana Amiinu +3 位作者 Andrés Alvarado González Zonghua Pu BibiMaryam Mousavi Shichun Mu 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2020年第5期839-846,共8页
Although carbon-supported platinum(Pt/C) is still considered the most active electrocatalyst for hydrogen evolution reaction(HER) and oxygen reduction reaction(ORR), its applications in metal–air batteries as a catho... Although carbon-supported platinum(Pt/C) is still considered the most active electrocatalyst for hydrogen evolution reaction(HER) and oxygen reduction reaction(ORR), its applications in metal–air batteries as a cathode catalyst, or for oxygen generation via water splitting electrolysis as an anode catalyst is mainly constrained by the insufficient kinetic activity and stability in the oxygen evolution reaction(OER). Here, MOF-253-derived nitrogen-doped carbon(N/C)-confined Pt single nanocrystals(Pt@N/C) have been synthesized and shown to be efficient catalysts for the OER. Even with low Pt mass loading of 6.1 wt%(Pt@N/C-10), the catalyst exhibits greatly improved activity and long-time stability as an efficient OER catalyst. Such high catalytic performance is attributed to the core-shell structure relationship, in which the active N-doped-C shell not only provides a protective shield to avoid rapid Pt nanocrystal oxidation at high potentials and inhibits the Pt migration and agglomeration, but also improves the conductivity and charge transfer kinetics. 展开更多
关键词 PT MOF-253 Carbon confinement Oxygen evolution reaction ELECTROCATALYST
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Quantum-confined superfluid: From nature to artificial 被引量:12
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作者 Liping Wen Xiqi Zhang +1 位作者 Ye Tian Lei Jiang 《Science China Materials》 SCIE EI CSCD 2018年第8期1027-1032,共6页
Biological ion channels show that ultrafast ions and molecules transmission are in a quantum way of single molecular or ionic chain with a certain number of molecules or ions, and we define it as "quantum-confined su... Biological ion channels show that ultrafast ions and molecules transmission are in a quantum way of single molecular or ionic chain with a certain number of molecules or ions, and we define it as "quantum-confined superfluid" (QSF). This ordered ultrafast flow in the confined channel can be considered as "quantum tunneling fluid effect" with a "tunneling distance", which is corresponding to the period of QSF. Recent research demonstrated that artificial biomimetic nanochannels also showed the phenomenon of QSF, such as ion and water channels. The introduction of QSF concept in the fields of chemistry and biology may create significant impact. As for chemistry, the QSF effect provides new ideas for accurate synthesis in organic, inorganic, polymer, etc. We believe the implementation of the idea of QSF will promote the development of QSF biochemistry, biophysics, bioinformatics and biomedical science. 展开更多
关键词 quantum-confined superfluid quantum tunneling fluid effect ion channels artificial nauochannels
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